Mechanisms of Surfactant-Mediated Crystallization of Colloidal Quantum Dots

表面活性剂介导的胶体量子点结晶机制

• 批准号: 2004008
• 负责人: Jonathan Owen
• 金额: $ 47.25万
• 依托单位: Columbia University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2020
• 资助国家: 美国
• 起止时间: 2020-09-01 至 2023-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2004008&HistoricalAwards=false
• 关键词: Mechanisms; Surfactant; Mediated; Crystallization; Colloidal

With support from the Macromolecular, Supramolecular, and Nanochemistry (MSN) Program in the Division of Chemistry, Professor Jonathan Owen at Columbia University is studying the fundamental processes that control the growth of nanometer scale crystals. With deeper understanding of crystal growth mechanisms, scientists can design and manufacture crystals with improved performance in solar cells, light emitting diodes, lasers, and infrared cameras capable of capturing images at night. In this project, crystal growth kinetics is monitored with X-rays generated at synchrotron light sources that allow the first moments of crystal formation to be visualized. Mathematical models are developed to describe the evolution of the growing crystals and predict the growth of new materials. Professor Owen develops an educational program that integrates the research with the education of high school, undergraduate and graduate student researchers, including students at New York City schools serving under-represented elementary, middle school, and high school students. The group communicates the value of research on nanoscale materials to the public.The concentration and temperature dependence of lead selenide and lead sulfide nucleation and growth is probed in this project using in situ optical spectroscopies and X-ray scattering. The solute concentration and the nanocrystal size and yield are monitored in real time. The atomic structure of intermediates formed during the nucleation phase is probed in situ using pair distribution function (PDF) analysis of X-ray scattering. These studies are complemented by ex situ studies of the precursor conversion reaction and the size dependence of the growth kinetics to arrive at a holistic understanding of each of the coupled phases of the reaction. Rate equation models and structure prediction methods are used to model the evolution of the solute and nanocrystals throughout nucleation and growth. Professor Owen is using a synergistic approach to help determine whether the nucleation mechanism follows a classical process involving a critical nucleus whose radius changes with the supersaturation, a rate limiting transition between specific “magic size” clusters, crystallization from an amorphous intermediate, or a molecular process. A deeper understanding of crystal nucleation growth can accelerate the design of a broad array of new materials for luminescent displays, solid state lighting, and photovoltaics. Professor Owen is also working with high school, undergraduate and graduate students closely on this project. He develops a laboratory module to teach high school students about luminescence and shares the teaching tools with local schools serving underrepresented minority students.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

在化学系高分子、超分子和纳米化学（MSN）项目的支持下，哥伦比亚大学乔纳森·欧文教授正在研究控制纳米级晶体生长的基本过程。通过对晶体生长机制的更深入了解，科学家们可以设计和制造具有改进性能的晶体，用于太阳能电池、发光二极管、激光器和能够在夜间捕获图像的红外摄像机。在该项目中，通过产生的 X 射线监测晶体生长动力学。同步加速器光源可以使晶体形成的最初时刻可视化，以描述生长晶体的演化并预测新材料的生长，欧文教授开发了一个将研究与高等教育相结合的教育计划。该小组向公众传达了纳米材料研究的价值。铅的浓度和温度依赖性。硒化物和该项目使用原位光学光谱和 X 射线散射来探测硫化铅的成核和生长，实时监测成核阶段形成的中间体的原子结构。使用 X 射线散射的对分布函数 (PDF) 分析，辅以前体转化反应的异位研究和生长动力学的尺寸依赖性，以得出整体结果。速率方程模型和结构预测方法用于模拟成核和生长过程中溶质和纳米晶体的演化，欧文教授正在使用协同方法来帮助确定成核机制是否遵循特定的规律。经典过程涉及半径随过饱和而变化的临界核、特定“神奇尺寸”簇之间的速率限制转变、非晶中间体的结晶或分子过程对晶体的更深入理解。成核生长可以加速一系列用于发光显示器、固态照明和光伏的新材料的设计，欧文教授还与高中生、本科生和研究生密切合作，开发了一个用于高中教学的实验室模块。该奖项反映了 NSF 的法定使命，并通过使用基金会的智力价值和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

Size Dependent Optical Properties and Structure of ZnS Nanocrystals Prepared from a Library of Thioureas

由硫脲库制备的 ZnS 纳米晶体的尺寸依赖性光学性质和结构

• DOI: 10.1021/acs.chemmater.1c03432
• 发表时间: 2022-01
• 期刊: Chemistry of Materials
• 影响因子: 8.6
• 作者: Bennett, Ellie;Greenberg, Matthew W.;Jordan, Abraham J.;Hamachi, Leslie S.;Banerjee, Soham;Billinge, Simon J.;Owen, Jonathan S.
• 通讯作者: Owen, Jonathan S.

Growth kinetics determine the polydispersity and size of PbS and PbSe nanocrystals

生长动力学决定 PbS 和 PbSe 纳米晶体的多分散性和尺寸

• DOI: 10.1039/d1sc06098h
• 发表时间: 2022-04-20
• 期刊: Chemical Science
• 影响因子: 8.4
• 作者: Campos, Michael P.;De Roo, Jonathan;Greenberg, Matthew W.;McMurtry, Brandon M.;Hendricks, Mark P.;Bennett, Ellie;Saenz, Natalie;Sfeir, Matthew Y.;Abecassis, Benjamin;Ghose, Sanjit K.;Owen, Jonathan S.
• 通讯作者: Owen, Jonathan S.

Synthesis of graded CdS 1−x Se x nanoplatelet alloys and heterostructures from pairs of chalcogenoureas with tailored conversion reactivity

利用具有定制转化反应性的成对硫属脲合成分级 CdS 1–x Se x 纳米片合金和异质结构

• DOI: 10.1039/d3sc03384h
• 发表时间: 2023-11-08
• 期刊: Chemical Science
• 影响因子: 8.4
• 作者: Saenz, Natalie;Hamachi, Leslie S.;Wolock, Anna;Goodge, Berit H.;Kuntzmann, Alexis;Dubertret, Benoit;Billinge, Isabel;Kourkoutis, Lena F.;Muller, David A.;Crowther, Andrew C.;Owen, Jonathan S.
• 通讯作者: Owen, Jonathan S.

Persistent nucleation and size dependent attachment kinetics produce monodisperse PbS nanocrystals

持久成核和尺寸依赖性附着动力学产生单分散 PbS 纳米晶体

• DOI: 10.1039/d1sc06134h
• 发表时间: 2022-05-04
• 期刊: Chemical Science
• 影响因子: 8.4
• 作者: Abecassis, Benjamin;Greenberg, Matthew W.;Bal, Vivekananda;McMurtry, Brandon M.;Campos, Michael P.;Guillemeney, Lilian;Mahler, Benoit;Prevost, Sylvain;Sharpnack, Lewis;Hendricks, Mark P.;DeRosha, Daniel;Bennett, Ellie;Saenz, Natalie;Peters, Baron;Owen, Jonathan S.
• 通讯作者: Owen, Jonathan S.