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arXiv:2310.17172 · Electronic Structure

Integrating subsystem embedding subalgebras and coupled cluster Green’s function: a theoretical foundation for quantum embedding in excitation manifold

Bo Peng, Karol Kowalski

Published Jan 12, 2024• 3 citations
arXivHTMLPDF

Abstract

Abstract In this study, we introduce a novel approach to coupled-cluster Green’s function (CCGF) embedding by seamlessly integrating conventional CCGF theory with the state-of-the-art sub-system embedding sub-algebras coupled cluster (SES-CC) formalism. This integration focuses primarily on delineating the characteristics of the sub-system and the corresponding segments of the Green’s function, defined explicitly by active orbitals. Crucially, our work involves the adaptation of the SES-CC paradigm, addressing the left eigenvalue problem through a distinct form of Hamiltonian similarity transformation. This advancement not only facilitates a comprehensive representation of the interaction between the embedded sub-system and its surrounding environment but also paves the way for the quantum mechanical description of multiple embedded domains, particularly by employing the emergent quantum flow algorithms. Our theoretical underpinnings further set the stage for a generalization to multiple embedded sub-systems. This expansion holds significant promise for the exploration and application of non-equilibrium quantum systems, enhancing the understanding of system–environment interactions. In doing so, the research underscores the potential of SES-CC embedding within the realm of quantum computations and multi-scale simulations, promising a good balance between accuracy and computational efficiency.

DOI
10.1088/2516-1075/ad1e3b

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Abstract In this study, we introduce a novel approach to coupled-cluster Green’s function (CCGF) embedding by seamlessly integrating conventional CCGF theory with the state-of-the-art sub-system embedding sub-algebras coupled cluster (SES-CC) formalism. This integration focuses primarily on delineating the characteristics of the sub-system and the corresponding segments of the Green’s function, defined explicitly by active orbitals. Crucially, our work involves the adaptation of the SES-CC paradigm, addressing the left eigenvalue problem through a distinct form of Hamiltonian similarity transformation. This advancement not only facilitates a comprehensive representation of the interaction between the embedded sub-system and its surrounding environment but also paves the way for the quantum mechanical description of multiple embedded domains, particularly by employing the emergent quantum flow algorithms. Our theoretical underpinnings further set the stage for a generalization to multiple embedded sub-systems. This expansion holds significant promise for the exploration and application of non-equilibrium quantum systems, enhancing the understanding of system–environment interactions. In doing so, the research underscores the potential of SES-CC embedding within the realm of quantum computations and multi-scale simulations, promising a good balance between accuracy and computational efficiency.
In this paper, we discuss the extension of the recently introduced subsystem embedding subalgebra coupled cluster (SES-CC) formalism to unitary CC formalisms. In analogy to the standard single-reference SES-CC formalism, its unitary CC extension allows one to include the dynamical (outside the active space) correlation effects in an SES induced complete active space (CAS) effective Hamiltonian. In contrast to the standard single-reference SES-CC theory, the unitary CC approach results in a Hermitian form of the effective Hamiltonian. Additionally, for the double unitary CC (DUCC) formalism, the corresponding CAS eigenvalue problem provides a rigorous separation of external cluster amplitudes that describe dynamical correlation effects—used to define the effective Hamiltonian—from those corresponding to the internal (inside the active space) excitations that define the components of eigenvectors associated with the energy of the entire system. The proposed formalism can be viewed as an efficient way of downfolding many-electron Hamiltonian to the low-energy model represented by a particular choice of CAS. In principle, this technique can be extended to any type of CAS representing an arbitrary energy window of a quantum system. The Hermitian character of low-dimensional effective Hamiltonians makes them an ideal target for several types of full configuration interaction type eigensolvers. As an example, we also discuss the algebraic form of the perturbative expansions of the effective DUCC Hamiltonians corresponding to composite unitary CC theories and discuss possible algorithms for hybrid classical and quantum computing. Given growing interest in quantum computing, we provide energies for H2 and Be systems obtained with the quantum phase estimator algorithm available in the Quantum Development Kit for the approximate DUCC Hamiltonians.
We discuss reduced-scaling strategies employing the recently introduced subsystem embedding subalgebra (SES) coupled-cluster (CC) formalism to describe quantum many-body systems. These strategies utilize properties of the SES CC formulations where the equations describing certain classes of subsystems can be integrated into computational flows composed of coupled eigenvalue problems of reduced dimensionality. Additionally, these flows can be determined at the level of the CC ansatz by the inclusion of selected classes of cluster amplitudes, which define the wave-function ``memory'' of possible partitioning of the many-body system into constituent subsystems. One of the possible ways of solving these coupled problems is through implementing procedures where the information is passed between the subsystems in a self-consistent manner. As a special case we consider local flow formulations where the local character of correlation effects can be closely related to the properties of subsystem embedding subalgebras employing a localized molecular basis. We also generalize flow equations to the time domain and to downfolding methods utilizing a double-exponential unitary CC ansatz, where the reduced dimensionality of constituent subproblems offers a possibility of efficient utilization of limited quantum resources in modeling realistic systems.
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In this paper, we discuss extending the sub-system embedding sub-algebra coupled cluster formalism and the double unitary coupled cluster (DUCC) ansatz to the time domain. An important part of the analysis is associated with proving the exactness of the DUCC ansatz based on the general many-body form of anti-Hermitian cluster operators defining external and internal excitations. Using these formalisms, it is possible to calculate the energy of the entire system as an eigenvalue of downfolded/effective Hamiltonian in the active space, which is identifiable with the sub-system of the composite system. It can also be shown that downfolded Hamiltonians integrate out Fermionic degrees of freedom that do not correspond to the physics encapsulated by the active space. In this paper, we extend these results to the time-dependent Schrödinger equation, showing that a similar construct is possible to partition a system into a sub-system that varies slowly in time and a remaining sub-system that corresponds to fast oscillations. This time-dependent formalism allows coupled cluster quantum dynamics to be extended to larger systems and for the formulation of novel quantum algorithms based on the quantum Lanczos approach, which has recently been considered in the literature.
The recently introduced coupled cluster (CC) downfolding techniques for reducing the dimensionality of quantum many-body problems recast the CC formalism in the form of the renormalization procedure allowing, for the construction of effective (or downfolded) Hamiltonians in small-dimensionality sub-space, usually identified with the so-called active space, of the entire Hilbert space. The resulting downfolded Hamiltonians integrate out the external (out-of-active-space) Fermionic degrees of freedom from the internal (in-the-active-space) parameters of the wave function, which can be determined as components of the eigenvectors of the downfolded Hamiltonians in the active space. This paper will discuss the extension of non-Hermitian (associated with standard CC formulations) and Hermitian (associated with the unitary CC approaches) downfolding formulations to composite quantum systems. The non-Hermitian formulation can provide a platform for developing local CC approaches, while the Hermitian one can serve as an ideal foundation for developing various quantum computing applications based on the limited quantum resources. We also discuss the algorithm for extracting the semi-analytical form of the inter-electron interactions in the active spaces.
The three key elements of a quantum simulation are state preparation, time evolution, and measurement. While the complexity scaling of time evolution and measurements are well known, many state preparation methods are strongly system-dependent and require prior knowledge of the system's eigenvalue spectrum. Here, we report on a quantum-classical implementation of the coupled-cluster Green's function (CCGF) method, which replaces explicit ground state preparation with the task of applying unitary operators to a simple product state. While our approach is broadly applicable to many models, we demonstrate it here for the Anderson impurity model (AIM). The method requires a number of TTT gates that grows as $ \mathcal{O} \left(N^5 \right)$ per time step to calculate the impurity Green's function in the time domain, where NNN is the total number of energy levels in the AIM. Since the number of TTT gates is analogous to the computational time complexity of a classical simulation, we achieve an order of magnitude improvement over a classical CCGF calculation of the same order, which requires $ \mathcal{O} \left(N^6 \right)$ computational resources per time step.