Orientated energy absorption from mid-infrared laser pulses in constrained water systems

TL;DR

This study uses molecular dynamics simulations to explore how polarized mid-infrared pulses induce orientation-dependent resonant energy absorption in water, leading to rapid heating and insights into biochemical energy transfer.

Contribution

It reveals the anisotropic energy absorption mechanisms in oriented water molecules under mid-infrared irradiation, highlighting the role of molecular orientation in vibrational excitation.

Findings

Rapid heating exceeding 100 K under 1 ps pulse

Orientation-dependent excitation of symmetric and asymmetric OH modes

Dominance of symmetric mode in parallel orientation, asymmetric in perpendicular orientation

Abstract

The energy acquisition based on resonant excitations are of great importance in chemical and biological systems. Here, the intramolecular resonant absorption of polarized mid-infrared pulses by bulk water and surface water is investigated using molecular dynamics simulation. The consequent heating based on the OH stretching vibrations is found to be very prompt, achieving more than 100 K temperature jump under irradiation of a pulse with 1 ps width and maximum intensity of 0.5 V/nm. A general anisotropic phenomenon is manifested as a result of preferential resonant excitation of symmetric or asymmetric OH stretching vibration, depending on the relationships between the orientations of water molecules and the polarized direction of the pulse. In the case of water molecules with the preferred dipole orientation, constrained by applied static electric field or spacial confinement, parallel to the polarized direction of the pulses, the energy absorption is dominated by the symmetric stretching mode (around 99 THz), while in the perpendicular case, the asymmetric stretching mode (around 101 THz) is more efficient. Since orientated water molecules are prevalent in chemical and biological systems, these findings concerning orientation-dependent excitation of intramolecular vibrations are of special significance to understood the energy absorption and transition in relevant biochemical processes.