arXiv subjects

Hugo Levy-Falk

Publications and source records attributed to Hugo Levy-Falk.

4 recordsLinked to original sources

arXiv2026

Breakdown of the optical saturation regime in molecular single-photon emitters

Solid-state single organic molecules, such as dibenzoterrylene (DBT) in organic matrices, are prominent deterministic single-photon sources, usually modeled as effective two-level systems (TLS). We show that single DBT molecules in anthracene nanocrystals, under strong continuous-wave driving, depart from this picture: instead of the expected saturation, fluorescence is strongly suppressed at high resonant pump power, while the linewidth broadens beyond the TLS prediction -- an \emph{anomalous saturation} regime. Comparing coherent and incoherent excitation and independently calibrating temperature via phonon-induced dephasing rules out laser-induced heating and intersystem crossing. Instead, a model of intensity-dependent excited-state absorption (ESA) toward a short-lived dark state quantitatively reproduces both the fluorescence suppression and the linewidth broadening. We further show that matrix quality mitigates this quenching, and that pulsed excitation schemes are strategic toward full population inversion, with direct implications for quantum nanophotonics and molecular optomechanics.

quant-ph↗

arXiv2026

Lattice quantum electrodynamics of a molecular emitter in a topological gap

Engineering the photonic environment using lattices of coupled resonators, which we refer to as lattice quantum electrodynamics (QED), provides a route to control both the spontaneous emission of individual quantum emitters and the photon-mediated interactions between them. Here we introduce an optical lattice QED platform based on individual dibenzoterrylene (DBT) molecules embedded in anthracene crystals and coupled to lattices of open optical microcavities. This hybrid architecture benefits from narrow-linewidth molecular emitters, site-resolved optical access, engineered coupled-resonator bands, and compatibility with established molecular frequency-tuning techniques. As a proof-of-principle demonstration, we observe emitter-photon bound states formed when the optical transition of a single molecule is tuned to the band gap of a Su-Schrieffer-Heeger (SSH) cavity lattice. These in-gap states display directional localization and photon emission on a single sublattice, inherited from the vacancy-induced topological edge modes of the underlying SSH lattice. Our results establish open-cavity lattices coupled to DBT molecules as a versatile architecture for engineering many-emitter quantum optical systems with controllable photon-mediated interactions.

quant-ph↗

arXiv2025

Collective Fluorescence of Graphene Quantum Dots on a surface

This study explores the organization of graphene quantum dots on the surface of monocrystalline halide perovskite. We show that graphene quantum dots tends to aggregate on the surface of perovskite unlike in solution or on other substrates, even at very low concentration of the initial solution that should yield single-molecule samples. Spectral analysis on small clusters shows a back-and-forth dynamical transition between an uncoupled, monomer-like state, and an excimer state. Following this "dance" between states, a drastic one-way increase in fluorescence intensity combined with a shortening of the excited state lifetime has been observed on some clusters. This behavior is related to the emission of a collective state that may be a consequence of the dynamical organization of graphene quantum dots under illumination on the surface of the perovksite.

cond-mat.mes-hall↗

arXiv2025

Hybrid interfaces at the single quantum level in fluorescent molecules

We theoretically investigate a single fluorescent molecule as a hybrid quantum optical device, in which multiple external laser sources exert control of the vibronic states. In the high-saturation regime, a coherent interaction is established between the vibrational and electronic degrees of freedom, and molecules can simulate several cavity QED models, whereby a specific vibrational mode plays the role of the cavity mode. Focusing on the specific example where the system is turned into an analogue simulator of the quantum Rabi model, the steady state exhibits vibrational bi-modality resulting in a statistical mixture of highly non-classical vibronic cat states. Applying our paradigm to molecules with prominent spatial asymmetry and combining an optical excitation with a THz(IR) driving, the system can be turned into a single photon transducer. Two possible implementations are discussed based on the coupling to a subwavelength THz patch antenna or a resonant metamaterial. In a nutshell, this work assesses the role of molecules as an optomechanical quantum toolbox for creating hybrid entangled states of electrons, photons, and vibrations, hence enabling frequency conversion over very different energy scales.

quant-ph↗