Optical absorption in boron clusters B6 and B 6 + : a first principles configuration interaction singles approach

The linear optical absorption spectra in neutral boron cluster B₆ and cationic B₆ ⁺ are calculated using a first principles correlated electron approach. The geometries of several low-lying isomers of these clusters were optimized at the coupled-cluster singles doubles (CCSD) level of theory. With these optimized ground-state geometries, excited states of different isomers were computed using the configuration-interaction singles (CIS) approach. The many-body wavefunctions of various excited states have been analyzed and the nature of optical excitation involved are found to be of collective, plasmonic type. We also benchmark our CIS results against more sophisticated equation-of-motion (EOM) CCSD approach for a few isomers.     

Coupled-cluster and configuration-interaction calculations for odd-A heavy nuclei

We compare coupled-cluster (CC) and configuration-interaction (CI) results for 55Ni and 57Ni obtained in the pf-shell basis, focusing on the practical equation-of-motion (EOM) CC approximations that can be applied to systems with dozens of correlated fermions. The weight of the reference state and the strength of correlation effects are controlled by the gap between the f7/2 orbit and the f5/2, p3/2, p1/2 orbits. Independent of the gap, the CC methods with up to 2p-2h components in the cluster operator and 3p-2h/3h-2p components in the EOMCC excitation operator are more accurate than the computationally more demanding CI approach with up to 3p-3h excitations and almost as accurate as the even more demanding CI approach truncated at 4p-4h excitations.     

Self-consistent RPA based on a many-body vacuum

Self-Consistent RPA is extended in a way so that it is compatible with a variational ansatz for the ground-state wave function as a fermionic many-body vacuum. Employing the usual equation-of-motion technique, we arrive at extended RPA equations of the Self-Consistent RPA structure. In principle the Pauli principle is, therefore, fully respected. However, the correlation functions entering the RPA matrix can only be obtained from a systematic expansion in powers of some combinations of RPA amplitudes. We demonstrate for a model case that this expansion may converge rapidly.     

Correlated ground state of the Hubbard model

The variational many-body approach or, more generally, the method of correlated basis functions initiated for a quantitative analysis of strongly interacting quantum fluids may be adapted with minor modifications for exploring the properties of lattice models. This is demonstrated by performing an explicit analysis of the paramagnetic ground state of the Hubbard model. In a first step of the approximation scheme we represent the correlated state by a spin-dependent wave function of Jastrow-type. We analyze in detail the associated density-matrix elements and set up the corresponding Fermi hypernetted-chain equations which determine the irreducible constituents of these quantities. The solutions are discussed and constructed by iteration in terms of cluster approximants. Specializing the input data and the formal results provides a Fermi hypernetted-chain analysis of the correlations induced by a ground state wave function of the Gutzwiller form.     

Efficient electronic structure theory via hierarchical scale-adaptive coupled-cluster formalism: I. Theory and computational complexity analysis

ABSTRACT

A novel reduced-scaling, general-order coupled-cluster approach is formulated by exploiting hierarchical representations of many-body tensors, combined with the recently suggested formalism of scale-adaptive tensor algebra. Inspired by the hierarchical techniques from the renormalisation group approach, H/H²-matrix algebra and fast multipole method, the computational scaling reduction in our formalism is achieved via coarsening of quantum many-body interactions at larger interaction scales, thus imposing a hierarchical structure on many-body tensors of coupled-cluster theory. In our approach, the interaction scale can be defined on any appropriate Euclidean domain (spatial domain, momentum-space domain, energy domain, etc.). We show that the hierarchically resolved many-body tensors can reduce the storage requirements to O(N), where N is the number of simulated quantum particles. Subsequently, we prove that any connected many-body diagram consisting of a finite number of arbitrary-order tensors, e.g. an arbitrary coupled-cluster diagram, can be evaluated in O(NlogN) floating-point operations. On top of that, we suggest an additional approximation to further reduce the computational complexity of higher order coupled-cluster equations, i.e. equations involving higher than double excitations, which otherwise would introduce a large prefactor into formal O(NlogN) scaling.     

A Light-Front Coupled Cluster Method

A new method for the nonperturbative solution of quantum field theories is described. The method adapts the exponential-operator technique of the standard many-body coupled-cluster method to the Fock-space eigenvalue problem for light-front Hamiltonians. This leads to an effective eigenvalue problem in the valence Fock sector and a set of nonlinear integral equations for the functions that define the exponential operator. The approach avoids at least some of the difficulties associated with the Fock-space truncation usually used.     

Properties of advanced coupled-cluster Green's function

ABSTRACT

We present an extension of the analysis previously applied to the retarded part of the coupled cluster (CC) Green's function to its advanced part. In analogy to our earlier studies for the retarded part, we demonstrate that the advanced CC Green's function is expressed in terms of connected diagrams only, which is a direct consequence of algebraic form of equations satisfied by CC amplitudes. We also demonstrate that ω-derivatives of the advanced CC Green's function can be calculated analytically and can be expressed in terms of connected diagrams only. We analyse the structure of connected diagrams and the role of intermediate operators which satisfy electron affinity equation-of-motion CC-type conditions.     

Microscopic approach to many-exciton complexes in self-assembled InGaAs/GaAs quantum dots

We present a numerical calculation of many-exciton complexes in self-assembled InAs/GaAs quantum dots. We apply continuum elasticity theory and atomistic valence-force-field method to calculate strain distribution, and make use of various methods, ranging from a quasi-atomistic tight-binding approach to the single-band effective-mass approximation, to obtain single-particle energy levels. The effect of strain is incorporated by the deformation potential theory. We expand multiexciton states in the basis of Slater determinants and solve the many-body problem by the configuration-interaction method. The dynamics of multiexcitons is studied by solving the rate equations, from which the excitation–power dependence of emission spectrum is obtained. The emission spectra calculated by the microscopic tight-binding approach are found to be in good agreement with those obtained by the simple effective-mass method.     

On the connectivity criteria in the open-shell coupled-cluster theory for general model spaces

In this paper we study the following aspects of the open-shell coupled-cluster (CC) theories: (a) we examine the current theoretical status regarding the existence or non-existence of a linked-cluster theorem, ensuring the connectedness of the cluster amplitudes and the effective Hamiltonian; (b) we lay down the necessary and sufficient conditions for connectivity for a general (incomplete) model space, involving valence particles as well as valence holes; and (c) critically re-assess the earlier theoretical works from a comprehensive and unifying view point.     

Medium-dependent dynamics in Fermi systems from a pair-composite viewpoint

We examine the effects of medium dependence of the two-body dynamics on the many-body properties of Fermion systems, with approximation ultimately aimed at lower densities for all temperatures. The dynamics are initially treated in terms of a pair-composite formulation given previously, and the underlying single-Fermion nature of the pair constituents allows interpretation via more conventional thermal many-body formalism. This permits construction of coupled equations for composite amplitudes and bound states, single-particle energy and momentum distributions, and macroscopic thermodynamic properties. We explore differences between our results and those of traditional theories which incorporate two-body correlations in some fashion, and we display explicitly how correct limiting results are recovered from our equations when the density and/or coupling strength is decreased. Finally, we provide an interpretation of our results via a form of quasiparticle quantum cluster expansion analogous to the familiar particle quantum cluster expansion.     

Molecular cluster perturbation theory. I. Formalism

We present second-order molecular cluster perturbation theory (MCPT(2)), a linear scaling methodology to calculate arbitrarily large systems with explicit calculation of individual wave functions in a coupled-cluster framework. This new MCPT(2) framework uses coupled-cluster perturbation theory and an expansion in terms of molecular dimer interactions to obtain molecular wave functions that are infinite order in both the electronic fluctuation operator and all possible dimer (and products of dimers) interactions. The MCPT(2) framework has been implemented in the new SIA/Aces4 parallel architecture, making use of the advanced dynamic memory control and fine-grained parallelism to perform very large explicit molecular cluster calculations. To illustrate the power of this method, we have computed energy shifts, lattice site dipole moments, and harmonic vibrational frequencies via explicit calculation of the bulk system for the polar and non-polar polymorphs of solid hydrogen fluoride. The explicit lattice size (without using any periodic boundary conditions) was expanded up to 1000 HF molecules, with 32,000 basis functions and 10,000 electrons. Our obtained HF lattice site dipole moments and harmonic vibrational frequencies agree well with the existing literature.     

Green's Functions in Coupled-Cluster Form

The Green's function and coupled-cluster (CC) methods are two important tools of quantum many-body theory. It seems worthwhile to find their connection. In the present paper we demonstrate this connection and give the expressions of the Green's functions in the CC form. Diagrammatic techniques are used to write explicit algebraic expressions.     

Weighted-Residual Methods for the Solution of Two-Particle Lippmann–Schwinger Equation Without Partial-Wave Decomposition

Recently there has been a growing interest in computational methods for quantum scattering equations that avoid the traditional decomposition of wave functions and scattering amplitudes into partial waves. The aim of the present work is to show that the weighted-residual approach in combination with local basis functions give rise to convenient computational schemes for the solution of the multi-variable integral equations without the partial wave expansion. The weighted-residual approach provides a unifying framework for various variational and degenerate-kernel methods for integral equations of scattering theory. Using a direct-product basis of localized quadratic interpolation polynomials, Galerkin, collocation and Schwinger variational realizations of the weighted-residual approach have been implemented for a model potential. It is demonstrated that, for a given expansion basis, Schwinger variational method exhibits better convergence with basis size than Galerkin and collocation methods. A novel hybrid-collocation method is implemented with promising results as well.     

The many-body problem within the Lee model

The structure of a field theoretical many-body problem is studied within the (non-static) Lee model. The explicit solvability of the renormalization problem allows the investigation of renormalization corrections in many-particle systems. Herefore, the renormalized equations are worked out for the N-V scattering and for the binding-energy problem of “N-V matter” — these cases taken in analogy to nucleon-nucleon scattering and nuclear matter. The N-V matter equations are obtained from a cluster expansion suitably defined for the field theoretical case. The ansatz for the correlated wave functions is chosen in such a way as to generate a two-hole-line expansion of the binding energy. The renormalized form of this field theoretical extension of Brueckner theory is discussed in detail revealing the medium effects on renormalization.     

Two-dimensional integrodifferential equations for unequal mass particle systems

The two-variable Integrodifferential Equation Approach (IDEA) valid for A nucleons is generalized to describe quantum mechanical systems consisting of A, unequal mass, particles. The method is based on an expansion of the wave function in Faddeev amplitudes for the various particle pairs and a subsequent expansion of them in terms of Potential Harmonics. Projecting the resulting Faddeev-type equations on a specific two-body space and spin-isospin channel one obtains coupled, two-variable, integrodifferential equations describing the system. These equations can be readily applied, for example, to hypernuclear systems such as the double hypernucleus ΛΛα which can be handled either as a three- or as a six-body problem. We demonstrate our approach by applying it to various single and double hypernuclei and compare the results to those obtained by other methods.     

The logarithmic discretization embedded cluster approximation

This work proposes a new approach to study transport properties of highly correlated local structures. The method, dubbed the logarithmic discretization embedded cluster approximation (LDECA), consists of diagonalizing a finite cluster containing the many-body terms of the Hamiltonian and embedding it into the rest of the system, combined with Wilson's idea of a logarithmic discretization of the representation of the band. A many-body formalism provides a solid theoretical foundation to the method.     

On the hierarchy equations of the wave-operator for open-shell systems

Starting with the open-shell analogue of the Gell Mann-Low theorem of many-body perturbation theory, a non-perturbative linear operator equation is derived for the linked part of the wave-operatorW for open-shell systems. It is shown that, for a proper treatment of the linked nature of the wave-operator, a separation into its connected and disconnected components has to be made, and this leads to a hierarchy of equations for the various connected components. It is proved that the set of equations can be cast into a form equivalent to the non-perturbative equations of the wave-operator recently derived by Mukherjee and others in a coupled-cluster or exp(T) type formalism if a consistent use is made of a ‘core-valence separability’ condition introduced earlier. A comparison of the coupled-cluster representation ofW with the perturbative representation reveals that various alternative forms ofW in the coupled-cluster representation are possible and these reflect alternative ways of realising the core-valence expansion of the wave-operator. In particular it is emphasised how the use of Mandelstam block-ordering simplifies the coupled-cluster theories to a considerable extent and a comparison is made with coupled-cluster methods for open-shells put forward very recently by Ey and Lindgren. Finally, it is shown how difference energies of interest may be derived in a compact manner using the Mandelstam block-ordering of the wave-operator.     

Electron correlations and many-body techniques in magnetism

Recent progress in the theory of magnetism and electron correlations is reviewed to clarify the theories developed in the last decade and their mutual relations. A historical development of the theory of magnetism is outlined, and the dynamical coherent potential approximation (CPA) which completely takes account of the dynamical spin and charge fluctuations within the single-site approximation is introduced. Both the dynamical effects on various magnetic properties and the many-body band structure are shown to be explained on the same footing. It is shown that the dynamical CPA is equivalent to the other single-site theories of strongly correlated electrons: the many-body CPA, the dynamical mean-field theory (DMFT), and the projection operator method CPA (PM-CPA). These theories are elucidated with use of a common concept of effective medium or coherent potential. The effects of orbital degeneracy and the realistic calculation scheme are discussed with an emphasis on Hund’s rule coupling. Non-local theories of magnetism and electron correlations which go beyond the single-site approximation are presented. They include the molecular dynamics approach to the magnetic short range order, the dynamical cluster methods as a direct extension of the DMFT, and the self-consistent projection operator approach as an extension of the PM-CPA with use of the incremental cluster expansion. The current problems of their approaches and their future perspective are discussed.     

On the orbital dependence of compact,weight-selected configuration interaction and coupled-cluster wave functions

We recently reported that very compact coupled-cluster wave functions may be generated by selecting the most important configurations, by weight, from the full coupled-cluster wave function. Here, we consider how the choice of orbitals may affect these wave functions in the case of the symmetric dissociation of H₂O. We employ unrestricted Hartree–Fock and complete-active-space self-consistent-field orbitals, as well as natural orbitals derived from a coupled-cluster singles and doubles wave function. For a given accuracy, some choices of orbitals can reduce the size of configuration interaction wave functions, but they have little effect on the weight-selected coupled-cluster wave functions.