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A dielectric materials 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 materials 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.
We present a method to control photodissociation by manipulating the bond softening mechanism occurring in strong shaped laser fields, by varying the chirp sign and magnitude of an ultra-short laser pulse. Manipulation of bond-softening is experiment
Nonlinear optical methods are becoming ubiquitous in many areas of modern photonics. They are, however, often limited to a certain range of input parameters, such as pulse energy and average power, since restrictions arise from, for example, parasiti
We consider a hybrid plasmon-exciton system comprised of a resonant molecular subsystem and three Au wires supporting a dipole mode which can be coupled to a dark mode in controllable fashion by variation of a symmetry parameter. The physics of such
We numerically demonstrate inhibition of absorption, optical transparency, and anomalous momentum states of phase locked harmonic pulses in semiconductors, at UV and extreme UV frequencies, in spectral regions where the dielectric constant of typical
We present a versatile electric trap for the exploration of a wide range of quantum phenomena in the interaction between polar molecules. The trap combines tunable fields, homogeneous over most of the trap volume, with steep gradient fields at the tr