Studying interactions among metal nanoclusters, host ligands and small-molecule analytes

该项目将研究包裹在核酸中的小金属纳米粒子的分子结构和光物理性质，称为dna模板银纳米团簇。银纳米团簇是令人着迷的荧光纳米材料，其颜色经常对周围化学环境的细微变化做出反应，使其成为检测小分子（例如，三磷酸腺苷）和重金属（例如，汞和铜）的新型传感器。然而，尚不清楚银纳米团簇如何与这些分析物相互作用并改变其物理或化学性质。此外，目前尚不清楚为什么某些银簇物种对特定的小分子分析物反应强烈，而对其他类似的化合物却没有反应。该项目旨在回答这些基本问题，最终目标是实现对银纳米簇传感器的分子和原子水平的理解。了解银纳米团簇的纳米级相互作用也将为各种生物和化学应用创造新的工具，例如化学物质的检测。主要研究人员将与当地K-12学生合作，开展名为“探索纳米医学与光”的推广项目。外展的目标是激发学生基于对银纳米团簇的新理解开发新工具，并鼓励他们在大学教育中走上科学、技术、工程和数学的道路。纳米传感器的未来发展受到可编程对特定分析物做出反应的功能纳米材料的缺乏的阻碍。Yeh教授和Brodbelt教授正在使用新颖的实验（基于芯片的高通量选择）和分析（激活电子光分离质谱）方法来筛选大量的银纳米团簇物种，并对它们与宿主配体、小分子分析物和重金属的相互作用有了基本的了解。主要研究人员还将利用深度神经网络对银簇对分析物的反应进行分类，并对银纳米簇进行原子建模。银纳米团簇由于其特殊的化学、物理和光学性质，为小分子和重金属传感提供了新的机会。分析化学、高通量筛选、光物理表征和深度学习分类的变革性整合不仅可以测试假设（分析物结合通过重新排列银簇周围的核碱基来重塑银簇的电子结构），而且还可以创建一个多功能工具包，用于许多应用，包括信号分子检测和污染传感。主要研究人员将与当地K-12学生合作，开展名为“探索纳米医学与光”的推广项目。外展的目标是激发学生基于对银纳米团簇的新理解开发新工具，并鼓励他们在大学教育中走上科学、技术、工程和数学的道路。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

This project will investigate the molecular structures and photophysical properties of small metallic nanoparticles encapsulated in nucleic acids, termed DNA-templated silver nanoclusters. Silver nanoclusters are fascinating fluorescent nanomaterials whose colors often respond to subtle changes in their surrounding chemical environment, making them novel sensors for detection of small molecules (e.g., adenosine triphosphate) and heavy metals (e.g., mercury and copper). However, it is not known how silver nanoclusters interact with these analytes and change their physical or chemical properties. In addition, it is not understood why certain silver cluster species respond strongly to specific small-molecule analytes but not to other similar compounds. The project seeks to answer these fundamental questions, with the end goal to achieve molecular and atomic level understanding of silver nanocluster sensors. Understanding the nanoscale interactions of silver nanoclusters will also create new tools for diverse biological and chemical applications, such as detection of chemicals. The principal investigators will work with local K-12 students in an outreach program named “Exploring Nanomedicine and Light”. The goal of the outreach is to intrigue the students to develop new tools based on the new understanding of silver nanoclusters and encourage them into a science, technology, engineering, and mathematics path in their college education.Future development of nanosensors is hampered by the scarcity of functional nanomaterials that can be programmed to respond to specific analytes. Professors Yeh and Brodbelt are using novel experimental (chip-based high-throughput selection) and analytical (activated electron photodetachment mass spectrometry) approaches to screen a large number of silver nanocluster species and develop a fundamental understanding of their interactions with host ligands, small-molecule analytes and heavy metals. The principal investigators will also take advantage of deep neural networks to classify the silver clusters’ responses to analytes and perform atomistic modeling of silver nanoclusters. Silver nanoclusters present new opportunities for small-molecule and heavy metal sensing because of their special chemical, physical and optical properties. The transformative integration of analytical chemistry, high-throughput screening, photophysical characterization and deep learning classification will not only allow the hypothesis to be tested (analyte binding reshapes silver cluster’s electronic structure through rearranging the nucleobases around the silver cluster) but also enable the creation of a versatile toolkit for numerous applications, including detection of signaling molecules and sensing of pollution. The principal investigators will work with local K-12 students in an outreach program named “Exploring Nanomedicine and Light”. The goal of the outreach is to intrigue the students to develop new tools based on the new understanding of silver nanoclusters and encourage them into a science, technology, engineering and mathematics path in their college education.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.