arXiv subjects

Johannes Flick

Publications and source records attributed to Johannes Flick.

At least 19 recordsLinked to original sources

arXiv2026

Modifying van der Waals Materials via Cavity Vacuum Fluctuations

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.

cond-mat.mtrl-sci↗

arXiv2026

Engineering molecular potential energy surfaces using magnetic cavity quantum electrodynamics

We investigate the effects of coupling a quantum-magnetic cavity field to molecules. Our high-precision auxiliary-field quantum Monte Carlo calculations capture the effect of the cavity field in the presence of electron correlations, and their interplay and competition. In H$_2$, we find that a strong enough cavity coupling makes the original bound ground state metastable, along with inverting the singlet-triplet gap. In ring molecules (e.g., H$_n$), the magnetic cavity coupling stabilizes symmetric geometries. As a consequence, open-shell rings such as H$_4$, H$_8$, or C$_4$H$_4$, which would undergo Jahn-Teller distortions outside of the cavity, obtain exotic spin or ring-current polarized, antiaromatic ground states. These effects are enhanced by increasing the molecule concentration inside the cavity. Our results suggest cavity quantum electrodynamics beyond the long-wavelength approximation as a promising avenue for cavity-altered chemistry.

physics.chem-ph↗

arXiv2026

Magnetically tunable telecom emission from Er3+ ions in layered WS2

Erbium ions (Er3+) provide a telecom-band optical transition with strong magnetic-dipole character, making them attractive for quantum communication and spin-photon interfaces. Identifying host environments that combine low decoherence with photonic compatibility, however, remains a central challenge. Here we investigate Er3+ emission in tungsten disulfide (WS2) flakes, a layered host offering low nuclear-spin density and narrow telecom emission. Using time- and polarization-resolved photoluminescence under modest magnetic fields (< 0.2 T), we observe pronounced dimming, lifetime extension, and rotation of the emission dipole when the field has an out-of-plane component, whereas in-plane fields produce little change. Effective model calculations of Er3+ in monolayer WS2 parametrized from density functional theory indicate that these effects arise primarily from Zeeman-induced mixing of near-degenerate crystal-field sublevels, which modifies the magnitude and orientation of the optical transition dipole moments. Comparative measurements in flakes of different thickness and numerical estimates of the local density of optical states further suggest a secondary contribution from dipole coupling to the anisotropic photonic environment of thin WS2 layers. These findings identify layered WS2 as a platform where magnetic fields can tune telecom emission through an interplay of crystal-field physics and anisotropic photonic coupling.

cond-mat.mes-hall↗

arXiv2026

Emission of nitrogen-vacancy centers in diamond shaped by topological photonic waveguide modes

As the ability to integrate single photon emitters into photonic architectures improves, so does the need to characterize and understand their interaction. Here, we use a scanning diamond nanocrystal to investigate the interplay between the emission of room-temperature nitrogen-vacancy (NV) centers and a proximal topological waveguide. In our experiments, NVs serve as local, spectrally broad light sources which we exploit to characterize the waveguide bandwidth as well as the correspondence between light injection site and directionality of wave propagation. Further, we find that near-field coupling to the waveguide influences the spectral shape and ellipticity of the NV photoluminescence, hence allowing us to reveal nanostructured light fields with a spatial resolution defined by the nanoparticle size. Our results expand on the sensing modalities afforded by color centers, and portend novel opportunities in the development of on-chip, quantum optics devices leveraging topological photonics to best manipulate and readout single-photon emitters.

physics.optics↗

arXiv2025

Super-Poissonian Squeezed Light in the Ground State of Strongly Coupled Light-matter Systems

Strong light-matter coupling enables hybrid states in which photonic and electronic degrees of freedom become correlated even in the ground state. While many-body effects in long-range dispersion interactions are known to reshape electronic properties under such conditions, their impact on quantum-optical observables remains largely unexplored. Here, we address this problem using quantum electrodynamical density-functional theory (QEDFT) combined with the recently developed photon-many-body dispersion (pMBD) functional, which can capture higher-order electron-photon correlations and multi-photon processes. We compute ground-state photonic observables including photon number fluctuations, second-order correlations, and quadrature variances, and find squeezing and super-Poissonian photon statistics emerging from light-matter interactions in the strong coupling regime. Our results demonstrate that capturing the full hierarchy of many-body, electron-photon and multi-photon correlations is essential for a consistent description of quantum-optical properties in strongly coupled molecular systems, establishing QEDFT as a first-principles framework for predicting nonclassical photonic features in the ground state of complex systems.

physics.chem-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

Neural network distillation of orbital dependent density functional theory

Density functional theory (DFT) offers a desirable balance between quantitative accuracy and computational efficiency in practical many-electron calculations. Its central component, the exchange-correlation energy functional, has been approximated with increasing levels of complexity ranging from strictly local approximations to nonlocal and orbital-dependent expressions with many tuned parameters. In this paper, we formulate a general way of rewriting complex density functionals using deep neural networks in a way that allows for simplified computation of Kohn-Sham potentials as well as higher functional derivatives through automatic differentiation, enabling access to highly nonlinear response functions and forces. These goals are achieved by using a recently developed class of robust neural network models capable of modeling functionals, as opposed to functions, with explicitly enforced spatial symmetries. Functionals treated in this way are then called global density approximations and can be seamlessly integrated with existing DFT workflows. Tests are performed for a dataset featuring a large variety of molecular structures and popular meta-generalized gradient approximation density functionals, where we successfully eliminate orbital dependencies coming from the kinetic energy density, and discover a high degree of transferability to a variety of physical systems. The presented framework is general and could be extended to more complex orbital and energy dependent functionals as well as refined with specialized datasets.

physics.chem-ph↗

arXiv2024

The light-matter correlation energy functional of the cavity-coupled two-dimensional electron gas via quantum Monte Carlo simulations

We perform extensive simulations of the two-dimensional cavity-coupled electron gas in a modulating potential as a minimal model for cavity quantum materials. These simulations are enabled by a newly developed quantum-electrodynamical (QED) auxiliary-field quantum Monte Carlo method. We present a procedure to greatly reduce finite-size effects in such calculations. Based on our results, we show that a modified version of weak-coupling perturbation theory is remarkably accurate for a large parameter region. We further provide a simple parameterization of the light-matter correlation energy as a functional of the cavity parameters and the electronic density. These results provide a numerical foundation for the development of the QED density functional theory, which was previously reliant on analytical approximations, to allow quantitative modeling of a wide range of systems with light-matter coupling.

cond-mat.str-el↗

arXiv2024

Quantum embedding study of strain and charge induced Stark effects on the NV$^{-}$ center in diamond

The NV$^{-}$ color center in diamond has been demonstrated as a powerful nanosensor for quantum metrology due to the sensitivity of its optical and spin properties to external electric, magnetic, and strain fields. In view of these applications, we use quantum embedding to derive a many-body description of strain and charge induced Stark effects on the NV$^{-}$ center. We quantify how strain longitudinal to the axis of NV$^{-}$ shifts the excited states in energy, while strain with a component transverse to the NV$^{-}$ axis splits the degeneracies of the $^{3}E$ and $^{1}E$ states. The largest effects are for the optically relevant $^{3}E$ manifold, which splits into $E_{x}$ and $E_{y}$ with transverse strain. From these responses we extract strain susceptibilities for the $E_{x/y}$ states within the quasi-linear regime. Additionally, we study the many-body dipole matrix elements of the NV$^{-}$ and find a permanent dipole 1.64 D at zero strain, which is somewhat smaller than that obtained from recent density functional theory calculations. We also determine the transition dipole between the $E_{x}$ and $E_{y}$ and how it evolves with strain.

cond-mat.mtrl-sci↗

arXiv2024

Photoinduced charge injection from shallow point defects in diamond into water

Thanks to its low or negative surface electron affinity and chemical inertness, diamond is attracting broad attention as a source material of solvated electrons produced by optical excitation of the solid-liquid interface. Unfortunately, its wide bandgap typically imposes the use of wavelengths in the ultra-violet range, hence complicating practical applications. Here we probe the photocurrent response of water surrounded by single-crystal diamond surfaces engineered to host shallow nitrogen-vacancy (NV) centers. We observe clear signatures of diamond-induced photocurrent generation throughout the visible range and for wavelengths reaching up to 594 nm. Experiments as a function of laser power suggest that NV centers and other co-existing defects - likely in the form of surface traps - contribute to carrier injection, though we find that NVs dominate the system response in the limit of high illumination intensities. Given our growing understanding of near-surface NV centers and adjacent point defects, these results open new perspectives in the application of diamond-liquid interfaces to photo-carrier-initiated chemical and spin processes in fluids.

cond-mat.mtrl-sci↗

arXiv2024

Cavity-Born Oppenheimer Approximation for Molecules and Materials via Electric Field Response

We present an ab initio method for computing vibro-polariton and phonon-polariton spectra of molecules and solids coupled to the photon modes of optical cavities. We demonstrate that if interactions of cavity photon modes with both nuclear and electronic degrees of freedom are treated on the level of the cavity Born-Oppenheimer approximation (CBOA), spectra can be expressed in terms of the matter response to electric fields and nuclear displacements which are readily available in standard density functional perturbation theory (DFPT) implementations. In this framework, results over a range of cavity parameters can be obtained without the need for additional electronic structure calculations, enabling efficient calculations on a wide range of parameters. Furthermore, this approach enables results to be more readily interpreted in terms of the more familiar cavity-independent molecular electric field response properties, such as polarizability and Born effective charges which enter into the vibro-polariton calculation. Using corresponding electric field response properties of bulk insulating systems, we are also able to obtain $Γ$ point phonon-polariton spectra of two dimensional (2D) insulators. Results for a selection of cavity-coupled molecular and 2D crystal systems are presented to demonstrate the method.

physics.chem-ph↗

arXiv2024

Probing electric-dipole-enabled transitions in the excited state of the nitrogen-vacancy center in diamond

The excited orbitals of color centers typically show stronger electric dipoles, which can serve as a resource for entanglement, emission tuning, or electric field sensing. Here, we use resonant laser excitation to expose strong transition dipoles in the excited state (ES) orbitals of the negatively charged nitrogen vacancy center in diamond. By applying microwave electric fields, we perform strong Rabi driving between ES orbitals, and show that the dressed states can be tuned in frequency and are protected against fluctuations of the transverse electric field. In contrast with previous results, we observe sharp microwave resonances between magnetic states of the ES orbitals, and find that they are broadened due to simultaneous electric dipole driving.

quant-ph↗

arXiv2024

Semiempirical $\textit{ab initio}$ modeling of bound states of deep defects in semiconductor quantum technologies

A significant hurdle in developing high-performance semiconductor quantum technologies utilizing deep defects is related to charge dynamics. Unfortunately, progress in modeling their charge dynamics has been hindered over recent decades due to the absence of appropriate multiscale models capable of accurately representing the atomic properties of these defects and their impact on device performance. Here, we present a semi-\textit{ab initio} method for modeling the bound states of deep defects in semiconductor quantum technologies, applied to the negatively charged nitrogen vacancy (NV$^-$) center in diamond. We employ density functional theory calculations to construct accurate potentials for an effective mass model, which allow us to unveil the structure of the bound hole states. We develop a model to calculate the nonradiative capture cross sections, which agrees with experiment within one order of magnitude. Finally, we present our attempt at constructing the photoionization spectrum of NV$^0\rightarrow$ NV$^-$ + bound hole, showing that the electronic transitions of the bound holes can be distinguished from phonon sidebands. This paper offers a practical and efficient solution to a long-standing challenge in understanding the charge dynamics of deep defects.

cond-mat.mes-hall↗

arXiv2024

Emergence of new optical resonances in single-layer transition metal dichalcogenides with atomic-size phase patterns

Atomic-scale control of light-matter interactions represent the ultimate frontier for many applications in photonics and quantum technology. Two-dimensional semiconductors, including transition metal dichalcogenides, are a promising platform to achieve such control due to the combination of an atomically thin geometry and convenient photophysical properties. Here, we demonstrate that a variety of durable polymorphic structures can be combined to generate additional optical resonances beyond the standard excitons. We theoretically predict and experimentally show that atomic-sized patches of 1T phase within the 1H matrix form unique electronic bands that give rise to new and robust optical resonances with strong absorption, circularly polarized emission and long radiative lifetime. The atomic manipulation of two-dimensional semiconductors opens unexplored scenarios for light harvesting devices and exciton-based photonics.

cond-mat.mes-hall↗

arXiv2024

Photon Many-body Dispersion: an Exchange-correlation Functional for Strongly Coupled Light-matter Systems

We introduce an electron-photon exchange-correlation functional for quantum electrodynamical density-functional theory (QEDFT). The approach, photon MBD (pMBD), is inspired by the many-body dispersion (MBD) method for weak intermolecular interactions, which is generalized to include both electronic and photonic (electromagnetic) degrees of freedom on the same footing. We demonstrate that pMBD accurately captures effects that arise in the context of strong light-matter interactions, such as anisotropic electron-photon interactions, beyond single-photon effects, and cavity modulated van der Waals interactions. Moreover, we show that pMBD is computationally efficient and allows simulations of large complex systems coupled to optical cavities.

physics.chem-ph↗

arXiv2024

Ab initio calculations of quantum light-matter interactions in general electromagnetic environments

The emerging field of strongly coupled light-matter systems has drawn significant attention in recent years due to the prospect of altering physical and chemical properties of molecules and materials. Because this emerging field draws on ideas from both condensed-matter physics and quantum optics, it has attracted attention from theoreticians from both fields. While the former employ accurate descriptions of the electronic structure of the matter the description of the electromagnetic environment is often oversimplified. Contrastingly, the latter often employs sophisticated descriptions of the electromagnetic environment, while using simple few-level approximations for the matter. Both approaches are problematic because the oversimplified descriptions of the electronic system are incapable of describing effects such as light-induced structural changes, while the oversimplified descriptions of the electromagnetic environments can lead to unphysical predictions because the light-matter interactions strengths are misrepresented. Here we overcome these shortcomings and present the first method which can quantitatively describe both the electronic system and general electromagnetic environments from first principles. We realize this by combining macroscopic QED (MQED) with Quantum Electrodynamical Density-functional Theory. To exemplify this approach, we consider an absorbing spherical cavity and study the impact of different parameters of both the environment and the electronic system on the transition from weak-to-strong coupling for different aromatic molecules. As part of this work, we also provide an easy-to-use tool to calculate the cavity coupling strengths for simple cavity setups. Our work is a step towards parameter-free ab initio calculations for strongly coupled quantum light-matter systems and will help bridge the gap between theoretical methods and experiments in the field.

quant-ph↗

arXiv2023

Simulating polaritonic ground states on noisy quantum devices

The recent advent of quantum algorithms for noisy quantum devices offers a new route toward simulating strong light-matter interactions of molecules in optical cavities for polaritonic chemistry. In this work, we introduce a general framework for simulating electron-photon coupled systems on small, noisy quantum devices. This method is based on the variational quantum eigensolver (VQE) with the polaritonic unitary coupled cluster (PUCC) ansatz. To achieve chemical accuracy, we exploit various symmetries in qubit reduction methods, such as electron-photon parity, and use recently developed error mitigation schemes, such as the reference zero-noise extrapolation method. We explore the robustness of the VQE-PUCC approach across a diverse set of regimes for the bond length, cavity frequency, and coupling strength of the H$_2$ molecule in an optical cavity. To quantify the performance, we measure two properties: ground-state energy, fundamentally relevant to chemical reactivity, and photon number, an experimentally accessible general indicator of electron-photon correlation.

quant-ph↗

arXiv2023

Detection and modeling of hole capture by single point defects under variable electric fields

Understanding carrier trapping in solids has proven key to semiconductor technologies but observations thus far have relied on ensembles of point defects, where the impact of neighboring traps or carrier screening is often important. Here, we investigate the capture of photo-generated holes by an individual negatively-charged nitrogen-vacancy (NV) center in diamond at room temperature. Using an externally gated potential to minimize space-charge effects, we find the capture probability under electric fields of variable sign and amplitude shows an asymmetric-bell-shaped response with maximum at zero voltage. To interpret these observations, we run semi-classical Monte Carlo simulations modeling carrier trapping through a cascade process of phonon emission, and obtain electric-field-dependent capture probabilities in good agreement with experiment. Since the mechanisms at play are insensitive to the trap characteristics, the capture cross sections we observe - largely exceeding those derived from ensemble measurements - should also be present in materials platforms other than diamond.

cond-mat.mes-hall↗