Evolution Of Density Matrix Research Articles

Simulating multipulse NMR spectra of polycrystalline solids in the frequency domain.

An approach is presented for simulating multipulse nuclear magnetic resonance (NMR) spectra of polycrystalline solids directly in the frequency domain. The approach integrates the symmetry pathway concept for multipulse NMR with efficient algorithms for calculating spinning sideband amplitudes and performing interpolated finite-element numerical integration over all crystallite orientations in a polycrystalline sample. The numerical efficiency is achieved through a set of assumptions used to approximate the evolution of a sparse density matrix through a pulse sequence as a set of individual transition pathway signals. The utility of this approach for simulating the spectra of complex materials, such as glasses and other structurally disordered materials, is demonstrated.

Bottomonium suppression from the three-loop QCD potential

We compute the suppression of bottomonium in the quark-gluon plasma using the three-loop QCD static potential. The potential describes the spin-averaged bottomonium spectrum below threshold with a less than 1% error. Within potential nonrelativistic quantum chromodynamics and an open quantum systems framework, we compute the evolution of the bottomonium density matrix. The values of the quarkonium transport coefficients are obtained from lattice QCD measurements of the bottomonium in-medium width and thermal mass shift; we additionally include for the first time a vacuum contribution to the dispersive coefficient γ. Using the three-loop potential and the values of the heavy quarkonium transport coefficients, we find that the resulting bottomonium nuclear modification factor is consistent with experimental observations, while at the same time reproducing the lattice measurements of the in-medium width. Published by the American Physical Society 2024

Fluorescence modulation of quantum dots in subsurface defects of optical elements by a linearly polarized light.

The limited excitation efficiency of quantum dots in the detection of subsurface defects in optical elements by quantum dot fluorescence gives rise to insufficient accuracy. To enhance the excitation efficiency of quantum dots, we studied the modulation of the polarization direction of linearly polarized incident light on quantum dot fluorescence. We first apply density matrix evolution theory to study the quantum dots interacting with linearly polarized incident light and emitting fluorescence. The fluorescence intensity exhibits cosine oscillations versus modulated laser polarization. It reaches a maximum value at the polarization angle zero, and then decreases as the angle becomes larger until π/2. The experimental results for the quantum dot in both solutions and subsurface defect of optical elements confirmed these results. For optical elements tagged with CdSe/ZnS quantum dots, the fluorescence intensity increases by 61.7%, and the area for the detected subsurface defects increases by 142.9%. Similarly, for C and InP/ZnS quantum dots, there are also increases in both the fluorescence intensity and the area of subsurface defects. Our study suggests that the subsurface defect detection in optical elements by the linearly polarized incident light could enhance the detection accuracy of subsurface defects in optical elements, and potentially achieve super-resolution imaging of subsurface defects.

Spin-Vibronic Dynamics in Open-Shell Systems beyond the Spin Hamiltonian Formalism.

Vibronic coupling has a dramatic influence over a large number of molecular processes, ranging from photochemistry to spin relaxation and electronic transport. The simulation of vibronic coupling with multireference wave function methods has been largely applied to organic compounds, and only early efforts are available for open-shell systems such as transition metal and lanthanide complexes. In this work, we derive a numerical strategy to differentiate the molecular electronic Hamiltonian in the context of multireference ab initio methods and inclusive of spin-orbit coupling effects. We then provide a formulation of open quantum system dynamics able to predict the time evolution of the electron density matrix under the influence of a Markovian phonon bath up to fourth-order perturbation theory. We apply our method to Co(II) and Dy(III) molecular complexes exhibiting long spin relaxation times and successfully validate our strategy against the use of an effective spin Hamiltonian. Our study sheds light on the nature of vibronic coupling, the importance of electronic excited states in spin relaxation, and the need for high-level computational chemistry to quantify it.

Evolution of spin coherence of radical pairs due to spin-selective recombination: Comparison of three models.

This study looked for a way to evaluate the validity of previously suggested models for describing the spin-selective recombination of radical pairs. As an example, for analysis, we used the conventional model, the model by Jones and Hore [Chem. Phys. Lett. 488, 90 (2010)], and the model by Salikhov [Am. J. Phys. Chem. 11, 67 (2022)]. To do this, analytical solutions to the evolution of the radical pair density matrix due to a radical pair's spin-selective recombination and singlet-triplet transitions in a strong magnetic field were obtained for the conventional model and the Jones and Hore model. Spin interactions included in the Hamiltonian were time-independent exchange interactions as well as Zeeman and hyperfine interactions. The most striking difference between the models' predictions appeared when considering the fraction of singlet pairs among all currently existing ones. In the Jones and Hore model, this ratio has the form of damped oscillations for any values of the spin-hamiltonian parameters. The conventional model and the Salikhov model both predicted that this ratio had the form of undamped oscillations in the absence of exchange interaction and at a sufficiently low recombination rate. Besides, the conventional model predicts the possibility of a resonance-like behavior of this ratio when singlet-triplet transitions in a part of the radical pair ensemble are completely suppressed by tuning the magnetic field strength. Possible experimental conditions in which distinguishing between the models seems to be most straightforward were suggested.

Phase transitions in the classical simulability of open quantum systems

We introduce a Langevin unravelling of the density matrix evolution of an open quantum system over matrix product states, which we term the time-dependent variational principle-Langevin equation. This allows the study of entanglement dynamics as a function of both temperature and coupling to the environment. As the strength of coupling to and temperature of the environment is increased, we find a transition where the entanglement of the individual trajectories saturates, permitting a classical simulation of the system for all times. This is the Hamiltonian open system counterpart of the saturation in entanglement found in random circuits with projective or weak measurements. If a system is open, there is a limit to the advantage in simulating its behaviour on a quantum computer, even when that evolution harbours important quantum effects. Moreover, if a quantum simulator is in this phase, it cannot simulate with quantum advantage.

Neutrino decoherence from generalised uncertainty

Quantum gravity models predict a minimal measurable length which gives rise to a modification in the uncertainty principle. One of the simplest manifestations of these generalised uncertainty principles is the linear quadratic generalised uncertainty principle which leads to a modified Heisenberg algebra. This can alter the usual von-Neumann evolution of density matrix to a Lindblad-type equation. We show how this can give rise to a decoherence in neutrino propagation in vacuum. The decoherence effects due to the linear quadratic generalised uncertainty principle are extremely minimal and is unlikely to be detectable in the existing or upcoming experimental facilities for any of the natural sources of neutrinos. We also show that, in principle, there can be other variants of generalised uncertainty principle which predicts verifiable decoherence effects for the cosmic neutrino background.

Understanding Traffic Jams Using Lindblad Superoperators

We propose a model to simulate different traffic-flow conditions in terms of quantum graphs hosting an (N+1)-level dot at each site. Our model allows us to keep track of the type and of the destination of each vehicle. The traffic flow inside the system is encoded in a proper set of Lindbladian local dissipators that describe the time evolution of the system density matrix. Taking advantage of the invariance of the Lindblad master equation under inhomogeneous transformations we derive the quantum Hamiltonian for the bulk dynamics in a proper experimental setup.

Incorporating Lindblad decay dynamics into mixed quantum-classical simulations.

We derive the L-mean-field Ehrenfest (MFE) method to incorporate Lindblad jump operator dynamics into the MFE approach. We map the density matrix evolution of Lindblad dynamics onto pure state coefficients using trajectory averages. We use simple assumptions to construct the L-MFE method that satisfies this exact mapping. This establishes a method that uses independent trajectories that exactly reproduce Lindblad decay dynamics using a wavefunction description, with deterministic changes of the magnitudes of the quantum expansion coefficients, while only adding on a stochastic phase. We further demonstrate that when including nuclei in the Ehrenfest dynamics, the L-MFE method gives semi-quantitatively accurate results, with the accuracy limited by the accuracy of the approximations present in the semiclassical MFE approach. This work provides a general framework to incorporate Lindblad dynamics into semiclassical or mixed quantum-classical simulations.

Exceptional spectral phase in a dissipative collective spin model

We study a model of a quantum collective spin weakly coupled to a spin-polarized Markovian environment and find that the spectrum is divided into two regions that we name normal and exceptional Liouvillian spectral phases. In the thermodynamic limit, the exceptional spectral phase displays the unique property of being made up exclusively of second order exceptional points. As a consequence, the evolution of any initial density matrix populating this region is slowed down and cannot be described by a linear combination of exponential decays. This phase is separated from the normal one by a critical line in which the density of Liouvillian eigenvalues diverges, a phenomenon analogous to that of excited-state quantum phase transitions observed in some closed quantum systems. In the limit of no bath polarization, this criticality is transferred onto the steady state, implying a dissipative quantum phase transition and the formation of a boundary time crystal.

Decoherence modeling of polarization mode dispersion for one- and two-photon states in optical fibers

We investigate the effects of polarization mode dispersion (PMD) on the propagation of single- and two-photon states in single-mode fibers. We look at PMD as decoherence due to the system's coupling with the bosonic environment involved in optical birefringence and a thermal bath, respectively. The evolution of the polarization density matrix is described by a master equation, and its solution is used to calculate the differential group delay (DGD) due to the fiber. The PMD effects on the dynamics of EPR states in optical fibers are investigated by using the same method. In both the short-time and long-time regimes, we find that PMD-induced and thermal-induced decoherence behave similarly.

Information retrieval and eigenstate coalescence in a non-Hermitian quantum system with anti- PT symmetry

Non-Hermitian systems with parity-time reversal ($\mathcal{PT}$) or anti-$\mathcal{PT}$ symmetry have attracted a wide range of interest owing to their unique characteristics and counterintuitive phenomena. One of the most extraordinary features is the presence of an exception point (EP), across which a phase transition with spontaneously broken $\mathcal{PT}$ symmetry takes place. We implement a Floquet Hamiltonian of a single qubit with anti-$\mathcal{PT}$ symmetry by periodically driving a dissipative quantum system of a single trapped ion. With stroboscopic emission and quantum state tomography, we obtain the time evolution of density matrix for an arbitrary initial state, and directly demonstrate information retrieval, eigenstates coalescence, and topological energy spectra as unique features of non-Hermitian systems.

Calibrating the unphysical divergence in TDDFT + U simulations of a correlated oxide

To simulate the photoexcited molecular dynamics of strongly correlated materials, we implement the Hubbard U term for the proper account of the on-site Coulomb interaction in the real-time time dependent density functional theory (TDDFT + U) molecular dynamics simulations. As a prototype example, we present first-principles simulations of excited state dynamics in a typical transition metal oxide (rutile TiO2) containing d-orbital electrons. We find an unphysical divergence originated from the overcoherence in the evolution of density matrix, which can be alleviated by a diagonalization procedure proposed here. Upon this correction, we identify an intrinsic charge localization dynamics in rutile TiO2 upon photoexcitation, which offers a microscopic understanding of the photoinduced processes in correlated transition metal oxides.

Quantum critical systems with dissipative boundaries

We study the effects of dissipative boundaries in many-body systems at continuous quantum transitions, when the parameters of the Hamiltonian driving the unitary dynamics are close to their critical values. As paradigmatic models, we consider fermionic wires subject to dissipative interactions at the boundaries, associated with pumping or loss of particles. They are induced by couplings with a Markovian baths, so that the evolution of the system density matrix can be described by a Lindblad master equation. We study the quantum evolution arising from variations of the Hamiltonian and dissipation parameters, starting at t=0 from the ground state of the critical Hamiltonian. Two different dynamic regimes emerge: (i) an early-time regime for times t ~ L, where the competition between coherent and incoherent drivings develops a dynamic finite-size scaling, obtained by extending the scaling framework describing the coherent critical dynamics of the closed system, to allow for the boundary dissipation; (ii) a large-time regime for t ~ L^3 whose dynamic scaling describes the late quantum evolution leading to the t->infty stationary states.

Simulating energy transfer dynamics in the Fenna-Matthews-Olson complex via the modified generalized quantum master equation.

The generalized quantum master equation (GQME) provides a general and formally exact framework for simulating the reduced dynamics of open quantum systems. The recently introduced modified approach to the GQME (M-GQME) corresponds to a specific implementation of the GQME that is geared toward simulating the dynamics of the electronic reduced density matrix in systems governed by an excitonic Hamiltonian. Such a Hamiltonian, which is often used for describing energy and charge transfer dynamics in complex molecular systems, is given in terms of diabatic electronic states that are coupled to each other and correspond to different nuclear Hamiltonians. Within the M-GQME approach, the effect of the nuclear degrees of freedom on the time evolution of the electronic density matrix is fully captured by a memory kernel superoperator, which can be obtained from short-lived (compared to the time scale of energy/charge transfer) projection-free inputs. In this paper, we test the ability of the M-GQME to predict the energy transfer dynamics within a seven-state benchmark model of the Fenna-Matthews-Olson (FMO) complex, with the short-lived projection-free inputs obtained via the Ehrenfest method. The M-GQME with Ehrenfest-based inputs is shown to yield accurate results across a wide parameter range. It is also found to dramatically outperform the direct application of the Ehrenfest method and to provide better-behaved convergence with respect to memory time in comparison to an alternative implementation of the GQME approach previously applied to the same FMO model.

Quantum Boltzmann equation for fermions: An attempt to calculate the NMR relaxation and decoherence times using quantum field theory techniques

Extracting macroscopic properties of a system from microscopic interactions has always been an interesting topic with the most diverse applications. Here, we use the quantum Boltzmann equation to investigate the density matrix evolution of a system of nucleons. Using the quantum field theory tools for constructing the density matrix operators and calculating the interactions is the main advantage of this equation. The right-hand side of this equation involves forward scattering and usual collision terms. As examples of application, we calculate the standard Bloch equations for the nucleon system in the presence of a constant and an oscillating magnetic field from the forward scattering term. We find the longitudinal and transverse (decoherence) relaxation times from the collision term by considering the nucleon-nucleon scattering.

Finite-Temperature, Anharmonicity, and Duschinsky Effects on the Two-Dimensional Electronic Spectra from Ab Initio Thermo-Field Gaussian Wavepacket Dynamics.

Accurate description of finite-temperature vibrational dynamics is indispensable in the computation of two-dimensional electronic spectra. Such simulations are often based on the density matrix evolution, statistical averaging of initial vibrational states, or approximate classical or semiclassical limits. While many practical approaches exist, they are often of limited accuracy and difficult to interpret. Here, we use the concept of thermo-field dynamics to derive an exact finite-temperature expression that lends itself to an intuitive wavepacket-based interpretation. Furthermore, an efficient method for computing finite-temperature two-dimensional spectra is obtained by combining the exact thermo-field dynamics approach with the thawed Gaussian approximation for the wavepacket dynamics, which is exact for any displaced, distorted, and Duschinsky-rotated harmonic potential but also accounts partially for anharmonicity effects in general potentials. Using this new method, we directly relate a symmetry breaking of the two-dimensional signal to the deviation from the conventional Brownian oscillator picture.

Bridging nano-optics and condensed matter formalisms in a unified description of inelastic scattering of relativistic electron beams

In the last decades, the blossoming of experimental breakthroughs in the domain of electron energy loss spectroscopy (EELS) has triggered a variety of theoretical developments. Those have to deal with completely different situations, from atomically resolved phonon mapping to electron circular dichroism passing by surface plasmon mapping. All of them rely on very different physical approximations and have not yet been reconciled, despite early attempts to do so. As an effort in that direction, we report on the development of a scalar relativistic quantum electrodynamic (QED) approach of the inelastic scattering of fast electrons. This theory can be adapted to describe all modern EELS experiments, and under the relevant approximations, can be reduced to most of the last EELS theories. In that aim, we present in this paper the state of the art and the basics of scalar relativistic QED relevant to the electron inelastic scattering. We then give a clear relation between the two once antagonist descriptions of the EELS, the retarded dyadic Green function, usually applied to describe photonic excitations and the quasi-static mixed dynamic form factor (MDFF), more adapted to describe core electronic excitations of material. Using the photon propagator in a material, expressed in the relevant gauges, as a tool to understand the interaction between a fast electron and a material, we extend this relation to a newly defined quantity, the relativistic MDFF. The relation between the dyadic Green function and the relativistic MDFF does depend only on the photon propagator and not on the specifics of the particle (here, a fast electron) probing the target. Therefore, it can be adapted to any spectroscopy where a relation between the electromagnetic and electronic properties of a material is needed. We then use this theory to establish two important EELS-related equations. The first one relates the spatially resolved EELS to the imaginary part of the photon propagator and the incoming and outgoing electron beam wavefunction, synthesizing the most common theories developed for analyzing spatially resolved EELS experiments. The second one shows that the evolution of the electron beam density matrix is proportional to the mutual coherence tensor, proving that quite universally, the electromagnetic correlations in the target are imprinted in the coherence properties of the probing electron beam.

Time dependent reduced density matrix functional theory at strong correlation: insights from a two-site Anderson impurity model.

The one-body density matrix has recently attracted considerable attention as a promising key quantity for the description of systems out of equilibrium. Its time evolution is given in terms of the two-body density matrix, and thus the central challenge is to find approximations to the latter. An extra layer of difficulty is added when dealing with strong electron correlations. In this work, we explore precisely this regime by looking at the two-site Anderson impurity model as a case study. To address the system's dynamics, we use an adiabatic approximation based on the exact ground-state two-body density matrix. We find that this adiabatic extension does not reproduce the exact results even for a slow switch-on of the external perturbation, and we trace back this behavior to the lack of an accurate imaginary part of the adiabatic approximation to the two-body density matrix. The attempt to restore an approximate imaginary part through a Hilbert transform of the real part works well only for very short times, but quickly deteriorates for longer times, with the one-body density matrix being pushed out of its N-representability domain. Our results thus pose an important constraint on practical prescriptions to perform the time evolution of the one-body density matrix.

Density matrix and purity evolution in dissipative two-level systems: II. Relaxation.

We investigate the time evolution of the reduced density matrix (RDM) and its purity in the dynamics of a two-level system coupled to a dissipative harmonic bath, when the system is initially placed in one of its eigenstates. We point out that the symmetry of the initial condition confines the motion of the RDM elements to a one-dimensional subspace and show that the purity always goes through its maximally mixed value at some time during relaxation, but subsequently recovers and (under low-temperature, weakly dissipative conditions) can rise to values that approach unity. These behaviors are quantified through accurate path integral calculations. Under low-temperature, weakly dissipative conditions, we observe unusual, nonmonotonic population dynamics when the two-level system is initially placed in its ground state. We also analyze the origin of the system-bath interactions responsible for the nonmonotonic behavior of purity during relaxation. Our results show that classical dephasing processes arising from site level fluctuations lead to a monotonic decay of purity, and that the quantum mechanical decoherence events associated with spontaneous phonon emission are responsible for the subsequent recovery of purity. Last, we show that coupling with a low-temperature bath can purify a mixed two-level system. In the case of the maximally mixed initial RDM, the purity increases monotonically even during short time.