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2018 numbers and records every Indian cricket fan should know
Stats 78 // 31 Dec 2018, 18:39 IST SHARE 2018 is set to end in a few hours' time and the year witnessed a lot of fantastic moments in cricket. There were a lot of fine innings by the batsmen, fiery spell by the bowlers, great catches etc. on the field and off it, there were a lot of controversies in the year including the Sandpaper gate, Mithali Raj-Ramesh Powar saga etc.The Indian team had a good year as they played a good brand of cricket throughout and ended up winning a few tournaments. 2018 was always going to be tough for the Indian team as they were scheduled to tour South Africa, England and Australia in the year and Virat Kohli and his men, though lost the series in South Africa and England, gave a lot of good memories as they played a fearless brand of cricket throughout and challenged the opposition in their own backyard.After losing the Test series in South Africa and England, India ended the year on a high as they took an unassailable … [Read more...] about 2018 numbers and records every Indian cricket fan should know
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India vs Australia, 4th Test: Dream11 Prediction, Fantasy Cricket Tips & Playing XI Updates
Feature 5 // 31 Dec 2018, 17:30 IST SHARE India completed a historic victory win over Australia in the last Test of 2018 with a 137-run win at Melbourne. The action moves to Sydney after the start of the new year, with the Indian team having a chance of clinching a series win for the first time Down Under.Ahead of the fourth Test, former India cricketer and Sportskeeda's Fantasy Cricket Mantra expert Hemang Badani has suggested his fantasy cricket tips.You can watch the video here."The wicket at Sydney might be a little different from what we say at Melbourne. It might have some turn", states Badani, who believes that spinners will have a key role to play on the track.As was the case in the last article, Badani has suggested two teams for more choice. "If you have two sides, you have the option of picking 22 different players, wherein you might get more points. If you happen to pick one side, pick side No.1".Here are Badani's suggestions:Fantasy … [Read more...] about India vs Australia, 4th Test: Dream11 Prediction, Fantasy Cricket Tips & Playing XI Updates
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Sri Lanka cricket rated most corrupt by ICC: Minister
December 31, 2018 timesofindia Leave a Comment
COLOMBO: Sri Lanka has been rated as the most corrupt cricket nation by the world governing body, the country's sports minister said on Monday. The International Cricket Council feels "Sri Lanka's cricket administration is corrupt from top to bottom", Harin Fernando said, adding that he had been shown a confidential report on the matter at a Dubai meeting. A host of scandals have rocked Sri Lankan cricket in recent years including a match-fixing controversy revealed in a sting operation carried out for a TV documentary. The ICC anti-corruption unit has regularly investigated cases in the island nation. The crisis-ridden Sri Lanka Cricket (SLC) is to hold delayed elections in February, which were due last May when the term of president Thilanga Sumathipala ended. Sumathipala has been accused of violating ICC rules by holding office despite alleged links to gambling. He denies the charges. "Unfortunately Sri Lanka is being ranked as one of the worst or the top worst country … [Read more...] about Sri Lanka cricket rated most corrupt by ICC: Minister
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5 cricketers who disappointed in 2018
Top 5 / Top 10 111 // 31 Dec 2018, 17:00 IST SHARE The year 2018 has almost ended, but there was no dearth of quality action in the field of cricket. There were numerous record-breaking performances and heartwarming gestures in the roller-coaster game, that gave fans a lot of reasons to remember the year.2019 will be a notable year too, especially because of the World Cup that will be played. In the lead-up to the big tournament, most teams would want their players to be in top form.However, there were a few big names, who would have walked into 2018 with a reputation of having a great year, but ended up disappointing their teams and their fans in international cricket.Let us take a look at five such players:#5 Quinton de KockThe talented left-handed batsmen has been one of the top performers for the South African team in the last half a decade. Stylish and effective, Quinton de Kock has also been a vital component behind the stumps for the Proteas … [Read more...] about 5 cricketers who disappointed in 2018
Cricket Cricket, Top 5 / Top 10, MS Dhoni, KL Rahul, MS Dhoni Net worth, Indian Cricket Team, Indian Cricket Team Under Kohli
Smriti Mandhana wins ICC 'Women's Cricketer' and 'ODI Player of the year' awards
DUBAI: Talented India vice-captain Smriti Mandhana was Monday adjudged 'Women's Cricketer of the Year' as well as the 'Women's ODI Player of the Year' by the ICC. Left-handed opener Mandhana won the Rachael Heyhoe Flint Award for the 'Women's Cricketer of the Year' for scoring 669 runs in 12 ODIs along with 622 runs in 25 T20 Internationals in 2018. Her ODI runs were scored at an average of 66.90 while strike-rate for T20I was an impressive 130.67. Mandhana played a crucial role in India's semi-final appearance at the Women's World T20 in the West Indies, where she scored 178 runs in five matches at a strike-rate of 125.35. She is currently ranked fourth in the ODI rankings and 10th in the rankings for T20Is, the ICC said in a statement. Mandhana became only the second India woman player to win an ICC award after fast bowler Jhulan Goswami, who was named the ICC Player of the Year in 2007. Reacting to the news, a delighted Mandhana said: "...when you get acknowledged for your … [Read more...] about Smriti Mandhana wins ICC 'Women's Cricketer' and 'ODI Player of the year' awards
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The ATO has recently expressed concerns about the increase in claims by taxpayers for certain work related expenses, including clothing and laundry expenses, and has advised that it is an area where it will be "increasing attention, scrutiny and education".
It has also reminded taxpayers that to be eligible for a deduction, clothing needs to be occupation-specific, protective, or a uniform that is unique to the organisation for whom the taxpayer works.
It is not correct that taxpayers can claim a standard deduction of $150 without spending money on appropriate clothing or laundry. While record-keeping requirements for laundry expenses are "relaxed" for claims up to the $150 threshold, taxpayers do need to be able to show how they calculated their deduction.


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Universiṭah ha-ʻIvrit bi-Yerushalayim
Existence: 1925-
Architectural Records in the Hadassah Archives
Identifier: I-578/RG 21
The materials in the record group mostly consist of reproductions of building plans of the Hadassah hospitals on Mount Scopus and Ein Kerem from the 1920s to the 2000s. Other properties documented in the record group include buildings managed by Youth Aliyah, Hadassah Youth Services, Young Judaea, Hadassah Israel Education Services, the National Office, and the Hadassah Medical Organization. These records document a core Hadassah function, the building of medical and social service facilities in Palestine/Israel.
Found in: American Jewish Historical Society / Architectural Records in the Hadassah Archives
Arthur A. Goren Papers
Identifier: P-985
This is the collection of Arthur A. Goren, a historian and professor of American Jewish history at the Hebrew University and Columbia University. This collection consists of his research material and professional files from his academic pursuits and career as a professor, primarily at Columbia University. Included in the collection are copies of articles and photocopies of archival material used for research, drafts of speeches and manuscripts, handwritten and typed research notes, correspondence, clippings, photographs, and teaching and course material such as syllabi, readings, notes, and bibliographies.
Found in: American Jewish Historical Society / Arthur A. Goren Papers
Bondi Family Collection
Identifier: LBIJER 915
The collection contains various materials pertaining to the Bondi family, mostly concerning Aron (Alfred) Bondi and his scientific career.
Found in: Leo Baeck Institute / Bondi Family Collection
Executive Functions Records in the Hadassah Archives
This record group includes documents created and maintained by the Office of the President, the Office of the Executive Director and the Chair of the Division Coordinators/Directors Committee. Prominent is the Henrietta Szold series, containing correspondence by and to Szold as well as printed materials written by and about her. The files in this record group were created by a national president or executive director, or for their use, or maintained in their office during their years in office. Included are correspondence, minutes, memos, publications, reports and subject files on topics with which these individuals were involved.
Dates: 1875, 1877-2011, 2015; Majority of material found within 1910 - 2000
Found in: American Jewish Historical Society / Executive Functions Records in the Hadassah Archives
Hadassah Medical Organization Records in the Hadassah Archives
Identifier: I-578/RG 2
The Hadassah Medical Organization Records in the Hadassah Archives document Hadassah's work in providing health care resources in Palestine/Israel since 1918. The activities documented revolve around the development of the Hadassah Hospital; health centers; dental centers; occupational and rehabilitative services; medical, nursing, dental, and pharmacy schools; as well as numerous educative and preventive projects, especially those aimed at infant care. The documents also reflect the history of the Yishuv (Jewish settlement in Palestine) and the establishment of the State of Israel. The record group contains articles, clippings, correspondence, financial records, fundraising material, minutes, personal accounts, press releases, publicity material, reports, and statistical reports.
Found in: American Jewish Historical Society / Hadassah Medical Organization Records in the Hadassah Archives
More about 'Universiṭah ha-ʻIvrit bi-Yerushalayim'
Name Forms
Also known by the following names:
Evreĭskiĭ universitet v Ierusalime
Hebrew University (Jerusalem)
Université hébraïque de Jérusalem
Jerusalem. Hebrew University
Jāmiʻah al-ʻIbrīyah fī Ūrushalīm
Hebreyisher Uniṿersiṭeṭ in Yerusholayim
Hebräische Universität von Jerusalem
Universiṭah ha-ʻIvrit, Yerushalayim
Universiṭah ha-ʻIvrit (Jerusalem)
Universidad Hebrea de Jerusalén
Hebrew University, Jerusalem
Hebreeuwse Universiteit van Jeruzalem
Uniwersytet Hebrajski w Jerozolimie
Universiṭah ha-ʻIvrit be-Erets-Yiśra'el
Hebrejská univerzita v Jeruzalémĕ
Université hébraïque à Jérusalem
Università ebraica di Gerusalemme
אונברסיטה העברית בירושלים
אוניברסיטה העברית
אוניברסיטה העברית בירושלים
אוניברסיטה העברית בישרולים
האוניברסיטה העברית
האוניברסיטה העברית בירושלים
The Hebrew University of Jerusalem
The Hebrew University
Hebrew U
ha-Universiṭah ha-ʻIvrit bi-Yerushalayim
ha-Universita ha-Ivrit B'irushalayim
Universita ha-Ivrit B'irushalayim
الجامعة العبرية في القدس
al-Jāmiʻah al-ʻIbrīyah fī al-Quds
al-Ǧāmiʻah al-ʻIbriyyah fil-Quds
جامعة العبرية في القدس
Jāmiʻah al-ʻIbrīyah fī al-Quds
Ǧāmiʻah al-ʻIbriyyah fil-Quds
HUJI
Kudüs Ibrani Üniversitesi
Subject: Israel X
Subject: Jerusalem X
New York (N.Y.) 3
Scopus, Mount 3
Hospitals -- Administration 2
Jewish architects 2
Jewish women--United States--Societies and clubs 2
Jews -- Palestine 2
Medical centers -- Design and construction 2
Minutes (administrative records) 2
Nursing schools 2

redpajama_set_name: RedPajamaCommonCrawl


text:
package org.terasology.core.world;

import org.terasology.world.biomes.BiomeRegistry;
import org.terasology.world.biomes.BiomeRegistrator;

/**
 * Registers all core biomes with the engine.
 */
public class CoreBiomes implements BiomeRegistrator {

    @Override
    public void registerBiomes(BiomeRegistry registry) {
        for (CoreBiome coreBiome : CoreBiome.values()) {
            registry.registerBiome(coreBiome);
        }
    }

}

redpajama_set_name: RedPajamaGithub


When I first found the House of Prayer, in 2006, it was like I was reading the bible for the first time. I would read it, sing it, paint it, it was alive in me. One of the first passages I meditated on that really consumed my heart was 1 Corinthians 2:6-13. I still remember the tune of the music playing in the room as I paced and sang these verses.
Have you ever experience that? Reading a verse over an over, as if obsessed? Like you know there is another layer of revelation there that you are determined to get to? And the more you say it, or sing it, the more you become fascinated with God? The more you become fascinated, the priorities in your life shift.
It starts out by feeling dull inside, and digging deep just to crack the book open. Your like, "I'm gonna just read one Psalm, wherever I land" Then you read a verse, and your like, "oh thats good!" You read it again, and again, and from there is where the choice is made -- move on with my busy schedule or "seek the Lord while He may be found". Have you experienced this? I do very often. Sometimes I chose to move on to my busy schedule. I never get more done, however. But when I choose to get in the "zone" in the spirit, my day plays out different. The things I thought were really important before I went to bed the night before, suddenly aren't as urgent.
I went back to these verses, which I do often, but i chose the road of pressing in deeper for another layer of revelation. As I did, I became absolutely filled and engulfed with this message, that GOD. IS. EVERYTHING.
God is everything. He is all we need. And His spirit dwells in me. There is nothing that men possess or that the world offers that is out of reach. HE IS EVERYTHING. He is all I need, and through Him, ALL is my inheritance. ALL I need is from Him, not something I must acquire from an individual, an organization, or spiritual understanding in the heavenlies- ALL is mine.
ALL is everything- understanding, revelation, love, peace, joy, endurance, equipping for my calling- ALL. ALL.
Oh! To live daily in the spirit! To not be swayed to the left or the right!! To be anchored in my fascination with Jesus all throughout the day! HE. IS. EVERYTHING. My ALL in ALL.
God is my ALL in ALL. He is my EVERYTHING.
You are my Father, my provider, my protector, my shield, my covering, you are ALL.
He is the TRUTH in a world that is confused. He is the TRUTH in a world that is bombarded with false-truths, half-truths, false realities, and magnificent lies. He is the TRUTH amidst loud, self-reliant voices. He is the TRUTH in a world that is hopeless, broken, discouraged, and fearful.
His TRUTH supersedes my reality.
His TRUTH supersedes my failure. His TRUTH is above all, and is ALL. HE. IS. ALL.
The spirit that lives in God, lives is us who have received Christ. The same spirit, the spirit that is in the Father, is in me. How marvelous is this understanding? How marvelous is this truth? That God knows our humanity, our frail condition, that He chooses foolish things of the world, and puts His spirit in us. Oh I tell you I am in awe of God. I am in awe of His goodness and majesty towards us who believe.


Namib I is the official information centre in the Namibian coastal town, Swakopmund. We specialise in information for the whole of Namibia. We help you plan your trips, your one-stop reservations for transport, tours, activities and also accommodations.


Yay! You're booked for a photography session. Now what? Location, location, location.
First thing, if we haven't already, let's pick a spot (or two) to take your photos. While Austin is not short on beautiful and interesting venues, it's always fun to choose a location that has personal meaning to you. A special location, like Jessica and Colin's choice of Mozart's for coffee, gives extra meaning and depth to your photos. But if nothing comes to mind, don't fret. I'm happy to help you choose a location that suits the look and feel you want for your photo session, whether it's a grassy field or your own backyard. If you're in Austin, here are some solid options I love (the scenery varies by season, of course)!
First and foremost, it's important to feel like yourself, because that will absolutely come across in your photos. Secondly, you should choose wardrobe pieces that aren't going to compete for attention in the photo. We want the focus to be on you and not really what you're wearing. So the best idea is to stick with solid colors or classic, small prints. When planning a shoot with multiple people, whether it's your whole family or just one other person, it's a good idea to coordinate your colors and styles without falling into the dreaded "matchy-matchy" look. It's a good idea to choose a starting point with one person's outfit and work outwards from there. My final piece of wardrobe advice is to consider your environment. Jessica's casual dress and heels worked perfectly for the downtown park, as it had paved pathways that made sense for stilettos. Make sure your footwear matches the terrain, unless the intent is a purposeful juxtaposition of wardrobe and scenery.
The week leading up to your portrait session is an important one. Do your best to get a good amount of sleep and stay hydrated. Your skin will thank you for it!
Check out those fingers and toes. Treat yourself to a manicure/pedicure, and if you are planning to show off a sparkly new engagement ring, consider getting it cleaned before your session. These small details will make your overall look polished and camera-ready.
I hope this helps get you ready for your session! As always, I'm here to answer any questions or bounce ideas back and forth. Looking forward to seeing you in front of the camera!


you need to make a jig to cut the angle that those require. your chop saw can only cut 45 to 90degrees. that angle is very small like 10 to 20 degrees. i have some 4 into 1 collectors in mild steel in the garage. they will fit 1.5" primaries.
you need to mark the pipe so that both cuts one the one pipe is 90 degrees from each other. if you get this wrong they wont fit properly.
the degrees depends on you. the larger the degree the more the primaries will angle out. see what angle works for you.
LOL Hooch you have to give some posters time to get on here, especially that early in the morning.
New Project Plans Need Some Help Please!!!!


We are pleased to announce that multi-year memberships are now available for purchase.
Beginning in 2020, the Journal of Foraminiferal Research will be published quarterly online, with two issues combined into a single printing that will be mailed twice per year.
If you are an active or recent member, your Username is your email address and your default Password is the first 7 letters of your last name (add 9's to the end of your last name to get to 7 characters if your last name is shorter than 7 letters).
New members must register for an account to purchase a Membership and conduct other transactions. Future visits to the website will only require login.
Please click the "Join/Renew" button below and follow the onscreen prompts. The membership is for the natural year (January 1 to December 31).
Additionally, please take a moment to update your address and contact information if any changes are needed.
*This website accepts Visa, Mastercard and Discover. We also accept bank transfers and checks via mail drawn in USD.
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text:
Telugu star Nandamuri Balakrishna's talk show 'Unstoppable With NBK' will feature 'RRR' director S.S. Rajamouli and the movie's music director M.M. Keeravani.
With the most popular celebrities appearing to chat with 'Akhanda' hero Balakrishna has been showing his perkiest side on the show.
Rajamouli and Keeravani have joined the sets of 'Unstoppable With NBK'.
As the duo shared a great time interacting with Balakrishna on his show, the audience is quite excited to watch the interesting episode.
"The men behind the biggest Indian movie are on the biggest talk show. #UnstoppableWithNBK Episode 5 is going to be a treat with @ssrajamouli garu and @mmkeeravani garu having a great time with our #NandamuriBalakrishna garu. Promo out soon," the makers wrote.
Balakrishna, who had hosted Telugu's superstar Mahesh Babu in the previous episode of 'Unstoppable With NBK', has had other bigwigs like Brahmanandam, Mohan Babu, and Nani in the previous episodes.
Balakrishna seems to be buoyed with the success of his latest movie 'Akhanda'.
TAGS: music director M.M. Keeravani, director S.S. Rajamouli, Nandamuri Balakrishna
#NTR Biopic: Mahanayakudu Released Date Locked


Back to the NBA tonight, it's a big occasion with the draft on everyone's lips Jimmy Butler supposedly making his debut for the Sixers. They gave up a few players to get him, but on paper do look very strong now. It will, of course, take time for him to gel with his teammates. Sixers have a bad away record, but Orlando do at home as well.


text:
package com.hpe.application.automation.tools.results.service.almentities;

public class AlmTestSetFolderImpl extends AlmEntityImpl implements
		AlmTestSetFolder {
	private static String restPrefix = "test-set-folders";
	public String getRestPrefix() {
		return restPrefix;
	}
}


Ghost Owl is the 3rd book in my Avian Series, preceded by Yellow-Billed Magpie and Red-Tailed Hawk. Each book is a stand-alone story, but features many of the same characters. It's nice to read them in order if you like, but it's not necessary.
Now that I've retired from teaching, I feel very blessed to have the time and resources to pursue my writing as it's been a passion of mine for over 40 years.
I'm very proud of this particular story. I hope it will touch your heart.
I'll be selling all my books at the party (including my short story collection, Rover) for the low low price of $5 each. If you're not in the Sacramento area, my books are all available at Amazon, and on Kindle as well.
I'm planning to be there. I might bring a friend.


Dr. Boll will be serving as producer on this one with Marcel Walz directing. Caroline Williams, Christa Campbell, Nick Principe, Jared Demetri Luciano, Manoush, Natalie Scheetz, Annika Strauss, and Sarah Hayden star.
Plot details are currently under wraps, but we'd expect lots of hammering, slicing, dicing, screaming, and all around general mayhem. You gotta like that, right? That's just how these movies roll. More soon!


text:
With One Accord: Affirming Catholic Teaching Using Protestant Principles
"All these with one accord devoted themselves to prayer" (Acts 1:14). The apostles and early Christians believed and worshiped in unity—in doctrine and practice following Jesus' wish that "they may be one" (John...
Pope Peter: Defending the Church's Most Distinctive Doctrine in a Time of Crisis
The papacy is no stranger to controversy. In many ways it's Catholicism's defining doctrine—but also its most divisive. From medieval pontiffs who acted like princes to a modern pope whose every casual statement sets off a social-media...
Why Catholic Bibles Are Bigger - Revised 2nd Edition
Did the Catholic Church add extra books to the Bible? Or did Protestant leaders have them removed? Find out the truth! Some differences between Catholicism and Protestantism can be tricky to grasp, but one of them just requires the ability to count:...
The Protestant's Dilemma
What if Protestantism were true? What if the Reformers really were heroes, the Bible the sole rule of faith, and Christ's Church just an invisible collection of loosely united believers? As an Evangelical, Devin Rose used to believe all of it...
The Fathers Know Best: Your Essential Guide to the Teachings of the Early Church
What Did Early Christians Really Believe? The Answer Will Surprise and Amaze You!The Fathers Know Best: Your Essential Guide to the Teachings of the Early Church is a unique resource that introduces you to the teachings of the first Christians in a way...
Why We're Catholic: Our Reasons For Faith, Hope, And Love
How can you believe all this stuff? This is the number-one question Catholics get asked—and, sometimes, we ask ourselves. Why do we believe that God exists, that he became a man and came to save us, that what looks like a wafer of bread...
Radio Replies: Classic Answers to Timeless Questions About the Catholic Faith
A must-have for every Catholic's bookshelf! Father Leslie Rumble was the godfather of radio apologists and one of the Catholic media superstars of his day. During the 1920s and 30s his show helped millions of people understand and explain the...
The Essential Catholic Survival Guide: Answers to Tough Questions About the Faith
Being Catholic isn't easy. Every Catholic will come face-to-face with anti-Catholic attacks that are launched against the Faith. Don't you owe it to yourself to make sure you have the very best in apologetic resources right at your...


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Cephas HAYS
Illinois State Journal, Saturday, 5 December 1953, page 8 column 3:
Cephas Hays, Of Girard, Dies
Girard, Dec. 4--Cephas Hays, 73, retired farmer and resident of North Otter township his entire life, died at 5:10 p. m. Friday in St. John's Hospital, Springfield, where he had been a patient since Nov. 26.
Mr. Hays was born Jan. 31, 1880 the son of John W. and Lucinda England Hays. In 1910 he married the former Ruth Hageler.
Surviving are his wife; a daughter, Mrs. Geraldine McElhanon, Springfield; two sons, Donald, Sunol, Calif., and Clifford, Virden; a brother, R. O. Hays, Girard; a sister, Mrs. E. A. Coe, Girard and six grandchildren.
He was a member of the Union Chapel Methodist church and served as North Otter township clerk for nearly 50 years.
The body was removed to the Berry funeral home, Girard. Funeral arrangements are incomplete.
echoalpha.info > Genealogy > H200 > Cephas HAYS (1880-1953)
Last updated 28 August 2001.


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Al Shabab terrorists strike two Christian churches in Garissa, kill 17 at least and injure scores of others
AL SHABAB TERROR STRIKE KILLS AT LEAST 17 IN CATHOLIC AND AIC CHURCHES
The bloodiest strike yet on Kenya was this morning perpetrated in the Northern Kenyan town of Garissa, where almost simultaneously two Christian churches were attacked by what is generally thought to be Islamist terrorists from the Al Shabab group, now fighting for survival in Somalia as allied forces are advancing on their last strongholds of Kismayu.
Reports from Kenyan contacts in Mombasa and Nairobi speak of at least 17 worshippers dead and scores of others seriously injured in the blasts and shootings, amongst them children.
The attack on Christian Sunday services was immediately seen as a declaration of war not just on Kenya as a nation but on Christianity too, adding a new dimension to the often cruel terror acts of Al Shabab, which has seen women being stoned to death for being raped, youths beheaded for refusing to be pressed into the service of terror and whatever businesses remain in areas under their shrinking control extorted for money to buy and pay for supplies.
A fleet of aircraft including medivac and intensive care equipped aircraft have been dispatched from Nairobis Wilson Airport when the extend of the terror strike became fully known and are expected to be landing at the Garissa airfield before 4 p.m. local time, then expected back in the capital before last light with the worst cases to receive the best possible medical care.
Regular sources in Kenya attributed the attack on the two churches to the ongoing high level of security in Nairobi, Mombasa and other key Kenyan towns, leaving the terrorists to seek out opportunistic targets like church services, which are not as tightly guarded until now, though two policemen deployed at the scenes were reportedly also killed by the attackers. In the big cities they can only hope to throw a grenade or something like that because security is now very very tight, especially for hotels, restaurants, public places even. So they have now looked for other locations nearer to the Somali border that they can sneak across at night and then hit and run back. It is sad that they claim to be Muslims because they are the devils breed for sure. No God fearing Muslim will condone such acts or commit such acts on other religions services and Christians are as far as we are concerned, as far as the Holy Quran is concerned, people of the book. There is no justification at all in what these murderers did said a regular source from Mombasa to me on the phone just now, who happens to be a practicing Muslim, though in our personal and professional relationship that is of no consequence or importance at all as we both see the value of the individual not in any way influenced by religion, ethnicity or cultural background.
Other sources expressed shock as apparently the news was slow in spreading across Kenya on a Sunday, but from other sources close to the state machinery it was learned that new add measures will now be put into place to also protect places of worship in the same way as other public gatherings are subject to security checks. Already high security in Nairobi and Mombasa was reportedly also stepped up further with yet more intense checks on cars and individuals while some hotels too have added an extra layer of security screening before vehicles can enter into the resort or hotel compounds or individuals are admitted into the premises.
Sincere and heartfelt condolences are expressed to the families and friends of those who lost loved ones in this mornings twin terror strikes.
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The stylized movement vocabulary known as house dance entails both rhythmic and lyrical elements that speak to the soul of the music and the dancer. Starting in New York City, and extending itself to underground dancers around the world, house has allowed very different people of all ages, races, and backgrounds to speak a common dance language, explore its variations, and work through what might be the widest range of movement, from rich and sensual floor movement to quick and slight body changes and footwork patterns and vocabulary. Though understanding the vocabulary, exploring the music, working through the tools of choreography, freestyle, and other exercises, one automatically is able to explore and express their feelings about the music, but dynamically understood as they are automatically sharing with the class and community.


As a constituent college of DU, Miranda House was linked to the National Knowledge Network with the DU Computer Centre planning and introducing state-of-art hardware, software and networking solutions. It laid a university wide fibre optic network that acts as the hub for ICT related activities at DU. Large number of computers in the college are on Miranda House LAN.
National Knowledge Network (NKN) is available on DU Intranet and accessed via the college Wi-Fi. The usage includes video conferencing and access to virtual classrooms. Faculty members use features like video lectures, and learning management system courses. Students and faculty have actively participated in all NKN events at DU that include direct address by Honourable President of India on several occasions.


If you have a back yard, getting outside to enjoy beautiful weather is likely a favorite past time. Whether you have a large yard or a small yard with limited space, you can create an inviting atmosphere with simple backyard projects.
As a parent, you know that getting your kids outside to play is important. Physical exercise builds strong bones and releases pent-up energy that creates anxiety and sleeping problems. Select a sunny spot in the yard away from trees and shrubs that you can easily see from the house. Consider a few pieces of equipment that your kids will enjoy like a swing set, a see-saw, a jungle gym or a trampoline. If you have the space, you can also include a place for lawn games like horseshoes, lawn bowling, shuffleboard or bat mitten. If your kids are toddler age, a simple sandbox filled with toys, pails and shovels will create a fun outdoor play area.
A cozy backyard fire pit will provide a warm gathering spot on cool evenings. It will create a comfortable place to relax with a glass of wine, enjoy conversations with family and friends, and roast marshmallows with the kids. Fire pits are affordable and easy to build. You can find DIY kits for in-ground and above-ground fire pits at most local home improvement stores or online. There are also more decorative, prefabricated fire pits that come in a variety of shapes, sizes and materials that can be placed in the back yard or on the patio or deck. These smaller, more decorative models are great for back yards with limited space.
An outdoor pavilion will create a comfortable backyard area for relaxation and entertaining. Since a pavilion typically has a closed roof and open walls, it provides a certain amount of shelter from hot sun and rain. To create more privacy and weather protection, you can install outdoor draperies or panels that can be closed when needed. A pavilion is simple and affordable to build and install in most backyard areas with some flat terrain. You can build it in a size that fits comfortably in your yard and suits your needs for outdoor activities. You can choose from building materials including wood, vinyl, fiberglass, and composites that fit comfortably within your budget.


Domain Name Forum - hosting with disaster recovery?
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You can check that which hosting servers provide disaster recovery solutions also. And you can take disaster recovery hosting services separately they will help you to protect your data from all type of problems.


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Rep. DeFazio Awarded NUCA's Top Industry Honor
by NUCA Staff
House Infrastructure Committee Chairman Wins Industry "We Dig America" Award
Chairman DeFazio was presented the award at the grand exterior steps of the U.S. House of Representatives on Nov. 3 in Washington, D.C.
In recognition of his tireless service to America's communities through his work as the chairman of the House Transportation and Infrastructure Committee, the National Utility Contractors Association (NUCA) on Nov. 3 awarded Rep. Peter DeFazio of Oregon its "We Dig America" award.
"NUCA is honored to give Chairman DeFazio our top industry award this year," said NUCA CEO Doug Carlson. "Without the chairman's support of key pieces of legislation at the right time, and his strong advocacy of these bills in the face of adversity, this legislation would not have made it out of Congress. We would be looking at an America still mired in broken water mains, unsafe drinking water, and unfulfilled promises. Chairman DeFazio's infrastructure bill will deliver lasting improvements in the lives of every American over the next several years."
Chairman DeFazio was presented the award at the grand exterior steps of the U.S. House of Representatives in Washington, D.C. It is the first time the association has awarded a lawmaker this top industry award at the U.S. Capitol Building.
Chairman DeFazio has been instrumental over the last year in supporting our industry and the work that our 570,000 employees perform each day to repair water main breaks, install new water and wastewater lines, and build complex facilities such as pumping stations and water treatment facilities. Our industry is thankful for Chairman DeFazio's work over the past year. The effect of his sponsorship of several pieces of legislation over the past sessions of Congress that will build and improve this nation's infrastructure, and his personal support of these initiatives, cannot be understated.
This award is presented to a non-NUCA member who has made a significant contribution to NUCA and the underground utility construction and excavation industry. The achievement must have national impact and the recipient must have national stature, both of which perfectly fit Chairman DeFazio.
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US7807265B2 - Partially passivated quantum dots, process for making, and sensors therefrom - Google Patents
Partially passivated quantum dots, process for making, and sensors therefrom Download PDF
nanocrystal
analyte
Swadeshmukul Santra
Subir Kumar Sabui
Paul H. Holloway
Heesun Yang
University of Florida Research Foundation Inc
University of Central Florida Research Foundation Inc (UCFRF)
2007-05-14 Application filed by University of Central Florida Research Foundation Inc (UCFRF) filed Critical University of Central Florida Research Foundation Inc (UCFRF)
2010-02-08 Assigned to UNIVERSITY OF FLORIDA RESEARCH FOUNDATION, INC. reassignment UNIVERSITY OF FLORIDA RESEARCH FOUNDATION, INC. ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: SABUI, SUBIR K., SANTRA, SWADESHMUKUL
2010-02-08 Assigned to UNIVERSITY OF FLORIDA RESEARCH FOUNDATION, INC. reassignment UNIVERSITY OF FLORIDA RESEARCH FOUNDATION, INC. ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: HOLLOWAY, PAUL H., YANG, HEESUN
G01—MEASURING; TESTING
G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
G01N33/00—Investigating or analysing materials by specific methods not covered by groups G01N1/00 - G01N31/00
G01N33/48—Biological material, e.g. blood, urine; Haemocytometers
G01N33/50—Chemical analysis of biological material, e.g. blood, urine; Testing involving biospecific ligand binding methods; Immunological testing
G01N33/58—Chemical analysis of biological material, e.g. blood, urine; Testing involving biospecific ligand binding methods; Immunological testing involving labelled substances
G01N33/588—Chemical analysis of biological material, e.g. blood, urine; Testing involving biospecific ligand binding methods; Immunological testing involving labelled substances with semiconductor nanocrystal label, e.g. quantum dots
B—PERFORMING OPERATIONS; TRANSPORTING
B82—NANOTECHNOLOGY
B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
B82Y15/00—Nanotechnology for interacting, sensing or actuating, e.g. quantum dots as markers in protein assays or molecular motors
G01N21/00—Investigating or analysing materials by the use of optical means, i.e. using infra-red, visible or ultra-violet light
G01N21/62—Systems in which the material investigated is excited whereby it emits light or causes a change in wavelength of the incident light
G01N21/63—Systems in which the material investigated is excited whereby it emits light or causes a change in wavelength of the incident light optically excited
G01N21/64—Fluorescence; Phosphorescence
G01N21/645—Specially adapted constructive features of fluorimeters
G01N21/648—Specially adapted constructive features of fluorimeters using evanescent coupling or surface plasmon coupling for the excitation of fluorescence
G01N21/6489—Photoluminescence of semiconductors
G01N21/75—Systems in which material is subjected to a chemical reaction, the progress or the result of the reaction being investigated
G01N21/77—Systems in which material is subjected to a chemical reaction, the progress or the result of the reaction being investigated by observing the effect on a chemical indicator
G01N21/7703—Systems in which material is subjected to a chemical reaction, the progress or the result of the reaction being investigated by observing the effect on a chemical indicator using reagent-clad optical fibres or optical waveguides
G01N2021/7769—Measurement method of reaction-produced change in sensor
G01N2021/7786—Fluorescence
Y10S977/00—Nanotechnology
Y10S977/70—Nanostructure
Y10S977/773—Nanoparticle, i.e. structure having three dimensions of 100 nm or less
Y10S977/813—Of specified inorganic semiconductor composition, e.g. periodic table group IV-VI compositions
Y10S977/824—Group II-VI nonoxide compounds, e.g. CdxMnyTe
Y10S977/832—Nanostructure having specified property, e.g. lattice-constant, thermal expansion coefficient
Y10S977/834—Optical properties of nanomaterial, e.g. specified transparency, opacity, or index of refraction
Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
Y10T428/00—Stock material or miscellaneous articles
Y10T428/29—Coated or structually defined flake, particle, cell, strand, strand portion, rod, filament, macroscopic fiber or mass thereof
Y10T428/2982—Particulate matter [e.g., sphere, flake, etc.]
Y10T428/2991—Coated
Y10T428/2998—Coated including synthetic resin or polymer
A partially passivating core shell particle includes a luminescent nanocrystal core, and a partially passivating semiconducting core shell on a surface of the nanocrystal. The shell allows selected analytes to alter a luminescent response of the core shell particle. A quantum dot-based sensing system includes at least one partially passivating core shell particle, a light source for irradiating the partially passivating core shell particle, and a light detector for receiving emissions from the particle, wherein emissions from the core shell particle change in response to the presence of at least one analyte.
The present application incorporates by reference and claims priority to U.S. Provisional Patent Application Ser. No. 60/799,948, entitled "PARTIALLY PASSIVATED QUANTUM DOTS, PROCESS FOR MAKING, AND SENSORS THEREFROM" filed May 12, 2006, and U.S. Provisional Patent Application Ser. No. 60/842,434, entitled "PARTIALLY PASSIVATED QUANTUM DOTS, PROCESS FOR MAKING, AND SENSORS THEREFROM" filed Sep. 6, 2006.
The invention is related to core/shell quantum dots, as well as sensors and methods of sensing analytes utilizing the same.
A quantum dot (Qdot) is a semiconductor crystal whose size is on the order of just a few nanometers. Qdots contain anywhere from 100 to 1,000 essentially free electrons and range from about 2 to 10 nanometers in size, or about 10 to 50 atoms, in diameter.
One of the optical features of excitonic Qdots noticeable to the unaided eye is coloration. While the material which makes up a quantum dot is significant, more significant in terms of coloration is the size. The larger the Qdot, the redder (the more towards the longer wavelength end of the electromagnetic spectrum) they fluorescence. The smaller the dot, the bluer (the more towards the short wavelength end) it is. The coloration is directly related to the energy levels of the Qdot. Quantitatively speaking, the bandgap energy that determines the energy (and hence color) of the fluoresced light is approximately inversely proportional to the square of the size of the Qdot. Larger Qdots have more energy levels which are more closely spaced. This allows the Qdot to absorb photons containing less energy, i.e. those closer to the red end of the spectrum.
Regarding fabrication, in semiconductors, Qdots are small regions of one material buried in another with a larger energy (band) gap. Qdots sometimes may occur spontaneously in quantum well structures due to monolayer fluctuations in the well's thickness. Self-assembled quantum dots nucleate spontaneously under certain conditions during molecular beam epitaxy (MBE) and metallorganic vapor phase epitaxy (MOVPE), when a material is grown on a substrate to which it is not lattice matched.
Being quasi-zero dimensional, quantum dots have a sharper density of states than higher-dimensional structures. As a result, they generally have superior transport and optical properties, and are currently being researched for use in diode lasers, amplifiers, and certain biological sensors.
More than a decade-long studies on colloidal luminescent Qdots have revealed that effective surface passivation is critical in making Qdots extremely bright and photostable. Continuous passivation coatings of sufficient thickness thus provide a reduction in the sensitivity of Qdots to various environmental conditions. As a result, Qdots are often passivated with a continuous coating to form core/shell structure comprising an encapulating shell having the Qdot core within.
A partially passivating core shell particle comprises a luminescent nanocrystal core, and a partially passivating semiconducting core shell on a surface of the nanocrystal. The shell is operable to allow selected analytes to alter a luminescent response of the core shell particle.
In one embodiment, the nanocrystal comprises a metal chalcogenide and the shell comprises a compositionally different metal chalcogenide. In this embodiment, the nanocrystal can comprise CdS and the core shell can comprise ZnS or ZnSe.
The nanocrystal can include a transition or lanthanide metal dopant. In one embodiment, the partially passivating core shell provides a band gap of at least 4 eV at 25 C. The composition can further comprise an analyte selective shell covalently attached to the core shell, such as a Macro-Cyclic Crown Ligand (MCCL).
A quantum dot-based sensing system comprises at least one partially passivating core shell particle including a luminescent nanocrystal core, and a partially passivating semiconducting core shell on a surface of the nanocrystal. The shell allows selected analytes to alter a luminescent response of the core shell particle. A light source is provided for irradiating the partially passivating core shell particle. A light detector receives emissions from the partially passivating core shell, wherein the emissions change in response to the presence of at least one analyte. The system can further comprise at least one optical fiber including a transmitting leg and a receiving leg, and a core portion located between the transmitting leg and the receiving leg covered with at least one of the partially passivated core shell particles. In one embodiment, an analyte selective shell is covalently attached to the partially passivating core shell, such as a MCCL.
The nanocrystal can comprise a metal chalcogenide and the partially passivating core shell can comprise a metal chalcogenide. In one embodiment, the nanocrystal comprises CdS and the partially passivating core shell comprises ZnS or ZnSe.
A method of sensing analytes comprising the steps of providing at least one partially passivating core shell particle comprising a luminescent nanocrystal core and a partially passivating semiconducting coating shell on a surface the nanocrystal, wherein the shell allows selected analytes to alter a luminescent response of the core shell particle. A fluid suspected of including at least one analyte is exposed to the partially passivating core shell particle. Based on a change in luminescent response of the core shell particle following exposure to the fluid it is determined whether the analyte is present in the fluid. The fluid can comprise water. The analyte can be a heavy metal cation, such as Hg, Cd or Pb.
A fuller understanding of the present invention and the features and benefits thereof will be obtained upon review of the following detailed description together with the accompanying drawings, in which:
FIG. 1 is a schematic representation of a partially passivated quantum dot (partially passivated Qdot) according to an embodiment of the invention.
FIG. 2( a) is a schematic representation of an exemplary Qdot-based Heavy Metal Detection Probe (QHMDP) according to the present invention. The QHMDP has a core-shell structure. The shell comprises Macro-Cyclic Crown based Ligands (shown as "Ln") capable of binding to specific heavy metal ions and a large energy gap material (e.g. ZnS) partially passivating a Qdot core. The MCCLs at least partially encapsulate the partially passivateds core. FIG. 2( b)-(d) show some exemplary MCCLs, shown as Ln1, Ln2 and Ln3, respectively.
FIGS. 3( a) and (b) show simplified representations of an intrisic and an extrinsic fiber optic based sensor system, respectively, according to an embodiments of the present invention.
FIG. 4 shows a flow chart for the synthesis of CdS:Mn/ZnS core/shell Qdots using a water-and-oil (W/O) microemulsion according to the invention.
FIG. 5 is a Table showing the experimental protocol used having a constant microemulsion composition to demonstrate a scale-down effect where the microemulsion volume becomes an important process control parameter.
FIG. 6 shows emission spectra for the various Qdot samples showing very significant spectral changes based solely on the microemulsion volume used in the microemulsion system (the scale-down effect).
FIG. 7 provides data including XPS data for the various samples described above evidencing a variation in Zn+2/Cd+2 ratio between the sample groups.
FIG. 8 shows the effect of metal ion concentration on the luminescence intensity for the metal ions Cd+2, Hg+2 and Pb+2, as a function of concentration of the metal ion.
The present invention is more particularly described in the following description and examples that are intended to be illustrative only since numerous modifications and variations therein will be apparent to those skilled in the art. As used in the specification and in the claims, the singular form "a," "an," and "the" may include plural referents unless the context clearly dictates otherwise. Also, as used in the specification and in the claims, the term "comprising" may include the embodiments "consisting of" and "consisting essentially of". In addition, unless indicated otherwise, a description of a layer being disposed on another layer, includes both embodiments where the layer is directly on the other layer or the layer has one or more intermediate layers interposed between the layer and the other layer.
As noted in the Background, it is well known to provide surface passivation layers for Qdots to achieve maximum brightness. Besides providing maximum brightness, such conventional passivation coatings are designed to also provide a reduction in the sensitivity of Qdots to various environmental conditions. Significantly, however, the Inventors have unexpectedly found that a partially passivating semiconductor coating layer disposed on the luminescent nanocrystal dot core which provides a significantly lower brightness compared to a fully passivated layer, provides useful sensing properties that can be used for a variety of chemical/biological sensing applications.
A partially passivating core shell particle according to the present invention comprises one or more partially passivated quantum dots. FIG. 1 shows an exemplary partially passivated quantum dot 100 according to an embodiment of the present invention. The nanocrystal core 105 has an average size less than 100 nm, generally being about 1 to 10 nm in size. A partially passivating semiconductor coating layer 110 is disposed on the surface of the luminescent nanocrystal core. As used herein, "partially passivated layer" or "partially passivating layer" is defined by reference to its luminescence intensity measured at the emission band (e.g. 590 nm for Mn doped CdS) as compared to the luminescence intensity of both a fully (optimal) passivated Qdot control and an unpassivated control. Specifically, partially passivated Qdots according to the present invention as defined herein to provide a luminescence intensity range as follows:
i) a maximum intensity level that is at least 30% less than the luminescence of a fully (optimal) passivated Qdot control, and
ii) a lower intensity level that is the greater of 85% less that the luminescence of the same fully passivated Qdot control and 30% more than the luminescence intensity of an unpassivated control.
The thickness of the semiconductor coating 110 is generally one to two atomic layers, but can be somewhat thicker, such as three to five atomic layers. The coating is preferably a wide band gap semiconductor, selected to have a larger band gap, such as 0.5 to 1 eV higher, as compared to the band gap provided by the core nanoparticle 105. The partially passivated surface coating according to the present invention exposes at least a portion of the exterior of the luminescent nanocrystalline material to external influences. Although shown in FIG. 1 as being a continuous coating, the surface coating can be discontinuous as well. The semiconductor coating 110 can be a luminescent or non-luminescent coating.
Although not required to practice the present invention, Applicants, not seeking to be bound by theory, believe that by using luminescent core nanoparticles having a significant portion of their surface area exposed to external influences allows certain materials to change the electron-hole recombination process behavior, which results in a change in the photoluminescence (PL) response. Through interaction of the luminescent nanocrystalline material with certain outside influences, and a resulting change in photoluminescence (PL) intensity or PL lifetime, certain outside influences can thus be sensed and identified based on unique PL signatures for a variety of analytes.
Although generally described using a CdS core and a ZnS coating, the invention is in no way limited to any particle luminescent nanocrystalline material or coating. Although the passivating coating is generally an inorganic layer, organic layers may also be used. In some embodiments, the luminescent nanocrystals can be doped with a transition or lanthanide metal.
In one specific embodiment, the luminescent nanocrystalline material is a doped metal chalcogenide, such as Mn doped CdS. CdS:Mn nanocrystals have been found to show efficient and broad photoluminescence (PL) around 2.1 eV. Similar PL is observed in bulk CdS:Mn. This is attributed to the intra-3d transition of Mn2+ ions. Moreover, the PL excitation spectrum of CdS:Mn nanocrystals has been found to be similar to the absorption spectrum of CdS nanocrystals. These observations suggest that efficient energy transfer of carriers occurs from CdS nanocrystals to Mn2+ ions.
As a result of partial surface passivation according to the present invention, compositions according to the invention behave as if the emission is internally quenched. This arrangement and the discovery of an efficient method to form partially passivating semiconductor coating layers disposed on the luminescent nanocrystals (described below) allows the formation of new Qdot-based analyte sensors. Such sensors have been found to provide high levels of sensitivity toward pH, various metal ions (including bivalent Cd, Pb, Hg cations) and certain organic molecules, and are expected to provide selectivity for organics including nitroaromatic explosives, such as TNT. It is expected that environmentally-sensitive Qdots will also have potential for the biosensing. For example, alteration in the Qdot PL signature is expected once reactive oxygen species (such as associated with superoxide, nitric oxide and peroxide) will interfere with the electron-hole recombination processes at the surface of the luminescent nanoparticle. Accordingly, portable heavy metal detection devices for Hg, Pb, As, Cd ions (samples including contaminated water) can make use of fluorescence signatures upon exposure to heavy metals.
Regarding heavy metal detection using partially passivated Qdots according to the invention, results obtained described below indicated significant sensitivity. Moreover, such Qdots were found to be extremely photostable in solution as was confirmed by the continuous exposure to 450 W Xenon excitation for several hours. However, in certain applications where multiple analytes may be present, such Qdots may not have sufficient selectivity. For instance, when exposed to both Hg2+ and Pb2+, luminescence quenching of the 584 nm Mn2+ 4T1-6A1 band was observed in each case. Moreover, an unknown contaminated soil or water sample may contain various cationic and anionic species, other than toxic heavy metal ions. In this situation, it would be challenging to selectively detect any specific heavy metal.
To improve selectivity of partially passivated Qdots according to the invention, a new core-shell-shell QHMDP design was developed by the present Inventors. Although described below as being a shell to improve heavy metal selectivity, selectivity enhancing shells can be used to improve selectivity for a variety of non-heavy metal analytes The core here is defined to be a partially passivated core/shell Qdot according to the present invention and is designed to achieve high optical sensitivity (e.g. luminescence quenching of Mn doped CdS 584 nm emission for both Hg2+ and Pb2+ ions). In one embodiment, The Qdot shell will be synthesized by covalently attaching the core to heavy metal selective ligands, such as Macro-Cyclic Crown Ligands (MCCLs), to provide a Qdot based Heavy Metal Detection Probe (QHMDP) 200 according to the present invention, as shown in FIG. 2( a). QHMDP 200 is shown having a Mn doped CdS core 205, a partially passivating ZnS coating 210, and a plurality of selective ligands 215 (shown as Ln) bound to the ZnS coating 210. In one embodiment the selective ligands 215 are MCCL which are designed to capture specific heavy metals from a mixture heavy metal ions. It is noted that the MCCL or other selective ligands 215 is preferably directly attached to the Qdot surface without a spacer. The purpose for direct attachment is to obtain essentially zero-space surface passivation that will create a non-flexible MCCL coating. In the case of a MCCL coating, such a robust coating should prevent undesired metal ions diffusion to the core. The shell design shown reduces interference due to non-specific binding of undesired metal ions. In a practical situation, however, there will always be a chance of non-specific interaction once the probe is allowed to interact with the sample for a longer period of time. Therefore, when implementing a detection method using QHMDPs according to the present invention, a brief exposure (e.g. <1 minute) of QHMDP to the sample and rapid detection procedure will generally be desirable.
FIGS. 2( b)-(d) show exemplary MCCL coatings for the selective detection of Pb+2, Hg+2, and Cd+2. Although generally covalently attached, it is possible to attach MCCLs to Qdots according to the present invention by certain non-covalent means. Ln1 shown in FIG. 2( b) is not a fully closed ring. As shown in FIG. 2( b)-(d), the MCCLs (e.g. Ln1, Ln2 and Ln3) are shown surrounding their respective selective analytes, Pb+2, Hg+2, and Cd+2, respectively.
MCCLs have been widely used in separation chemistry and treatment of heavy metal poisoning. During the past two decades, several synthetic strategies have been developed to make metal selective MCCLs. Crown ether based chemosensors for the specific detection of Hg (shown in FIG. 2( c)) are disclosed in Yoon, S., et al., Screening mercury levels in fish with a selective fluorescent chemosensor. Journal of the American Chemical Society, 2005. 127(46): p. 16030-16031; hereafter "Yoon et al."]. Crown ether based chemosensors for the specific detection of Pb (shown in FIG. 2( b)) are disclosed in He, Q. W., et al., A selective fluorescent sensor for detecting lead in living cells. Journal of the American Chemical Society, 2006. 128(29): p. 9316-9317; hereafter "He et al."] at trace amounts in living species (e.g. mercury ion detection in fish, intra-cellular lead ion detection in HEK cells). In the chemosensor design disclosed in Yoon et al., a fluorescent reporter molecule (e.g. fluorescein) was covalently attached to a heavy metal specific MCCL ligand. The fluorescein emission was internally quenched in this construct. Upon binding to heavy metal ions, the fluorescein emission was restored. The increase in the emission intensity was directly proportional to the toxic heavy metal ion concentration. The restoration of fluorescein emission clearly indicated that the binding of heavy metals has a direct influence on the electronic states of the fluorescent reporter molecule, drastically reducing non-radiative pathways.
The present invention replaces fluorescein reporter molecules with highly-sensitive, photostable and environmentally sensitive Qdot probes according to the invention. For example, for the detection of Cd2+, Ln3 (FIG. 2( d) can be used. Ln3 shown in FIG. 2( d) is disclosed in Bronson et al. [Bronson, R. T., et al., Efficient immobilization of a cadmium chemosensor in a thin film: Generation of a cadmium sensor prototype. Organic Letters, 2005. 7(6): p. 1105-1108].
The present invention can be used in a variety of sensor systems. Sensor systems generally comprise a light source for irradiating the partially passivated Qdots. A light detector is provided for receiving emissions (typically fluorescence) from the nanocrystals, wherein the emissions change (intensity, wavelength, decay time) in response to the presence of at least one analyte. A detector for measuring electrical conductivity of the nanocrystals can also be included. The analyte can be in liquid or vapor form. The nanocrystals can be secured to a surface or held in solution. For example, the nanoparticles can be arranged on a packed bead bed or in a particle dispersion on a substrate. In another embodiment, selective shell covered partially passivated Qdots according to the invention are dip coated inside the core of a fiberoptic fiber.
FIG. 3( a) shows an intrinsic fiber-optic based hand-held sensor probe 300 according to an embodiment of the present invention. The fiber includes a transmitting leg 305 and a receiving leg 310. Between the transmitting leg 305 and a receiving leg 310 is a core portion 312 having at least one, and generally a plurality of selective shell covered partially passivated Qdots according to the invention coated inside to provide analyte specificity. An inlet region 316 to core region 312 is provided for introducing samples suspected of including one or more targets. A light source (e.g. laser) 315 and lens 320 are provided for coupling light into the transmitting leg 305 of the fiber. A detector 325 is coupled to the output of receiving leg 310. Although not shown, a supervisory computer and processor is preferably included for characterizing the luminescence intensity and/or luminescent lifetime and determining whether a specific analyte is present. By providing multiple fibers all having different selective shells between light source/lens and detector, probes according to the present invention can be used to simultaneously sense a plurality of different analytes.
FIG. 3( b) shows an extrinsic fiber-optic based hand-held sensor probe 350 according to an embodiment of the present invention. The fiber includes a transmitting leg 355 and a receiving leg 360. Probe 350 includes positions for insertion of plates having selective shell covered partially passivated Qdots according to the invention coated thereon. As with FIG. 3( a), although not shown, a supervisory computer and processor is preferably included for generating a luminescence spectrum from data provided and determining whether a specific analyte is present. Probes according to the invention are expected to rapidly and selectively detect toxic heavy metal ions at trace levels, such as in the range between parts per billion (ppb) or parts per trillion (ppt).
Besides detecting highly toxic heavy metal ions (Cd2+, Hg2+, Pb2+ and As3+ ions), biological reactive species (nitric oxide, super oxide and peroxides), or explosives (e.g. explosive nitro-aromatics) as noted above, nanosensors according to the present invention can also be useful for detection of sodium, potassium, magnesium ions, as well as amino acids and other materials.
Reactive oxygen species (ROS), such as superoxide, nitric oxide, and peroxides are of particular interest as they are responsible for oxidative stress and ageing. Superoxides are known to cause oxidative stress and are directly linked to many neurodegerative diseases such as Alzheimer's, Parkinson's, and Huntington's diseases. Nitric oxide (NO) is an important bioregulatory agent in a range of physiological processes from vasodilation and platelet aggregation to neurotransmission and penile erection. In biology, hydrogen peroxide is considered as a reactive oxygen species that could lead to serious tissue damage. Sensitive detection of these ROS is highly desirable for early diagnosis and monitoring disease progression. Superoxide radicals will be generated in solution by the reaction between xanthine oxidase and hypoxanthine, followed by the treatment with Qdots. Sodium (Z)-1-(N,N-diethylamino)diazen-1-ium-1,2-diolate will be used to generate nitric oxide in solution and will then be treated with Qdots. ROS will generally interfere with the electron-hole recombination processes allowing the effect of ROS to be assessed by monitoring PL characteristics (PL emission, PLE and lifetime measurements) of Qdots according to the present invention.
Detection of explosive nitro-aromatics is important for Homeland Security reasons as these materials fall under the category of cheap and dirty explosives. Electron-deficient explosive nitro-aromatics could behave as surface traps for the electron hole recombination process. It is expected that sensitive responses will be provided by partially passivated Qdots according to the invention. Exemplary explosive nitro-aromatics include 2,4,6 trinitrotoluene (TNT), peroxides and picric acid.
A new room temperature operable synthesis protocol allows synthesis of doped semiconductor nanocrystals, such as CdS:Mn nanocrystals, having variety of surface passivation layers, such as a ZnS layer. Through controlling the process as described below, the surface passivation layer can be continuous or sufficiently thin or discontinuous to be partially passivating. Regarding the new process, as demonstrated in the Examples below, solution volume has unexpectedly been found to be a process parameter which enables formation of a partially passivating passivation layer.
Generally, the method comprises the steps of providing a metal ion comprising water-in-oil micellular solution, the metal ion comprising at least a first and a second metal, providing a chalcogenide ion comprising water-in-oil micellular solution, and mixing the metal ion comprising water-in-oil micellular solution and the chalcogenide ion comprising water-in-oil micellular solution, wherein a stoichiometric surplus of the chalcogenide is provided. A plurality of first or second metal chalcogenide nanoparticles are formed. A third metal comprising water-in-oil micellular solution is then sequentially or simultaneously added, wherein a coating comprising the third metal and chalcogenide forms on the plurality of first or second metal chalcogenide nanoparticles. By using a total volume of reactants sufficiently low, generally less than 400 ml, a partially passivating coating layers is formed on the nanoparticles. Nanoparticles formed by the present method also generally include a plurality of surfactant molecules on their outer surface.
FIG. 4 shows a flow chart for one method suitable for the synthesis of CdS:Mn/ZnS core/shell Qdots using a water-and-oil (W/O) microemulsion according to the invention. In this embodiment, the oil is heptane and the surfactant is sodium dioctyl sulfosuccinate (AOT, 99%, Sigma Chemical Co., St. Louis, Mo.). The water/AOT ratio can be about 10.
It should be understood that the Examples described below are provided for illustrative purposes only and do not in any way define the scope of the invention.
While attempting to synthesize CdS:Mn/ZnS Qdots on a small scale (small volume) using a AOT/heptane W/O microemulsion system based on the process described in FIG. 4, an unexpected dramatic scale-down effect of reaction volume on the growth of the ZnS surface passivation layer (shell) onto the CdS:Mn Qdot core was discovered. The Table shown in FIG. 5 described below details the scale-down protocol of Qdot synthesis showing a constant composition using different microemulsion volumes, from about 700 ml to 35 ml.
FIG. 6 shows emission spectra for the various Qdot samples surprisingly showing very significant spectral changes based only the microemulsion volume used in the microemulsion system, referred to herein as the scale-down effect. For all sensing tests 50 μg of nanoparticles were dispersed in 3 ml of methanol along with less than 1% water (V/V). QD1-4 which resulted in a continuous coatings was found to be the brightest. QD1, QD1-8 and QD1-16 which resulted in a partially passivating coating were found to have intermediate (moderate) emission intensity. QD1-20 which resulted in a minimal coating was found to have the lowest emission intensity. Except QD1-20, all samples showed only variation in luminescence intensity at 584 nm, confirming the effect of surface passivation. Sample QD1-20 showed dual emission at 584 nm and 645 nm. The emission at 645 nm could be due to the ionic defect emission (e.g. sulfur vacancies).
As expected, well-surface passivated Qdots showed the brightest intensity and the poorly-passivated Qdots showed very weak emission. However, Qdots with complete surface passivation are expected to be insensitive to the outside environment, while Qdots with partial surface passivation were found to be responsive to the outside environment. As noted above, partially passivated Qdots are believed to possess localized surface states in the band gap as well as ionic defects (e.g. sulfur vacancies in case of CdS:Mn/ZnS Qdots). Therefore, the Inventors determined that the partially passivated Qdots can be used as an environmentally-sensitive probe as it is possible to further quench or enhance the luminescence intensity of the Qdots in the presence of certain analytes.
Several experiments were conducted. Using a dioctyl sulfosuccinate, sodium salt (AOT)/heptane/water W/O microemulsion technique, CdS:Mn core/ZnS shell Qdots were produced based on the process flow described generally in FIG. 4. Typically, Cd(CH3COO)2.2H2O, Mn(CH3COO)2, Na2S, and Zn(CH3COO)2 were used for the preparation of (Cd2++Mn2+), S2−, and Zn2+ containing the standard aqueous solutions. Each aqueous solution was stirred with an AOT/heptane solution, forming the micellar solution. Mn doped CdS core nanocrystals were formed by mixing (Cd2++Mn2+) and S2− containing micellar solutions rapidly for 10-15 min. The W0 value for the W/O microemulsion was 10. For the growth of a shell layer, a Zn2+-containing micellar solution was added at a very slow rate (1.5 ml/min) into the CdS:Mn nanocrystal micellar solution (having maintained a surplus of sulfur ions to support the ZnS shell growth). The nucleation and growth of a separate ZnS phase were suppressed by the very slow addition of the Zn2+-containing micellar solution.
The Table shown in FIG. 5 shows the microemulsion composition used for all samples. Note that in all samples, the relative ratio of Cd2+, Mn2+, Zn2+ and S2− ions are identical. The microemulsion volume was varied from 700 ml (QD1) to 35 ml (QD 1-20). Traditionally, one would expect to obtain Qdots with similar intensities, irrespective of total microemulsion volume. However, the observations obtained showed this was not the case (see FIG. 7 described below). The brightness of sample QD 1-4 was the maximum followed by the gradual decrease in luminescence intensity from QD 1 to QD 1-8 to QD1-16 that showed a yellow emission from Mn2+ 4T1-6A1 transition at the ˜584 nm under a hand-held 366 nm multi-band UV light source. It is believed that the QD 1-4 sample had a well-passivating ZnS layer as it showed the brightest Mn emission. X-ray photoelectron spectroscopy (XPS) analysis reported in FIG. 7 described below showed drastic deviation of [Zn2+] to [Cd2+] molar ratio (X0 value) from the calculated value of 8. X0 values for QD1, QD1-4, QD 1-8 and QD 1-16 samples were 6.02, 8.17, 11.13 and 3.31, respectively. Note that the experimental X0 value of the brightest sample (QD 1-4) was very close to the calculated value (i.e. 8). Fluorescence emission spectra recorded for all samples clearly showed drastic scale-down effect on the surface passivation process of the Qdots as shown in FIG. 6.
FIG. 7 provides a table including XPS data for the various samples described above. Significantly, the Zn+2/Cd+2 ratio varied from the nominal calculated value of 8, to values above and below 8. A high Zn+2/Cd+2 ratio may be evidence of a partially passivated surface.
To demonstrate the environmental sensitivity of partially passivated Qdots according to the invention, QD 1 and QD1-8 were intentionally selected as the test samples as they are about 2 and 7.4 times dimmer than QD 1-4 and thus should be partially surface-passivated. As noted above, for fluorescence measurements, all experimental Qdot solutions (concentration: 50 μg/ml) were prepared at room temperature in methanol containing DI water (maximum 0.01% (V/V)). Again, all experimental Qdot solutions were transparent and no light-scattering was observed in the visible range. When exposed to highly toxic heavy metal ions (e.g. Cd2+, Hg2+, Pb2+ ions etc.), quenching of 584 nm Qdot emission was observed in a unique fashion for each type of metal ion. It was observed that with respect to luminescence quenching, both QD1 and QD1-8 samples had similar response.
FIG. 8 shows the effect of increased amounts of metal ion concentration on the luminescence intensity of QD1-8. The luminescence quenching efficiency of Hg2+ was at least three orders of magnitude higher than Cd2+ ions. The higher sensitivity of Qdots towards Hg2+ could be attributed to the high reactivity of Hg2+ ions towards Qdots, forming metal-like products such as HgS, CdHgS etc. Unlike Hg2+ ion, the luminescence intensity of QD1-8 measured at 584 nm increased first, reached a maximum at around 3 mM Cd2+ ion concentration, and then decreased. The initial enhancement in luminescence intensity could be due to the formation of the Cd(OH)2 layer over the CdS:Mn partially passivated core, which resulted in the reduction of the non-radiative recombination of charge carriers (electron-hole recombination without luminescence). Further, the decrease in the luminescence intensity with the increase in Cd2+ ions could not be explained without further investigation.
Different analytes were found to provide characteristic luminescent signatures as shown in FIG. 8. Once cataloged, such signatures allow unambiguous identification of particular analytes. For example, when exposed to Pb2+ ions, the luminescence spectral characteristics of QD1-8 (lower right) was quite different as compared to the spectral characteristics obtained from Cd2+ and Hg2+ ions (left). For exposure to Pb2+, a decrease in emission intensity at 584 nm was noticed and a new emission (upper left) peak at ˜643 nm appeared as the Pb2+ concentration increased from 0.166 mM to 14.28 mM (upper right). Several control spectral experiments were performed including emission spectra of pure methanol, methanol-water mixture, 14.28 mM PbCl2 in methanol and emission spectra in the presence of room-light to confirm the unusually sharp peak (much like a scattering peak) in the emission spectra. With a 370 nm UV exposure, 643 nm deep-red emission from 14.28 mM PbCl2 treated QD1-8 a sample was seen visually. The emission data obtained demonstrates that partially passivated Qdots can be used as environment sensitive probes which provide identification of specific analytes. To obtain improved selectivity in samples containing several analytes, the Qdot-based Heavy Metal Detection Probes (QHMDP) according to the present invention having Macro-Cyclic Crown based Ligands described above relative to FIGS. 2( b)-(d) can be used.
It is to be understood that while the invention has been described in conjunction with the preferred specific embodiments thereof, that the foregoing description as well as the examples which follow are intended to illustrate and not limit the scope of the invention. Other aspects, advantages and modifications within the scope of the invention will be apparent to those skilled in the art to which the invention pertains.
1. A core shell particle, comprising:
a luminescent nanocrystal core, and
a partially passivating semiconducting shell on a surface said nanocrystal, and
an analyte selective shell covalently attached to said semiconductor shell.
2. The core shell particle of claim 1, wherein said nanocrystal comprises a metal chalcogenide and said semiconductor shell comprises a compositionally different metal chalcogenide.
3. The core shell particle of claim 2, wherein said nanocrystal comprises CdS and said semiconductor shell comprises ZnS or ZnSe.
4. The core shell particle of claim 1, wherein said nanocrystal includes a transition or lanthanide metal dopant.
5. The core shell particle of claim 1, wherein said semiconductor shell provides a band gap of at least 4 eV at 25° C.
6. The core shell particle of claim 1, wherein said analyte selective shell comprises a Macro-Cyclic Crown Ligand (MCCL).
7. A quantum dot-based sensing system, comprising:
at least one core shell particle including a luminescent nanocrystal core, and
a partially passivating semiconducting shell on a surface said nanocrystal,
an analyte selective shell covalently attached to said semiconductor shell;
a light source for irradiating said core shell particle, and a
light detector for receiving emissions from said core shell particle, wherein said emissions change in response to the presence of at least one analyte.
8. The system of claim 7, further comprising at least one optical fiber including a transmitting leg and a receiving leg, and a core portion located between said transmitting leg and said receiving leg covered with at least one of said core shell particles.
9. The system of claim 7, wherein said analyte selective shell comprises a Macro-Cyclic Crown Ligand (MCCL).
10. The system of claim 7, wherein said nanocrystal comprises a metal chalcogenide and said semiconducting shell comprises a compositionally different metal chalcogenide.
11. The system of claim 10, wherein said nanocrystal comprises CdS and said semiconducting shell comprises ZnS or ZnSe.
12. A method of sensing analytes, comprising the steps of:
providing at least one core shell particle comprising a luminescent nanocrystal core and a partially passivating semiconducting shell on a surface said nanocrystal, and an analyte selective shell covalently attached to said semiconductor shell;
exposing a fluid suspected of including at least one analyte to said core shell particle, and
determining whether said analyte is present in said fluid based on a change in luminescent response of said core shell particle following exposure to said fluid.
13. The method of claim 12, wherein said fluid comprises water.
14. The method of claim 12, wherein said analyte is selected from the group of heavy metal cations.
15. The method of claim 14, wherein said heavy metal cation comprises Hg, Cd or Pb.
16. The method of claim 12, wherein when said analyte is present in said fluid said change in luminescent response of said core shell particle following exposure to said fluid comprises an enhanced luminescent response.
17. The method of claim 12, wherein said analyte selective shell comprises a Macro-Cyclic Crown Ligand (MCCL).
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text:
{-# LANGUAGE GeneralizedNewtypeDeriving #-}  -- haskell-mode wants this
{-# LANGUAGE LambdaCase #-}

module PPL2.CodeGen.Builder where

import PPL2.Prelude
import PPL2.VM.Types

-- ----------------------------------------

newtype Builder a = BU {unBU :: ([a] -> [a])}

instance Semigroup (Builder a) where
  BU x <> BU y = BU $ x . y

instance Monoid (Builder a) where
  mempty = BU id

builder2List :: Builder a -> [a]
builder2List = ($ []) . unBU

-- ----------------------------------------

type Code = Builder AInstr

gi :: AInstr -> Code
gi i = BU (i:)

toACode :: Code -> ACode
toACode = builder2List

-- ----------------------------------------

gLoad :: Address -> Code
gLoad = gi . Load

gLoadInt :: Int -> Code
gLoadInt = gi . LoadI

gLoadInd :: Code
gLoadInd = gi LoadInd

gLoadLab :: Label -> Code
gLoadLab = gi . LoadLab

gStore :: Address -> Code
gStore = gi . Store

gStoreInd :: Code
gStoreInd = gi StoreInd

gPop :: Code
gPop = gi Pop

gDup :: Offset -> Code
gDup = gi . Dup

gComp :: Mnemonic -> Code
gComp = gi . Comp

gJump :: Label -> Code
gJump = gi . Jump

gLabel :: Label -> Code
gLabel = gi . Label

gSRJump :: Label -> Code
gSRJump = gi . SRJump

gSRJumpInd :: Code
gSRJumpInd = gi SRJumpInd

gBr :: Bool -> Label -> Code
gBr b = gi . Br b
{-
gBrFalse :: Label -> Code
gBrFalse = gi . Br False

gBrTrue :: Label -> Code
gBrTrue = gi . Br True
-- -}
gEnter :: Offset -> Code
gEnter = gi . Enter

gLeave :: Code
gLeave = gi Leave

gTerminate :: Code
gTerminate = gi Term

-- ----------------------------------------