Coherent chemistry with THz pulses: Ultrafast field-driven isomerization of LiNC

Abstract

The ability to coherently rearrange structures at the atomic scale is among the grand challenges of physical science. Some of the primary obstacles are nonadiabatic increases in energy, such as intramolecular vibrational relaxation (IVR) and electronic excitations. Motivated by recent advances in strong terahertz (THz) pulse generation, we investigate the potential of THz to circumvent these obstacles. Employing TDDFT-Ehrenfest simulations, we discover that strong THz pulses can drive isomerization of the LiNC molecule over barriers greater than 0.2 eV with very low ionization rates and, in the best case, less than 3 meV of residual excess energy. This work points to new possibilities in predictively manipulating chemical bonds in molecules and materials.