arXiv subjects

Michael Reitz

Publications and source records attributed to Michael Reitz.

18 recordsLinked to original sources

arXiv2026

Full-wave nonlinear microscopy reveals guided channel for ultrafast polariton transport

We show how finite-difference time-domain (FDTD) simulations can be extended to model ultrafast nonlinear microscopy, enabling the prediction of spatially-resolved pump--probe signals in arbitrary electromagnetic environments. Focusing on polariton transport in strongly coupled light--matter systems, we develop a perturbative framework to study the ultrafast propagation of hybrid light--matter excitations in nanophotonic structures. We first apply the framework to a standard distributed Bragg reflector (DBR) cavity, reproducing established results for polariton transport from a multimode Tavis--Cummings model. We then consider the full modal landscape of the same cavity, including guided modes below the light line that are typically neglected in single-mode-family descriptions. Exploiting these modes, we design compact mode converters that transfer radiative cavity polaritons into photon-like guided polaritons and back, utilizing the guided modes for low-loss propagation. Despite molecular dephasing, this enables transport of molecular excitation over a millimeter, an order of magnitude beyond current transport experiments. We further compute the pump--probe differential transmission signal, providing an experimental signature of the mechanism. Our results show that the modal landscape of a photonic cavity can be engineered to bypass limitations commonly assumed to be intrinsic to the transport of molecular polaritons.

quant-ph↗

arXiv2026

Multidimensional semiclassical single- and double-quantum spectroscopy of anharmonic molecular polaritons

We present a general and efficient approach to compute phase-resolved multidimensional spectra of anharmonic molecular polaritons, based on a semiclassical evolution of the molecular Hamiltonian and cavity field in the large-$\mathcal{N}$ limit of many molecules coupled to a confined photonic mode. By systematically expanding the response in both amplitudes and phases of the input fields, our method enables a transparent and computationally simple construction of phase-cycled two-dimensional single- and double-quantum polariton spectra from the underlying nonlinear signal components. Here, phase cycling acts as an analogue of phase matching with oblique pulses, allowing for the isolation of the contributing nonlinear pathways in Liouville space. We specialize to vibrational polaritons and benchmark the method through direct comparison with experimentally measured single-quantum spectra, providing an explanation for the longstanding puzzle of the polariton bleach effect observed at short waiting times. Further, we show how the imprint of various types of anharmonicities on the double-excitation manifold can be directly probed and analyzed through double-quantum coherence spectroscopy. Taken together, our results establish a practical and powerful framework for the modeling and interpretation of nonlinear spectroscopic experiments on strongly coupled light-matter platforms and for guiding the design of cavity-enhanced molecular platforms.

quant-ph↗

arXiv2026

Dynamical Drexhage Effect: Amplified Emission in Time-Modulated Electromagnetic Environments

We investigate the effect of nonrelativistic motion on the emission dynamics of a dipole emitter moving next to a reflecting interface. Within the formalism of macroscopic QED, we obtain a general equation of motion for the dipole amplitude in terms of the dyadic Green's function, yielding a dynamical extension of the Drexhage effect. At short dipole-surface distances, the dipole can be described as a parametric oscillator featuring time-dependent dampings and Lamb shifts, both arising from the self-induced modulation of the surrounding electromagnetic environment. Importantly, these time-dependent parameters do not always average out, leading to amplification of the dipole amplitude and the radiated intensity when considering certain sinusoidal trajectories with specific modulation amplitudes and frequencies. We derive threshold modulation amplitudes as function of the relative permittivities at the interface. Qualitatively, in the vicinity of certain epsilon-near-zero materials, amplification is possible purely by modulation of the damping. Our findings open up avenues for the dynamic control of light-matter interaction in nanophotonic environments.

physics.optics↗

arXiv2025

Towards coherent polaritonic circuits operating at room temperature

Polariton condensation is a potential system state for performing analog computations, given that it exhibits quantum behavior at macroscopic scales readily probed with low-cost optical methods. Current methods of fabricating devices in polariton microcavities largely involve patterning the devices via e-beam lithography before the cavity is completed, which offers less flexibility in device creation and reduces the maximum possible refractive index contrast. Moreover, the momentum and spatial distributions of the condensate are highly dependent on the host platform, and it has been difficult to preserve the desired behavior when modifying a given cavity. Here we introduce a method that addresses both of these challenges with the creation of polaritonic circuits of arbitrary forms etched via Focused Ion Beam into an organic microcavity based on Rhodamine 3B Perchlorate within a Small Molecule Ionic Isolation Lattices complex. We demonstrate room temperature condensation and propagation of polaritons in rectangular and trapezoidal waveguides by analyzing spatial and angle-resolved photoluminescence. We also discuss the blue-shifting and non-zero momentum of the condensate and show that it is strongly confined up to several higher energy levels. As an example, we report the spatial profiles of condensation in custom devices, such as a ring waveguide, a Y-splitter, and a Mach-Zehnder interferometer. This work represents a first step towards the realization of more complex, fully integrated, coherent polaritonic circuits operating at room temperature.

physics.optics↗

arXiv2025

Mapping molecular polariton transport via pump-probe microscopy

We demonstrate how the transport properties of molecular polaritons in optical cavities can be extracted from a microscopic modeling of pump-probe spectroscopy. Our approach combines a mean-field treatment of the light-matter Hamiltonian with a perturbative expansion of both light and matter components, along with spatial coarse-graining. This approach extends semiclassical cavity spectroscopy to multimode light-matter interactions, providing full access to spatially resolved transient spectra. By simulating a microscopy experiment with counter-propagating pump and probe pulses, we compute the differential transmission and show how molecular dephasing and persistent dark exciton populations drive sub-group-velocity transport of the root-mean-square displacement. We analyze transport across the polariton dispersion, showing how velocity renormalization correlates with excitonic weight, consistent with experimental observations, and further its dependence on the rate of molecular dephasing. Our results highlight the need to consider measured spectroscopic observables when characterizing transport in polaritonic systems.

quant-ph↗

arXiv2025

Quantum theory of surface lattice resonances

The collective interactions of nanoparticles arranged in periodic structures give rise to high-$Q$ in-plane diffractive modes known as surface lattice resonances. While these resonances and their broader implications have been extensively studied within the framework of classical electrodynamics and linear response theory, a quantum optical theory capable of describing the dynamics of these structures, especially in the presence of material nonlinearities beyond \textit{ad hoc} few-mode approximations, is largely missing. To this end, we consider a lattice of metallic nanoparticles coupled to the electromagnetic field and derive the quantum input--output relations within the electric dipole approximation. As applications, we analyze coupling between the nanoparticle array and external quantum emitters, and show how the formalism extends to molecular optomechanics, where the high $Q$-factors of SLRs enable coupling to collective vibrational modes. We further consider arrays composed of saturable excitonic emitters, demonstrating how emitter nonlinearities can be used to switch the SLR condition between electronic transitions. Using a perturbative approach that accounts for population dynamics, we show how these effects can be probed in pump--probe experiments and give rise to nonlinear phase-matching phenomena. Our work provides a microscopic framework for modeling SLRs interacting with quantum emitters without phenomenological descriptions of the electromagnetic environment.

quant-ph↗

arXiv2024

Nonlinear semiclassical spectroscopy of ultrafast molecular polariton dynamics

We introduce a theoretical framework that allows for the systematic and efficient description of the ultrafast nonlinear response of molecular polaritons, i.e., hybrid light-matter states, in the collective regime of large numbers of molecules $\mathcal N$ coupled to the cavity photon mode. Our approach is based on a semiclassical, mean-field evolution of the molecular Hamiltonian and the cavity field, which is complemented by a perturbative expansion of both light and matter counterparts in the input fields entering the cavity. In addition, expansion in terms of the pulse phases enables us to disentangle different excitation pathways in Liouville space, thereby distinguishing contributions to the nonlinear response. The formalism extends traditional free-space nonlinear spectroscopy by incorporating the feedback of matter onto the light field via the induced polarization. We demonstrate the utility of the framework by applying it to the calculation of pump-probe polariton spectra and show how, by storing the pulses, the cavity facilitates additional excitation pathways, which can be used to isolate purely bright state contributions. Our method, which does not scale with $\mathcal N$, is broadly applicable and can be extended to model a wide range of current experiments investigating the dynamical nonlinear response of hybrid light-matter states.

quant-ph↗

arXiv2023

Metasurface-based hybrid optical cavities for chiral sensing

Quantum metasurfaces, i.e., two-dimensional subwavelength arrays of quantum emitters, can be employed as mirrors towards the design of hybrid cavities, where the optical response is given by the interplay of a cavity-confined field and the surface modes supported by the arrays. We show that, under external magnetic field control, stacked layers of quantum metasurfaces can serve as helicity-preserving cavities. These structures exhibit ultranarrow resonances and can enhance the intensity of the incoming field by orders of magnitude, while simultaneously preserving the handedness of the field circulating inside the resonator, as opposed to conventional cavities. The rapid phase shift in the cavity transmission around the resonance can be exploited for the sensitive detection of chiral scatterers passing through the cavity. We discuss possible applications of these resonators as sensors for the discrimination of chiral molecules.

quant-ph↗

arXiv2023

Hybrid THz architectures for molecular polaritonics

Physical and chemical properties of materials can be modified by a resonant optical mode. Such recent demonstrations have mostly relied on a planar cavity geometry, others have relied on a plasmonic resonator. However, the combination of these two device architectures have remained largely unexplored, especially in the context of maximizing light-matter interactions. Here, we investigate several schemes of electromagnetic field confinement aimed at facilitating the collective coupling of a localized photonic mode to molecular vibrations in the terahertz region. The key aspects are the use of metasurface plasmonic structures combined with standard Fabry-Perot configurations and the deposition of a thin layer of glucose, via a spray coating technique, within a tightly focused electromagnetic mode volume. More importantly, we demonstrate enhanced vacuum Rabi splittings reaching up to 200 GHz when combining plasmonic resonances, photonic cavity modes and low-energy molecular resonances. Furthermore, we demonstrate how a cavity mode can be utilized to enhance the zero-point electric field amplitude of a plasmonic resonator. Our study provides key insight into the design of polaritonic platforms with organic molecules to harvest the unique properties of hybrid light-matter states.

physics.optics↗

arXiv2022

Linear optical elements based on cooperative subwavelength emitter arrays

We describe applications of two-dimensional subwavelength quantum emitter arrays as efficient optical elements in the linear regime. For normally incident light, the cooperative optical response, stemming from emitter-emitter dipole exchanges, allows the control of the array's transmission, its resonance frequency, and bandwidth. Operations on fully polarized incident light, such as generic linear and circular polarizers as well as phase retarders can be engineered and described in terms of Jones matrices. Our analytical approach and accompanying numerical simulations identify optimal regimes for such operations and reveal the importance of adjusting the array geometry and of the careful tuning of the external magnetic fields amplitude and direction.

quant-ph↗

arXiv2022

Cooperative subwavelength molecular quantum emitter arrays

Dipole-coupled subwavelength quantum emitter arrays respond cooperatively to external light fields as they may host collective delocalized excitations (a form of excitons) with super- or subradiant character. Deeply subwavelength separations typically occur in molecular ensembles, where in addition to photon-electron interactions, electron-vibron couplings and vibrational relaxation processes play an important role. We provide analytical and numerical results on the modification of super- and subradiance in molecular rings of dipoles including excitations of the vibrational degrees of freedom. While vibrations are typically considered detrimental to coherent dynamics, we show that molecular dimers or rings can be operated as platforms for the preparation of long-lived dark superposition states aided by vibrational relaxation. In closed ring configurations, we extend previous predictions for the generation of coherent light from ideal quantum emitters to molecular emitters, quantifying the role of vibronic coupling onto the output intensity and coherence.

quant-ph↗

arXiv2021

Cooperative quantum phenomena in light-matter platforms

Quantum cooperativity is evident in light-matter platforms where quantum emitter ensembles are interfaced with confined optical modes and are coupled via the ubiquitous electromagnetic quantum vacuum. Cooperative effects can find applications, among other areas, in topological quantum optics, in quantum metrology or in quantum information. This tutorial provides a set of theoretical tools to tackle the behavior responsible for the onset of cooperativity by extending open quantum system dynamics methods, such as the master equation and quantum Langevin equations, to electron-photon interactions in strongly coupled and correlated quantum emitter ensembles. The methods are illustrated on a wide range of current research topics such as the design of nanoscale coherent light sources, highly-reflective quantum metasurfaces or low intracavity power superradiant lasers. The analytical approaches are developed for ensembles of identical two-level quantum emitters and then extended to more complex systems where frequency disorder or vibronic couplings are taken into account. The relevance of the approach ranges from atoms in optical lattices to quantum dots or molecular systems in solid-state environments.

quant-ph↗

arXiv2020

Floquet engineering of molecular dynamics via infrared coupling

We discuss Floquet engineering of dissipative molecular systems through periodic driving of an infrared-active vibrational transition, either directly or via a cavity mode. Following a polaron quantum Langevin equations approach, we derive correlation functions and stationary quantities showing strongly modified optical response of the infrared-dressed molecule. The coherent excitation of molecular vibrational modes, in combination with the modulation of electronic degrees of freedom due to vibronic coupling can lead to both enhanced vibronic coherence as well as control over vibrational sideband amplitudes. The additional coupling to an infrared cavity allows for the controlled suppression of undesired sidebands, an effect stemming from the Purcell enhancement of vibrational relaxation rates.

quant-ph↗

arXiv2020

Molecular polaritonics in dense mesoscopic disordered ensembles

We study the dependence of the vacuum Rabi splitting (VRS) on frequency disorder, vibrations, near-field effects and density in molecular polaritonics. In the mesoscopic limit, static frequency disorder alone can already introduce a loss mechanism from polaritonic states into a dark state reservoir, which we quantitatively describe, providing an analytical scaling of the VRS with the level of disorder. Disorder additionally can split a molecular ensemble into donor-type and acceptor-type molecules and the combination of vibronic coupling, dipole-dipole interactions and vibrational relaxation induces an incoherent FRET (F\"{o}rster resonance energy transfer) migration of excitations within the collective molecular state. This is equivalent to a dissipative disorder and has the effect of saturating and even reducing the VRS in the mesoscopic, high-density limit. Overall, this analysis allows to quantify the crucial role played by dark states in cavity quantum electrodynamics with mesoscopic, disordered ensembles.

quant-ph↗

arXiv2019

Molecule-photon interactions in phononic environments

Molecules constitute compact hybrid quantum optical systems that can interface photons, electronic degrees of freedom, localized mechanical vibrations and phonons. In particular, the strong vibronic interaction between electrons and nuclear motion in a molecule resembles the optomechanical radiation pressure Hamiltonian. While molecular vibrations are often in the ground state even at elevated temperatures, one still needs to get a handle on decoherence channels associated with phonons before an efficient quantum optical network based on opto-vibrational interactions in solid-state molecular systems could be realized. As a step towards a better understanding of decoherence in phononic environments, we take here an open quantum system approach to the non-equilibrium dynamics of guest molecules embedded in a crystal, identifying regimes of Markovian versus non-Markovian vibrational relaxation. A stochastic treatment based on quantum Langevin equations predicts collective vibron-vibron dynamics that resembles processes of sub- and superradiance for radiative transitions. This in turn leads to the possibility of decoupling intramolecular vibrations from the phononic bath, allowing for enhanced coherence times of collective vibrations. For molecular polaritonics in strongly confined geometries, we also show that the imprint of opto-vibrational couplings onto the emerging output field results in effective polariton cross-talk rates for finite bath occupancies.

quant-ph↗

arXiv2018

Langevin Approach to Quantum Optics with Molecules

We investigate the interaction between light and molecular systems modeled as quantum emitters coupled to a multitude of vibrational modes via a Holstein-type interaction. We follow a quantum Langevin equations approach that allows for analytical derivations of absorption and fluorescence profiles of molecules driven by classical fields or coupled to quantized optical modes. We retrieve analytical expressions for the modification of the radiative emission branching ratio in the Purcell regime and for the asymmetric cavity transmission associated with dissipative cross-talk between upper and lower polaritons in the strong coupling regime. We also characterize the F\"{o}rster resonance energy transfer process between donor-acceptor molecules mediated by the vacuum or by a cavity mode.

quant-ph↗

arXiv2018

Enhanced collective Purcell effect of coupled quantum emitter systems

Cavity-embedded quantum emitters show strong modifications of free space radiation properties such as an enhanced decay known as the Purcell effect. The central parameter is the cooperativity $C$, the ratio of the square of the coherent cavity coupling strength over the product of cavity and emitter decay rates. For a single emitter, $C$ is independent of the transition dipole moment and dictated by geometric cavity properties such as finesse and mode waist. In a recent work [Phys. Rev. Lett. 119, 093601 (2017)] we have shown that collective excitations in ensembles of dipole-dipole coupled quantum emitters show a disentanglement between the coherent coupling to the cavity mode and spontaneous free space decay. This leads to a strong enhancement of the cavity cooperativity around certain collective subradiant antiresonances. Here, we present a quantum Langevin equations approach aimed at providing results beyond the classical coupled dipoles model. We show that the subradiantly enhanced cooperativity imprints its effects onto the cavity output field quantum correlations while also strongly increasing the cavity-emitter system's collective Kerr nonlinear effect.

quant-ph↗

arXiv2018

Energy transfer and correlations in cavity-embedded donor-acceptor configurations

The rate of energy transfer in donor-acceptor systems can be manipulated via the common interaction with the confined electromagnetic modes of a micro-cavity. We analyze the competition between the near-field short range dipole-dipole energy exchange processes and the cavity mediated long-range interactions in a simplified model consisting of effective two-level quantum emitters that could be relevant for molecules in experiments under cryogenic conditions. We find that free-space collective incoherent interactions, typically associated with sub- and superradiance, can modify the traditional resonant energy transfer scaling with distance. The same holds true for cavity-mediated collective incoherent interactions in a weak-coupling but strong-cooperativity regime. In the strong coupling regime, we elucidate the effect of pumping into cavity polaritons and analytically identify an optimal energy flow regime characterized by equal donor/acceptor Hopfield coefficients in the middle polariton. Finally we quantify the build-up of quantum correlations in the donor-acceptor system via the two-qubit concurrence as a measure of entanglement.

quant-ph↗