arXiv subjects

Marvin F. Schumacher

Publications and source records attributed to Marvin F. Schumacher.

3 recordsLinked to original sources

arXiv2026

Strong coupling regimes of an organic exciton mirror in a microcavity

The coherent, periodic energy transfer between light- and matter excitations characterizes the strong coupling regime of cavity exciton-polaritons, resulting, in the simplest case, in a Rabi-doublet in the spectral domain. We demonstrate a peculiar regime of strong light-matter coupling, which arises when photonic cavity modes couple to an ultra-thin excitonic mirror. We embed a 12 nm J-aggregated thin film in an open microcavity and tune the coupling strength from weak to the onset of ultrastrong coupling. At resonance, the excitonic mirror selectively changes dielectric to metallic field boundary conditions adding a 2π phase, which links optical cavity modes of different order. Our work gives an exciting perspective to ultra-fast cavity switches and photonic devices based on excitonic optical elements.

cond-mat.mes-hall↗

arXiv2025

Mapping the Optical Landscape of a Squaraine Molecule in the Visible and Ultraviolet Energy Range

Although squaraine dyes are commonly praised as candidates for light-based applications, little is known about their excited state landscape beyond the low-energy visible light region. Our work aims for an improved understanding of the photophysical properties of squaraines at the example of N-isobutyl substituted anilino-squaraine (SQIB) by extending ground-state and excited-state absorption spectroscopy of the molecule into the ultraviolet up to 6.5~eV. In addition, we distinguish the relative transition dipole moments of the excited state absorption peaks with the help of transient absorption anisotropy experiments. To relate experimental features to specific states, we employ a set of ab initio methods including time-dependent density functional theory (TDDFT), the Bethe-Salpeter equation (BSE) and n-electron valence perturbation theory on top of a self-consistent complete active space (CASSCF/NEVPT2). Our assignment is complemented by vibronic simulations and a discussion of two-photon absorption measurements. Through this joint effort, we are able to provide a consistent picture of the optical behavior of SQIB across the visible and ultraviolet light regime, and assign a total of twelve electronically excited states to our experimental data.

physics.chem-ph↗

arXiv2023

Plasmon mediated coherent population oscillations in molecular aggregates

The strong coherent coupling of quantum emitters to vacuum fluctuations of the light field offers opportunities for manipulating the optical and transport properties of nanomaterials, with potential applications ranging from ultrasensitive all-optical switching to creating polariton condensates. Often, ubiquitous decoherence processes at ambient conditions limit these couplings to such short time scales that the quantum dynamics of the interacting system remains elusive. Prominent examples are strongly coupled exciton-plasmon systems, which, so far, have mostly been investigated by linear optical spectroscopy. Here, we use ultrafast two-dimensional electronic spectroscopy to probe the quantum dynamics of J-aggregate excitons collectively coupled to the spatially structured plasmonic fields of a gold nanoslit array. We observe rich coherent Rabi oscillation dynamics reflecting a plasmon-driven coherent exciton population transfer over mesoscopic distances at room temperature. This opens up new opportunities to manipulate the coherent transport of matter excitations by coupling to vacuum fields.

cond-mat.mes-hall↗