权益分类	功能权益	普通用户	{{item.name}}会员
{{category.name}}	{{benefitItem.name}}

Nonperturbative theory of femtosecond time-resolved spectroscopy: optical N-wave mixing and strong-pulse spectroscopies

飞秒时间分辨光谱的非微扰理论：光学 N 波混频和强脉冲光谱

基本信息

批准号：
226726153
负责人：
Professor Dr. Wolfgang Domcke
金额：
--
依托单位：
Lehrstuhl für Theoretische Chemie
依托单位国家：
德国
项目类别：
Research Grants
财政年份：
2012
资助国家：
德国
起止时间：
2011-12-31 至 2019-12-31
项目状态：
已结题

来源：
https://gepris.dfg.de/gepris/projekt/226726153?language=en
关键词：
Nonperturbative theory femtosecond time resolved

项目摘要

This research project aims at the further development of the theory of multiple-pulse UV/vis laser spectroscopy of polyatomic molecules. Deviating from the main-stream approach, which is based on the formalism of perturbative nonlinear optics, we elaborate a nonperturbative description of femtosecond time-resolved spectroscopy. In the weak-field regime, the nonperturbative theory is computationally more efficient than the traditional approach when applied to complex material systems. In the strong-field regime, there is no alternative to a nonperturbative description. We will investigate the potential of two-dimensional UV/vis spectroscopy and of polarization-sensitive pump-probe spectroscopy (two examples of four-wave-mixing spectroscopies) for the detection of ultrafast dynamics at conical intersections of electronic potential-energy surfaces. We will perform computational simulations of the signals of two novel six-wave-mixing spectroscopies (femtosecond stimulated Raman spectroscopy and heterodyned three-dimensional optical spectroscopy). We will develop a theoretical description of the novel and very promising technique of femtosecond double-pump single-molecule spectroscopy and will consider applications. We will explore to which extent strong-field phenomena, such as electronic Rabi cycling, can provide novel spectroscopic information on the ultrafast nonadiabatic dynamics of complex molecular systems.

本研究旨在进一步发展多原子分子的多脉冲紫外/维斯光激光光谱理论。偏离主流的方法，这是基于微扰非线性光学的形式主义，我们阐述了飞秒时间分辨光谱的非微扰描述。在弱场区，非微扰理论在计算复杂物质系统时比传统方法更有效。在强场区，除了非微扰描述之外，别无选择。我们将研究二维紫外/维斯光谱和偏振敏感泵浦-探测光谱（四波混合光谱的两个例子）在电子势能面的圆锥形交叉点的超快动力学检测的潜力。我们将对两种新颖的六波混频光谱（飞秒受激拉曼光谱和外差三维光谱）的信号进行计算模拟。我们将对飞秒双泵浦单分子光谱这一新颖且非常有前途的技术进行理论描述，并考虑其应用。我们将探讨在何种程度上强场现象，如电子拉比循环，可以提供新的光谱信息的超快非绝热动力学的复杂分子系统。