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

Lina Bielke1, Samuel Schöpa1, Falk-Erik Wiechmann1,2, Franziska Fennel1,2, and Dieter Bauer1,2,*

  • *Contact author: dieter.bauer@uni-rostock.de
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Phys. Rev. A 113, 043106 – Published 3 April, 2026

DOI: https://doi.org/10.1103/7ljs-sbpy

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)]. There it was found that the laser-polarization-dependent harmonic yield was 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.

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Phys. Rev. A 113, 043106– Published 3 April, 2026
  • Received 3 December 2025
  • Accepted 11 March 2026
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