Light-Induced Ultrafast Molecular Dynamics: From Photochemistry to Optochemistry

Abstract

By precisely controlling the waveform of ultrashort laser fields, electronic and nuclear motions in molecules can be steered on extremely short time scales, even in the attosecond regime. This new research field, termed “optochemistry”, presents the light field in the time-frequency domain and opens new avenues for tailoring molecular reactions beyond photochemistry. This Perspective summarizes the ultrafast laser techniques employed in recent years for manipulating the molecular reactions based on waveform control of intense ultrashort laser pulses, where the chemical reactions can take place in isolated molecules, clusters, and various nanosystems. The underlying mechanisms for the coherent control of molecular dynamics are explicitly explored. Challenges and opportunities coexist in the field of optochemistry. Advanced technologies and theoretical modeling are still being pursued, with great prospects for controlling chemical reactions with unprecedented spatiotemporal precision.

Attosecond ionization time delays in strong-field physics

“…In addition to the advancements in exploring quantum dynamics at ever faster rates and on ever shorter timescales, interdisciplinary integration with other fields holds promising prospects, leading to ultrafast chemistry, [3,170,171] ultrafast nanophysics, [172,173] and ultrafast quantum information science, [174][175][176][177][178][179] offering fertile ground for innovative research. Continued exploration in the realm of ultrafast science promises an ever broader scope, contributing to the expansion of human knowledge on an ever increasing scale.…”

“…In the 1980s, femtosecond lasers started to develop, enabling the production of the movie of a chemical reaction. [1] Starting in the 2000s, laser sources with attosecond duration have matured, making possible the observation and control of electronic processes [2] and the formation and breakage of chemical bonds, [3] which are the fastest resolvable physical processes up to date.…”

The quantum trajectory‐guided adaptive Gaussian methodology in the Libra software package

“…Nonadiabatic effects of electron‐nuclear interactions are essential in many chemical processes [1–6], including photophysics and photochemistry involving charge and energy transfer, and reactive dynamics in the condensed phase. The systems exhibiting electronically nonadiabatic behavior range from electron and/or proton transfer in chemical and biological systems [4, 5, 7], to light‐harvesting materials [6, 8–12], to reaction control and optochemistry [13]. Therefore, the development of time‐dependent nonadiabatic dynamics methods has received a lot of attention from many theorists utilizing a variety of approaches [14–18].…”

The Quantum Trajectory-quided Adaptive Gaussian Methodology in the Libra Software Package

“…The systems exhibiting electronically nonadiabatic behavior range from electron and/or proton transfer in chemical and biological systems, 4,5,7 to light-harvesting materials, 6,[8][9][10][11][12] to reaction control and optochemistry. 13 Therefore, the development of time-dependent nonadiabatic dynamics methods has received a lot of attention from many theorists utilizing a variety of approaches. [14][15][16][17][18] Given the expense and unfavorable scaling of exact quantum dynamics methods, an often-employed strategy is to combine a classical treatment of the nuclei with a semi-classical or quantum description of electrons.…”