Understanding Emerging Photon Avalanching Processes in Lanthanide-Based Nanomaterials

了解镧系纳米材料中新兴的光子雪崩过程

• 批准号: 2203510
• 负责人: Peter Schuck
• 金额: $ 52万
• 依托单位: Columbia University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2022
• 资助国家: 美国
• 起止时间: 2022-06-15 至 2025-05-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2203510&HistoricalAwards=false
• 关键词: Understanding; Emerging; Photon; Avalanching; Processes

With support from the Macromolecular, Supramolecular, and Nanochemistry (MSN) program in the Division of Chemistry, Professor P. James Schuck of Columbia University is studying the photon avalanching behavior in lanthanide-based nanoparticles. When nanoparticles absorb light of one color, they often emit light of another color, in a process known as photoluminescence. In most cases, the intensity of the photoluminescence scales with the intensity of the exciting light. Double the light and photoluminescence is twice as bright. However, that is not always the case. Sometimes the absorption of light can make a nanoparticle more likely to absorb more light. In these cases, the brightness of the photoluminescence would more than double when the intensity of the exciting light doubles. This property is known as photon avalanching, and it could be used in a variety of emerging applications. However, there are only a few examples of substances that exhibit photon avalanching behavior and much remains to be learned about this unusual property. Professor Schuck and his students will use a combined experimental and theoretical approach to unlock fundamental insights about what controls the photon avalanching in these unique nanostructures. Their discoveries could impact technologies ranging from efficient upconverting lasers and image processing to infrared quantum counting, solid-state lighting and broadband photonics, all of which rely on rapid and energy efficient light-material interactions. The project will also promote STEM education, engaging graduate, undergraduate, and underrepresented high school students through research and teaching activities highlighting non-traditional links between chemistry and engineering disciplines.This project aims to fundamentally understand and develop new avalanching nanoparticles through a synergistic effort that combines advanced characterization, theoretical modeling, precision synthesis and hierarchical nanoparticle design. Avalanching nanoparticles will be investigated using single-particle imaging and optical spectroscopy approaches, revealing critical mechanistic parameters and essential links that define, and ultimately limit, the photon avalanching response in this new class of materials. In addition, improved models of photon avalanching in nanoparticles will be developed, enabling the quantitative derivation of the roles of distinct energy transfer (ET) processes and recombination pathways – and the prediction of nanochemistry-dependent avalanching properties – when combined with our experimental measurements. The research is expected to establish foundational science and strategies for jump-starting the field of photon avalanching nanostructures, with potential for ultrasensitive imaging, light harvesting, and compact quantum photonics.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.

在化学系大分子、超分子和纳米化学(MSN)计划的支持下，哥伦比亚大学的P.James Schuck教授正在研究稀土纳米粒子中的光子雪崩行为。当纳米颗粒吸收一种颜色的光时，它们通常会发射另一种颜色的光，这一过程被称为光致发光。在大多数情况下，光致发光的强度随激发光的强度而变化。光和光致发光都是原来的两倍。然而，情况并不总是如此。有时，光的吸收会使纳米颗粒更有可能吸收更多的光。在这些情况下，当激发光的强度加倍时，光致发光的亮度将增加一倍以上。这种特性被称为光子雪崩，它可以用于各种新兴的应用中。然而，显示出光子雪崩行为的物质只有几个例子，关于这种不寻常的性质还有很多需要了解。舒克教授和他的学生将使用实验和理论相结合的方法，揭示是什么控制了这些独特的纳米结构中的光子雪崩。他们的发现可能会影响从高效上转换激光和图像处理到红外量子计数、固态照明和宽带光子学等一系列技术，所有这些技术都依赖于快速且节能的光-材料相互作用。该项目还将促进STEM教育，通过强调化学和工程学科之间的非传统联系的研究和教学活动，吸引研究生、本科生和代表性不足的高中生。该项目旨在通过结合先进的表征、理论建模、精确合成和分级纳米颗粒设计的协同努力，从根本上了解和开发新的雪崩纳米颗粒。雪崩纳米粒子将使用单粒子成像和光学光谱学方法进行研究，揭示定义并最终限制这类新材料中的光子雪崩响应的关键机械参数和基本环节。此外，还将开发改进的纳米粒子中的光子雪崩模型，与我们的实验测量相结合，能够定量推导不同的能量转移(ET)过程和复合路径的作用，并预测依赖于纳米化学的雪崩特性。这项研究有望建立基础科学和战略，以启动光子雪崩纳米结构领域，具有超灵敏成像、光收集和紧凑量子光子的潜力。这一奖项反映了NSF的法定使命，并通过使用基金会的智力优势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

Indefinite and bidirectional near-infrared nanocrystal photoswitching

• DOI: 10.1038/s41586-023-06076-7
• 发表时间: 2022-09
• 期刊: Nature
• 影响因子: 64.8
• 作者: Changhwan Lee;Emma Z. Xu;K. Kwock;Ayelet Teitelboim;Yawei Liu;H. Park;Benedikt Ursprung;Mark E. Ziffer;Yuzuka Karube;N. Fardian-Melamed;C. Pedroso;Jongwoo Kim;Stefanie D. Pritzl;S. Nam;Theobald Lohmueller;J. Owen;P. Ercius;Y. Suh;B. Cohen;E. Chan;P. Schuck