Hauptinhalt
Eingereicht - im peer-review-Prozess
Inhalt ausklappen Inhalt einklappen K. Gadge, M. Merboldt, M. Schüler, J. P. Bange, W. Bennecke, M. A. Sentef, M. Reutzel, S. Mathias, S. R. Manmana, A comparative study of perturbative and nonequilibrium Green's function approaches for Floquet sidebands in periodically driven quantum systems, arXiv:2601.14443 (2026).
We compare two complementary theoretical approaches to compute and interpret Floquet sidebands in periodically driven quantum materials: a first-order perturbative approach (first-order perturbative Born approximation, PB1) and time-dependent nonequilibrium Green's functions (tdNEGF). Using graphene as a model Dirac system, we disentangle in pump-probe setups Floquet-dressed initial states, Volkov-dressed final states (also known as laser-assisted photoelectric effect, LAPE), and their interference. We quantify how photoemission matrix elements, polarization, incidence angle, and near-surface screening shape the momentum-resolved sideband intensity observed in tr-ARPES. PB1 yields an analytical expression for the momentum-dependent sideband intensity, and for graphene it captures the correct symmetry trends, such as the magnitude of the intensities when considering the interference between the Floquet and Volkov states and photoemission matrix elements. tdNEGF reproduces the full energy-momentum-resolved spectra, including hybridization gaps and spectral-weight redistribution. We find qualitative agreement between PB1 and tdNEGF once matrix elements are included; quantitative differences arise near hybridization regions and at specific angles where higher-order processes and self-energies are essential. Thus, for systems with simple band structures and away from these regions, the two approaches can be used in a complementary way.
https://arxiv.org/abs/2601.14443Inhalt ausklappen Inhalt einklappen W. Bennecke, T. L. Dinh, J.P. Bange, D. Schmitt, M. Merboldt, L. Weinhagen, B. van W., F. Frassetto, L. Poletto, M. Reutzel, D. Steil, D.R. Luke, S. Mathias, GS Jansen, Table-top three-dimensional photoemission orbital tomography with a femtosecond extreme ultraviolet light source, arXiv:2502.18269 (2025).
Two-dimensional transition metal dichalcogenides (TMDs) and organic semiconductors (OSCs) have emerged as promising material platforms for next-generation optoelectronic devices. The combination of both is predicted to yield emergent properties while retaining the advantages of their individual components. In OSCs the optoelectronic response is typically dominated by localized Frenkel-type excitons, whereas TMDs host delocalized Wannier-type excitons. However, much less is known about the spatial and electronic characteristics of excitons at hybrid TMD/OSC interfaces, which ultimately determine the possible energy and charge transfer mechanisms across the 2D-organic interface. Here, we use ultrafast momentum microscopy and many-body perturbation theory to elucidate a hybrid exciton at an TMD/OSC interface that forms via the ultrafast resonant Förster energy transfer process. We show that this hybrid exciton has both Frenkel- and Wannier-type contributions: Concomitant intra- and interlayer electron-hole transitions within the OSC layer and across the TMD/OSC interface, respectively, give rise to an exciton wavefunction with mixed Frenkel-Wannier character. By combining theory and experiment, our work provides previously inaccessible insights into the nature of hybrid excitons at TMD/OSC interfaces. It thus paves the way to a fundamental understanding of charge and energy transfer processes across 2D-organic heterostructures.
https://arxiv.org/abs/2502.18269, https://arxiv.org/abs/2411.14993