Density Matrix Perturbation Research Articles

A modified least squares-based tomography with density matrix perturbation and linear entropy consideration along with performance analysis

Quantum state tomography identifies target quantum states by performing repetitive measurements on identical copies. In this paper, we have two key contributions aimed at improving traditional post-processing computational complexity and sample complexity of quantum tomography protocols. In the first case, we propose a new low-cost positivity constraint method based on density matrix perturbation after the least squares (LS) estimation of the density matrix. In the second case, we propose a new cost function with the maximum linear entropy and LS method to improve the sample average trace distance with reasonably low sample complexity. We call it the LS with the maximum entropy (LSME) method. Our proposed algorithm does not follow the iterative optimization technique, which is true for existing maximum likelihood and entropy-based ones. Performance analysis is conducted for our proposed methods by studying how they compare to the existing techniques for different sample complexities and dimensionalities. Extensive numerical simulations have been conducted to demonstrate the advantages of the proposed tomography algorithms.

Semi-Empirical Shadow Molecular Dynamics: A PyTorch Implementation.

Extended Lagrangian Born-Oppenheimer molecular dynamics (XL-BOMD) in its most recent shadow potential energy version has been implemented in the semiempirical PyTorch-based software PySeQM. The implementation includes finite electronic temperatures, canonical density matrix perturbation theory, and an adaptive Krylov subspace approximation for the integration of the electronic equations of motion within the XL-BOMB approach (KSA-XL-BOMD). The PyTorch implementation leverages the use of GPU and machine learning hardware accelerators for the simulations. The new XL-BOMD formulation allows studying more challenging chemical systems with charge instabilities and low electronic energy gaps. The current public release of PySeQM continues our development of modular architecture for large-scale simulations employing semi-empirical quantum-mechanical treatment. Applied to molecular dynamics, simulation of 840 carbon atoms, one integration time step executes in 4 s on a single Nvidia RTX A6000 GPU.

Controlling Rotationally Resolved Two-Dimensional Infrared Spectra with Polarization.

Recent advancements in infrared frequency combs will enable facile recording of coherent two-dimensional infrared spectra of gas-phase molecules with rotational resolution (RR2DIR). Using time-dependent density-matrix perturbation theory and angular momentum algebra techniques, we derive new polarization conditions unique to freely rotating molecules and absent in the condensed phase. These polarization conditions can be used to suppress parts of 2DIR rovibrational response, clarifying complicated RR2DIR spectra. With the polarization control methods described here, RR2DIR spectroscopy can be a powerful tool for studying complex gas mixtures of polyatomic molecules.

Analysis of All-Optical Generation of Graphene Surface Plasmons by a Frequency-Difference Process

The generation of graphene surface plasmons (SPs) by a frequency-difference nonlinear (NL) process caused by the interaction of two optical beams was experimentally demonstrated several years ago by measuring the differential reflectance of the probe beam. However, the understanding of these results requires much larger second-order optical conductivities of graphene than calculations performed so far can yield. In this work, we carefully calculate the relevant NL conductivities and show that, indeed, the experimental observations of the differential reflectance must have originated from physical processes beyond the coherent frequency-difference generation of SPs described by the density-matrix perturbation theory approach, presumably by hot-electron effects. We also suggest an alternative way of detecting optically generated SPs, which can be feasible at lower powers of the optical pulses. Such additional experiments are expected to help understand the remaining discrepancy between the theory and the existing experimental data.

Differential privacy protection scheme based on community density aggregation and matrix perturbation

With the development and popularity of social networks, the security issues of personal data await effective solution. We propose a differential privacy protection scheme for social network data based on community density aggregation and matrix perturbation (MPCD) and introduce the correlation coefficient k to preserve differential privacy and availability of edge-related data. We adopt a community structure rapid identification algorithm to identify social network structure labels, to realize the label aggregation of community nodes. Combined with the structure of a binary tree, we use the adaptive method to identify the dense regions for the generated upper triangular adjacency matrix. We perturb the edge connection probability of the identified dense regions and reconstruct a disturbed adjacency matrix by edge optimal allocation to publish the final network graph, which can improve the efficiency of the algorithm and data availability. In addition, we experimentally evaluate our approach on four social network datasets and show that the published network graph has better data availability and privacy protection, with higher execution efficiency than the four classical schemes.

Computational Protocol to Evaluate Electron-Phonon Interactions Within Density Matrix Perturbation Theory.

We present a computational protocol, based on density matrix perturbation theory, to obtain non-adiabatic, frequency-dependent electron–phonon self-energies for molecules and solids. Our approach enables the evaluation of electron–phonon interaction using hybrid functionals, for spin-polarized systems, and the computational overhead to include dynamical and non-adiabatic terms in the evaluation of electron–phonon self-energies is negligible. We discuss results for molecules, as well as pristine and defective solids.

Polarized induced phase grating in a quantized four-level graphene monolayer system.

We discuss the electromagnetically induced grating (EIG) and electromagnetically induced phase grating (EIPG) in a four-level quantized graphene monolayer system. By using the density matrix technique and perturbation theory, we first obtain the self-Kerr nonlinear susceptibility of the graphene system; afterwards, we study the amplitude and phase modulations of the probe light. We discovered that the EIG and EIPG can be found by controlling the elliptically polarized coupling fields that interact with the monolayer graphene system. Owing to the phase modulation of the transmitted light beam, we recognized that the probe strength can also additionally switch from zeroth-order to high-order diffraction. Moreover, we found that the diffraction performance of the grating may be adjusted through tuning the polarization of the coupling light.

Quantum Perturbation Theory Using Tensor Cores and a Deep Neural Network.

Time-independent quantum response calculations are performed using Tensor cores. This is achieved by mapping density matrix perturbation theory onto the computational structure of a deep neural network. The main computational cost of each deep layer is dominated by tensor contractions, i.e., dense matrix-matrix multiplications, in mixed-precision arithmetics, which achieves close to peak performance. Quantum response calculations are demonstrated and analyzed using self-consistent charge density-functional tight-binding theory as well as coupled-perturbed Hartree-Fock theory. For linear response calculations, a novel parameter-free convergence criterion is presented that is well-suited for numerically noisy low-precision floating point operations and we demonstrate a peak performance of almost 200 Tflops using the Tensor cores of two Nvidia A100 GPUs.

Spatio-temporal properties of pulse propagation in a graphene quantum system

In this paper we have theoretically studied the spatial-temporal evolution of electromagnetic light propagation through a four-level graphene quantum system by using density matrix method and perturbation theory. The four-level graphene quantum medium interacted by an elliptical polarized coupling and a weak probe lights, respectively. We present the analytical solution for solving the Maxwell–Bloch equations for graphene and electromagnetic field in space and time domains. Then, we have analyzed the dynamic control of pulse propagation and optical dual switching in such a laser-driven quantum system. Our theoretical findings show that by adjusting the optical parameters such as elliptical angle i.e. phase difference between right-and-left circularly polarized, one can easily control the absorption spectrum and pulse propagation of the probe light in graphene medium. Our results may have potential applications in designing the new quantum devices for usage in quantum information processing.

Paramagnetic NMR Shielding Tensors and Ring Currents: Efficient Implementation and Application to Heavy Element Compounds.

We present an efficient implementation of paramagnetic NMR shielding tensors and shifts in a nonrelativistic and scalar-relativistic density functional theory framework. For the latter, we make use of the scalar exact two-component Hamiltonian in its local approximation, and generally we apply the well established (multipole-accelerated) resolution of the identity approximation and the seminumerical exchange approximation. The perturbed density matrix of a paramagnetic NMR shielding calculation is further used to study the magnetically induced current density and ring currents of open-shell systems as illustrated for [U@Bi12]3-. [U@Bi12]3- features delocalized highest occupied molecular orbitals and sustains a net diatropic ring current of ca. 18 nA/T through the Bi12 torus similar to the all-metal aromatic heavy-element cluster [Th@Bi12]4-.

Influence of position dependent effective mass on impurity binding energy and absorption in quantum wells with the Konwent potential

In this work, we perform a theoretical investigation on the effect of position-dependent effective mass on binding energy and optical absorption coefficient for donor impurities in single and double quantum wells defined by Konwent potential. We have used the diagonalization method by choosing a wave function based on the trigonometric orthonormal base functions that are solutions of an infinite square quantum well to get the energy spectrum of the system, the variational method for impurity binding energy is used and also linear absorption coefficient is deduced from the density matrix approach and perturbation expansion method. Numerical results reveal that impurity binding energy as well as the linear optical absorption coefficient are remarkably affected by the confinement potential parameters, position of an impurity and the approach used for the effective electron mass. Moreover, it is seen that with an appropriate choice of the structure parameters and position dependence effective mass distribution, the optical response of the system can be tailored in a controllable manner.

Notes on density matrix perturbation theory.

Density matrix perturbation theory (DMPT) is known as a promising alternative to the Rayleigh-Schrödinger perturbation theory, in which the sum-over-states (SOS) is replaced by algorithms with perturbed density matrices as the input variables. In this article, we formulate and discuss three types of DMPT, with two of them based only on density matrices: the approach of Kussmann and Ochsenfeld [J. Chem. Phys. 127, 054103 (2007)] is reformulated via the Sylvester equation and the recursive DMPT of Niklasson and Challacombe [Phys. Rev. Lett. 92, 193001 (2004)] is extended to the hole-particle canonical purification (HPCP) from Truflandier et al. [J. Chem. Phys. 144, 091102 (2016)]. A comparison of the computational performances shows that the aforementioned methods outperform the standard SOS. The HPCP-DMPT demonstrates stable convergence profiles but at a higher computational cost when compared to the original recursive polynomial method.

Orbital magneto-optical response of periodic insulators from first principles

Magneto-optical response, i.e. optical response in the presence of a magnetic field, is commonly used for characterization of materials and in optical communications. However, quantum mechanical description of electric and magnetic fields in crystals is not straightforward as the position operator is ill defined. We present a reformulation of the density matrix perturbation theory for time-dependent electromagnetic fields under periodic boundary conditions, which allows us to treat the orbital magneto-optical response of solids at the ab initio level. The efficiency of the computational scheme proposed is comparable to standard linear-response calculations of absorption spectra and the results of tests for molecules and solids agree with the available experimental data. A clear signature of the valley Zeeman effect is revealed in the continuum magneto-optical spectrum of a single layer of hexagonal boron nitride. The present formalism opens the path towards the study of magneto-optical effects in strongly driven low-dimensional systems.

A Joint Spectral Similarity Measure for Graphs Classification

In spite of the simple linear relationship between the adjacency A and the Laplacian L matrices, L=D−A where D is the degrees matrix, these matrices seem to reveal informations about the graph in different ways, where it appears that some details are detected only by one of them, as in the case of cospectral graphs. Based on this observation, a new graphs similarity measure, referred to as joint spectral similarity (JSS) incorporating both spectral information from A and L is introduced. A weighting parameter to control the relative influence of each matrix is used. Furthermore, to highlight the overlapping and the unequal contributions of these matrices for graph representation, they are compared in terms of the so called Von Neumann entropy (VN), connectivity and complexity measures. The graph is viewed as a quantum system and thus, the calculated VN entropy of its perturbed density matrix emphasizes the overlapping in terms of information quantity of A and L matrices. The impact of matrix representation is strongly illustrated by classification findings on real and conceptual graphs based on JSS measure.The obtained results show the effectiveness of the JSS measure in terms of graph classification accuracies and also highlight varying information overlapping rates of A and L, and point out their different ways in recovering structural information of the graph.

Chiral Mott insulators in frustrated Bose-Hubbard models on ladders and two-dimensional lattices: A combined perturbative and density matrix renormalization group study

We study the fully gapped chiral Mott insulator (CMI) of frustrated Bose-Hubbard models on ladders and two-dimensional lattices by perturbative strong-coupling analysis and density matrix renormalization group (DMRG). First we show the existence of a low-lying exciton state on all geometries carrying the correct quantum numbers responsible for the condensation of excitons and formation of the CMI in the intermediate interaction regime. Then we perform systematic DMRG simulations on several two-leg ladder systems with $\pi$-flux and carefully characterize the two quantum phase transitions. We discuss the possibility to extend the generally very small CMI window by including repulsive nearest-neighbour interactions or changing density and coupling ratios.

A Perturbative Density Matrix Renormalization Group Algorithm for Large Active Spaces.

We describe a low cost alternative to the standard variational DMRG (density matrix renormalization group) algorithm that is analogous to the combination of the selected configuration interaction plus perturbation theory (SCI+PT). We denote the resulting method p-DMRG (perturbative DMRG) to distinguish it from the standard variational DMRG. p-DMRG is expected to be useful for systems with very large active spaces, for which variational DMRG becomes too expensive. Similar to SCI+PT, in p-DMRG, a zeroth-order wave function is first obtained by a standard DMRG calculation but with a small bond dimension. Then, the residual correlation is recovered by a second-order perturbative treatment. We discuss the choice of partitioning for perturbation theory, which is crucial for its accuracy and robustness. To circumvent the problem of a large bond dimension in the first-order wave function, we use a sum of matrix product states to expand the first-order wave function, yielding substantial savings in computational cost and memory. We also propose extrapolation schemes to reduce the errors in the zeroth- and first-order wave functions. Numerical results for Cr2 with a (28e, 76o) active space and 1,3-butadiene with an (22e, 82o) active space reveal that p-DMRG provides ground state energies of a similar quality to variational DMRG with very large bond dimensions but at a significantly lower computational cost. This suggests that p-DMRG will be an efficient tool for benchmark studies in the future.

Communication: An efficient stochastic algorithm for the perturbative density matrix renormalization group in large active spaces

We present an efficient stochastic algorithm for the recently introduced perturbative density matrix renormalization group method for large active spaces. The stochastic implementation bypasses the computational bottleneck involved in solving the first order equation in the earlier deterministic algorithm. We demonstrate the efficiency and accuracy of the algorithm on the C2 and Cr2 molecular benchmark systems.

Gauge invariance of excitonic linear and nonlinear optical response

We study the equivalence of four different approaches to calculate the excitonic linear and nonlinear optical response of multiband semiconductors. These four methods derive from two choices of gauge, i.e. length and velocity gauges, and two ways of computing the current density, i.e. direct evaluation and evaluation via the time-derivative of the polarization density. The linear and quadratic response functions are obtained for all methods by employing a perturbative density matrix approach within the mean-field approximation. The equivalence of all four methods is shown rigorously, when a correct interaction Hamiltonian is employed for the velocity gauge approaches. The correct interaction is written as a series of commutators containing the unperturbed Hamiltonian and position operators, which becomes equivalent to the conventional velocity gauge interaction in the limit of infinite Coulomb screening and infinitely many bands. As a case study, the theory is applied to hexagonal boron nitride monolayers, and the linear and nonlinear optical response found in different approaches are compared.

Double-dark-resonance-enhanced Kerr nonlinearity in a single layer of graphene nanostructure

In this paper, a novel scheme is proposed for the giant enhanced Kerr nonlinearity in a single layer of graphene nanostructure based on quantum optics and nonlinear optical sciences. The linear and the nonlinear susceptibility of the monolayer graphene system are presented in details by using the density matrix method and perturbation theory. After deriving the equations of motion in the steady-state regime, we analytically solve the linear and nonlinear susceptibility of the system. Our numerical results show that the giant enhanced Kerr nonlinearity can be obtained in the double-dark-resonance condition with zero linear and nonlinear absorption. Our results may have potential applications in quantum information science in infrared and terahertz regimes.

Level sequence and splitting identification of closely spaced energy levels by angle-resolved analysis of fluorescence light

The angular distribution and linear polarization of the fluorescence light following the resonant photoexcitation is investigated within the framework of the density matrix and second-order perturbation theory. Emphasis has been placed on "signatures" for determining the level sequence and splitting of intermediate (partially) overlapping resonances, if analyzed as a function of the photon energy of the incident light. Detailed computations within the multiconfiguration Dirac-Fock method have been performed especially for the $1s^{2}2s^{2}2p^{6}3s\;\, J_{i}=1/2 \,+\, \gamma_{1} \:\rightarrow\: (1s^{2}2s2p^{6}3s)_{1}3p_{3/2}\;\, J=1/2, \, 3/2 \:\rightarrow\: 1s^{2}2s^{2}2p^{6}3s\;\, J_{f}=1/2 \,+\, \gamma_{2}$ photoexcitation and subsequent fluorescence emission of atomic sodium. A remarkably strong dependence of the angular distribution and linear polarization of the $\gamma_{2}$ fluorescence emission is found upon the level sequence and splitting of the intermediate $(1s^{2}2s2p^{6}3s)_{1}3p_{3/2}\;\, J=1/2, \, 3/2$ overlapping resonances owing to their finite lifetime (linewidth). We therefore suggest that accurate measurements of the angular distribution and linear polarization might help identify the sequence and small splittings of closely-spaced energy levels, even if they can not be spectroscopically resolved.