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arXiv:2608.28521

Modifying van der Waals Materials via Cavity Vacuum Fluctuations

Mohammad Hassan, Cankut Tasci, Leonardo A. Cunha, Johannes Flick

cond-mat.mtrl-sciphysics.chem-phphysics.opticsquant-phSubmitted Aug 28, 2026• Announced Aug 31, 2026
v1 · Aug 28, 2026v2 · Oct 5, 2026
arXivHTMLPDF

Abstract

In the field of cavity quantum materials, vacuum fluctuations of optical cavities are used for modifying ground-state properties of quantum materials without external driving. Here, one example is the van der Waals (vdW)/dispersion interaction in layered 2D vdW materials, where non-additive long-range correlations can dominate the interlayer binding. While cavity-induced changes of such interactions have been predicted and described using ab initio methods for molecular systems, no efficient description exists yet for extended materials. In this Letter, we close this gap by introducing a periodic formulation of the photon many-body dispersion (pMBD) functional within quantum electrodynamical density-functional theory (QEDFT). Applying this method with efficient $\textbf{q}$-point sampling to bilayer hBN and graphene, we predict cavity-modified stacking, increased equilibrium interlayer distances, and softened layer breathing modes with increasing light-matter coupling strength. Our results establish cavity vacuum fluctuations as a tuning knob for the structural properties of vdW materials.

Comments
6 pages, 2 figures

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In the field of cavity quantum materials, vacuum fluctuations of optical cavities are used for modifying ground-state properties of quantum materials without external driving. Here, one example is the van der Waals (vdW)/dispersion interaction in layered 2D vdW materials, where non-additive long-range correlations can dominate the interlayer binding. While cavity-induced changes of such interactions have been predicted and described using ab initio methods for molecular systems, no efficient description exists yet for extended materials. In this Letter, we close this gap by introducing a periodic formulation of the photon many-body dispersion (pMBD) functional within quantum electrodynamical density-functional theory (QEDFT). Applying this method with efficient q\textbf{q}q-point sampling to bilayer hBN and graphene, we predict cavity-modified stacking, increased equilibrium interlayer distances, and softened layer breathing modes with increasing light-matter coupling strength. Our results establish cavity vacuum fluctuations as a tuning knob for the structural properties of vdW materials.
Summary form only given. The topic of quantum cavity electrodynamics is to describe the coupling between the fluctuations of an atomic system and the vacuum e.m. field, when special boundary conditions are imposed by a cavity to the vacuum field. A realistic description of these boundary conditions is hence of crucial importance. For such a purpose, the unavoidable dispersive spectral properties of any material cavity cannot be ignored when dealing with (temporal) fluctuations. For these reasons, we have embarked on an (experimental) analysis of the resonant long-range coupling between atomic excitation and the surface modes of a cavity (most often restricted to a simple wall, i.e. a flat open cavity). In our present investigations, we are concerned with the exploration of the dissipative counterpart of the resonant atom-surface van der Waals coupling.
We discuss how the presence of two-dimensional (2D) materials, such as graphene, can significantly affect two intrinsically quantum phenomena that have traditionally served as probes of the fundamental van der Waals (VDW) interaction. First, we show theoretically that Quantum Reflection (QR) of slow atoms off attractive VDW potential tails (due to interactions with 2D materials) is very strongly dependent on material characteristics (such as band structure, doping and screening level, etc). Secondly, we analyze manifestations of such 2D effects for many atoms forming a confined Bose-Einstein condensate (BEC) placed near 2D materials, which in turn makes the BEC frequency sensitive to the interface. In both cases we find that relatively small 2D material changes (either by external factors such as strain or doping, or by using gapped 2D materials instead of graphene) can have a profound effect on the above phenomena. In particular, Quantum Reflection at a given energy can experience a significant enhancement or supression (relative to conventionally used bulk materials) making 2D quantum materials an attractive playground for the study of many-body phenomena at the interface of atomic and solid state physics. *This work received support under NASA grant number 80NSSC19M0143.
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, in particular, 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.
Abstract We consider the resonant van der Waals (vdW) interaction between two correlated identical two-level atoms (at least one of which being excited) within the framework of macroscopic cavity quantum electrodynamics in linear, dispersing and absorbing media. The interaction of both atoms with the body-assisted electromagnetic field of the cavity is assumed to be strong. Our time-independent evaluation is based on an extended Jaynes–Cummings model. For a system prepared in a superposition of its dressed states, we derive the general form of the vdW forces, using a Lorentzian single-mode approximation. We demonstrate the applicability of this approach by considering the case of a planar cavity and showing the position dependence of Rabi oscillations. We also show that in the limiting case of weak coupling, our results reproduce the perturbative ones for the case where the field is initially in vacuum state while the atomic state is in a superposition of two correlated states sharing one excitation.
When in a quantum optical system the coupling between matter and cavity mode becomes comparable to the bare excitation frequency, we enter a non-perturbative coupling regime, as perturbation theory fails describing the system’s dynamics. While recent advances in Cavity Quantum Electrodynamics allowed to achieve very high values of the coupling strength, thanks to the resonators properties optimization and the employment of solid-state devices, an ever growing interest has been shown about the possibility of significantly modify materials’ properties. It has been demonstrated that the chemical structure of molecules strongly coupled to a photon mode can be altered, which opens the possibility to manipulate and control chemical reactions. The aim of this thesis is to explore non-perturbative regimes on several quantum systems, and to investigate the effects of the coupling upon their properties, such as internal degrees of freedom or electronic states structure. I first developed a novel theory to determine the polariton spectrum of a dipolar ensamble in which a Ising-like dipole-dipole interaction in the 2 non-perturbative regime is considered. A further important focus is the investigation of the saturation effects due to the inclusion of the inter-dipole interaction, and the interplay between the latter and light-matter coupling strength. I also explored specifically the influence of the coupling on the rotational degrees of freedom of an ensemble of two-dimensional freely rotating dipoles, all coupled to a single cavity mode, finding that they are driven by the collective light-matter coupling to undergo a crossover between an isotropic and an aligned phase. I then investigated the case of cavity-embedded doped quantum wells, demonstrating that not only it is possible to couple a discrete cavity mode and bound-to-continuum transitions, but also that a novel bound exciton state appears, induced by the coupling strength. This results shows how light–matter coupling can be used to tune both optical and electronic properties of semiconductor heterostructures beyond those permitted by mere crystal properties. Finally, I explored the physics of an array of THz metamaterial resonators coupled to cyclotron resonances of a two-dimensional electron gas, developing a multiple-mode theory that takes in account the interaction between multiple photon modes mediated by the electrons. My results show that this cross-interaction, due to the strong two-dimensional geometry of the optically active medium, leads to the hybridization of different uncoupled photon modes, and manifests as a visible change of the distribution of the coupled electromagnetic field.
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 JJJ 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 JJJ, 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 ttt-JJJ 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.