Coherent Nonlinear Spectroscopy with Multiple Mode-Locked Lasers

Abstract

Coherent multidimensional spectroscopy has been widely used to study the structure and dynamics of chemical and biological systems. Each ultrashort pulse from a single mode-locked laser is split into multiple pulses by beam splitters. Their arrival times at a given molecular sample are controlled with mechanical time-delay generators for time-resolved measurements of molecular responses. Such nonlinear vibrational, electronic, or vibrational-electronic spectroscopy can now be carried out with multiple mode-locked lasers with highly stabilized repetition and sometimes carrier-envelope-offset frequencies. By precisely controlling the repetition frequencies of multiple mode-locked lasers, one can achieve automatic delay time scanning, known as asynchronous optical sampling, to investigate various relaxation processes associated with photochemical or photobiological phenomena at one sweep in time. In this Perspective, the current developments and applications of multiple mode-locked laser-based techniques to time-resolved nonlinear spectroscopy of chromophores in condensed phases are discussed. The author's perspective on this approach is also presented.