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Markus Penz

Publications and source records attributed to Markus Penz.

At least 19 recordsLinked to original sources
arXiv2026

Moreau-Yosida-based Kohn-Sham Inversion for Periodic Systems

Density-potential inversion for periodic systems within Moreau-Yosida-regularised density-functional theory is investigated, both theoretically and numerically. We develop the framework in a periodic homogeneous Sobolev space and use it to recover the exchange-correlation potential of Kohn-Sham theory through a limiting procedure. A key analytical ingredient is the proof of lower semicontinuity of the non-interacting kinetic-energy functional in the chosen topology. The proximal mapping, together with its algorithmic evaluation, plays a central role in the resulting inversion scheme. Numerical experiments illustrate the performance and properties of the method for both the Kohn-Sham and Gross-Pitaevskii equations.

math.NA↗
arXiv2026

Unified Framework for Functional Theories of Quantum Systems

We introduce and study a unified framework for density-functional theory and its variants for quantum systems on finite-dimensional Hilbert spaces. These theories seek to reduce the complexity inherent in the many-body quantum problem by describing ground states through reduced variables. The central ingredients of our unified framework are a generalized choice of basic observables, whose expectation values define precisely those reduced variables, and a fixed part of the Hamiltonian characterizing the class of quantum systems under consideration. It is this minimal structure, which we call the scope of a functional theory, that is necessary and sufficient for the formulation of a functional theory. In particular, it allows one to define the universal functionals, establish their convexity and differentiability properties, address representability questions, and prove a Hohenberg-Kohn-type uniqueness result. A purification construction also relates ensemble and weighted-ensemble functionals to the pure-state variant. Particular emphasis is placed on functional theories with Lie-algebra observable structures, connecting the variational framework to symplectic geometry. The result of this work is a systematic mathematical formulation in which structural results can be proved once and applied across a broad class of finite-dimensional functional theories.

math-ph↗
arXiv2026

Capturing electron correlation at mean-field cost: Assessment of i-DMFT and the underlying correlation conjecture

Accurately treating strong electron correlation in quantum chemistry typically requires multireference wave-function methods with steep computational scaling. The recently proposed i-DMFT method promises near configuration-interaction accuracy at mean-field cost by invoking an empirical linear relation between correlation energy and entropy (Collins' conjecture), whose validity remains unclear. We systematically assess this relation across a range of di- and polyatomic molecules, including diverse bond types, third-row elements, different types of geometric distortions, and excited states. We find that the conjectured linearity holds for bond-breaking processes dominated by electron redistribution within orbital pairs, but breaks down for heterolytic dissociation and excited states. In simple molecules, i-DMFT provides a reasonable description of total energies, but does not reliably reproduce reduced density matrices or individual energy components. It further degrades in more complex cases such as ethylene. Based on these results, we formulate criteria for the validity of the conjecture and outline implications for entropy-based reduced density matrix functionals.

physics.chem-ph↗
arXiv2025

Perspective on Moreau-Yosida Regularization in Density-Functional Theory

Within density-functional theory, Moreau-Yosida regularization enables both a reformulation of the theory and a mathematically well-defined definition of the Kohn-Sham approach. It is further employed in density-potential inversion schemes and, through the choice of topology for the density and potential space, can be directly linked to classical field theories. This perspective collects various appearances of the regularization technique within density-functional theory alongside possibilities for their future development.

cond-mat.mtrl-sci↗
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

Constrained Search in Imaginary Time

We introduce an imaginary-time evolution method to evaluate the pure-state constrained-search functional from density-functional theory formulated on finite lattices. Simultaneously, it yields a potential that produces a prescribed density of an eigenstate. Besides being a computational scheme, this allows one to gain theoretical insights into the density-potential mapping. The method can be generalized to the optimization of the expectation value of a general self-adjoint operator on a finite-dimensional Hilbert space under a finite number of expectation-value constraints for commuting self-adjoint operators.

cond-mat.mtrl-sci↗
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

Adaptation of Moreau-Yosida regularization to the modulus of convexity

We study a generalization of Moreau-Yosida regularization that is adapted to the geometry of Banach spaces where the dual space is uniformly convex with modulus of convexity of power type. Important properties for regularized convex functions are given, in particular strong monotonicity of the subdifferential of their convex conjugate and H\"older-continuity of their gradient.

math.FA↗
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

Density-functional theory for the Dicke Hamiltonian

A detailed analysis of density-functional theory for quantum-electrodynamical model systems is provided. In particular, the quantum Rabi model, the Dicke model, and a generalization of the latter to multiple modes are considered. We prove a Hohenberg-Kohn theorem that manifests the magnetization and displacement as internal variables, along with several representability results. The constrained-search functionals for pure states and ensembles are introduced and analyzed. We find the optimizers for the pure-state constrained-search functional to be low-lying eigenstates of the Hamiltonian and, based on the properties of the optimizers, we formulate an adiabatic-connection formula. In the reduced case of the Rabi model we can even show differentiability of the universal density functional, which amounts to unique pure-state v-representability.

math-ph↗
arXiv2024

Geometrical Perspective on Spin-Lattice Density-Functional Theory

A recently developed viewpoint on the fundamentals of density-functional theory for finite interacting spin-lattice systems that centers around the notion of degeneracy regions is presented. It allows for an entirely geometrical description of the Hohenberg-Kohn theorem and v-representability. The phenomena receive exemplification by an Anderson impurity model and other small-lattice examples. The case of adiabatic change and the time-dependent setting are examined as well.

cond-mat.mtrl-sci↗
arXiv2024

Electron-Photon Exchange-Correlation Approximation for QEDFT

Quantum-electrodynamical density-functional theory (QEDFT) provides a promising avenue for exploring complex light-matter interactions in optical cavities for real materials. Similar to conventional density-functional theory, the Kohn-Sham formulation of QEDFT needs approximations for the generally unknown exchange-correlation functional. In addition to the usual electron-electron exchange-correlation potential, an approximation for the electron-photon exchange-correlation potential is needed. A recent electron-photon exchange functional [C. Sch\"afer et al., Proc. Natl. Acad. Sci. USA, 118, e2110464118 (2021), https://www.pnas.org/doi/abs/10.1073/pnas.2110464118], derived from the equation of motion of the non-relativistic Pauli-Fierz Hamiltonian, shows robust performance in one-dimensional systems across weak- and strong-coupling regimes. Yet, its performance in reproducing electron densities in higher dimensions remains unexplored. Here we consider this QEDFT functional approximation from one to three-dimensional finite systems and across weak to strong light-matter couplings. The electron-photon exchange approximation provides excellent results in the ultra-strong-coupling regime. However, to ensure accuracy also in the weak-coupling regime across higher dimensions, we introduce a computationally efficient renormalization factor for the electron-photon exchange functional, which accounts for part of the electron-photon correlation contribution. These findings extend the applicability of photon-exchange-based functionals to realistic cavity-matter systems, fostering the field of cavity QED (quantum electrodynamics) materials engineering.

physics.comp-ph↗
arXiv2023

Solution of the v-representability problem on a one-dimensional torus

We provide a solution to the v-representability problem for a non-relativistic quantum many-particle system on a ring domain in terms of Sobolev spaces and their duals. Any one-particle density that is square-integrable, has a square-integrable weak derivative, and is gapped away from zero can be realized from the solution of a many-particle Schr\"odinger equation, with or without interactions, by choosing a corresponding external potential. This potential can contain a distributional contribution but still gives rise to a self-adjoint Hamiltonian. Importantly, this allows for a well-defined Kohn-Sham procedure but, on the other hand, invalidates the usual proof of the Hohenberg-Kohn theorem.

math-ph↗
arXiv2023

Exchange-only virial relation from the adiabatic connection

The exchange-only virial relation due to Levy and Perdew is revisited. Invoking the adiabatic connection, we introduce the exchange energy in terms of the right-derivative of the universal density functional w.r.t. the coupling strength $\lambda$ at $\lambda=0$. This agrees with the Levy-Perdew definition of the exchange energy as a high-density limit of the full exchange-correlation energy. By relying on $v$-representability for a fixed density at varying coupling strength, we prove an exchange-only virial relation without an explicit local-exchange potential. Instead, the relation is in terms of a limit ($\lambda \searrow 0$) involving the exchange-correlation potential $v_\mathrm{xc}^\lambda$, which exists by assumption of $v$-representability. On the other hand, a local-exchange potential $v_\mathrm{x}$ is not warranted to exist as such a limit.

physics.chem-ph↗
arXiv2023

Weakened Topological Protection of the Quantum Hall Effect in a Cavity

We study the quantum Hall effect in a two-dimensional homogeneous electron gas coupled to a quantum cavity field. As initially pointed out by Kohn, Galilean invariance for a homogeneous quantum Hall system implies that the electronic center of mass (CM) decouples from the electron-electron interaction, and the energy of the CM mode, also known as Kohn mode, is equal to the single particle cyclotron transition. In this work, we point out that strong light-matter hybridization between the Kohn mode and the cavity photons gives rise to collective hybrid modes between the Landau levels and the photons. We provide the exact solution for the collective Landau polaritons and we demonstrate the weakening of topological protection at zero temperature due to the existence of the lower polariton mode which is softer than the Kohn mode. This provides an intrinsic mechanism for the recently observed topological breakdown of the quantum Hall effect in a cavity [Appugliese et al., Science 375, 1030-1034 (2022)]. Importantly, our theory predicts the cavity suppression of the thermal activation gap in the quantum Hall transport. Our work paves the way for future developments in the cavity control of quantum materials.

cond-mat.mes-hall↗
arXiv2023

The structure of the density-potential mapping. Part II: Including magnetic fields

The Hohenberg-Kohn theorem of density-functional theory (DFT) is broadly considered the conceptual basis for a full characterization of an electronic system in its ground state by just the one-body particle density. In this Part~II of a series of two articles, we aim at clarifying the status of this theorem within different extensions of DFT including magnetic fields. We will in particular discuss current-density-functional theory (CDFT) and review the different formulations known in the literature, including the conventional paramagnetic CDFT and some non-standard alternatives. For the former, it is known that the Hohenberg-Kohn theorem is no longer valid due to counterexamples. Nonetheless, paramagnetic CDFT has the mathematical framework closest to standard DFT and, just like in standard DFT, non-differentiability of the density functional can be mitigated through Moreau-Yosida regularization. Interesting insights can be drawn from both Maxwell-Schr\"odinger DFT and quantum-electrodynamical DFT, which are also discussed here.

physics.chem-ph↗
arXiv2022

Density-potential inversion from Moreau-Yosida regularization

For a quantum-mechanical many-electron system, given a density, the Zhao-Morrison-Parr method allows to compute the effective potential that yields precisely that density. In this work, we demonstrate how this and similar inversion procedures mathematically relate to the Moreau-Yosida regularization of density functionals on Banach spaces. It is shown that these inversion procedures can in fact be understood as a limit process as the regularization parameter approaches zero. This sheds new insight on the role of Moreau-Yosida regularization in density-functional theory and allows to systematically improve density-potential inversion. Our results apply to the Kohn-Sham setting with fractional occupation that determines an effective one-body potential that in turn reproduces an interacting density.

physics.chem-ph↗
arXiv2022

The structure of the density-potential mapping. Part I: Standard density-functional theory

The Hohenberg-Kohn theorem of density-functional theory (DFT) is broadly considered the conceptual basis for a full characterization of an electronic system in its ground state by just the one-body particle density. Part I of this review aims at clarifying the status of the Hohenberg-Kohn theorem within DFT and Part II at different extensions of the theory that include magnetic fields. We collect evidence that the Hohenberg-Kohn theorem does not so much form the basis of DFT, but is rather the consequence of a more comprehensive mathematical framework. Such results are especially useful when it comes to the construction of generalized DFTs.

physics.chem-ph↗