Ground-state Density Matrix Research Articles

Behavior of quantum coherence in quantum phase transitions of two-dimensional XY and ising models

We investigate the quantum coherence behavior of the ground states of 2D Heisenberg XY model and 2D Ising model with a transverse field on square lattices using the Quantum Renormalization Group (QRG) method. Our analysis focused on the ground state density matrix and its marginal states, revealing non-analytic behavior of quantum coherence (especially two-site coherence) near the critical point. This behavior allowed us to detect quantum phase transitions (QPT) in these models. By examining the scaling behavior of the maximum derivative of quantum coherence with system size, we determined the critical exponent of coherence for both models and the length exponent of the Ising model. Additionally, we investigated the time evolution of coherence in both models. Our results closely align with those obtained from entanglement analysis, that is while quantum coherence requires fewer computational calculations compared to discord and entanglement approaches.

Triangular lattice Hubbard model physics at intermediate temperatures

Moire systems offer an exciting playground to study many-body effects of strongly correlated electrons in regimes that are not easily accessible in conventional material settings. Motivated by a recent experiment on $\text{WSe}_2/\text{WS}_2$ moire bilayers [Y. Tang et al., Nature 579, 353-358 (2020)], which realizes a triangular superlattice with a small hopping (of approximately 10 Kelvin), with tunable density of holes, we explore the Hubbard model on the triangular lattice for intermediate temperatures $t \lesssim T < U$. Employing finite temperature Lanczos calculations, and closely following the fitting protocols used in the experiment, we recover the observed trends in the reported Curie-Weiss temperature $\Theta$ with filling, using the reported interaction strength $U/t=20$. We focus on the large increase of $|\Theta|$ on decreasing the density below half filling and the sign change of $\Theta$ at higher fillings, which signals the onset of ferromagnetism. The increase in $|\Theta|$ is also seen in the $t$-$J$ model (the low energy limit of the Hubbard model) in the intermediate temperature range, which we clarify is opposite to the trend in its high temperature limit. Differences between the low, intermediate and high temperature regimes are discussed. Our numerical calculations also capture the crossover between short-range antiferromagnetic to ferromagnetic order in the intermediate temperature regime, a result broadly consistent with the experimental findings. We find that this behavior is a finite-temperature remnant of the underlying zero temperature phase transition, which we explore with ground state density matrix renormalization group calculations. We provide evidence of ferromagnetism characterized by weak (but robust) correlations that explain the small $\Theta$ seen in the experiment.

Scaled opposite-spin atomic-orbital based algebraic diagrammatic construction scheme for the polarization propagator with asymptotic linear-scaling effort: Theory and implementation.

A novel local approach for the quantum-chemical computation of excited states is presented, where the concept of the atomic-orbital formulation of the second-order Møller-Plesset energy expression is extended to the second-order algebraic diagrammatic construction scheme by virtue of the Laplace transform. The scaled opposite-spin second-order algebraic diagrammatic construction method with Cholesky decomposed densities and density-fitting, or CDD-DF-SOS-ADC(2) for short, exploits the sparsity of the two-electron repulsion integrals, the atomic ground-state density matrix, and the atomic transition density matrix to drastically reduce the computational effort. By using a local density-fitting approximation, it is shown that asymptotically linear scaling can be achieved for linear carboxylic acids. For electron-dense systems, sub-cubic scaling can be achieved if the excitation is local, and hence the transition density is sparse. Furthermore, the memory footprint and accuracy of the CDD-DF-SOS-ADC(2) method are explored in detail.

Electrodynamics of Topologically Ordered Quantum Phases in Dirac Materials.

First-principles calculations of the electronic ground state in tantalum arsenide are combined with tight-binding calculations of the field dependence of its transport model equivalent on the graphene monolayer to study the emergence of topologically ordered quantum states, and to obtain topological phase diagrams. Our calculations include the degrees of freedom for nuclear, electronic, and photonic interactions explicitly within the quasistatic approximation to the time-propagation-dependent density functional theory. This field-theoretic approach allows us to determine the non-linear response of the ground state density matrix to the applied electromagnetic field at distinct quantum phase transition points. Our results suggest the existence of a facile electronic switch between trivial and topologically ordered quantum states that may be realizable through the application of a perpendicular electric or magnetic field alongside a staggered-sublattice potential in the underlying lattice. Signatures of the near field electrodynamics in nanoclusters show the formation of a quantum fluid phase at the topological quantum phase transition points. The emergent carrier density wave transport phase is discussed to show that transmission through the collective excitation mode in multilayer heterostructures is a unique possibility in plasmonic, optoelectronic, and photonic applications when atomic clusters of Dirac materials are integrated within nanostructures, as patterned or continuous surfaces.

Ground-state phase diagram of the t-t′-J model

We report results of large-scale ground-state density matrix renormalization group (DMRG) calculations on t-[Formula: see text]-J cylinders with circumferences 6 and 8. We determine a rough phase diagram that appears to approximate the two-dimensional (2D) system. While for many properties, positive and negative [Formula: see text] values ([Formula: see text]) appear to correspond to electron- and hole-doped cuprate systems, respectively, the behavior of superconductivity itself shows an inconsistency between the model and the materials. The [Formula: see text] (hole-doped) region shows antiferromagnetism limited to very low doping, stripes more generally, and the familiar Fermi surface of the hole-doped cuprates. However, we find [Formula: see text] strongly suppresses superconductivity. The [Formula: see text] (electron-doped) region shows the expected circular Fermi pocket of holes around the [Formula: see text] point and a broad low-doped region of coexisting antiferromagnetism and d-wave pairing with a triplet p component at wavevector [Formula: see text] induced by the antiferromagnetism and d-wave pairing. The pairing for the electron low-doped system with [Formula: see text] is strong and unambiguous in the DMRG simulations. At larger doping another broad region with stripes in addition to weaker d-wave pairing and striped p-wave pairing appears. In a small doping region near [Formula: see text] for [Formula: see text], we find an unconventional type of stripe involving unpaired holes located predominantly on chains spaced three lattice spacings apart. The undoped two-leg ladder regions in between mimic the short-ranged spin correlations seen in two-leg Heisenberg ladders.

Phase diagram of the quantum Ising model on a triangular lattice under external field

Quantum Ising model on a triangular lattice hosts a finite temperature Berezinskii-Kosterlitz-Thouless (BKT) phase with emergent U(1) symmetry, and it will transit into an up-up-down (UUD) phase with $C_3$ symmetry breaking upon an infinitesimal external field along the longitudinal direction, but the overall phase diagram spanned by the axes of external field and temperature remains opaque due to the lack of systematic invesitgations with controlled methodologies. By means of quantum Monte Carlo at finite temperature and ground state density matrix renormalization group simulations, we map out the phase diagram of triangular quantum Ising model. Stemming from the upper BKT temperature at zero field, we obtain the phase boundary between the UUD and paramagnetic phases with its 2D $q=3$ Potts universality at weak field and weakly first order transition at strong field. Originated from the lower BKT temperature at zero field, we analyze the low temperature phase boundary between the clock phase and the UUD phase with Ising symmetry breaking at weak fields and the quantum phase transition between the UUD and fully polarized phases at strong fields. The accurate many-body numerical results are consistent with our field theoretical analysis. The experimental relevance towards the BKT magnet TmMgGaO$_4$ and programmable quantum simulators are also discussed.

Post-processing of the plane-wave approximation of Schrödinger equations. Part II: Kohn–Sham models

Abstract In this article, we provide a priori estimates for a perturbation-based post-processing method of the plane-wave approximation of nonlinear Kohn–Sham local density approximation (LDA) models with pseudopotentials, relying on Cancès et al. (2020, Post-processing of the plane-wave approximation of Schrödinger equations. Part I: linear operators. IMA Journal of Numerical Analysis, draa044) for the proofs of such estimates in the case of linear Schrödinger equations. As in Cancès et al. (2016, A perturbation-method-based post-processing for the plane-wave discretization of Kohn–Sham models. J. Comput. Phys., 307, 446–459), where these a priori results were announced and tested numerically, we use a periodic setting and the problem is discretized with plane waves (Fourier series). This post-processing method consists of performing a full computation in a coarse plane-wave basis and then to compute corrections based on the first-order perturbation theory in a fine basis, which numerically only requires the computation of the residuals of the ground-state orbitals in the fine basis. We show that this procedure asymptotically improves the accuracy of two quantities of interest: the ground-state density matrix, i.e. the orthogonal projector on the lowest $N$ eigenvectors, and the ground-state energy.

Post-processing of the planewave approximation of Schrödinger equations. Part I: linear operators

Abstract In this article we prove a priori error estimates for the perturbation-based post-processing of the plane-wave approximation of Schrödinger equations introduced and tested numerically in previous works (Cancès, Dusson, Maday, Stamm and Vohralík, (2014), A perturbation-method-based a posteriori estimator for the planewave discretization of nonlinear Schrödinger equations. C. R. Math., 352, 941--946; Cancès, Dusson, Maday, Stamm and Vohralík, (2016), A perturbation-method-based postprocessing for the planewave discretization of Kohn–Sham models. J. Comput. Phys., 307, 446--459.) We consider here a Schrödinger operator ${{\mathscr{H}} \,}= -\frac{1}{2}\varDelta +{\mathscr{V}}$ on $L^2(\varOmega )$, where $\varOmega $ is a cubic box with periodic boundary conditions and where ${\mathscr{V}}$ is a multiplicative operator by a regular-enough function ${\mathscr{V}}$. The quantities of interest are, on the one hand, the ground-state energy defined as the sum of the lowest $N$ eigenvalues of ${{\mathscr{H}} \,}$, and, on the other hand, the ground-state density matrix that is the spectral projector on the vector space spanned by the associated eigenvectors. Such a problem is central in first-principle molecular simulation, since it corresponds to the so-called linear subproblem in Kohn–Sham density functional theory. Interpreting the exact eigenpairs of ${{\mathscr{H}} \,}$ as perturbations of the numerical eigenpairs obtained by a variational approximation in a plane-wave (i.e., Fourier) basis we compute first-order corrections for the eigenfunctions, which are turned into corrections on the ground-state density matrix. This allows us to increase the accuracy by a factor proportional to the inverse of the kinetic energy cutoff ${E_{\textrm{c}}}^{-1}$ of both the ground-state energy and the ground-state density matrix in Hilbert–Schmidt norm at a low computational extra cost. Indeed, the computation of the corrections only requires the computation of the residual of the solution in a larger plane-wave basis and two fast Fourier transforms per eigenvalue.

QM–MM Ehrenfest dynamics from first principles: photodissociation of diazirine in aqueous solution

This article describes an implementation of Ehrenfest molecular dynamics based on TDDFT and Gaussian basis sets, optimized for hybrid QM–MM simulations in GPU. The present method makes use of the equations of motion proposed by Chen et al. (J Chem Phys 135:044126, 2011), which, at variance with previous formulations of the Ehrenfest dynamics, takes into account the movement of the localized basis functions, thus improving accuracy and energy conservation. This methodology is used to explore the evolution and the stability of excited state dynamics for two different constructions of the initial excited state, consisting in the linear response TDDFT $$S_1$$ solution, and in the ground state density matrix where the HOMO–LUMO occupancies have been switched, which is a widespread approach to model photoexcitation in electron dynamics simulations. It is found that the second kind of starting state leads to a larger numerical noise and to a poorer stability of the dynamics, aside from “awakening” inner electronic modes that become manifest in the frequency spectrum, and which are absent if the dynamics departs from the linear response TDDFT density matrix. Then, the method is applied to investigate the photodissociation of the diazirine molecule, CH $$_2$$ N $$_2$$ , both in vacuum and in aqueous solution. Diazirine decomposes into carbene and molecular nitrogen upon irradiation with UV light, and for this reason it has been widely adopted to photolabel biomolecules through the insertion of carbenes in the macromolecular surface. Our simulations suggest that the quantum yield of the dissociative reaction experiences a decrease in solution with respect to the gas phase, that can be understood in terms of the vibrational relaxation facilitated by the solvent molecules. Besides, the present results indicate that the isomerization and dissociation mechanism occur fully on the $$S_1$$ excited state.

Zero-temperature limit of thermodynamic quantum master equations

We investigate the zero-temperature limit of thermodynamic quantum master equations that govern the time evolution of density matrices for dissipative quantum systems. The quantum master equations for $T=0$ and for $T&gt;0$ possess completely different structures: (i) the equation for $T=0$ is linear in the deviation from the ground-state density matrix, whereas the equation for $T&gt;0$, in general, is seriously nonlinear, and (ii) the Gibbs state is obtained as the steady-state solution of the nonlinear equation for $T&gt;0$, whereas the ground state cannot be found from the equation for $T=0$. Nevertheless, the equation for $T=0$ can reproduce the behavior for $T\ensuremath{\gtrsim}0$ remarkably well. We discuss some implications of that observation for dissipative quantum field theory.

Orbital Magnetization as a Local Property

The modern expressions for polarization P and orbital magnetization M are k-space integrals. But a genuine bulk property should also be expressible in r space, as an unambiguous function of the ground-state density matrix, "nearsighted" in insulators, independently of the boundary conditions--either periodic or open. While P--owing to its "quantum" indeterminacy--is not a bulk property in this sense, M is. We provide its r-space expression for any insulator, even with a nonzero Chern invariant. Simulations on a model Hamiltonian validate our theory.

Mean-field models for disordered crystals

In this article, we set up a functional setting for mean-field electronic structure models of Hartree–Fock or Kohn–Sham types for disordered quantum systems. In the first part, we establish important properties of stochastic fermionic one-body density matrices, assuming that they are stationary under the ergodic action of a translation group. In particular, we prove Hoffmann-Ostenhof and Lieb–Thirring inequalities for ergodic density matrices, and deduce some weak compactness properties of the set of such matrices. We also discuss the representability problem for the associated one-particle densities. In the second part, we investigate the problem of solving Poissonʼs equation for a given stationary charge distribution, using the Yukawa potential to appropriately define the Coulomb self-interaction in the limit when the Yukawa parameter goes to zero. Finally, in the last part of the article, we use these tools to study a specific mean-field model (reduced Hartree–Fock, rHF) for a disordered crystal where the nuclei are classical particles whose positions and charges are random. We prove the existence of a minimizer of the energy per unit volume and the uniqueness of the ground state density. For (short-range) Yukawa interactions, we prove in addition that the rHF ground state density matrix satisfies a self-consistent equation, and that our model is the thermodynamic limit of the supercell model.

Bulk-edge correspondence in entanglement spectra

Li and Haldane conjectured and numerically substantiated that the entanglement spectrum of the reduced density matrix of ground-states of time-reversal breaking topological phases (fractional quantum Hall states) contains information about the counting of their edge modes when the ground-state is cut in two spatially distinct regions and one of the regions is traced out. We analytically substantiate this conjecture for a series of FQH states defined as unique zero modes of pseudopotential Hamiltonians by finding a one to one map between the thermodynamic limit counting of two different entanglement spectra: the particle entanglement spectrum, whose counting of eigenvalues for each good quantum number is identical (up to accidental degeneracies) to the counting of bulk quasiholes, and the orbital entanglement spectrum (the Li-Haldane spectrum). As the particle entanglement spectrum is related to bulk quasihole physics and the orbital entanglement spectrum is related to edge physics, our map can be thought of as a mathematically sound microscopic description of bulk-edge correspondence in entanglement spectra. By using a set of clustering operators which have their origin in conformal field theory (CFT) operator expansions, we show that the counting of the orbital entanglement spectrum eigenvalues in the thermodynamic limit must be identical to the counting of quasiholes in the bulk. The latter equals the counting of edge modes at a hard-wall boundary placed on the sample. Moreover, we show this to be true even for CFT states which are likely bulk gapless, such as the Gaffnian wavefunction.

Minimally entangled typical thermal state algorithms

We discuss a method based on sampling minimally entangled typical thermal states (METTS) that can simulate finite temperature quantum systems with a computational cost comparable to the ground state density matrix renormalization group (DMRG). Detailed implementation of each step of the method is presented, along with efficient algorithms for working with matrix product states and matrix product operators. Furthermore, we explore how the properties of METTS can reveal characteristic order and excitations of systems and discuss why METTS form an efficient basis for sampling. Finally, we explore the extent to which the average entanglement of a METTS ensemble is minimal.

The Dielectric Permittivity of Crystals in the Reduced Hartree–Fock Approximation

In a recent article (Canc\`es, Deleurence and Lewin, Commun. Math. Phys., 281 (2008), pp. 129-177), we have rigorously derived, by means of bulk limit arguments, a new variational model to describe the electronic ground state of insulating or semiconducting crystals in the presence of local defects. In this so-called reduced Hartree-Fock model, the ground state electronic density matrix is decomposed as $\gamma = \gamma^0_{\rm per} + Q_{\nu,\epsilon_{\rm F}}$, where $\gamma^0_{\rm per}$ is the ground state density matrix of the host crystal and $Q_{\nu,\epsilon_{\rm F}}$ the modification of the electronic density matrix generated by a modification $\nu$ of the nuclear charge of the host crystal, the Fermi level $\epsilon_{\rm F}$ being kept fixed. The purpose of the present article is twofold. First, we study more in details the mathematical properties of the density matrix $Q_{\nu,\epsilon_{\rm F}}$ (which is known to be a self-adjoint Hilbert-Schmidt operator on $L^2(\R^3)$). We show in particular that if $\int_{\RR^3} \nu \neq 0$, $Q_{\nu,\epsilon_{\rm F}}$ is not trace-class. Moreover, the associated density of charge is not in $L^1(\R^3)$ if the crystal exhibits anisotropic dielectric properties. These results are obtained by analyzing, for a small defect $\nu$, the linear and nonlinear terms of the resolvent expansion of $Q_{\nu,\epsilon_{\rm F}}$. Second, we show that, after an appropriate rescaling, the potential generated by the microscopic total charge (nuclear plus electronic contributions) of the crystal in the presence of the defect, converges to a homogenized electrostatic potential solution to a Poisson equation involving the macroscopic dielectric permittivity of the crystal. This provides an alternative (and rigorous) derivation of the Adler-Wiser formula.

Nonresonant interaction of femtosecond laser pulse with centrosymmetric molecules

We have derived a system of equations that describes the evolution of the density matrix of a centrosymmetric molecule interacting with a single nonresonant femtosecond laser pulse. The dynamics of the ground electronic state is expressed in terms of the effective Hamiltonian and the coherences between the ground an excited electronic states are functionals of the ground state density matrix. Using the time-dependent perturbation theory, we have calculated the energy deposited in the molecule as a result of rotational stimulated Raman scattering. The effective absorption coefficient is found to be proportional to the fourth power of the pulse amplitude and has a resonance-like dependence with respect to the pulse duration.

Transport through quantum dots: a combined DMRG and embedded-cluster approximation study

The numerical analysis of strongly interacting nanostructures requires powerful techniques. Recently developed methods, such as the time-dependent density matrix renormalization group (tDMRG) approach or the embedded-cluster approximation (ECA), rely on the numerical solution of clusters of finite size. For the interpretation of numerical results, it is therefore crucial to understand finite-size effects in detail. In this work, we present a careful finite-size analysis for the examples of one quantum dot, as well as three serially connected quantum dots. Depending on “odd-even” effects, physically quite different results may emerge from clusters that do not differ much in their size. We provide a solution to a recent controversy over results obtained with ECA for three quantum dots. In particular, using the optimum clusters discussed in this paper, the parameter range in which ECA can reliably be applied is increased, as we show for the case of three quantum dots. As a practical procedure, we propose that a comparison of results for static quantities against those of quasi-exact methods, such as the ground-state density matrix renormalization group (DMRG) method or exact diagonalization, serves to identify the optimum cluster type. In the examples studied here, we find that to observe signatures of the Kondo effect in finite systems, the best clusters involving dots and leads must have a total z-component of the spin equal to zero.

Density matrices for finite segments of Heisenberg chains of arbitrary length

We derive a multiple integral representing the ground-state density matrix of a segment of length m of the XXZ spin chain on L lattice sites, which depends on L only parametrically. This allows us to treat chains of arbitrary finite length. Specializing to the isotropic limit of the XXX chain we show for small m that the multiple integrals factorize. We conjecture that this property holds for arbitrary m and suggest an exponential formula for the density matrix which involves only a double Cauchy type integral in the exponent. We demonstrate the efficiency of our formula by computing the next-to-nearest neighbour zz-correlation function for chain lengths ranging from two to macroscopic numbers.

Applications and generalizations of Fisher–Hartwig asymptotics

Fisher–Hartwig asymptotics refers to the large n form of a class of Toeplitz determinants with singular generating functions. This class of Toeplitz determinants occurs in the study of the spin–spin correlations for the two-dimensional Ising model, and the ground state density matrix of the impenetrable Bose gas, amongst other problems in mathematical physics. We give a new application of the original Fisher–Hartwig formula to the asymptotic decay of the Ising correlations above Tc, while the study of the Bose gas density matrix leads us to generalize the Fisher–Hartwig formula to the asymptotic form of random matrix averages over the classical groups and the Gaussian and Laguerre unitary matrix ensembles. Another viewpoint of our generalizations is that they extend to Hankel determinants the Fisher–Hartwig asymptotic form known for Toeplitz determinants.

Polariton laser: thermodynamics and quantum kinetic theory

Cavity exciton–polaritons are considered to be two-dimensional weakly interacting true bosons. We analyse their thermodynamic properties and show that they can exhibit local condensation or Kosterlitz–Thouless phase transition towards superfluidity, so that polariton lasing can be achieved. The dynamical evolution of the condensate in a non-resonantly pumped cavity is described by a quantum kinetic formalism. The distribution function of polaritons is described by a semi-classical Boltzmann equation. A master equation for the ground-state density matrix is derived in the framework of the Born–Markov approximation. The dynamics of the ground-state population and its coherence are deduced.