Time-dependent Density Matrix Research Articles

CoOMBE: A suite of open-source programs for the integration of the optical Bloch equations and Maxwell-Bloch equations

The programs described in this article and distributed with it aim (1) at integrating the optical Bloch equations governing the time evolution of the density matrix representing the quantum state of an atomic system driven by laser or microwave fields, and (2) at integrating the 1D Maxwell-Bloch equations for one or two laser fields co-propagating in an atomic vapour. The rotating wave approximation is assumed. These programs can also be used for more general quantum dynamical systems governed by the Lindblad master equation. They are written in Fortran 90; however, their use does not require any knowledge of Fortran programming. Methods for solving the optical Bloch equations in the rate equations limit, for calculating the steady-state density matrix and for formulating the optical Bloch equations in the weak probe approximation are also described. Program summaryProgram Title: CoOMBECPC Library link to program files:https://doi.org/10.17632/5wsg9d52dk.1Developers' repository link:https://github.com/durham-qlm/CoOMBELicensing provisions: GPLv3Programming language: Fortran 90Nature of problem: The present programs can be used for the following operations: (1) Integrating the optical-Bloch equations within the rotating wave approximation for a multi-state atomic system. At the choice of the user, the calculation will return either the time-dependent density matrix at given times or the density matrix in the long time limit if the system evolves into a steady state in that limit. The calculation can be done with or without averaging over the thermal velocity distribution of the atoms. The number of atomic states which can be included in the calculation is limited only by the CPU time available and possibly by memory requirements. An arbitrarily large number of laser or microwave fields can be included in the calculation if these fields are all CW. This number is currently limited to one or two for fields that are not all CW. The calculation can be done in the weak probe approximation, or in the rate equations approximation, or without assuming either of these two approximations. Calculating refractive indexes, absorption coefficients and complex susceptibilities is also possible. (2) Integrating the 1D Maxwell-Bloch equations in the slowly varying envelope approximation for one or two fields co-propagating in a single-species atomic vapour. Although geared towards the case of atoms interacting with laser fields, this code can also be used for more general quantum systems with similar equations of motion (e.g., molecular systems, spin systems, etc.).Solution method: The Lindblad master equation is expressed as a system of homogeneous first order linear differential equations, which are transformed as required and solved to obtain the density matrix representing the state of the atomic system. A variety of methods are offered to this end. The same approach is also used in the calculation of the polarisation of the medium when integrating the Maxwell-Bloch equations. The latter are integrated over space using predictor-corrector methods. The library includes a general driving program making it possible to use these codes without additional program development. The distribution also includes examples of the use of a container for running these programs without a pre-installed Fortran compiler.

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.

Kylin-V: An open-source package calculating the dynamic and spectroscopic properties of large systems.

Quantum dynamics simulation and computational spectroscopy serve as indispensable tools for the theoretical understanding of various fundamental physical and chemical processes, ranging from charge transfer to photochemical reactions. When simulating realistic systems, the primary challenge stems from the overwhelming number of degrees of freedom and the pronounced many-body correlations. Here, we present Kylin-V, an innovative quantum dynamics package designed for accurate and efficient simulations of dynamics and spectroscopic properties of vibronic Hamiltonians for molecular systems and their aggregates. Kylin-V supports various quantum dynamics and computational spectroscopy methods, such as time-dependent density matrix renormalization group and our recently proposed single-site and hierarchical mapping approaches, as well as vibrational heat-bath configuration interaction. In this paper, we introduce the methodologies implemented in Kylin-V and illustrate their performances through a diverse collection of numerical examples.

Theoretical investigation of distal charge separation in a perylenediimide trimer

An exciton–phonon (ex–ph) model based on our recently developed block interaction product basis framework is introduced to simulate the distal charge separation (CS) process in aggregated perylenediimide (PDI) trimer incorporating the quantum dynamic method, i.e., the time-dependent density matrix renormalization group. The electronic Hamiltonian in the ex–ph model is represented by nine constructed diabatic states, which include three local excited (LE) states and six charge transfer (CT) states from both the neighboring and distal chromophores. These diabatic states are automatically generated from the direct products of the leading localized neutral or ionic states of each chromophore’s reduced density matrix, which are obtained from ab initio quantum chemical calculation of the subsystem consisting of the targeted chromophore and its nearest neighbors, thus considering the interaction of the adjacent environment. In order to quantum-dynamically simulate the distal CS process with massive coupled vibrational modes in molecular aggregates, we used our recently proposed hierarchical mapping approach to renormalize these modes and truncate those vibrational modes that are not effectively coupled with electronic states accordingly. The simulation result demonstrates that the formation of the distal CS process undergoes an intermediate state of adjacent CT, i.e., starts from the LE states, passes through an adjacent CT state to generate the intermediates (∼200 fs), and then formalizes the targeted distal CS via further charge transference (∼1 ps). This finding agrees well with the results observed in the experiment, indicating that our scheme is capable of quantitatively investigating the CS process in a realistic aggregated PDI trimer and can also be potentially applied to exploring CS and other photoinduced processes in larger systems.

Random-matrix model for thermalization

We show that for a system governed by a random-matrix Hamiltonian (a member of the time-reversal invariant Gaussian Orthogonal Ensemble (GOE) of random matrices of dimension N), all functions Tr(Aρ(t)) in the ensemble thermalize: For N→∞ every such function tends to the value Tr(Aρeq(∞))+Tr(Aρ(0))g2(t) . Here ρ(t) is the time-dependent density matrix of the system, A is a Hermitean operator standing for an observable, and ρeq(∞) is the equilibrium density matrix at infinite temperature. The oscillatory function g(t) is the Fourier transform of the average GOE level density and falls off as 1/|t|3/2 for large t. With g(t)=g(−t) , thermalization is symmetric in time. Analogous results, including the symmetry in time of thermalization, are derived for the time-reversal non-invariant Gaussian Unitary Ensemble of random matrices. Comparison with the ‘eigenstate thermalization hypothesis’ of (Srednicki 1999 J. Phys. A: Math. Gen. 32 1163) shows overall agreement but raises significant questions.

Thermalization of closed chaotic many-body quantum systems

We investigate thermalization of a closed chaotic many-body quantum system by combining the Hartree–Fock approach with the Bohigas–Giannoni–Schmit conjecture. The conjecture implies that locally, the residual interaction causes the statistics of eigenvalues and eigenfunctions of the full Hamiltonian to agree with random-matrix predictions. The agreement is confined to an interval Δ (the correlation width). The results are used to calculate Tr(Aρ(t)) . Here ρ(t) is the time-dependent density matrix of the system, and A represents an observable. In the semiclassical regime, the average ⟨Tr(Aρ(t))⟩ decays on the time scale ℏ/Δ toward an asymptotic value. If the energy spread of the system is of order Δ, that value is given by Tr(Aρeq) where ρeq is the density matrix of statistical equilibrium. The correlation width Δ is the central parameter of our approach. We argue that Δ occurs generically in chaotic quantum systems and plays the same central role.

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.

Divergent Nonlinear Response from Quasiparticle Interactions.

We demonstrate that nonlinear response functions in many-body systems carry a sharp signature of interactions between gapped low-energy quasiparticles. Such interactions are challenging to deduce from linear response measurements. The signature takes the form of a divergent-in-time contribution to the response-linear in time in the case when quasiparticles propagate ballistically-that is absent for free bosonic excitations. We give a physically transparent semiclassical picture of this singular behavior. While the semiclassical picture applies to a broad class of systems we benchmark it in two simple models: in the Ising chain using a form-factor expansion, and in a nonintegrable model-the spin-1 Affleck-Kennedy-Lieb-Tasaki chain-using time-dependent density matrix renormalization group simulations. We comment on extensions of these results to finite temperatures.

Auger spectroscopy beyond the ultra-short core-hole relaxation time approximation

We present a time-dependent computational approach to study Auger electron spectroscopy (AES) beyond the ultra-short core-hole relaxation time approximation and, as a test case, we apply it to the paradigmatic example of a one-dimensional Mott insulator represented by a half-filled Hubbard chain. The Auger spectrum is usually calculated by assuming that, after the creation of a core-hole, the system thermalizes almost instantaneously. This leads to a relatively simple analytical expression that uses the ground-state with a core-hole as a reference state and ignores all the transient dynamics related to the screening of the core-hole. In this picture, the response of the system can be associated to the pair spectral function. On the other hand, in our numerical calculations, the core hole is created by a light pulse, allowing one to study the transient dynamics of the system in terms of the pulse duration and in the non-perturbative regime. Time-dependent density matrix renormalization group calculations reveal that the relaxation process involves the creation of a polarization cloud of doublon excitations that have an effect similar to photo-doping. As a consequence, there is a leak of spectral weight to higher energies into what otherwise would be the Mott gap. For longer pulses, these excited states, mostly comprised of doublons, can dominate the spectrum. By changing the duration of the light-pulse, the entire screening process can be resolved in time.

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.

Simulating noise on a quantum processor: interactions between a qubit and resonant two-level system bath

Material defects fundamentally limit the coherence times of superconducting qubits, and manufacturing completely defect-free devices is not yet possible. Therefore, understanding the interactions between defects and a qubit in a real quantum processor design is essential. We build a model that incorporates the standard tunneling model, the electric field distributions in the qubit, and open quantum system dynamics, and draws from the current understanding of two-level system (TLS) theory. Specifically, we start with one million TLSs distributed on the surface of a qubit and pick the 200 systems that are most strongly coupled to the qubit. We then perform a full Lindbladian simulation that explicitly includes the coherent coupling between the qubit and the TLS bath to model the time dependent density matrix of resonant TLS defects and the qubit. We find that the 200 most strongly coupled TLSs can accurately describe the qubit energy relaxation time. This work confirms that resonant TLSs located in areas where the electric field is strong can significantly affect the qubit relaxation time, even if they are located far from the Josephson junction (JJ). Similarly, a strongly-coupled resonant TLS located in the JJ does not guarantee a reduced qubit relaxation time if a more strongly coupled TLS is far from the JJ. In addition to the coupling strengths between TLSs and the qubit, the model predicts that the geometry of the device and the TLS relaxation time play a significant role in qubit dynamics. Our work can provide guidance for future quantum processor designs with improved qubit coherence times.

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.

Traces of electron-phonon coupling in one-dimensional cuprates

The appearance of certain spectral features in one-dimensional (1D) cuprate materials has been attributed to a strong, extended attractive coupling between electrons. Here, using time-dependent density matrix renormalization group methods on a Hubbard-extended Holstein model, we show that extended electron-phonon (e–ph) coupling presents an obvious choice to produce such an attractive interaction that reproduces the observed spectral features and doping dependence seen in angle-resolved photoemission experiments: diminished 3kF spectral weight, prominent spectral intensity of a holon-folding branch, and the correct holon band width. While extended e–ph coupling does not qualitatively alter the ground state of the 1D system compared to the Hubbard model, it quantitatively enhances the long-range superconducting correlations and suppresses spin correlations. Such an extended e–ph interaction may be an important missing ingredient in describing the physics of the structurally similar two-dimensional high-temperature superconducting layered cuprates, which may tip the balance between intertwined orders in favor of uniform d-wave superconductivity.

Hierarchical Mapping for Efficient Simulation of Strong System-Environment Interactions.

Quantum dynamics (QD) simulation is a powerful tool for interpreting ultrafast spectroscopy experiments and unraveling their microscopic mechanism in out-of-equilibrium excited state behaviors in various chemical, biological, and material systems. Although state-of-the-art numerical QD approaches such as the time-dependent density matrix renormalization group (TD-DMRG) already greatly extended the solvable system size of general linearly coupled exciton-phonon models with up to a few hundred phonon modes, the accurate simulation of larger system sizes or strong system-environment interactions is still computationally highly challenging. Based on quantum information theory (QIT), in this work, we realize that only a small number of effective phonon modes couple to the excitonic system directly regardless of a large or even infinite number of modes in the condensed phase environment. On top of the identified small number of direct effective modes, we propose a hierarchical mapping (HM) approach through performing block Lanczos transformations on the remaining indirect modes, which transforms the Hamiltonian matrix to a nearly block-tridiagonal form and eliminates the long-range interactions. Numerical tests on model spin-boson systems and realistic singlet fission models in a rubrene crystal environment with up to 7000 modes and strong system-environment interactions indicate HM can reduce the system size by 1-2 orders of magnitude and accelerate the calculation by ∼80% without losing accuracy.

Atomic-Scale Defects Might Determine the Second Harmonic Generation from Plasmonic Graphene Nanostructures.

In this work, we theoretically investigate the impact of the atomic scale lattice imperfections of graphene nanoflakes on their nonlinear response enhanced by the resonance between an incident electromagnetic field and localized plasmon. As a case study, we address the second harmonic generation from graphene plasmonic nanoantennas of different symmetries with missing carbon atom vacancy defects in the honeycomb lattice. Using the many-body time-dependent density matrix approach, we find that one defect in the nanoflake comprising over five thousand carbon atoms can strongly impact the nonlinear hyperpolarizability and override the symmetry constraints. The effect reported here cannot be captured using the relaxation time approximation within the quantum or classical framework. Results obtained in this work have thus important implications for the design of nonlinear graphene devices.

DYNAMICS OF THE THREE-QUBITS TAVIS — CUMMINGS MODEL

In this article, we have studied the entanglement dynamics of three identical qubits (natural or artificial two-level atoms) resonantly interacting with the one mode of the thermal field of a microwave lossless resonator via one-photon transitions. An exact solution of the quantum time Schrodinger equation is found for the total wave function of the system for the initial separable and entangled states of qubits and the Fock initial state of the resonator. On the basis of this solution, an exact solution of the quantum Liouville equation for the total time-dependent density matrix of the system in the case of a thermal field of the resonator is constructed. The exact solution for the full density matrix is used to calculate the criterion of entanglement of pairs of qubits negativity. The resultsof numerical simulation of the time dependence of the negativity of pairs of qubits showed that with an increase in the intensity of the thermal resonator field, the degree of entanglement of pairs of qubits decreases. It is also shown that In the model under consideration, for any initial states of qubits and intensities of the thermal field of the resonator, the effect of sudden death of entanglement takes place. This behavior of the entanglement parameter in the model under consideration differs from that in the two-qubit model. For two-qubit model, the effect of the sudden death of entanglement takes place only for the initial entangled states of qubits and intense thermal fields of the resonator.

The Irreversible Quantum Dynamics of the Three-Level su(1, 1) Bosonic Model

We study the quantum dynamics of the opened three-level su(1, 1) bosonic model. The effective non-Hermitian Hamiltonians describing the system of the Lindblad equation in the short time limit are constructed. The obtained non-Hermitian Hamiltonians are exactly solvable by the Algebraic Bethe Ansatz. This approach allows representing biorthogonal and nonorthogonal bases of the system. We analyze the biorthogonal expectation values of a number of particles in the zero mode and represent it in the determinantal form. The time-dependent density matrix satisfying the Lindblad master equation is found in terms of the nonorthogonal basis.

Formation of spin and charge ordering in the extended Hubbard model during a finite-time quantum quench

We investigate the formation of charge and spin ordering by starting from a non-interacting state and studying how it evolves in time under a Hamiltonian with finite electronic interactions. We consider the one-dimensional, half-filled extended Hubbard model, which we solve within time-dependent density matrix renormalization group. By employing linear finite-time quenches in the onsite and nearest-neighbor interactions, we find the existence of impulse, intermediate, and adiabatic regimes of time evolution. For the quenches we analyze, we observe that the adiabatic regime is reached with distinct ramping time scales depending on whether the charge density wave (CDW) or the spin density wave (SDW) is formed. The former needs to be slower than the latter to prevent entangled excited states from being accessed during the quench. More interestingly, in the intermediate regime, we observe an enhancement of the entanglement entropy with respect to its initial value, which precedes the formation of the CDW ordering; a similar enhancement is not seen in the quench towards SDW. Our findings also show that the breaking of the system integrability, by turning on the nearest-neighbor interactions, does not give rise to significant changes in the non-equilibrium behavior within the adiabatic approximation.

One-particle entanglement for one-dimensional spinless fermions after an interaction quantum quench

Particle entanglement provides information on quantum correlations in systems of indistinguishable particles. Here, we study the one particle entanglement entropy for an integrable model of spinless, interacting fermions both at equilibrium and after an interaction quantum quench. Using both large scale exact diagonalization and time dependent density matrix renormalization group calculations, we numerically compute the one body reduced density matrix for the J-V model, as well as its post-quench dynamics. We include an analysis of the fermionic momentum distribution, showcasing its time evolution after a quantum quench. Our numerical results, extrapolated to the thermodynamic limit, can be compared with field theoretic bosonization in the Tomonaga-Luttinger liquid regime. Excellent agreement is obtained using an interaction cutoff that can be determined uniquely in the ground state.