Density Matrix Renormalization Group Method Research Articles

Efficient simulation of open quantum systems coupled to a reservoir through multiple channels.

It is challenging to simulate open quantum systems that are connected to a reservoir through multiple channels. For example, vibrations may induce fluctuations in both energy gaps and electronic couplings, which represent two independent channels of system-bath couplings. Systems of this kind are ubiquitous in the processes of excited state radiationless decay. Combined with density matrix renormalization group (DMRG) and matrix product states (MPS) methods, we develop an interaction-picture chain mapping strategy for vibrational reservoirs to simulate the dynamics of these open systems, resulting in time-dependent spatially local system-bath couplings in the chain-mapped Hamiltonian. This transformation causes the entanglement generated by the system-bath interactions to be restricted within a narrow frequency window of vibrational modes, enabling efficient DMRG/MPS dynamical simulations. We demonstrate the utility of this approach by simulating singlet fission dynamics using a generalized spin-boson Hamiltonian with both diagonal and off-diagonal system-bath couplings. This approach generalizes an earlier interaction-picture chain mapping scheme, allowing for efficient and exact simulation of systems with multi-channel system-bath couplings using matrix product states, which may further our understanding of nonlocal exciton-phonon couplings in exciton transport and the non-Condon effect in energy and electron transfer.

Parallel Implementation of the Density Matrix Renormalization Group Method Achieving a Quarter petaFLOPS Performance on a Single DGX-H100 GPU Node.

We report cutting edge performance results on a single node hybrid CPU-multi-GPU implementation of the spin adapted ab initio Density Matrix Renormalization Group (DMRG) method on current state-of-the-art NVIDIA DGX-H100 architectures. We evaluate the performance of the DMRG electronic structure calculations for the active compounds of the FeMoco, the primary cofactor of nitrogenase, and cytochrome P450 (CYP) enzymes with complete active space (CAS) sizes of up to 113 electrons in 76 orbitals [CAS(113, 76)] and 63 electrons in 58 orbitals [CAS(63, 58)], respectively. We achieve 246 teraFLOPS of sustained performance, an improvement of more than 2.5× compared to the performance achieved on the DGX-A100 architectures and an 80× acceleration compared to an OpenMP parallelized implementation on a 128-core CPU architecture. Our work highlights the ability of tensor network algorithms to efficiently utilize high-performance multi-GPU hardware and shows that the combination of tensor networks with modern large-scale GPU accelerators can pave the way toward solving some of the most challenging problems in quantum chemistry and beyond.

TD-DMRG Study of Exciton Dynamics with both Thermal and Static Disorders for Fenna-Matthews-Olson Complex.

Photosynthesis is a fundamental process that converts solar energy into chemical energy. Understanding the microscopic mechanisms of energy transfer in photosynthetic systems is crucial for the development of novel optoelectronic materials. Simulating these processes poses significant challenges due to the intricate interactions between electrons and phonons, compounded by static disorder. In this work, we present a numerically nearly exact study using the time-dependent density matrix renormalization group (TD-DMRG) method to simulate the quantum dynamics of the Fenna-Matthews-Olson (FMO) complex considering an eight-site model with both thermal and static disorders. We employ the thermo-field dynamics formalism for temperature effects. We merge all electronic interactions into one large matrix product state (MPS) site, boosting accuracy efficiently without increasing complexity. Previous combined experimental and computational studies indicated that the static disorders range from 30 to 90 cm-1 for different FMO sites. We employ a Gaussian distribution and the auxiliary bosonic operator approach to consider the static disorder in our TD-DMRG algorithm. We investigate the impact of different initial excitation sites, temperatures, and degrees of static disorder on the exciton dynamics and temporal coherence. It is found that under the influence of the experimentally determined static disorder strength, the exciton population evolution shows a non-negligible difference at zero temperature, while it is hardly affected at room temperature.

Variational Adiabatic Transport of Tensor Networks

We discuss a tensor network method for constructing the adiabatic gauge potential—the generator of adiabatic transformations—as a matrix product operator, which allows us to adiabatically transport matrix product states. Adiabatic evolution of tensor networks offers a wide range of applications, of which two are explored in this paper: improving tensor network optimization and scanning phase diagrams. By efficiently transporting eigenstates to quantum criticality and performing intermediary density-matrix renormalization group (DMRG) optimizations along the way, we demonstrate that we can compute ground and low-lying excited states faster and more reliably than a standard DMRG method at or near quantum criticality. We demonstrate a simple automated step size adjustment and detection of the critical point based on the norm of the adiabatic gauge potential. Remarkably, we are able to reliably transport states through the critical point of the models we study. Published by the American Physical Society 2024

Two-dimensional quantum lattice models via mode optimized hybrid CPU-GPU density matrix renormalization group method

Two-dimensional quantum lattice models via mode optimized hybrid CPU-GPU density matrix renormalization group method

Using Kondo entanglement to induce spin correlations between disconnected quantum dots

We investigate the entanglement between the spins of two quantum dots that are not simultaneously connected to the same system. Quantum entanglement among localized spins is a crucial property for the advancement of quantum computing and quantum information. Generating and controlling an entangled state between quantum dots have garnered significant attention in recent years for this reason. In this study, we demonstrate that information about the spin orientation of a quantum dot can be preserved, utilizing Kondo entanglement, within a reservoir of electrons. Subsequently, this information can be transmitted to another dot after the initial dot has been decoupled from the reservoirs. We employ a double quantum dot system in a parallel geometry to establish the initial state, where each dot interacts with reservoirs of different symmetries. A specific phase in the couplings is chosen to induce antiferromagnetic spin correlation between the dots. The time evolution of the initial state is analyzed using the time-dependent density matrix renormalization group method. Our findings reveal that a partially entangled state between the dots can be achieved, even when they are not simultaneously connected. This entangled state arises transiently and dissipates in the stationary state. The stability of the state observed during the transient phase is demonstrated. To comprehend the details of these phenomena, we employ a canonical transformation of real space.

Possible chiral spin liquid state in the S = 1/2 kagome Heisenberg model

The nature of the ground state for the S = 1/2 Kagome Heisenberg antiferromagnet (KHAF) has been elusive. We revisit this challenging problem and provide numerical evidence that its ground state is a chiral spin liquid. Combining the density matrix renormalization group method with analytical analyses, we demonstrate that the previously observed chiral spin liquid phase in the KHAF with longer-range couplings is stable in a broader region of the phase diagram. We characterize the nature of the ground state by computing energy derivatives, revealing the ground-state degeneracy arising from the spontaneous breaking of the time-reversal symmetry, and targeting the semion sector. We further investigate the phase diagram in the vicinity of the KHAF and observe a 3×3\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\sqrt{3}\ imes \\sqrt{3}$$\\end{document} magnetically ordered phase and two valence-bond crystal phases.

Block-Correlated Coupled Cluster Theory with up to Four-Pair Correlation for Accurate Static Correlation of Strongly Correlated Systems.

A block-correlated coupled cluster method with up to four-pair correlation based on the generalized valence bond wave function (GVB-BCCC4) is first implemented, which offers an alternative method for electronic structure calculations of strongly correlated systems. We developed some techniques to derive a set of compact and cost-effective equations for GVB-BCCC4, which include the definition of n-block (n = 1-4) Hamiltonian matrices, the combination of excitation operators, and the definition of independent amplitudes. We then applied the GVB-BCCC4 method to investigate several potential energy surfaces of strongly correlated systems with singlet ground states. Our calculations demonstrate that the GVB-BCCC4 method can provide nearly exact static correlation energies as the density matrix renormalization group method (on the basis of the same GVB orbitals). This work highlights the significance of four-pair correlation in quantitative descriptions of static correlation energy for strongly correlated systems.

Predicting the FCI Energy of Large Systems to Chemical Accuracy from Restricted Active Space Density Matrix Renormalization Group Calculations.

We theoretically derive and validate with large scale simulations a remarkably accurate power law scaling of errors for the restricted active space density matrix renormalization group (DMRG-RAS) method [J. Phys. Chem. A 126, 9709] in electronic structure calculations. This yields a new extrapolation method, DMRG-RAS-X, which reaches chemical accuracy for strongly correlated systems such as the chromium dimer, dicarbon up to a large cc-pVQZ basis and even a large chemical complex such as the FeMoco with significantly lower computational demands than those of previous methods. The method is free of empirical parameters, performed robustly and reliably in all examples we tested, and has the potential to become a vital alternative method for electronic structure calculations in quantum chemistry and more generally for the computation of strong correlations in nuclear and condensed matter physics.

Hilbert space multireference coupled cluster tailored by matrix product states

In the past decade, the quantum chemical version of the density matrix renormalization group method has established itself as the method of choice for strongly correlated molecular systems. However, despite its favorable scaling, in practice, it is not suitable for computations of dynamic correlation. Several approaches to include that in post-DMRG methods exist; in our group, we focused on the tailored coupled cluster (TCC) approach. This method works well in many situations; however, in exactly degenerate cases (with two or more determinants of equal weight), it exhibits a bias toward the reference determinant representing the Fermi vacuum. Although sometimes it is possible to use a compensation scheme to avoid this bias for energy differences, it is certainly a drawback. In order to overcome this bias of the TCC method, we have developed a Hilbert-space multireference version of tailored CC, which can treat several determinants on an equal footing. We have implemented and compared the performance of three Hilbert-space multireference coupled cluster (MRCC) variants—the state universal one and the Brillouin–Wigner and Mukherjee’s state specific ones. We have assessed these approaches on the cyclobutadiene and tetramethyleneethane molecules, which are both diradicals with exactly degenerate determinants at a certain geometry. We have also investigated the sensitivity of the results on the orbital rotation of the highest occupied and lowest unoccupied molecular orbital (HOMO–LUMO) pair, as it is well known that Hilbert-space MRCC methods are not invariant to such transformations.

Strong electron correlation from partition density functional theory

Standard approximations for the exchange–correlation functional in Kohn–Sham density functional theory (KS-DFT) typically lead to unacceptably large errors when applied to strongly correlated electronic systems. Partition-DFT (PDFT) is a formally exact reformulation of KS-DFT in which the ground-state density and energy of a system are obtained through self-consistent calculations on isolated fragments, with a partition energy representing inter-fragment interactions. Here, we show how typical errors of the local density approximation (LDA) in KS-DFT can be largely suppressed through a simple approximation, the multi-fragment overlap approximation (MFOA), for the partition energy in PDFT. Our method is illustrated on simple models of one-dimensional strongly correlated linear hydrogen chains. The MFOA, when used in combination with the LDA for the fragments, improves LDA dissociation curves of hydrogen chains and produces results that are comparable to those of spin-unrestricted LDA, but without breaking the spin symmetry. MFOA also induces a correction to the LDA electron density that partially captures the correct density dimerization in strongly correlated hydrogen chains. Moreover, with an additional correction to the partition energy that is specific to the one-dimensional LDA, the approximation is shown to produce dissociation energies in quantitative agreement with calculations based on the density matrix renormalization group method.

Soliton confinement in a quantum circuit

Confinement of topological excitations into particle-like states - typically associated with theories of elementary particles - are known to occur in condensed matter systems, arising as domain-wall confinement in quantum spin chains. However, investigation of confinement in the condensed matter setting has rarely ventured beyond lattice spin systems. Here we analyze the confinement of sine-Gordon solitons into mesonic bound states in a perturbed quantum sine-Gordon model. The latter describes the scaling limit of a one-dimensional, quantum electronic circuit (QEC) array, constructed using experimentally-demonstrated QEC elements. The scaling limit is reached faster for the QEC array compared to spin chains, allowing investigation of the strong-coupling regime of this model. We compute the string tension of confinement of sine-Gordon solitons and the changes in the low-lying energy spectrum. These results, obtained using the density matrix renormalization group method, could be verified in a quench experiment using state-of-the-art QEC technologies.

A time-dependent momentum-resolved scattering approach to core-level spectroscopies

While new light sources allow for unprecedented resolution in experiments with X-rays, a theoretical understanding of the scattering cross-section is lacking. In the particular case of strongly correlated electron systems, numerical techniques are quite limited, since conventional approaches rely on calculating a response function (Kramers-Heisenberg formula) that is obtained from a perturbative analysis of scattering processes in the frequency domain. This requires a knowledge of a full set of eigenstates in order to account for all intermediate processes away from equilibrium, limiting the applicability to small tractable systems. In this work, we present an alternative paradigm, recasting the problem in the time domain and explicitly solving the time-dependent Schrödinger equation without the limitations of perturbation theory: a faithful simulation of the scattering processes taking place in actual experiments, including photons and core electrons. We show how this approach can yield the full time and momentum resolved Resonant Inelastic X-Ray Scattering (RIXS) spectrum of strongly interacting many-body systems. We demonstrate the formalism with an application to Mott insulating Hubbard chains using the time-dependent density matrix renormalization group method, which does not require a priory knowledge of the eigenstates and can solve very large systems with dozens of orbitals. This approach can readily be applied to systems out of equilibrium without modification and generalized to other spectroscopies.

Quantum correlations in the frustrated XY model on the honeycomb lattice

We have investigated the spin-1/2 XY frustrated antiferromagnetic Heisenberg honeycomb model, which features an intermediate region in its ground state phase diagram that is not well understood. The two dominant phases in the diagram are the quantum spin-liquid (QSL) and the antiferromagnetic Ising order. Quantum correlations suggest that the QSL phase is likely to exhibit entanglement. To explore this possibility, we utilized numerical Lanczos and density matrix renormalization group (DMRG) methods to calculate concurrence, quantum discord (QD), and entanglement entropy. The results of our study indicate the existence of quantum entanglement within the intermediate region, implying a greater probability for the dominance of the quantum spin-liquid (QSL) phase over the antiferromagnetic Ising order. This discovery underscores the importance of considering quantum correlations in comprehending the model’s behavior and provides insight into the complex nature of quantum systems.

Time-Dependent Density Matrix Renormalization Group Method for Quantum Transport with Phonon Coupling in Molecular Junction.

Quantum transport in molecular junctions has attracted great attention. The charge motion in a molecular junction can cause geometric deformation, leading to strong electron phonon coupling, which was often overlooked. We have formulated a nearly exact method to assess the time-dependent current and occupation number in the molecular junction modeled by the electron-phonon coupled bridge state using the time-dependent density matrix renormalization group (TD-DMRG) method. The oscillation period and amplitude of the current are found to be dependent on the electron phonon coupling strength and energy level alignment with the electrodes. In an attempt to better understand these phenomena, we have devised a new approximation that explains the bistability phenomenon and the behavior of steady currents in the strong electron-phonon coupling regime. Comparisons have been made with the multilayer-multiconfiguration time-dependent Hartree (ML-MCTDH) method and the analytical result in the purely electronic limit. Furthermore, we explore the entropy of different orderings, extending to the electron phonon model problems. Regarding finite temperature, the thermal Bogoliubov transformation of both fermions and bosons is used and compared with imaginary time evolution results.

Minimizing non-radiative decay in molecular aggregates through control of excitonic coupling

The widely known “Energy Gap Law” (EGL) predicts a monotonically exponential increase in the non-radiative decay rate (knr) as the energy gap narrows, which hinders the development of near-infrared (NIR) emissive molecular materials. Recently, several experiments proposed that the exciton delocalization in molecular aggregates could counteract EGL to facilitate NIR emission. In this work, the nearly exact time-dependent density matrix renormalization group (TD-DMRG) method is developed to evaluate the non-radiative decay rate for exciton-phonon coupled molecular aggregates. Systematical numerical simulations show, by increasing the excitonic coupling, knr will first decrease, then reach a minimum, and finally start to increase to follow EGL, which is an overall result of two opposite effects of a smaller energy gap and a smaller effective electron-phonon coupling. This anomalous non-monotonic behavior is found robust in a number of models, including dimer, one-dimensional chain, and two-dimensional square lattice. The optimal excitonic coupling strength that gives the minimum knr is about half of the monomer reorganization energy and is also influenced by system size, dimensionality, and temperature.

Magnetic-field-driven rise and fall of a bipartite entanglement in a spin-liquid phase of a spin-1/2 Heisenberg branched chain

The spin-1/2 Heisenberg branched chain with the unit cell composed of three spins in the main backbone and one spin at a side branching of one-dimensional chain is investigated with the help of density-matrix renormalization group (DMRG) and quantum Monte Carlo (QMC) methods. The DMRG simulations were employed to calculate zero-temperature magnetization curves and to construct the ground-state phase diagram, which is composed from four different ground states classified as gapped zero-plateau and one-half plateau phase, a gapless spin-liquid phase and a fully saturated phase. It is shown that the one-half magnetization plateau vanishes at the Kosterlitz–Thouless quantum critical point, which is wedged into a parameter space of the gapless quantum spin-liquid phase. The bipartite quantum entanglement between four distinct nearest-neighbor pairs of the spin-1/2 Heisenberg branched chain is quantified through the concurrence. It is found that the concurrence varies continuously within the quantum spin-liquid phase, where it may display a continuous rise, a continuous fall or eventually an intriguing rise-and-fall behavior. On the contrary, the concurrence is kept constant within two gapful zero- and one-half plateau phases. Temperature and magnetic-field dependencies of the magnetization and magnetic susceptibility computed within the QMC method uncover clear signatures of the quantum critical point at finite temperatures.

Quantum Circuit Matrix Product State Ansatz for Large-Scale Simulations of Molecules.

As demonstrated in the density matrix renormalization group (DMRG) method, approximating many-body wave function of electrons using a matrix product state (MPS) is a promising way to solve electronic structure problems. The expressibility of an MPS is determined by the size of the matrices or, in other words, the bond dimension, which unfortunately may be required to be very large in quantum chemistry simulations. In this study, we propose to calculate the ground state energies of molecular systems by variationally optimizing quantum circuit MPS (QCMPS) with a relatively small number of qubits. It is demonstrated that with carefully chosen circuit structure and orbital localization scheme, QCMPS can reach a similar accuracy as that achieved in DMRG with an exponentially large bond dimension. QCMPS simulation of a linear hydrogen molecular chain with 50 orbitals can reach the chemical accuracy using only 6 qubits at a moderate circuit depth. These results suggest that QCMPS is a promising wave function ansatz in the variational quantum eigensolver algorithm for molecular systems.

Three Lagrangians for the complete-active space coupled-cluster method.

Three fully variational formulations of the complete-active space coupled-cluster method are derived. The formulations include the ability to approximate the model vectors by smooth manifolds, thereby opening up the possibility for overcoming the exponential wall of scaling for model spaces of complete-active space type. In particular, model vectors of matrix-product states are considered, and it is argued that the present variational formulation allows not only favorably scaling multireference coupled-cluster calculations but also systematic correction of tailored coupled-cluster calculations and of quantum chemical density-matrix renormalization group methods, which are fast and polynomial scaling but lack the ability to properly resolve dynamical correlation at chemical accuracy. The extension of the variational formulations to the time domain is also discussed, with derivations of abstract evolution equations.

Spontaneous dimerization, spin-nematic order, and deconfined quantum critical point in a spin-1 Kitaev chain with tunable single-ion anisotropy

Kitaev-type spin chains have been demonstrated to be fertile playgrounds in which exotic phases and unconventional phase transitions are ready to appear. In this work, we use the density-matrix renormalization-group method to study the quantum phase diagram of a spin-1 Kitaev chain with a tunable negative single-ion anisotropy (SIA). When the strength of the SIA is small, the ground state is revealed to be a spin-nematic phase, which escapes conventional magnetic order but is characterized by a finite spin-nematic correlation because of the breaking spin-rotational symmetry. As the SIA increases, the spin-nematic phase is taken over by either a dimerized phase or an antiferromagnetic phase through an Ising-type phase transition, depending on the direction of the easy axis. For large enough SIA, the dimerized phase and the antiferromagnetic phase undergo a ``Landau-forbidden'' continuous phase transition, suggesting new platform of deconfined quantum critical point in spin-1 Kitaev chain.