2019/10/25 by Yuya Morimoto, Morimoto, Yuya, Yasushi Shinohara +9
Chemistry · Physics and Astronomy · #Atomic Physics (physics.atom-ph) #Chemical Physics (physics.chem-ph) #FOS: Physical sciences #Laser-Matter Interactions and Applications #Molecular spectroscopy and chirality #Optics (physics.optics) #Spectroscopy and Quantum Chemical Studies
paper · pdf · doi:10.48550/arxiv.1910.11821
openalex publication_date 2019/10/25 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28
A dielectric material's response to light is macroscopically described by electric displacement fields due to polarization and susceptibility, but the atomistic origin is light-cycle-driven motion of electron densities in the restoring forces of the atomic environment. Here we report how the macroscopic nonlinear-optical response of a heteronuclear crystal relates to the alignment and orientation of its chemical bonds. Substantial nonlinear emission is only observed if the electric field of an optical single-cycle pulse points from the less electronegative to the more electronegative element and not vice versa. This asymmetry is a consequence of the unbalanced real-space motion of valence charges along the direction of the bonds. These results connect a material's chemical structure to the optical response and may facilitate the comprehension and design of novel materials for applications in optics and lasers on basis of the atoms and how they connect.