arXiv subjects

Lina Bielke

Publications and source records attributed to Lina Bielke.

3 recordsLinked to original sources

arXiv2025

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

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.

quant-ph↗

arXiv2025

High-Order Harmonic Generation in Organic Molecular Crystals

High-order harmonic generation (HHG) is a powerful tool for probing electronic structure and ultrafast dynamics in matter. Traditionally studied in atomic and molecular gases, HHG has recently been extended to condensed matter, enabling all-optical investigations of electronic and crystal structures. Here, we experimentally demonstrate HHG in a new class of materials: thin organic molecular crystals with perfectly aligned molecules, using pentacene as a model system. Organic molecular crystals, characterized by weak intermolecular coupling, flat electronic bands, and large unit cells, differ fundamentally from conventional covalent or ionic crystals and have attracted significant interest as promising candidates for organic electronics. We show that pentacene crystals endure laser intensities sufficient for efficient HHG up to the 17th order. The harmonic yield as a function of laser polarization reveals a strong dependence on intermolecular interactions, with higher harmonic orders particularly sensitive to both nearest- and next-nearest-neighbor couplings. Model calculations indicate that weaker intermolecular interactions necessitate probing with higher harmonic orders to resolve the crystal structure. These findings suggest that HHG may serve as a powerful tool for probing the electronic structure of organic molecular crystals, enhancing all-optical techniques for studying electronic properties and ultrafast dynamics in complex organic materials.

physics.optics↗

arXiv2023

Formation of the solid-state high-order harmonic generation plateau through destructive interference

In frequently studied two-band models for solid-state high-harmonic generation, interband harmonics in principle can range from the minimum to the maximum bandgap. However, it is known that a laser-intensity dependent cutoff exists that may be well below the maximum bandgap unless the laser intensity is so high that the electrons explore the entire Brillouin zone. We show that this laser-intensity dependent cutoff is formed by destructive interference of the emission of electrons starting at different initial states in the Brillouin zone. The calculations in this work are for Su-Schrieffer-Heeger chains but our findings apply to other two-band systems as well. Only when the sampling of the Brillouin zone is fine enough or, equivalently, a finite chain is long enough in position space, the destructive interference is complete and forms the cutoff. For coarser sampling and shorter chains all harmonics between minimum and maximum bandgap are emitted. A time-frequency analysis shows how certain trajectories are responsible for the formation of the cutoff.

physics.optics↗