Molecular Radiative and Relaxation Processes

加州大学欧文分校的Shaul Mukamel得到了化学系化学理论、模型和计算方法计划的支持，该计划研究光和物质如何相互作用。激光和其他光源是人们可以用来探测、测量甚至控制分子行为的工具。在这个项目中，通过结合光的波动特性，如相位和偏振，设计了光与分子相互作用的新方法。尽管人们很好地理解了光的单个小组件(光子)与分子的相互作用，但多个光子可以组合成脉冲，以新的方式影响分子。这些光子和分子的相互作用最好地用量子力学来描述，量子力学是对亚原子粒子运动和相互作用的数学描述，结合了能量量子化、波粒二象性、测不准原理等概念。在这个项目中开发的方法将在这个框架内提供新的信息。这一领域的成功可能会带来量子计算机等新技术。为了对预测进行基准测试，该项目包括与世界各地的领先实验小组进行广泛的合作和学生交流。穆卡迈尔教授正在开发方法来研究复杂分子对超快激光脉冲序列的反应，这提供了电子和振动动力学和相关性的多维视角。设计了涉及新型脉冲序列的实验技术。发展了分析它们的理论和计算工具，并广泛应用于凝聚相中的分子。开发了用于解释和分析这些信号的模型和实用计算工具。探索了利用光的量子性质、光子纠缠和光子符合探测的新型光谱技术。这为探测分子和发色团聚集体提供了额外的工具，因为它们提供了经典光无法获得的信息。将单个纠缠光子的符合测量和干涉测量相结合的探测方案被应用于研究分子络合物中的基元电荷和能量迁移过程。在微腔中操纵分子属性(极化化学)和相干控制方案被用来优化和提炼非线性光学信号。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。

Shaul Mukamel of the University of California, Irvine is supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry to study how light and matter interact. Lasers and other light sources are tools with which one can probe, measure, and even control the behavior of molecules. In this project, new ways to interact light with molecules are designed by incorporating the wave properties of light such as phase and polarization. Although the interaction of a single small package (photon) of light with a molecule is quite well understood, multiple photons can be combined into pulses that influence molecules in new ways. These interactions of photons and molecules are best described by quantum mechanics, a the mathematical description of the motion and interaction of subatomic particles, incorporating the concepts of quantization of energy, wave-particle duality, the uncertainty principle, etc. The methods developed in this project will provide new information within this framework. Success in this area could lead to new technologies such as quantum computers. To benchmark the predictions, the project includes extensive collaborations and student exchanges with leading experimental groups all over the world.Professor Mukamel is developing methods to study the response of complex molecules to sequences of ultrafast optical laser pulses that provide a multidimensional view of electronic and vibrational dynamics and correlations. Experimental techniques involving novel pulse sequences are designed. Theoretical and computational tools for their analysis are developed and broadly applied to molecules in the condensed phase. Models and practical computational tools are developed for the interpretation and analysis of these signals. Novel spectroscopic techniques, which make use of the quantum nature of light, photon entanglement and photon coincidence detection are explored. These provide additional tools for probing molecules and chromophore aggregates by providing information that is not accessible by classical light. Detection schemes that combine coincidence measurements of individual entangled photons and interferometry are applied to study the elementary charge and energy migration processes in molecular complexes. Manipulating molecular properties in microcavities (polariton chemistry) and coherent control schemes are employed to optimize and refine nonlinear optical signals.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.