Probing Laser-Induced Plasma Generation in Liquid Water

• Published in: Journal of the American Chemical Society Vol. 143; no. 27; pp. 10382 - 10388
• Main Authors: Xu, Jiyu, Chen, Daqiang, Meng, Sheng
• Format: Journal Article
• Language: English
• Published: American Chemical Society 14-07-2021
• ISSN: 0002-7863; 1520-5126
• DOI: 10.1021/jacs.1c04675

Understanding photoexcitation dynamics in liquid water is of crucial significance for both fundamental scientific exploration and technological applications. Despite the observations of photoinduced macroscopic phenomena, the initial atomistic movements and associated energy transfer pathways immediately following laser irradiation are hard to track due to the extreme complexity of laser–water interaction and its ultrafast time scale. We explore the femtosecond evolution of liquid water upon intense photoexcitation based on nonadiabatic quantum dynamics simulations. Separate ionic and electronic dynamics were explicitly monitored with tremendous details unveiled on an unprecedented microscopic level. Water was found to undergo the two-step heating processes. The strong-field effects and electronic excitations dominate the first-stage heating and pressurization. Subsequent relaxation of ionic and electronic subsystems further increases the ionic temperature but releases the large internal pressure. The water molecules are stretched during the laser pulses, and the electronic excitations result in the proton transfers after laser pulses. Intense laser pulses violently excite liquid water, giving rise to severe molecular dissociation and plasma generation during the laser pulses. The laser-induced water plasma is characterized by a high fraction of free protons (∼50%), nonequilibrium ionic and electronic distributions, and a metallic electronic density of states.