Search

Fanpy is a free and open-source Python library for developing and testing multideterminant wavefunctions and related ab initio methods in electronic structure theory. The main use of Fanpy is to quickly prototype new methods by making it easier to convert the mathematical formulation of a new wavefunction ansatze to a working implementation. Fanpy is designed based on our recently introduced Flexible Ansatz for N-electron Configuration Interaction (FANCI) framework, where multideterminant wavefunctions are represented by their overlaps with Slater determinants of orthonormal spin-orbitals. In the simplest case, a new wavefunction ansatz can be implemented by simply writing a function for evaluating its overlap with an arbitrary Slater determinant. Fanpy is modular in both implementation and theory: the wavefunction model, the system's Hamiltonian, and the choice of objective function are all independent modules. This modular structure makes it easy for users to mix and match different methods and for developers to quickly explore new ideas. Fanpy is written purely in Python with standard dependencies, making it accessible for various operating systems. In addition, it adheres to principles of modern software development, including comprehensive documentation, extensive testing, quality assurance, and continuous integration and delivery protocols. This article is considered to be the official release notes for the Fanpy library.

Eigenvectors of the reduced Bardeen-Cooper-Schrieffer (BCS) Hamiltonian, Richardson-Gaudin (RG) states, are used as a variational wavefunction ansatz for strongly correlated electronic systems. These states are geminal products whose coefficients are solutions of non-linear equations. Previous results showed an un-physical apparent avoided crossing in ground state dissociation curves for hydrogen chains. In this paper, it is shown that each seniority-zero state of the molecular Coulomb Hamiltonian corresponds directly to an RG state. However, the seniority-zero ground state does not correspond to the ground state of a reduced BCS Hamiltonian. The difficulty is in choosing the correct RG state. The systems studied showed a clear choice, and we expect that it should always be possible to reason physically which state to choose. Published under an exclusive license by AIP Publishing.

We are grateful for constructive comments from K.-L. Cai, O. Denisov, F. de Soto, T. Frederico, J. Friedrich, C. Mezrag, V. Mokeev, W.-D. Nowak, C. Quintans, G. Salme and J. Segovia. Work supported by: National Natural Science Foundation of China (Grant nos. 12135007, 11805097); Helmholtz-Zentrum Dresden-Rossendorf High Potential Programme; Spanish Ministry of Science and Innovation (MICINN) (Grant nos. PID2020-113334GB, PID2019-107844GBC22); Generalitat Valenciana (Grant no. Prometeo/2019/087); Junta de Andalucia (Grant nos. P18-FR-5057, UHU-1264517, UHU EPIT2021); and STRONG-2020 "The strong interaction at the frontier of knowledge: fundamental research and applications" which received funding from the European Union's Horizon 2020 research and innovation programme (grant no. 824093)., Analyses of the pion valence-quark distribution function (DF), u(pi) (x; sigma), which explicitly incorporate the behaviour of the pion wave function prescribed by quantum chromodynamics (QCD), predict u(pi) (x similar or equal to 1; sigma) similar to (1 - x)(beta(sigma)), beta(sigma greater than or similar to m(p)) > 2, where mp is the proton mass. Nevertheless, more than forty years after the first experiment to collect data suitable for extracting the x similar or equal to 1 behaviour of up, the empirical status remains uncertain because some methods used to fit existing data return a result for up that violates this constraint. Such disagreement entails one of the following conclusions: the analysis concerned is incomplete; not all data being considered are a true expression of qualities intrinsic to the pion; or QCD, as it is currently understood, is not the theory of strong interactions. New, precise data are necessary before a final conclusion is possible. In developing these positions, we exploit a single proposition, viz. there is an effective charge which defines an evolution scheme for parton DFs that is all-orders exact. This proposition has numerous corollaries, which can be used to test the character of any DF, whether fitted or calculated., National Natural Science Foundation of China (NSFC) 12135007 11805097, Spanish Government European Commission PID2020-113334GB PID2019-107844GBC22, Generalitat Valenciana European Commission, General Electric Prometeo/2019/087, Junta de Andalucia P18-FR-5057 UHU-1264517 UHU EPIT2021, STRONG-2020 "The strong interaction at the frontier of knowledge: fundamental research and applications" - European Union's Horizon 2020 research and innovation programme 824093, Helmholtz-Zentrum Dresden-Rossendorf High Potential Programme

We compute the differential yield for quark anti-quark dijet production in high-energy electron-proton and electron-nucleus collisions at small $x$ as a function of the relative momentum $\boldsymbol{P}_\perp$ and momentum imbalance $\boldsymbol{k}_\perp$ of the dijet system for different photon virtualities $Q^2$, and study the elliptic and quadrangular anisotropies in the relative angle between $\boldsymbol{P}_\perp$ and $\boldsymbol{k}_\perp$. We review and extend the analysis in [1], which compared the results of the Color Glass Condensate (CGC) with those obtained using the transverse momentum dependent (TMD) framework. In particular, we include in our comparison the improved TMD (ITMD) framework, which resums kinematic power corrections of the ratio $k_\perp$ over the hard scale $Q_\perp$. By comparing ITMD and CGC results we are able to isolate genuine higher saturation contributions in the ratio $Q_s/Q_\perp$ which are resummed only in the CGC. These saturation contributions are in addition to those in the Weizs\"ackerWilliams gluon TMD that appear in powers of $Q_s/k_\perp$. We provide numerical estimates of these contributions for inclusive dijet production at the future Electron-Ion Collider, and identify kinematic windows where they can become relevant in the measurement of dijet and dihadron azimuthal correlations. We argue that such measurements will allow the detailed experimental study of both kinematic power corrections and genuine gluon saturation effects., Comment: v3: typos corrected post-publication. v2: 52 pages, 13 figures, matches published version

We study coherent diffractive photon and vector meson production in electron-proton and electron-nucleus collisions within the Color Glass Condensate effective field theory. We show that electron-photon and electron-vector meson azimuthal angle correlations are sensitive to non-trivial spatial correlations in the gluon distribution of the target, and perform explicit calculations using spatially dependent McLerran-Venugopalan initial color charge configurations coupled to the numerical solution of small $x$ JIMWLK evolution equations. We compute the cross-section differentially in $Q^2$ and $|t|$ and find sizeable anisotropies in the electron-photon and electron-$\mathrm{J}/��$ azimuthal correlations ($v_{1,2} \approx 2 - 10 \%$) in electron-proton collisions for the kinematics of the future Electron-Ion Collider. In electron-gold collisions these modulations are found to be significantly smaller ($v_{1,2}, 32 figures, 18 figures

We develop an extension of the Gutzwiller Approximation (GA) formalism that includes the effects of Coulomb interactions of arbitrary range (including density density, exchange, pair hopping and Coulomb assisted hopping terms). This formalism reduces to the ordinary GA formalism for the multi-band Hubbard models in the presence of only local interactions. This is accomplished by combining the 1/z expansion -- where z is the coordination number and only the leading order terms contribute in the limit of infinite dimensions -- with a P^2-I expansion, where P is the Gutzwiller projector. The method is conveniently formulated in terms of a Gutzwiller Lagrange function. We apply our theory to the extended single band Hubbard model. Similarly to the usual Brinkman-Rice mechanism we find a Mott transition. A valence skipping transition is observed, where the occupation of the empty and doubly occupied states for the Gutzwiller wavefunction is enhanced with respect to the uncorrelated Slater determinant wavefunction., 13+23 pages (1+4 figures) comments welcome; v2: typos corrected, submitted to PRB; v3: Added Section II which presents our results in a simple intuitive manner

Building on the success of Quantum Monte Carlo techniques such as diffusion Monte Carlo, alternative stochastic approaches to solve electronic structure problems have emerged over the past decade. The full configuration interaction quantum Monte Carlo (FCIQMC) method allows one to systematically approach the exact solution of such problems, for cases where very high accuracy is desired. The introduction of FCIQMC has subsequently led to the development of coupled cluster Monte Carlo (CCMC) and density matrix quantum Monte Carlo (DMQMC), allowing stochastic sampling of the coupled cluster wave function and the exact thermal density matrix, respectively. In this Article, we describe the HANDE-QMC code, an open source implementation of FCIQMC, CCMC and DMQMC, including initiator and semistochastic adaptations. We describe our code and demonstrate its use on three example systems; a molecule (nitric oxide), a model solid (the uniform electron gas), and a real solid (diamond). An illustrative tutorial is also included. Public domain – authored by a U.S. government employee

In methods like geminal-based approaches or coupled cluster that are solved using the projected Schr\"odinger equation, direct computation of the 2-electron reduced density matrix (2-RDM) is impractical and one falls back to a 2-RDM based on response theory. However, the 2-RDMs from response theory are not $N$-representable. That is, the response 2-RDM does not correspond to an actual physical $N$-electron wave function. We present a new algorithm for making these non-$N$-representable 2-RDMs approximately $N$-representable, i.e. it has the right symmetry and normalization and it fulfills the $P$-, $Q$- and $G$-conditions. Next to an algorithm which can be applied to any 2-RDM, we have also developed a 2-RDM optimization procedure specifically for seniority-zero 2-RDMs. We aim to find the 2-RDM with the right properties that is the closest (in the sense of the Frobenius norm) to the non-N-representable 2-RDM by minimizing the square norm of the difference between the initial 2-RDM and the targeted 2-RDM under the constraint that the trace is normalized and the 2-RDM, $Q$- and $G$-matrices are positive semidefinite, i.e. their eigenvalues are non-negative. Our method is suitable for fixing non-N-respresentable 2-RDMs which are close to being N-representable. Through the N-representability optimization algorithm we add a small correction to the initial 2-RDM such that it fulfills the most important N-representability conditions., Comment: 13 pages, 8 figures

We present a new variational tree tensor network state (TTNS) ansatz, the three-legged tree tensor network state (T3NS). Physical tensors are interspersed with branching tensors. Physical tensors have one physical index and at most two virtual indices, as in the matrix product state (MPS) ansatz of the density matrix renormalization group (DMRG). Branching tensors have no physical index, but up to three virtual indices. In this way, advantages of DMRG, in particular a low computational cost and a simple implementation of symmetries, are combined with advantages of TTNS, namely incorporating more entanglement. Our code is capable of simulating quantum chemical Hamiltonians, and we present several proof-of-principle calculations on LiF, N$_2$ and the bis($\mu$-oxo) and $\mu - \eta^2 : \eta^2$ peroxo isomers of $[\mathrm{Cu}_2\mathrm{O}_2]^{2+}$., Comment: 14 pages, 8 figures

We present the inner products of eigenstates in integrable Richardson-Gaudin models from two different perspectives and derive two classes of Gaudin-like determinant expressions for such inner products. The requirement that one of the states is on-shell arises naturally by demanding that a state has a dual representation. By implicitly combining these different representations, inner products can be recast as domain wall boundary partition functions. The structure of all involved matrices in terms of Cauchy matrices is made explicit and used to show how one of the classes returns the Slavnov determinant formula. This framework provides a further connection between two different approaches for integrable models, one in which everything is expressed in terms of rapidities satisfying Bethe equations, and one in which everything is expressed in terms of the eigenvalues of conserved charges, satisfying quadratic equations., 21+16 pages, minor revisions compared to the previous version

We present the extension of variational Monte Carlo (VMC) to the calculation of electronic excitation energies and oscillator strengths using time-dependent linear-response theory. By exploiting the analogy existing between the linear method for wave-function optimisation and the generalised eigenvalue equation of linear-response theory, we formulate the equations of linear-response VMC (LR-VMC). This LR-VMC approach involves the first-and second-order derivatives of the wave function with respect to the parameters. We perform first tests of the LR-VMC method within the Tamm-Dancoff approximation using single-determinant Jastrow-Slater wave functions with different Slater basis sets on some singlet and triplet excitations of the beryllium atom. Comparison with reference experimental data and with configuration-interaction-singles (CIS) results shows that LR-VMC generally outperforms CIS for excitation energies and is thus a promising approach for calculating electronic excited-state properties of atoms and molecules., Advances in Quantum Chemistry, 2017, Novel Electronic Structure Theory: General Innovations and Strongly Correlated Systems

The electric dipole polarizability quantifies the low-energy behaviour of the dipole strength and is related to critical observables such as the radii of the proton and neutron distributions. Its computation is challenging because most of the dipole strength lies in the scattering continuum. In this paper we combine integral transforms with the coupled-cluster method and compute the dipole polarizability using bound-state techniques. Employing different interactions from chiral effective field theory, we confirm the strong correlation between the dipole polarizability and the charge radius, and study its dependence on three-nucleon forces. We find good agreement with data for the 4He, 40Ca, and 16O nuclei, and predict the dipole polarizability for the rare nucleus 22O., 12 pages, 11 figures

A first quantized free photon is a complex massless vector field $A=(A^\mu)$ whose field strength satisfies Maxwell's equations in vacuum. We construct the Hilbert space $\mathscr{H}$ of the photon by endowing the vector space of the fields $A$ in the temporal-Coulomb gauge with a positive-definite and relativistically invariant inner product. We give an explicit expression for this inner product, identify the Hamiltonian for the photon with the generator of time translations in $\mathscr{H}$, determine the operators representing the momentum and the helicity of the photon, and introduce a chirality operator whose eigenfunctions correspond to fields having a definite sign of energy. We also construct a position operator for the photon whose components commute with each other and with the chirality and helicity operators. This allows for the construction of the localized states of the photon with a definite sign of energy and helicity. We derive an explicit formula for the latter and compute the corresponding electric and magnetic fields. These turn out to diverge not just at the point where the photon is localized but on a plane containing this point. We identify the axis normal to this plane with an associated symmetry axis, and show that each choice of this axis specifies a particular position operator, a corresponding position basis, and a position representation of the quantum mechanics of photon. In particular, we examine the position wave functions determined by such a position basis, elucidate their relationship with the Riemann-Silberstein and Landau-Peierls wave functions, and give an explicit formula for the probability density of the spatial localization of the photon., Comment: 35 pages, 2 figures, slightly expanded published version

We present results of the first ab initio lattice QCD calculation of the normalization constants and first moments of the leading twist distribution amplitudes of the full baryon octet, corresponding to the small transverse distance limit of the associated S-wave light-cone wave functions. The P-wave (higher twist) normalization constants are evaluated as well. The calculation is done using N-f = 2 + 1 flavors of dynamical (clover) fermions on lattices of different volumes and pion masses down to 222 MeV. Significant SU(3) flavor symmetry violation effects in the shape of the distribution amplitudes are observed., SCOAP3

Semilocal density functional theory is the most used computational method for electronic structure calculations in theoretical solid-state physics and quantum chemistry of large systems, providing good accuracy with a very attractive computational cost. Nevertheless, because of the non-locality of the exchange-correlation hole outside a metal surface, it was always considered inappropriate to describe the correct surface asymptotics. Here, we derive, within the semilocal density functional theory formalism, an exact condition for the image-like surface asymptotics of both the exchange-correlation energy per particle and potential. We show that this condition can be easily incorporated into a practical computational tool, at the simple meta-generalized-gradient approximation level of theory. Using this tool, we also show that the Airy-gas model exhibits asymptotic properties that are closely related to the ones at metal surfaces. This result highlights the relevance of the linear effective potential model to the metal surface asymptotics., Comment: 6 pages, 4 figures

Density matrix embedding theory (DMET) provides a theoretical framework to treat finite fragments in the presence of a surrounding molecular or bulk environment, even when there is significant correlation or entanglement between the two. In this work, we give a practically oriented and explicit description of the numerical and theoretical formulation of DMET. We also describe in detail how to perform self-consistent DMET optimizations. We explore different embedding strategies with and without a self-consistency condition in hydrogen rings, beryllium rings, and a sample S$_{\text{N}}$2 reaction. The source code for the calculations in this work can be obtained from \url{https://github.com/sebwouters/qc-dmet}., Comment: 41 pages, 10 figures

We present an efficient approach to the electron correlation problem that is well-suited for strongly interacting many-body systems, but requires only mean-field-like computational cost. %which is based on orbital optimization of electron pairs. The performance of our approach is illustrated for the one-dimensional Hubbard model with periodic boundary conditions for different chain lengths, and for the non-relativistic quantum chemical Hamiltonian exploring the symmetric dissociation of the H$_{50}$ hydrogen chain., 4 pages, 4 figures

The density matrix renormalization group (DMRG) has become an indispensable numerical tool to find exact eigenstates of finite-size quantum systems with strong correlation. In the fields of condensed matter, nuclear structure and molecular electronic structure, it has significantly extended the system sizes that can be handled compared to full configuration interaction, without losing numerical accuracy. For quantum chemistry (QC), the most efficient implementations of DMRG require the incorporation of particle number, spin and point group symmetries in the underlying matrix product state (MPS) ansatz, as well as the use of so-called complementary operators. The symmetries introduce a sparse block structure in the MPS ansatz and in the intermediary contracted tensors. If a symmetry is non-abelian, the Wigner-Eckart theorem allows to factorize a tensor into a Clebsch-Gordan coefficient and a reduced tensor. In addition, the fermion signs have to be carefully tracked. Because of these challenges, implementing DMRG efficiently for QC is not straightforward. Efficient and freely available implementations are therefore highly desired. In this work we present CheMPS2, our free open-source spin-adapted implementation of DMRG for ab initio QC. Around CheMPS2, we have implemented the augmented Hessian Newton-Raphson complete active space self-consistent field method, with exact Hessian. The bond dissociation curves of the 12 lowest states of the carbon dimer were obtained at the DMRG(28 orbitals, 12 electrons, D$_{\mathsf{SU(2)}}$=2500)/cc-pVDZ level of theory. The contribution of $1s$ core correlation to the $X^1\Sigma_g^+$ bond dissociation curve of the carbon dimer was estimated by comparing energies at the DMRG(36o, 12e, D$_{\mathsf{SU(2)}}$=2500)/cc-pCVDZ and DMRG-SCF(34o, 8e, D$_{\mathsf{SU(2)}}$=2500)/cc-pCVDZ levels of theory., Comment: 16 pages, 13 figures

During the past 15 years, the density matrix renormalization group (DMRG) has become increasingly important for ab initio quantum chemistry. Its underlying wavefunction ansatz, the matrix product state (MPS), is a low-rank decomposition of the full configuration interaction tensor. The virtual dimension of the MPS, the rank of the decomposition, controls the size of the corner of the many-body Hilbert space that can be reached with the ansatz. This parameter can be systematically increased until numerical convergence is reached. The MPS ansatz naturally captures exponentially decaying correlation functions. Therefore DMRG works extremely well for noncritical one-dimensional systems. The active orbital spaces in quantum chemistry are however often far from one-dimensional, and relatively large virtual dimensions are required to use DMRG for ab initio quantum chemistry (QC-DMRG). The QC-DMRG algorithm, its computational cost, and its properties are discussed. Two important aspects to reduce the computational cost are given special attention: the orbital choice and ordering, and the exploitation of the symmetry group of the Hamiltonian. With these considerations, the QC-DMRG algorithm allows to find numerically exact solutions in active spaces of up to 40 electrons in 40 orbitals., Comment: 24 pages; 10 figures; based on arXiv:1405.1225; invited review for European Physical Journal D

The similarities between Hartree-Fock (HF) theory and the density-matrix renormalization group (DMRG) are explored. Both methods can be formulated as the variational optimization of a wave-function ansatz. Linearization of the time-dependent variational principle near a variational minimum allows to derive the random phase approximation (RPA). We show that the non-redundant parametrization of the matrix product state (MPS) tangent space [J. Haegeman et al., Phys. Rev. Lett. 107, 070601 (2011)] leads to the Thouless theorem for MPS, i.e. an explicit non-redundant parametrization of the entire MPS manifold, starting from a specific MPS reference. Excitation operators are identified, which extends the analogy between HF and DMRG to the Tamm-Dancoff approximation (TDA), the configuration interaction (CI) expansion, and coupled cluster theory. For a small one-dimensional Hubbard chain, we use a CI-MPS ansatz with single and double excitations to improve on the ground state and to calculate low-lying excitation energies. For a symmetry-broken ground state of this model, we show that RPA-MPS allows to retrieve the Goldstone mode. We also discuss calculations of the RPA-MPS correlation energy. With the long-range quantum chemical Pariser-Parr-Pople Hamiltonian, low-lying TDA-MPS and RPA-MPS excitation energies for polyenes are obtained., Comment: 16 pages, 3 figures and 1 table

We report a theoretical study of the collective optical response of a two-dimensional array of nonlinear cavities in the impenetrable photon regime under a strong artificial magnetic field. Taking advantage of the non-equilibrium nature of the photon gas, we propose an experimentally viable all-optical scheme to generate and detect strongly correlated photon states which are optical analogs of the Laughlin states of fractional quantum Hall physics., 6 pages including the Supplemental Material (accepted for publication in Phys. Rev. Lett.)

We present a time-dependent density-functional method able to describe the photoelectron spectrum of atoms and molecules when excited by laser pulses. This computationally feasible scheme is based on a geometrical partitioning that efficiently gives access to photoelectron spectroscopy in time-dependent density-functional calculations. By using a geometrical approach, we provide a simple description of momentum-resolved photoemission including multiphoton effects. The approach is validated by comparison with results in the literature and exact calculations. Furthermore, we present numerical photoelectron angular distributions for randomly oriented nitrogen molecules in a short near-infrared intense laser pulse and helium-(I) angular spectra for aligned carbon monoxide and benzene., Financial suport was provided by Spanish (FIS2011-65702-C02-01 and PIB2010US-00652), ACI-Promociona (ACI2009-1036), Grupos Consolidados UPV/EHU del Gobierno Vasco (IT-319-07), and the European Research Council Advanced Grant DYNamo (ERC-2010-AdG–Proposal No. 267374). Computational time was granted by i2basque and BSC Red Espanola de Supercomputacion. M.A.L.M. acknowledges support from the French ANR (ANR-08-CEXC8-008-01).

We calculate the linear and non-linear susceptibilities of periodic longitudinal chains of hydrogen dimers with different bond-length alternations using a diffusion quantum Monte Carlo approach. These quantities are derived from the changes in electronic polarization as a function of applied finite electric field - an approach we recently introduced and made possible by the use of a Berry-phase, many-body electric-enthalpy functional. Calculated susceptibilities and hyper-susceptibilities are found to be in excellent agreement with the best estimates available from quantum chemistry - usually extrapolations to the infinite-chain limit of calculations for chains of finite length. It is found that while exchange effects dominate the proper description of the susceptibilities, second hyper-susceptibilities are greatly affected by electronic correlations. We also assess how different approximations to the nodal surface of the many-body wavefunction affect the accuracy of the calculated susceptibilities., 9 pages; accepted on J. Chem. Phys

We perform $GW$ calculations on atoms and diatomic molecules at different levels of self-consistency and investigate the effects of self-consistency on total energies, ionization potentials and on particle number conservation. We further propose a partially self-consistent $GW$ scheme in which we keep the correlation part of the self-energy fixed within the self-consistency cycle. This approximation is compared to the fully self-consistent $GW$ results and to the $G W_0$ and the $G_0W_0$ approximations. Total energies, ionization potentials and two-electron removal energies obtained with our partially self-consistent $GW$ approximation are in excellent agreement with fully self-consistent $GW$ results while requiring only a fraction of the computational effort. We also find that self-consistent and partially self-consistent schemes provide ionization energies of similar quality as the $G_0W_0$ values but yield better total energies and energy differences., 11 pages, 3 figures, 3 tables

We present a quantum Monte Carlo study of the hydrogen-benzene system where binding is very weak. We demonstrate that the binding is well described at both variational Monte Carlo (VMC) and diffusion Monte Carlo (DMC) levels by a Jastrow correlated single determinant geminal wave function with an optimized compact basis set that includes diffuse orbitals. Agreement between VMC and fixed-node DMC binding energies is found to be within 0.18 mHa, suggesting the calculations are well-converged with respect to the basis. Essentially the same binding is also found in independent DMC calculations using a different trial wave function of a more conventional Slater-Jastrow form, supporting our conclusion that the binding energy is accurate and includes all effects of correlation. We compare with empirical models and previous calculations, and we discuss the physical mechanisms of the interaction, the role of diffuse basis functions, and the charge redistribution in the bond., Comment: 12 pages, 4 figures

We theoretically study the efficiency of energy harvesting in linear exciton chains with an energy bias, where the initial excitation is taking place at the high-energy end of the chain and the energy is harvested (trapped) at the other end. The efficiency is characterized by means of the average time for the exciton to be trapped after the initial excitation. The exciton transport is treated as the intraband energy relaxation over the states obtained by numerically diagonalizing the Frenkel Hamiltonian that corresponds to the biased chain. The relevant intraband scattering rates are obtained from a linear exciton-phonon interaction. Numerical solution of the Pauli master equation that describes the relaxation and trapping processes, reveals a complicated interplay of factors that determine the overall harvesting efficiency. Specifically, if the trapping step is slower than or comparable to the intraband relaxation, this efficiency shows a nonmonotonic dependence on the bias: it first increases when introducing a bias, reaches a maximum at an optimal bias value, and then decreases again because of dynamic (Bloch) localization of the exciton states. Effects of on-site (diagonal) disorder, leading to Anderson localization, are addressed as well., Comment: 9 pages, 6 figures, to appear in Journal of Chemical Physics

4 pages.-- ISI Article Identifier: 000248297600103.-- ArXiv pre-print available at: http://arxiv.org/abs/hep-ph/0610287, Contribution to: Few-Body Problems in Physics - FB 18, 18th International IUPAP Conference on Few-Body Problems in Physics (Santos, Brazil, Aug 21-26, 2006)., We present an exact method based on a hyperspherical harmonic expansion to study systems made of quarks and antiquarks of the same flavor. Our formalism reproduces and improves the results obtained with variational approaches. This analysis shows that identical-flavor four-quark systems with non-exotic 2(++) quantum numbers may be bound independently of the quark mass. 0(+-) and 1(+-) states become attractive only for larger quarks masses., This work has been partially funded by MCyT under Contract No. FPA2004-05616, by JCyL under Contract No. SA104/04, and by GV under Contract No. GV05/276.

Based on exact limits and quantum Monte Carlo simulations, we obtain, at any density and spin polarization, an accurate estimate for the energy of a modified homogeneous electron gas where electrons repel each other only with a long-range coulombic tail. This allows us to construct an analytic local-spin-density exchange-correlation functional appropriate to new, multideterminantal versions of the density functional theory, where quantum chemistry and approximate exchange-correlation functionals are combined to optimally describe both long- and short-range electron correlations., Comment: revised version, ti appear in PRB

The question of how density functional theory (DFT) compares with Hartree-Fock (HF) for the computation of momentum-space properties is addressed in relation to systems for which (near) exact Kohn-Sham (KS) and HF one-electron matrices are known. This makes it possible to objectively compare HF and exact KS and hence to assess the potential of DFT for momentum space studies. The systems considered are the Moshinsky atom, the Hooke's atom and light two-electron ions, for which expressions for correlated density-matrices or momentum densities have been derived in closed-form. The results obtained show that it is necessary to make a distinction between true and approximate DFT., Comment: 30 pages, accepted for publication in J. Chem. Phys. (2006)

We discuss the application of an extended version of the coupled cluster method to systems exhibiting a quantum phase transition. We use thr lattice O(4) nonlinear sigma model in (1 + 1) and (3 + 1) dimensions as an example. We show how simple predictions get modified, leading to the absence of a phase transition in (1 + 1) dimensions, and strong indications for a phase transition in (3 + 1) dimensions.

In this article, we present new results of high-order coupled cluster method (CCM) calculations, based on a N\'eel model state with spins aligned in the $z$-direction, for both the ground- and excited-state properties of the spin-half {\it XXZ} model on the linear chain, the square lattice, and the simple cubic lattice. In particular, the high-order CCM formalism is extended to treat the excited states of lattice quantum spin systems for the first time. Completely new results for the excitation energy gap of the spin-half {\it XXZ} model for these lattices are thus determined. These high-order calculations are based on a localised approximation scheme called the LSUB$m$ scheme in which we retain all $k$-body correlations defined on all possible locales of $m$ adjacent lattice sites ($k \le m$). The ``raw'' CCM LSUB$m$ results are seen to provide very good results for the ground-state energy, sublattice magnetisation, and the value of the lowest-lying excitation energy for each of these systems. However, in order to obtain even better results, two types of extrapolation scheme of the LSUB$m$ results to the limit $m \to \infty$ (i.e., the exact solution in the thermodynamic limit) are presented. The extrapolated results provide extremely accurate results for the ground- and excited-state properties of these systems across a wide range of values of the anisotropy parameter., Comment: 31 Pages, 5 Figures

We report a systematic study of the weak chemical bond between two benzene molecules. We first show that it is possible to obtain a very good description of the C_2 dimer and the benzene molecule, by using pseudopotentials for the chemically inert 1s electrons, and a resonating valence bond wave function as a variational ansatz, expanded on a relatively small Gaussian basis set. We employ an improved version of the stochastic reconfiguration technique to optimize the many-body wave function, which is the starting point for highly accurate simulations based on the lattice regularized diffusion Monte Carlo (LRDMC) method. This projection technique provides a rigorous variational upper bound for the total energy, even in the presence of pseudopotentials, and allows to improve systematically the accuracy of the trial wave function, which already yields a large fraction of the dynamical and non-dynamical electron correlation. We show that the energy dispersion of two benzene molecules in the parallel displaced geometry is significantly deeper than the face-to-face configuration. However, contrary to previous studies based on post Hartree-Fock methods, the binding energy remains weak (~ 2 kcal/mol) also in this geometry, and its value is in agreement with the most accurate and recent experimental findings., Comment: 12 pages, 6 figures, submitted to the Journal of Chemical Physics

In this article, new results are presented for the zero-temperature ground-state properties of the spin-half transverse Ising model on various lattices using three different approximate techniques. These are, respectively, the coupled cluster method, the correlated basis function method, and the variational quantum Monte Carlo method. The methods, at different levels of approximation, are used to study the ground-state properties of these systems, and the results are found to be in excellent agreement both with each other and with results of exact calculations for the linear chain and results of exact cumulant series expansions for lattices of higher spatial dimension. The different techniques used are compared and contrasted in the light of these results, and the constructions of the approximate ground-state wave functions are especially discussed., Comment: 28 Pages, 4 Figures, 1 Table

The NL-eEDM collaboration is building an experimental setup to search for the permanent electric dipole moment of the electron in a slow beam of cold barium fluoride molecules [Eur. Phys. J. D, 72, 197 (2018)]. Knowledge of molecular properties of BaF is thus needed to plan the measurements and in particular to determine an optimal laser-cooling scheme. Accurate and reliable theoretical predictions of these properties require incorporation of both high-order correlation and relativistic effects in the calculations. In this work theoretical investigations of the ground and the lowest excited states of BaF and its lighter homologues, CaF and SrF, are carried out in the framework of the relativistic Fock-space coupled cluster (FSCC) and multireference configuration interaction (MRCI) methods. Using the calculated molecular properties, we determine the Franck-Condon factors (FCFs) for the $A^2\Pi_{1/2} \rightarrow X^2\Sigma^{+}_{1/2}$ transition, which was successfully used for cooling CaF and SrF and is now considered for BaF. For all three species, the FCFs are found to be highly diagonal. Calculations are also performed for the $B^2\Sigma^{+}_{1/2} \rightarrow X^2\Sigma^{+}_{1/2}$ transition recently exploited for laser-cooling of CaF; it is shown that this transition is not suitable for laser-cooling of BaF, due to the non-diagonal nature of the FCFs in this system. Special attention is given to the properties of the $A'^2\Delta$ state, which in the case of BaF causes a leak channel, in contrast to CaF and SrF species where this state is energetically above the excited states used in laser-cooling. We also present the dipole moments of the ground and the excited states of the three molecules and the transition dipole moments (TDMs) between the different states., Comment: Minor changes; The following article has been submitted to the Journal of Chemical Physics. After it is published, it will be found at https://publishing.aip.org/resources/librarians/products/journals/