Van Leeuwen Theorem Research Articles

Extended Time-Dependent Density Functional Theory for Multibody Densities.

Time-dependent density functional theory (TDDFT) is widely used for understanding and predicting properties and behaviors of matter. As one of the fundamental theorems in TDDFT, Van Leeuwen theorem [Phys. Rev. Lett. 82, 3863 (1999)PRLTAO0031-900710.1103/PhysRevLett.82.3863] guarantees how to construct a unique potential with the same one-body density evolution. Here we extend Van Leeuwen theorem by exploring truncation criteria in Bogoliubov-Born-Green-Kirkwood-Yvon (BBGKY) hierarchy. Our generalized theorem demonstrates the existence of a unique nonlocal potential to accurately reconstruct the multibody density evolution in binary interacting systems. Under nonstringent conditions, truncation of the BBGKY-hierarchy equations aligns with the behavior of multibody density evolution and maintains consistency in the reduced equations. Based on this theorem, we further construct a static many-body potential and extend the well-known Casida equation for multiple-excitation energy. The extended TDDFT provides an accurate and first-principles framework capable of describing the kinetic processes of correlated systems, including strongly coupled particle transport, multiple-excitation, and ionization processes.

Normal modes, rotational inertia, and thermal fluctuations of trapped ion crystals

The normal modes of a trapped ion crystal are derived using an approach based on the Hermitian properties of the system's dynamical matrix. This method is equivalent to the standard Bogoliubov method, but for classical systems, it is arguably simpler and more general in that canonical coordinates are not necessary. The theory is developed for stable, unstable, and neutrally stable systems. The method is then applied to ion crystals in a Penning trap. Reduced eigenvalue problems for the case of large applied magnetic fields are developed, for which the spectrum breaks into E × B drift modes, axial modes, and cyclotron modes. Thermal fluctuation levels in these modes are analyzed and shown to be consistent with the Bohr–van-Leeuwen theorem, provided that neutrally stable modes associated with crystal rotations are included in the analysis. An expression for the rotational inertia of the crystal is derived, and a magnetic contribution to this inertia, which dominates in large magnetic fields, is described. An unusual limit is discovered for the special case of spherically symmetric confinement, in which the rotational inertia does not exist and changes in angular momentum leave the rotation frequency unaffected.

Imaginary-Time Time-Dependent Density Functional Theory and Its Application for Robust Convergence of Electronic States.

Reliable and robust convergence to the electronic ground state within density functional theory (DFT) Kohn-Sham (KS) calculations remains a thorny issue in many systems of interest. In such cases, charge sloshing can delay or completely hinder the convergence. Here, we use an approach based on transforming the time-dependent DFT equations to imaginary time, followed by imaginary-time evolution, as a reliable alternative to the self-consistent field (SCF) procedure for determining the KS ground state. We discuss the theoretical and technical aspects of this approach and show that the KS ground state should be expected to be the long-imaginary-time output of the evolution, independent of the exchange-correlation functional or the level of theory used to simulate the system. By maintaining self-consistency between the single-particle wave functions (orbitals) and the electronic density throughout the determination of the stationary state, our method avoids the typical difficulties encountered in SCF. To demonstrate dependability of our approach, we apply it to selected systems which struggle to converge with SCF schemes. In addition, through the van Leeuwen theorem, we affirm the physical meaningfulness of imaginary-time TDDFT, justifying its use in certain topics of statistical mechanics such as in computing imaginary-time path integrals.

Density response from kinetic theory and time-dependent density-functional theory for matter under extreme conditions

The density linear response function for an inhomogeneous system of electrons in equilibrium with an array of fixed ions is considered. Two routes to its evaluation for extreme conditions (e.g., warm dense matter) are considered. The first is from a recently developed short-time kinetic equation; the second is from time-dependent density functional theory (tdDFT). The result from the latter approach agrees with that from kinetic theory in the "adiabatic approximation", providing support and context for each. Both provide a connection to the phenomenological Kubo-Greenwood method for calculating transport properties. A brief proof of the van Leeuwen theorem (an essential underpinning of tdDFT) extended to the mixed states of equilibrium ensembles is given.

Time-dependent generalized Kohn–Sham theory

Generalized Kohn–Sham (GKS) theory extends the realm of density functional theory (DFT) by providing a rigorous basis for non-multiplicative potentials, the use of which is outside original Kohn–Sham theory. GKS theory is of increasing importance as it underlies commonly used approximations, notably (conventional or range-separated) hybrid functionals and meta-generalized-gradient-approximation (meta-GGA) functionals. While this approach is often extended in practice to time-dependent DFT (TDDFT), the theoretical foundation for this extension has been lacking, because the Runge–Gross theorem and the van Leeuwen theorem that serve as the basis of TDDFT have not been generalized to non-multiplicative potentials. Here, we provide the necessary generalization. Specifically, we show that with one simple but non-trivial additional caveat – upholding the continuity equation in the GKS electron gas – the Runge–Gross and van Leeuwen theorems apply to time-dependent GKS theory. We also discuss how this is manifested in common GKS-based approximations.

Bohr–van Leeuwen theorem in non-commutative space

Bohr–van Leeuwen theorem has been studied in non-commutative space where the space coordinates do not commute. It has been found that in non-commutative space Bohr–van Leeuwen theorem, in general, is not satisfied and a classical treatment of the partition function of charged particles in a magnetic field gives rise to non zero magnetization.

A rigorous proof of the Bohr–van Leeuwen theorem in the semiclassical limit

The original formulation of the Bohr–van Leeuwen (BvL) theorem states that, in a uniform magnetic field and in thermal equilibrium, the magnetization of an electron gas in the classical Drude–Lorentz model vanishes identically. This stems from classical statistics which assign the canonical momenta all values ranging from -∞ to ∞ that makes the free energy density magnetic-field-independent. When considering a classical (Maxwell–Boltzmann) interacting electron gas, it is usually admitted that the BvL theorem holds upon condition that the potentials modeling the interactions are particle-velocities-independent and do not cause the system to rotate after turning on the magnetic field. From a rigorous viewpoint, when treating large macroscopic systems, one expects the BvL theorem to hold provided the thermodynamic limit of the free energy density exists (and the equivalence of ensemble holds). This requires suitable assumptions on the many-body interactions potential and on the possible external potentials to prevent the system from collapsing or flying apart. Starting from quantum statistical mechanics, the purpose of this paper is to give, within the linear-response theory, a proof of the BvL theorem in the semiclassical limit when considering a dilute electron gas in the canonical conditions subjected to a class of translational invariant external potentials.

CLASSICAL DIAMAGNETISM REVISITED

The well-known Bohr–van Leeuwen Theorem states that the orbital diamagnetism of classical charged particles is identically zero in equilibrium. However, results based on real space–time approach using the classical Langevin equation predicts non-zero diamagnetism for classical unbounded (finite or infinite) systems. Here we show that the recently discovered Fluctuation Theorems, namely, the Jarzynski Equality or the Crooks Fluctuation Theorem surprisingly predicts a free energy that depends on magnetic field as well as on the friction coefficient, in outright contradiction to the canonical equilibrium results. However, in the cases where the Langevin approach is consistent with the equilibrium results, the Fluctuation Theorems lead to results in conformity with equilibrium statistical mechanics. The latter is demonstrated analytically through a simple example that has been discussed recently.

Bohr–van Leeuwen theorem and the thermal Casimir effect for conductors

The problem of estimating the thermal corrections to Casimir and Casimir-Polder interactions in systems involving conducting plates has attracted considerable attention in the recent literature on dispersion forces. Alternative theoretical models, based on distinct low-frequency extrapolations of the plates reflection coefficient for transverse electric (TE) modes, provide widely different predictions for the magnitude of this correction. In this paper we examine the most widely used prescriptions for this reflection coefficient from the point of view of their consistency with the Bohr-van Leeuwen theorem of classical statistical physics, stating that at thermal equilibrium transverse electromagnetic fields decouple from matter in the classical limit. We find that the theorem is satisfied if and only if the TE reflection coefficient vanishes at zero frequency in the classical limit. This criterion appears to rule out some of the models that have been considered recently for describing the thermal correction to the Casimir pressure with non-magnetic metallic plates.

Nonequilibrium work distributions for a trapped Brownian particle in a time-dependent magnetic field

We study the dynamics of a trapped, charged Brownian particle in the presence of a time-dependent magnetic field. We calculate work distributions for different time-dependent protocols numerically. In our problem, thermodynamic work is related to variation of the vector potential with time as opposed to the earlier studies where the work is related to time variation of the potentials, a quantity that depends only on the coordinates of the particle. Using the Jarzynski and the Crooks equalities, we show that the free energy of the particle is independent of the magnetic field, thus complementing the Bohr-van Leeuwen theorem. We also show that our system exhibits a parametric resonance in a certain parameter space.

On the decoupling between classical Coulomb matter and radiation

We consider a model of matter coupled to radiation at equilibrium. Matter is described by a one-component plasma of classical point charges with Coulomb interactions, while radiation is represented by the classical transverse potential vector in Coulomb gauge. Using a straightforward generalization of the Bohr–van Leeuwen theorem, we show that the equilibrium properties of classical Coulomb matter remain unaffected by the presence of the classical radiation. As far as the real world is concerned, this decoupling does survive at large distances where both matter and radiation can be treated classically. This invalidates all the large-distances predictions, for the charge correlations, of the so-called Darwin models which incorporate retarded electromagnetic interactions beyond the instantaneous Coulomb potential. A second related important consequence is that the first relativistic corrections to the Coulomb thermodynamical quantities must be evaluated within the theory of quantum electrodynamics at finite temperature, even in a weakly relativistic and almost classical regime for matter.

On the radical theory of Andrunakievich varieties

In 1978 Anderson and Gardner investigated semisimple classes and recently Buys and Gerber developed the theory of special radicals in Andrunakievich varieties. In this note we continue the study of radical theory in Andrunakievich varieties. Sharpening some of the results of Anderson and Gardner we prove versions of Sands' Theorem characterizing semisimple classes by regularity, coinductivity and being closed under extensions. In the proof we follow a new method which avoids calculations with defining identities of the variety. We generalize van Leeuwen's Theorem characterizing semisimple classes of hereditary radicals as classes being regular and closed under essential extensions and subdirect sums.

Orbital diamagnetism of a charged Brownian particle undergoing a birth-death process

Considers the magnetic response of a charged Brownian particle undergoing a stochastic birth-death process. The latter simulates the electron-hole pair production and recombination in semiconductors. The authors obtain non-zero, orbital diamagnetism which can be large without violating the Van Leeuwen theorem (1921).