Theoretical Development of Nonlinear Surface-Selective Spectroscopies of Hydrogen-Bonded Systems

韦恩州立大学的弗拉基米尔切尔尼亚克获得了理论和计算化学项目的一项奖励，用于研究开发表征表面选择性光谱信息的方法，特别是氢键系统。 这项工作特别集中在这些系统的超快动力学模型的开发上，包括：（i）开发和验证能够对表面信号进行无背景检测的时间分辨的偶数阶非线性光谱技术;（ii）开发有效的信号处理算法;和（iii）发展降维经典和半经典的超快动力学随机模型，包括量子效应。 氢键是发生在化学和生物学中的基本非共价相互作用之一，并且负责分子组装体的许多独特性质。 了解复杂氢键系统的一般动力学特征将有助于我们了解一般的生物分子系统，也将有助于开发新的技术应用，依赖于对这种重要的化学相互作用的更好的理解。 在这项工作中开发的处理实验数据的理论方法和方法对于解释实验至关重要，但也可以扩展到其他类型的研究，如单分子光谱学，光纤通信以及各种技术应用中的光和能量转换。 Chernyak通过底特律公立学校系统运行的"高中生学徒计划"，让代表性不足的少数民族高中生参与他的研究小组。 因此，这项工作对新技术的开发和培训多样化的科学工作队伍产生了更广泛的影响。

Vladimir Chernyak of Wayne State University is supported by an award from the Theoretical and Computational Chemistry program for research to develop methods to characterize surface-selective spectroscopic information, particularly for hydrogen-bonded systems. The work is specifically focused on the development of models for ultrafast dynamics of these systems and includes: (i) the development and validation of time-resolved, even-order nonlinear spectroscopic techniques capable of background-free detection of the surface signal; (ii) development of efficient signal processing algorithms; and (iii) development of reduced-dimensionality classical and semi-classical stochastic models for ultrafast dynamics including quantum effects. Hydrogen bonding is one of the fundamental non-covalent interactions that occur in chemistry and biology and is responsible for many unique properties of molecular assemblies. Understanding the general dynamical features of complex hydrogen-bonded systems will help us understand biomolecular systems in general and will also aid in developing new technological applications that rest on an improved understanding of this important chemical interaction. The theoretical approaches and methods for processing experimental data that are being developed in this work are critical for interpreting experiments but may also be extended to other types of studies such as single-molecule spectroscopy, optical fiber communications and light and energy conversion in a variety of technological applications. Chernyak is involving under-represented minority high school students in his research group through a "High School Student Apprentice Program" run by the Detroit Public School System. The work is, thus, having a broader impact both on the development of new technology and on the training of a diverse scientific workforce.