arXiv subjects

Michael Ruggenthaler

Publications and source records attributed to Michael Ruggenthaler.

At least 19 recordsLinked to original sources

arXiv2026

Robustness of quantized Hall resistivity under cavity coupling at zero temperature

Recent experiments have shown that strong light-matter coupling in electromagnetic cavities can modify transport properties of quantum Hall systems through the formation of Landau polaritons, prompting questions about the robustness of topological protection. While earlier theory demonstrated that the Hall conductivity can be modified at finite temperature and finite polariton lifetime (or finite broadening), experiments primarily probe the resistivity tensor. Our phenomenological model reveals an asymmetry between conductivity and resistivity in quantum Hall systems under strong light-matter interaction, showing that at zero temperature the Hall resistivity remains completely immune to cavity-induced modifications arising from polariton broadening, independent of the light-matter coupling strength. These results provide a deeper explanation for the absence of renormalization in the von Klitzing constant in experiments probing the even QH plateaus through the Hall resistivity at low temperature, and clarify the distinct roles of dissipation and strong light-matter coupling in hybrid light-matter systems.

cond-mat.mes-hall↗

arXiv2026

Cavity-mediated localization and collective electron correlation phases

Collective strong coupling of molecular ensembles to optical cavities opens a route to modifying matter through genuinely collective electronic correlations. Yet even in the absence of a cavity, Coulomb correlations are notoriously difficult to describe, and cavity coupling adds transverse correlation channels extending over the entire molecular ensemble. Here we show that this seemingly intractable problem admits a controlled description by spin glass theory, i.e., by the analytically solvable spherical Sherrington-Kirkpatrick model. Our results predict two collective correlation phases, a paracorrelated phase and a spin-glass correlation phase, beyond the conventional uncorrelated molecular regime. These phases reveal an entropy-driven localization-delocalization mechanism that transfers molecular electronic states into collectively degenerate cavity-dressed states. Analytic calculation suggest that this collective correlated state can either remain insulating or even turn metallic if the entropic occupations favor a fractional filling. Our work reveals cavity-mediated electron correlations as a microscopic mechanism for emergent phases in strongly coupled molecular ensembles.

quant-ph↗

arXiv2026

Linear and nonlinear vibrational excitation driven by molecular polaritons

Following our recent numerical study [arXiv:2601.16299 (2026)], we investigate vibrational excitation induced by transient optical driving in molecular ensembles strongly coupled to a cavity mode using the field-driven Holstein--Tavis--Cummings model. We analyze how pulsed excitation redistributes energy among electronic, photonic, and vibrational degrees of freedom in molecular polaritons. Vibrational dynamics are examined over a broad range of pulse durations and intensities within both the single-excitation approximation and a mean-field description of collective light--matter coupling. Despite their distinct formulations and microscopic descriptions, these two approaches yield consistent scaling relations for vibrational excitation. In particular, we disentangle linear and nonlinear contributions to vibrational excitation, which are reflected in distinct quadratic and quartic scaling behaviors with respect to the driving field amplitude (that is, linear and quadratic dependence on the incident pulse intensity). The microscopic origin of the nonlinear component is identified as a polariton-mediated intrapulse stimulated Raman-like process, enabled by a pulse spectral bandwidth large enough to overlap both upper and lower polaritons (rather than a conventional multi-pulse scheme). These results establish a unified framework for understanding vibrational excitation under pulsed polariton driving and provide guidance for the interpretation and control of ultrafast polariton experiments. Discrepancies between the mean-field and single-excitation approaches under certain pulsed conditions are identified and analyzed.

physics.chem-ph↗

arXiv2026

Fluctuation engineering in cavity quantum materials

Coupling tailored electromagnetic fluctuations to materials provides a resource for controlling correlated quantum matter. By structuring the frequency, spatial, and modal distribution of fluctuations through a new generation of cavity quantum materials, vacuum and thermal spectra can shift phase boundaries and stabilize or suppress orders. This review organizes the field around a fluctuation-focused perspective, surveying a practical design toolbox and recent milestones, and outlining theory-experiment challenges in realistic, multimode, beyond-long-wavelength regimes. We highlight photonic observables and map opportunities for equilibrium and driven control across superconducting, magnetic, moire, and topological platforms.

cond-mat.mes-hall↗

arXiv2026

Unified ab initio quantum-electrodynamical density-functional theory for cavity-modified electron-phonon-photon coupling in solids

Quantum-electrodynamical density-functional theory (QEDFT) provides a first-principles framework for describing materials coupled to quantized electromagnetic fields. While QEDFT has successfully captured cavity-induced modifications of electronic structures in atoms and molecules, a fully self-consistent and accurate framework to simulate and predict the structural, phonon-related, polarization and optical response of periodic solids in optical cavities has remained elusive. Here, we introduce a unified QEDFT approach that combines collective light-matter coupling parameter in the electronic ground state, density functional perturbation theory for phonons, and real-time time-dependent QEDFT for optical excitations. This framework enables ab initio calculations of cavity-modified electronic and phononic dispersions, Born effective charges, dielectric tensors, and both resonant and non-resonant optical absorption spectra. Using wurtzite gallium nitride (GaN) in an optical cavity as a case study, we demonstrate that the quantized vacuum field reshapes electronic, phononic and polarization properties, producing experimentally accessible signatures in the dielectric function and absorption spectra. These results establish QEDFT as a general first-principles platform for predicting and exploring cavity-modified quantum materials.

cond-mat.mtrl-sci↗

arXiv2026

Cavity Control of Strongly Correlated Electrons Beyond Resonant Coupling

Interfacing materials with electromagnetic cavities offers a route to modify equilibrium properties through structured vacuum fluctuations. The coupling between light and correlated electrons lacks a characteristic energy scale, making vacuum induced ground state modifications of such systems inherently off-resonant and sensitive to the full photon mode structure. We develop a consistent cavity-QED formalism for dispersive electromagnetic environments in the Coulomb gauge, capturing both dynamical dressing via the vector potential and static screening by the dielectric. With this formalism, we perform a non-perturbative study of the cavity-induced modification of magnetism in the Hubbard model close to half-filling, including all cavity modes and with parameters determined from first principles. At half-filling, we show that the modification of the magnetic exchange interaction $J$ is controlled by a generalized Purcell factor, proportional to the frequency integrated photonic density of states relative to free space. This result identifies polaritonic surface cavities as promising platforms to modify correlated systems. For the surface cavity a competition between static screening and dynamical dressing via the vector potential leads to a net enhancement of $J$, directly observable in two-magnon Raman spectroscopy. The inclusion of screening is essential to obtain even qualitatively correct results. At weak doping, a variational exact diagonalization of the cavity-coupled $t$-$J$ polaron reveals that a low-frequency surface cavity can reverse the nodal-antinodal dichotomy of the bare polaron dispersion. This effect lies beyond mean field theory and is observable via ARPES measurements. Our framework establishes a concrete design principle linking cavity geometry to material response in the off-resonant regime, which will guide future experimental and theoretical explorations.

quant-ph↗

arXiv2026

Collective Rabi-driven vibrational activation in molecular polaritons

Molecular polaritons arise from electronic or vibrational strong coupling (ESC and VSC) with confined electromagnetic fields. While these have been widely studied, the influence of electron-nuclear dynamics in driven cavities remains largely unknown. Here, we report a previously unrecognized mechanism of vibrational activation that emerges under collective ESC in driven optical cavities. Using simulations that self-consistently combine Maxwell's equations with quantum molecular dynamics, we show that collective electronic Rabi oscillations coherently drive nuclear motion. This effect is captured using both vibrational wave-packet dynamics in a minimal two-level model and atomistic simulations based on time-dependent density-functional tight-binding theory. Vibrational activation depends non-monotonically on the Rabi frequency and is maximized when the collective polaritonic splitting resonates with a molecular vibrational mode. The mechanism exhibits features consistent with a stimulated Raman-like relaxation mechanism. Our predictions are robust under realistic cavity conditions and provide the conditions in which they could be verified experimentally.

physics.comp-ph↗

arXiv2025

Testing electron-photon exchange-correlation functional performance for many-electron systems under weak and strong light-matter coupling

We present results of a photon-free exchange-correlation functional within the local density approximation (pxcLDA) for quantum electrodynamics density functional theory (QEDFT) that efficiently describes the electron density of many-electron systems across weak to strong light-matter coupling. Building on previous work [I-Te. Lu et al., Phys. Rev. A 109, 052823 (2024)] that captured electron-photon correlations via an exchange-correlation functional derived from the nonrelativistic Pauli-Fierz Hamiltonian and tested on one-electron systems, we use a simple procedure to compute a renormalization factor describing electron-photon correlations and inhomogeneity in the weak-coupling regime by comparing it with quantum electrodynamics coupled-cluster, and previous QEDFT optimized effective potential methods. Across various atoms and molecules, pxcLDA reproduces cavity-modified densities in close agreement with these references. The renormalization factor approaches unity as the system size or collective coupling increases, reflecting an electron-photon exchange-dominated behavior and improved accuracy for larger systems. This approach now offers a practical route to applying QEDFT functionals based on electron density to realistic electron systems.

quant-ph↗

arXiv2025

Multimode equilibrium approximations in light-matter systems from weak to strong coupling

In this work, we detail different approaches to treat multi-mode photonic environments within non-relativistic quantum electrodynamics in the long-wavelength approximation efficiently. Specifically we show that for equilibrium properties of coupled light-matter systems, we can approximately capture the effects of multi-mode photonic environments on matter systems by either only keeping the polarization part of the electric field in the length-gauge formulation or by a few effective modes. We present a comprehensive set of approximation methods designed to accurately capture equilibrium phenomena in quantum light-matter systems across a range of complex photonic environments, from weak to strong coupling. These methods are applied to atomic and molecular models as well as to a two-dimensional quantum ring, demonstrating the versatility of our approach and laying the groundwork for first-principles simulations of real materials in cavity quantum electrodynamics.

quant-ph↗

arXiv2025

Density-Functional Tight Binding Meets Maxwell: Unraveling the Mysteries of (Strong) Light-Matter Coupling Efficiently

Controlling chemical and material properties through strong light-matter coupling in optical cavities has gained considerable attention over the past decade. However, the underlying mechanisms remain insufficiently understood, and a significant gap persists between experimental observations and theoretical descriptions. This challenge arises from the intrinsically multi-scale nature of the problem, where non-perturbative feedback occurs across different spatial and temporal scales. Collective coupling between a macroscopic ensemble of molecules and a photonic environment, such as Fabry-Perot cavity, can strongly influence the microscopic properties of individual molecules, while microscopic details of the ensemble in turn affect the macroscopic coupling. To address this complexity, we present an efficient computational framework that combines density-functional tight binding (DFTB) with finite-difference time-domain (FDTD) simulations for Maxwell's equations (DFTB+Maxwell). This approach allows for a self-consistent treatment of both the cavity and microscopic details of the molecular ensemble. We demonstrate the potential for this method by tackling several open questions. First, we calculate non-perturbatively two-dimensional spectroscopic observable that directly connect to well-established experimental protocols. Second, we provide local, molecule-resolved information within collectively coupled ensembles, which is difficult to obtain experimentally. Third, we show how cavity designs can be optimized to target specific microscopic applications. Finally, we outline future directions to enhance the predictive power of this framework, including extension to finite temperature, condensed phases, and correlated quantum effects.

physics.chem-ph↗

arXiv2025

Molecular polariton dynamics in realistic cavities

The large number of degrees of freedom involved in polaritonic chemistry processes considerably restricts the systems that can be described by any ab initio approach, due to the resulting high computational cost. Semiclassical methods that treat light classically offer a promising route for overcoming these limitations. In this work, we present a new implementation that combines the numerical propagation of Maxwell's equations to simulate realistic cavities with quantum electron dynamics at the density functional tight-binding (DFTB) theory level. This implementation allows for the simulation of a large number of molecules described at the atomistic level, interacting with cavity modes obtained by numerically solving Maxwell's equations. By mimicking experimental setups, our approach enables the calculation of transmission spectra, in which we observe the corresponding polaritonic signals. In addition, we have access to local information, revealing complex responses of individual molecules that depend on the number, geometry, position, and orientation of the molecules inside the cavity.

physics.comp-ph↗

arXiv2025

v-Representability on a one-dimensional torus at elevated temperatures

We extend a previous result [Sutter et al., J. Phys. A: Math. Theor. 57, 475202 (2024)] to give an explicit form of the set of $v$-representable densities on the one-dimensional torus with any fixed number of particles in contact with a heat bath at finite temperature. The particle interaction has to satisfy some mild assumptions but is kept entirely general otherwise. For densities, we consider the Sobolev space $H^1$ and exploit the convexity of the functionals. This leads to a broader set of potentials than the usual $L^p$ spaces and encompasses distributions. By including temperature and thus considering all excited states in the Gibbs ensemble, G\^ateaux differentiability of the thermal universal functional is guaranteed. This yields $v$-representability and it is demonstrated that the given set of $v$-representable densities is even maximal.

math-ph↗

arXiv2025

Linear-Response Quantum-Electrodynamical Density Functional Theory Based on Two-Component X2C Hamiltonians

Linear-response quantum electrodynamical density functional theory (QEDFT) enables the description of molecular spectra under strong coupling to quantized photonic modes, such as those in optical cavities. Recently, this approach was extended to the relativistic domain using the four-component Dirac-Coulomb Hamiltonian. To provide a computationally efficient yet accurate alternative-particularly for modeling 2D spectra or collective coupling for large, heavy-element systems-this article introduces a two-component linear-response QEDFT method based on exact two-component (X2C) Hamiltonian models. We derive how the parent four-component Hamiltonian for coupled electron-photon systems undergoes the X2C transformation. Moreover, we show that, under common weak-field and dipole approximations, it suffices to apply the X2C transformation only during the ground-state self-consistent field procedure, with the subsequent calculations performed fully in the two-component regime using the same X2C decoupling matrix. The current implementation includes the atomic mean-field (amfX2C), extended atomic mean-field (eamfX2C), and molecular mean-field (mmfX2C) Hamiltonian models. Benchmark calculations demonstrate that the X2C approach closely reproduces reference four-component results, enabling us to efficiently tackle systems that would be otherwise computationally too expensive. As applications, we compute 2D spectra of a mercury porphyrin complex in a Fabry-Perot cavity, demonstrating off-resonant coupling and the appearance of multiple polaritonic branches. We also study a chain of AuH molecules, showing that collective coupling can locally modify chemical properties of a molecule with a perturbed bond length.

physics.chem-ph↗

arXiv2025

Local-density correlation functional from the force-balance equation

The force-balance equation of time-dependent density-functional theory presents a promising route towards obtaining approximate functionals, however, so far, no practical correlation functionals have been derived this way. In this work, starting from a correlated wavefunction proposed originally by Colle and Salvetti [Theoret. Chim. Acta 37, 329 (1975)], we derive an analytical correlation-energy functional for the ground state based on the force-balance equation. The new functional is compared to the local-density correlation of the homogeneous electron gas and we find an increased performance for atomic systems, while it performs slightly worse on solids. From this point onward, the new force-based correlation functional can be systematically improved.

physics.chem-ph↗

arXiv2025

Cavity engineering of solid-state materials without external driving

Confining electromagnetic fields inside an optical cavity can enhance the light-matter coupling between quantum materials embedded inside the cavity and the confined photon fields. When the interaction between the matter and the photon fields is strong enough, even the quantum vacuum field fluctuations of the photons confined in the cavity can alter the properties of the cavity-embedded solid-state materials at equilibrium and room temperature. This approach to engineering materials with light avoids fundamental issues of laser-induced transient matter states. To clearly differentiate this field from phenomena in driven systems, we call this emerging field cavity materials engineering. In this review, we first present theoretical frameworks, especially, ab initio methods, for describing light-matter interactions in solid-state materials embedded inside a realistic optical cavity. Next, we overview a few experimental breakthroughs in this domain, detailing how the ground state properties of materials can be altered within such confined photonic environments. Moreover, we discuss state-of-the-art theoretical proposals for tailoring material properties within cavities. Finally, we outline the key challenges and promising avenues for future research in this exciting field.

cond-mat.mtrl-sci↗

arXiv2025

The 2025 Roadmap to Ultrafast Dynamics: Frontiers of Theoretical and Computational Modelling

The exploration of ultrafast phenomena is a frontier of condensed matter research, where the interplay of theory, computation, and experiment is unveiling new opportunities for understanding and engineering quantum materials. With the advent of advanced experimental techniques and computational tools, it has become possible to probe and manipulate nonequilibrium processes at unprecedented temporal and spatial resolutions, providing insights into the dynamical behavior of matter under extreme conditions. These capabilities have the potential to revolutionize fields ranging from optoelectronics and quantum information to catalysis and energy storage. This Roadmap captures the collective progress and vision of leading researchers, addressing challenges and opportunities across key areas of ultrafast science. Contributions in this Roadmap span the development of ab initio methods for time-resolved spectroscopy, the dynamics of driven correlated systems, the engineering of materials in optical cavities, and the adoption of FAIR principles for data sharing and analysis. Together, these efforts highlight the interdisciplinary nature of ultrafast research and its reliance on cutting-edge methodologies, including quantum electrodynamical density-functional theory, correlated electronic structure methods, nonequilibrium Green's function approaches, quantum and ab initio simulations.

cond-mat.mtrl-sci↗

arXiv2024

Quantum-Electrodynamical Density-Functional Theory Exemplified by the Quantum Rabi Model

The key features of density-functional theory (DFT) within a minimalistic implementation of quantum electrodynamics are demonstrated, thus allowing to study elementary properties of quantum-electrodynamical density-functional theory (QEDFT). We primarily employ the quantum Rabi model, that describes a two-level system coupled to a single photon mode, and also discuss the Dicke model, where multiple two-level systems couple to the same photon mode. In these settings, the density variables of the system are the polarization and the displacement of the photon field. We give analytical expressions for the constrained-search functional and the exchange-correlation potential and compare to established results from QEDFT. We further derive a form for the adiabatic connection that is almost explicit in the density variables, up to only a non-explicit correlation term that gets bounded both analytically and numerically. This allows several key features of DFT to be studied without approximations.

quant-ph↗

arXiv2024

Surface-mediated ultra-strong cavity coupling of two-dimensional itinerant electrons

Engineering phases of matter in cavities requires effective light-matter coupling strengths that are on the same order of magnitude as the bare system energetics, coined the ultra-strong coupling regime. For models of itinerant electron systems, which do not have discrete energy levels, a clear definition of this regime is outstanding to date. Here we argue that a change of the electronic mass exceeding $10\%$ of its bare value may serve as such a definition. We propose a quantitative computational scheme for obtaining the electronic mass in relation to its bare vacuum value and show that coupling to surface polariton modes can induce such mass changes. Our results have important implications for cavity design principles that enable the engineering of electronic properties with quantum light.

cond-mat.str-el↗