CAREER: From Quantum to Classical and Back: Bringing 2D Spectroscopy Insights into Focus

职业生涯：从量子到经典再回归：聚焦二维光谱学见解

• 批准号: 2236625
• 负责人: Michael Reppert
• 金额: $ 65万
• 依托单位: Purdue University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2023
• 资助国家: 美国
• 起止时间: 2023-02-01 至 2028-01-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2236625&HistoricalAwards=false
• 关键词: CAREER; Quantum; Classical; Back; Bringing

Mike Reppert of Purdue University is supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry to explore the interplay between quantum and classical coherence in two-dimensional (2D) spectroscopy. Two-dimensional infrared (2DIR) spectroscopy and two-dimensional electronic spectroscopy (2DES) use ultrafast laser pulses to monitor the motion of atoms and electrons on timescales faster than one trillionth of a second. Such experiments have the potential to provide unprecedented insight into fundamental biological processes such as protein folding and photosynthesis. However, the data they produce is often difficult to interpret, limiting their usefulness in real-world applications. Dr. Reppert and his research group are developing new theoretical tools to better understand the physical origins of 2DIR and 2DES signals (especially the distinct roles played by quantum and classical effects), paving the way for more transparent and efficient interpretation of 2D data. Newly developed 2DIR simulation methods will be made available to other researchers by incorporating them into an online application for protein 2DIR simulations. In addition, the Reppert group will work with K-12 educators to develop 2D acoustic experiments that demonstrate the working principles of 2DES and 2DIR measurements using audible signals. Together, these efforts are expand expand both accessibility to these spectroscopic tools and the application of these 2D methods to a broad class of problems in the chemical sciences. Despite the impressive array of quantum and semiclassical dynamics methods available for simulating two-dimensional (2D) optical spectra, a surprising gap remains in the 2D theory arsenal: no classical theory for 2D spectroscopy or systematic framework for classifying quantum effects has been thoroughly developed. On the one hand, this limitation leaves largely unexplored the potential numerical advantages of fully classical simulations; on the other hand, the inability to systematically classify quantum and classical effects obscures the physical origins of coherence in coupled molecular systems. To explore these issues, the Reppert group is working to develop a systematic, diagrammatic framework for disentangling quantum and classical contributions to coherent vibrational dynamics, beginning with the relatively simple case of 2D infrared (2DIR) spectroscopy and working toward more complex vibronic dynamics and the quantitative interpretation of Amide I (protein C=O stretch) 2DIR experiments. To test the limits of classical models for coherent nonlinear processes, a new class of 2D measurements investigating acoustic nonlinear response will be designed and implemented experimentally. The broader impact of this work will be maximized by developing educational materials (K-12 through graduate level) that illustrate nonlinear processes through conceptually approachable “ball and spring” models. In addition, the Reppert group will incorporate newly developed Amide I simulation methods into the AmideSpec app, offering a research-grade online tool for interpreting protein 2DIR data to researchers around the globe.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.

迈克（Mike）的曲目由化学理论的奖励支持，以探索二维（2D）光谱中的量子和经典连贯性之间的解释。为了在时间刻度上监测原子和电子的运动，比蛋白质折叠和光合作用的速度要快。了解2DIR和信号的物理起源（尤其是量子和经典效应所起的独特角色），将通过将它们纳入蛋白质2DIR模拟的Anline在线在线应用程序中，从而提供其他研究人员。为了开发2D，使用可听见的信号证明了2DIR测量的工作原理。光谱，令人惊讶的差距仍然存在于2D理论库中：没有用于2D光谱的经典理论或用于分类量子效率</s> </s> </s> </s> </s> </s> </s> </s> </s> </s> </s> </s> </s> </s> </s> </s> </s> </s> </s> </s> </s> </s的经典理论。 > </s> </s> </s> </s> </s> </s> </s> </s> </s> </s> </s> </s>完全阶级的dvantages，以系统地经典的效应遮盖了phe耦合分子系统中的相干性探索这些相干的经典贡献，对相干性OWARD更为复杂截面过程，将设计和实施这项工作的新的2D测量结果。 Modition Despec应用程序，为全球研究人员提供了研究级的在线工具，该奖项反映了NSF'SF'Story Dismiss D通过基金会的知识分子优点和更广泛的影响审查标准通过评估来降低了支持。