arXiv subjects

C. J. Umrigar

Publications and source records attributed to C. J. Umrigar.

52 records · Page 3Linked to original sources

arXiv2007

Incipient Wigner Localization in Circular Quantum Dots

We study the development of electron-electron correlations in circular quantum dots as the density is decreased. We consider a wide range of both electron number, N<=20, and electron gas parameter, r_s<18, using the diffusion quantum Monte Carlo technique. Features associated with correlation appear to develop very differently in quantum dots than in bulk. The main reason is that translational symmetry is necessarily broken in a dot, leading to density modulation and inhomogeneity. Electron-electron interactions act to enhance this modulation ultimately leading to localization. This process appears to be completely smooth and occurs over a wide range of density. Thus there is a broad regime of ``incipient'' Wigner crystallization in these quantum dots. Our specific conclusions are: (i) The density develops sharp rings while the pair density shows both radial and angular inhomogeneity. (ii) The spin of the ground state is consistent with Hund's (first) rule throughout our entire range of r_s for all 4<N<20. (iii) The addition energy curve first becomes smoother as interactions strengthen -- the mesoscopic fluctuations are damped by correlation -- and then starts to show features characteristic of the classical addition energy. (iv) Localization effects are stronger for a smaller number of electrons. (v) Finally, the gap to certain spin excitations becomes small at the strong interaction (large r_s) side of our regime.

cond-mat.mes-hall↗

arXiv2006

Alleviation of the Fermion-sign problem by optimization of many-body wave functions

We present a simple, robust and highly efficient method for optimizing all parameters of many-body wave functions in quantum Monte Carlo calculations, applicable to continuum systems and lattice models. Based on a strong zero-variance principle, diagonalization of the Hamiltonian matrix in the space spanned by the wav e function and its derivatives determines the optimal parameters. It systematically reduces the fixed-node error, as demonstrated by the calculation of the binding energy of the small but challenging C$_2$ molecule to the experimental accuracy of 0.02 eV.

cond-mat.other↗

arXiv2006

Correlation Induced Inhomogeneity in Circular Quantum Dots

Properties of the "electron gas" - in which conduction electrons interact by means of Coulomb forces but ionic potentials are neglected - change dramatically depending on the balance between kinetic energy and Coulomb repulsion. The limits are well understood. For very weak interactions (high density), the system behaves as a Fermi liquid, with delocalized electrons. In contrast, in the strongly interacting limit (low density), the electrons localize and order into a Wigner crystal phase. The physics at intermediate densities, however, remains a subject of fundamental research. Here, we study the intermediate-density electron gas confined to a circular disc, where the degree of confinement can be tuned to control the density. Using accurate quantum Monte Carlo techniques, we show that the electron-electron correlation induced by an increase of the interaction first smoothly causes rings, and then angular modulation, without any signature of a sharp transition in this density range. This suggests that inhomogeneities in a confined system, which exist even without interactions, are significantly enhanced by correlations.

cond-mat.mes-hall↗

arXiv2005

The maximum density droplet to lower density droplet transition in quantum dots

We show that, Landau level mixing in two-dimensional quantum dot wave functions can be taken into account very effectively by multiplying the exact lowest Landau level wave functions by a Jastrow factor which is optimized by variance minimization. The comparison between exact diagonalization and fixed phase diffusion Monte Carlo results suggests that the phase of the many-body wave functions are not affected much by Landau level mixing. We apply these wave functions to study the transition from the maximum density droplet state (incipient integer quantum Hall state with angular momentum L=N(N-1)/2) to lower density droplet states (L>N(N-1)/2).

cond-mat.mes-hall↗

arXiv2005

Interaction Effects in the Mesoscopic Regime: A Quantum Monte Carlo Study of Irregular Quantum Dots

We address the issue of accurately treating interaction effects in the mesoscopic regime by investigating the ground state properties of isolated irregular quantum dots. Quantum Monte Carlo techniques are used to calculate the distributions of ground state spin and addition energy. We find a reduced probability of high spin and a somewhat larger even/odd alternation in the addition energy from quantum Monte Carlo than in local spin density functional theory. In both approaches, the even/odd effect gets smaller with increasing number of electrons, contrary to the theoretical understanding of large dots. We argue that the local spin density approximation over predicts the effects of interactions in quantum dots.

cond-mat.mes-hall↗

arXiv2005

Energy and variance optimization of many body wave functions

We present a simple, robust and efficient method for varying the parameters in a many-body wave function to optimize the expectation value of the energy. The effectiveness of the method is demonstrated by optimizing the parameters in flexible Jastrow factors, that include 3-body electron-electron-nucleus correlation terms, for the NO$_2$ and decapentaene (C$_{10}$H$_{12}$) molecules. The basic idea is to add terms to the straightforward expression for the Hessian that are zero when the integrals are performed exactly, but that cancel much of the statistical fluctuations for a finite Monte Carlo sample. The method is compared to what is currently the most popular method for optimizing many-body wave functions, namely minimization of the variance of the local energy. The most efficient wave function is obtained by optimizing a linear combination of the energy and the variance.

cond-mat.other↗

arXiv2003

Erratum: Diffusion Monte Carlo study of circular quantum dots

Several of the energies in Tables I and II of our previous paper are incorrect. Most of the errors are due to incorrectly inputting the symmetry of some of the states, others are due to incorrectly converting or transcribing the energies. In particular, for N=4 we had a near degeneracy and a violation of Hund's first rule. The corrected result has $|L=0,S=1>$ as the ground state, as predicted by Hund's rule. Hund's first rule is satisfied for all $N$ for the confining potential used. We present corrected versions of Tables I and II.

cond-mat↗

arXiv2000

Diffusion Monte Carlo study of circular quantum dots

We present ground and excited state energies obtained from Diffusion Monte Carlo (DMC) calculations, using accurate multiconfiguration wave functions, for $N$ electrons ($N\le13$) confined to a circular quantum dot. We analyze the electron-electron pair correlation functions and compare the density and correlation energies to the predictions of local spin density approximation theory (LSDA). The DMC estimated change in electrochemical potential as function of the number of electrons in the dot is compared to that from LSDA and Hartree-Fock (HF) calculations.

cond-mat↗

arXiv1999

Correlated sampling in quantum Monte Carlo: a route to forces

In order to find the equilibrium geometries of molecules and solids and to perform ab initio molecular dynamics, it is necessary to calculate the forces on the nuclei. We present a correlated sampling method to efficiently calculate numerical forces and potential energy surfaces in diffusion Monte Carlo. It employs a novel coordinate transformation, earlier used in variational Monte Carlo, to greatly reduce the statistical error. Results are presented for first-row diatomic molecules.

cond-mat↗

arXiv1998

Monte Carlo Eigenvalue Methods in Quantum Mechanics and Statistical Mechanics

In this review we discuss, from a unified point of view, a variety of Monte Carlo methods used to solve eigenvalue problems in statistical mechanics and quantum mechanics. Although the applications of these methods differ widely, the underlying mathematics is quite similar in that they are stochastic implementations of the power method. In all cases, optimized trial states can be used to reduce the errors of Monte Carlo estimates.

cond-mat↗

arXiv1997

Excitation energies from density functional perturbation theory

We consider two perturbative schemes to calculate excitation energies, each employing the Kohn-Sham Hamiltonian as the unperturbed system. Using accurate exchange-correlation potentials generated from essentially exact densities and their exchange components determined by a recently proposed method, we evaluate energy differences between the ground state and excited states in first-order perturbation theory for the Helium, ionized Lithium and Beryllium atoms. It was recently observed that the zeroth-order excitations energies, simply given by the difference of the Kohn-Sham eigenvalues, almost always lie between the singlet and triplet experimental excitations energies, corrected for relativistic and finite nuclear mass effects. The first-order corrections provide about a factor of two improvement in one of the perturbative schemes but not in the other. The excitation energies within perturbation theory are compared to the excitations obtained within $Δ$SCF and time-dependent density functional theory. We also calculate the excitation energies in perturbation theory using approximate functionals such as the local density approximation and the optimized effective potential method with and without the Colle-Salvetti correlation contribution.

cond-mat↗

arXiv1997

Accuracy of Electronic Wave Functions in Quantum Monte Carlo: the Effect of High-Order Correlations

Compact and accurate wave functions can be constructed by quantum Monte Carlo methods. Typically, these wave functions consist of a sum of a small number of Slater determinants multiplied by a Jastrow factor. In this paper we study the importance of including high-order, nucleus-three-electron correlations in the Jastrow factor. An efficient algorithm based on the theory of invariants is used to compute the high-body correlations. We observe significant improvements in the variational Monte Carlo energy and in the fluctuations of the local energies but not in the fixed-node diffusion Monte Carlo energies. Improvements for the ground states of physical, fermionic atoms are found to be smaller than those for the ground states of fictitious, bosonic atoms, indicating that errors in the nodal surfaces of the fermionic wave functions are a limiting factor.

cond-mat↗

arXiv1996

A critical assessment of the Self-Interaction Corrected Local Density Functional method and its algorithmic implementation

We calculate the electronic structure of several atoms and small molecules by direct minimization of the Self-Interaction Corrected Local Density Approximation (SIC-LDA) functional. To do this we first derive an expression for the gradient of this functional under the constraint that the orbitals be orthogonal and show that previously given expressions do not correctly incorporate this constraint. In our atomic calculations the SIC-LDA yields total energies, ionization energies and charge densities that are superior to results obtained with the Local Density Approximation (LDA). However, for molecules SIC-LDA gives bond lengths and reaction energies that are inferior to those obtained from LDA. The nonlocal BLYP functional, which we include as a representative GGA functional, outperforms both LDA and SIC-LDA for all ground state properties we considered.

cond-mat↗

arXiv1996

Monte Carlo Optimization of Trial Wave Functions in Quantum Mechanics and Statistical Mechanics

This review covers applications of quantum Monte Carlo methods to quantum mechanical problems in the study of electronic and atomic structure, as well as applications to statistical mechanical problems both of static and dynamic nature. The common thread in all these applications is optimization of many-parameter trial states, which is done by minimization of the variance of the local or, more generally for arbitrary eigenvalue problems, minimization of the variance of the configurational eigenvalue.

chem-ph↗

arXiv1996

Generalized gradient approximations to density functional theory: comparison with exact results

In order to assess the accuracy of commonly used approximate exchange-correlation density functionals, we present a comparison of accurate exchange and correlation potentials, exchange energy densities and energy components with the corresponding approximate quantities. Four systems are used as illustrative examples: the model system of two electrons in a harmonic potential and the He, Be and Ne atoms. A new ingredient in the paper is the separation of the exchange-correlation potential into exchange and correlation according to the density functional theory definition.

cond-mat↗

arXiv1996

Separation of the Exchange-Correlation Potential into Exchange plus Correlation: an Optimized Effective Potential Approach

Most approximate exchange-correlation functionals used within density functional theory are constructed as the sum of two distinct contributions for exchange and correlation. Separating the exchange component from the entire functional is useful since, for exchange, exact relations exist under uniform density scaling and spin scaling. In the past, accurate exchange-correlation potentials have been generated from essentially exact densities constructed using information from either quantum chemistry or quantum Monte Carlo calculations but they have not been correctly decomposed into their separate exchange and correlation components, except for two-electron systems. exchange and correlation components (except for two-electron systems). Using a recently proposed method, equivalent to the solution of an optimized effective potential problem with the corresponding orbitals replaced by the exact Kohn-Sham orbitals, we obtain the separation according to the density functional theory definition. We compare the results for the Ne and Be atoms with those obtained by the previously used approximate separation scheme.

cond-mat↗