Nonadiabatic molecular dynamics simulation of in a strong laser field**Xi Zhao was supported by Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy (Grant No. DE-FG02-86ER13491), the National Natural Science Foundation of China (Grant No. 11904192); Ji-Gen Chen was supported by the National Natural Science Foundation of China (Grant No. 11975012);

Abstract

We investigate the alignment dependence of the strong laser dissociation dynamics of molecule in the frame of real-time and real-space time-dependent density function theory coupled with nonadiabatic quantum molecular dynamics (TDDFT-MD) simulation. This work is based on a recent experiment study “ultrafast electron diffraction imaging of bond breaking in di-ionized acetylene” [Wolter et al, Science 354, 308–312 (2016)]. Our simulations are in excellent agreement with the experimental data and the analysis confirms that the alignment dependence of the proton dissociation dynamics comes from the electron response of the driving laser pulse. Our results validate the ability of the TDDFT-MD method to reveal the underlying mechanism of experimentally observed and control molecular dissociation dynamics.