High-harmonic generation from two weakly coupled molecules: a simple tight-binding model

TL;DR

This paper models high-harmonic generation in weakly coupled molecules using a simple tight-binding approach, revealing how laser polarization and intermolecular interactions influence harmonic yields.

Contribution

It introduces a two-dimensional tight-binding model to analyze the effects of molecular coupling and laser polarization on high-harmonic generation.

Findings

Lower harmonic intensities peak when polarization aligns with molecular axes.

Higher harmonics show maximum yield along the intermolecular axis.

The harmonic order at which yield flips depends on coupling strength.

Abstract

The generation of high harmonics is a strongly nonlinear effect that allows to probe properties of the target and to study electron dynamics in matter. It has been investigated in many different kinds of targets, including molecular gases, liquids and solids. Recently, high-harmonic generation was studied in organic molecular crystals by Wiechmann et al. [Nat. Commun. 16, 9890 (2025)]. It was found that the laser-polarization-dependent harmonic yield is sensitive to the weak couplings between nearest- and next-nearest-neighbor molecules. In this paper, the impact of the laser polarization angle and the intermolecular interaction on the harmonic yield is examined in detail using a simple but insightful two-dimensional tight-binding system that models a molecular dimer, i.e. two weakly coupled molecules. We find that the intensities of lower harmonic orders tend to maximize for a laser polarization direction aligning with the molecular axes, whereas higher harmonic orders rather show the strongest yield for a polarization direction along the intermolecular axis. We further demonstrate that the harmonic order at which the maximum flips from the molecular to the intermolecular direction strongly depends on the intermolecular coupling strength. To gain a deeper insight into the origins of the findings, we include a detailed adiabatic analysis, showing that the flipping of the maximum yield towards the intermolecular direction is already contained qualitatively in the adiabatically following states.