arXiv subjects

Norm M. Tubman

Publications and source records attributed to Norm M. Tubman.

At least 55 records · Page 3Linked to original sources

arXiv2020

Are multi-quasiparticle interactions important in molecular ionization?

Photo-emission spectroscopy directly probes individual electronic states, ranging from single excitations to high-energy satellites, which simultaneously represent multiple quasiparticles (QPs) and encode information about electronic correlation. First-principles description of the spectra requires an efficient and accurate treatment of all many-body effects. This is especially challenging for inner valence excitations where the single QP picture breaks down. Here, we provide the full valence spectra of small closed-shell molecules, exploring the independent and interacting quasiparticle regimes, computed with the fully-correlated adaptive sampling configuration interaction (ASCI) method. We critically compare these results to calculations with the many-body perturbation theory, based on the $GW$ and vertex corrected $GWΓ$ approaches. The latter explicitly accounts for two-QP quantum interactions, which have been often neglected. We demonstrate that for molecular systems, the vertex correction universally improves the theoretical spectra, and it is crucial for accurate prediction of QPs as well as capturing the rich satellite structures of high-energy excitations. $GWΓ$ offers a unified description across all relevant energy scales. Our results suggest that the multi-QP regime corresponds to dynamical correlations, which can be described via perturbation theory.

physics.chem-ph↗

arXiv2020

Observation of separated dynamics of charge and spin in the Fermi-Hubbard model

Strongly correlated quantum systems give rise to many exotic physical phenomena, including high-temperature superconductivity. Simulating these systems on quantum computers may avoid the prohibitively high computational cost incurred in classical approaches. However, systematic errors and decoherence effects presented in current quantum devices make it difficult to achieve this. Here, we simulate the dynamics of the one-dimensional Fermi-Hubbard model using 16 qubits on a digital superconducting quantum processor. We observe separations in the spreading velocities of charge and spin densities in the highly excited regime, a regime that is beyond the conventional quasiparticle picture. To minimize systematic errors, we introduce an accurate gate calibration procedure that is fast enough to capture temporal drifts of the gate parameters. We also employ a sequence of error-mitigation techniques to reduce decoherence effects and residual systematic errors. These procedures allow us to simulate the time evolution of the model faithfully despite having over 600 two-qubit gates in our circuits. Our experiment charts a path to practical quantum simulation of strongly correlated phenomena using available quantum devices.

quant-ph↗

arXiv2020

CASSCF with Extremely Large Active Spaces using the Adaptive Sampling Configuration Interaction Method

The complete active space self-consistent field (CASSCF) method is the principal approach employed for studying strongly correlated systems. However, exact CASSCF can only be performed on small active spaces of ~20 electrons in ~20 orbitals due to exponential growth in the computational cost. We show that employing the Adaptive Sampling Configuration Interaction (ASCI) method as an approximate Full CI solver in the active space allows CASSCF-like calculations within chemical accuracy (<1 kcal/mol for relative energies) in active spaces with more than ~50 active electrons in ~50 active orbitals, significantly increasing the sizes of systems amenable to accurate multiconfigurational treatment. The main challenge with using any selected CI-based approximate CASSCF is the orbital optimization problem; they tend to exhibit large numbers of local minima in orbital space due to their lack of invariance to active-active rotations (in addition to the local minima that exist in exact CASSCF). We highlight methods that can avoid spurious local extrema as a practical solution to the orbital optimization problem. We employ ASCI-SCF to demonstrate lack of polyradical character in moderately sized periacenes with up to 52 correlated electrons and compare against heat-bath CI on an iron porphyrin system with more than 40 correlated electrons.

physics.comp-ph↗

arXiv2019

Modern Approaches to Exact Diagonalization and Selected Configuration Interaction with the Adaptive Sampling CI Method

Recent advances in selected CI, including the adaptive sampling configuration interaction (ASCI) algorithm and its heat bath extension, have made the ASCI approach competitive with the most accurate techniques available, and hence an increasingly powerful tool in solving quantum Hamiltonians. In this work, we show that a useful paradigm for generating efficient selected CI/exact diagonalization algorithms is driven by fast sorting algorithms, much in the same way iterative diagonalization is based on the paradigm of matrix vector multiplication. We present several new algorithms for all parts of performing a selected CI, which includes new ASCI search, dynamic bit masking, fast orbital rotations, fast diagonal matrix elements, and residue arrays. The algorithms presented here are fast and scalable, and we find that because they are built on fast sorting algorithms they are more efficient than all other approaches we considered. After introducing these techniques we present ASCI results applied to a large range of systems and basis sets in order to demonstrate the types of simulations that can be practically treated at the full-CI level with modern methods and hardware, presenting double- and triple-zeta benchmark data for the G1 dataset. The largest of these calculations is Si$_{2}$H$_{6}$ which is a simulation of 34 electrons in 152 orbitals. We also present some preliminary results for fast deterministic perturbation theory simulations that use hash functions to maintain high efficiency for treating large basis sets.

physics.comp-ph↗

arXiv2019

Dynamical Mean-Field Theory Simulations with the Adaptive Sampling Configuration Interaction Method

In the pursuit of accurate descriptions of strongly correlated quantum many-body systems, dynamical mean-field theory (DMFT) has been an invaluable tool for elucidating the spectral properties and quantum phases of both phenomenological models and ab initio descriptions of real materials. Key to the DMFT process is the self-consistent map of the original system into an Anderson impurity model, the ground state of which is computed using an impurity solver. The power of the method is thus limited by the complexity of the impurity model the solver can handle. Simulating realistic systems generally requires many correlated sites. By adapting the recently proposed adaptive sampling configuration interaction (ASCI) method as an impurity solver, we enable much more efficient zero temperature DMFT simulations. The key feature of the ASCI method is that it selects only the most relevant Hilbert space degrees of freedom to describe the ground state. This reduces the numerical complexity of the calculation, which will allow us to pursue future DMFT simulations with more correlated impurity sites than in previous works. Here we present the ASCI-DMFT method and example calculations on the one-dimensional and two-dimensional Hubbard models that exemplify its efficient convergence and timing properties. We show that the ASCI approach is several orders of magnitude faster than the current best published ground state DMFT simulations, which allows us to study the bath discretization error in simulations with small clusters, as well as to address cluster sizes beyond the current state of the art. Our approach can also be adapted for other embedding methods such as density matrix embedding theory and self-energy embedding theory.

cond-mat.str-el↗

arXiv2019

Optimizing quantum heuristics with meta-learning

Variational quantum algorithms, a class of quantum heuristics, are promising candidates for the demonstration of useful quantum computation. Finding the best way to amplify the performance of these methods on hardware is an important task. Here, we evaluate the optimization of quantum heuristics with an existing class of techniques called `meta-learners'. We compare the performance of a meta-learner to Bayesian optimization, evolutionary strategies, L-BFGS-B and Nelder-Mead approaches, for two quantum heuristics (quantum alternating operator ansatz and variational quantum eigensolver), on three problems, in three simulation environments. We show that the meta-learner comes near to the global optima more frequently than all other optimizers we tested in a noisy parameter setting environment. We also find that the meta-learner is generally more resistant to noise, for example seeing a smaller reduction in performance in Noisy and Sampling environments and performs better on average by a `gain' metric than its closest comparable competitor L-BFGS-B. These results are an important indication that meta-learning and associated machine learning methods will be integral to the useful application of noisy near-term quantum computers.

quant-ph↗

arXiv2019

From Ansätze to Z-gates: a NASA View of Quantum Computing

For the last few years, the NASA Quantum Artificial Intelligence Laboratory (QuAIL) has been performing research to assess the potential impact of quantum computers on challenging computational problems relevant to future NASA missions. A key aspect of this research is devising methods to most effectively utilize emerging quantum computing hardware. Research questions include what experiments on early quantum hardware would give the most insight into the potential impact of quantum computing, the design of algorithms to explore on such hardware, and the development of tools to minimize the quantum resource requirements. We survey work relevant to these questions, with a particular emphasis on our recent work in quantum algorithms and applications, in elucidating mechanisms of quantum mechanics and their uses for quantum computational purposes, and in simulation, compilation, and physics-inspired classical algorithms. To our early application thrusts in planning and scheduling, fault diagnosis, and machine learning, we add thrusts related to robustness of communication networks and the simulation of many-body systems for material science and chemistry. We provide a brief update on quantum annealing work, but concentrate on gate-model quantum computing research advances within the last couple of years.

quant-ph↗

arXiv2018

Postponing the orthogonality catastrophe: efficient state preparation for electronic structure simulations on quantum devices

Despite significant work on resource estimation for quantum simulation of electronic systems, the challenge of preparing states with sufficient ground state support has so far been largely neglected. In this work we investigate this issue in several systems of interest, including organic molecules, transition metal complexes, the uniform electron gas, Hubbard models, and quantum impurity models arising from embedding formalisms such as dynamical mean-field theory. Our approach uses a state-of-the-art classical technique for high-fidelity ground state approximation. We find that easy-to-prepare single Slater determinants such as the Hartree-Fock state often have surprisingly robust support on the ground state for many applications of interest. For the most difficult systems, single-determinant reference states may be insufficient, but low-complexity reference states may suffice. For this we introduce a method for preparation of multi-determinant states on quantum computers.

quant-ph↗

arXiv2018

An efficient deterministic perturbation theory for selected configuration interaction methods

The interplay between advances in stochastic and deterministic algorithms has recently led to development of interesting new selected configuration interaction (SCI) methods for solving the many body Schrödinger equation. The performance of these SCI methods can be greatly improved with a second order perturbation theory (PT2) correction, which is often evaluated in a stochastic or hybrid-stochastic manner. In this work, we present a highly efficient, fully deterministic PT2 algorithm for SCI methods and demonstrate that our approach is orders of magnitude faster than recent proposals for stochastic SCI+PT2. We also show that it is important to have a compact reference SCI wave function, in order to obtain optimal SCI+PT2 energies. This indicates that it advantageous to use accurate search algorithms such as 'ASCI search' rather than more approximate approaches. Our deterministic PT2 algorithm is based on sorting techniques that have been developed for modern computing architectures and is inherently straightforward to use on parallel computing architectures. Related architectures such as GPU implementations can be also used to further increase the efficiency. Overall, we demonstrate that the algorithms presented in this work allow for efficient evaluation of trillions of PT2 contributions with modest computing resources.

cond-mat.str-el↗

arXiv2018

QMCPACK : An open source ab initio Quantum Monte Carlo package for the electronic structure of atoms, molecules, and solids

QMCPACK is an open source quantum Monte Carlo package for ab-initio electronic structure calculations. It supports calculations of metallic and insulating solids, molecules, atoms, and some model Hamiltonians. Implemented real space quantum Monte Carlo algorithms include variational, diffusion, and reptation Monte Carlo. QMCPACK uses Slater-Jastrow type trial wave functions in conjunction with a sophisticated optimizer capable of optimizing tens of thousands of parameters. The orbital space auxiliary field quantum Monte Carlo method is also implemented, enabling cross validation between different highly accurate methods. The code is specifically optimized for calculations with large numbers of electrons on the latest high performance computing architectures, including multicore central processing unit (CPU) and graphical processing unit (GPU) systems. We detail the program's capabilities, outline its structure, and give examples of its use in current research calculations. The package is available at http://www.qmcpack.org .

physics.comp-ph↗

arXiv2017

Cluster decomposition of full configuration interaction wave functions: a tool for chemical interpretation of systems with strong correlation

Approximate full configuration interaction (FCI) calculations have recently become tractable for systems of unforeseen size thanks to stochastic and adaptive approximations to the exponentially scaling FCI problem. The result of an FCI calculation is a weighted set of electronic configurations, which can also be expressed in terms of excitations from a reference configuration. The excitation amplitudes contain information on the complexity of the electronic wave function, but this information is contaminated by contributions from disconnected excitations, i.e. those excitations that are just products of independent lower-level excitations. The unwanted contributions can be removed via a cluster decomposition procedure, making it possible to examine the importance of connected excitations in complicated multireference molecules which are outside the reach of conventional algorithms. We present an implementation of the cluster decomposition analysis and apply it to both true FCI wave functions, as well as wave functions generated from the adaptive sampling CI (ASCI) algorithm. The cluster decomposition is useful for interpreting calculations in chemical studies, as a diagnostic for the convergence of various excitation manifolds, as well as as a guidepost for polynomially scaling electronic structure models. Applications are presented for (i) the double dissociation of water, (ii) the carbon dimer, (iii) the π space of polyacenes, as well as (iv) the chromium dimer. While the cluster amplitudes exhibit rapid decay with increasing rank for the first three systems, even connected octuple excitations still appear important in Cr$_2$, suggesting that spin-restricted single-reference coupled-cluster approaches may not be tractable for some problems in transition metal chemistry.

cond-mat.str-el↗

arXiv2017

Monte Carlo Tensor Network Renormalization

Techniques for approximately contracting tensor networks are limited in how efficiently they can make use of parallel computing resources. In this work we demonstrate and characterize a Monte Carlo approach to the tensor network renormalization group method which can be used straightforwardly on modern computing architectures. We demonstrate the efficiency of the technique and show that Monte Carlo tensor network renormalization provides an attractive path to improving the accuracy of a wide class of challenging computations while also providing useful estimates of uncertainty and a statistical guarantee of unbiased results.

cond-mat.str-el↗

arXiv2016

Measuring quantum entanglement, machine learning and wave function tomography: Bridging theory and experiment with the quantum gas microscope

There is an enormous amount of information that can be extracted from the data of a quantum gas microscope that has yet to be fully explored. The quantum gas microscope has been used to directly measure magnetic order, dynamic correlations, Pauli blocking, and many other physical phenomena in several recent groundbreaking experiments. However, the analysis of the data from a quantum gas microscope can be pushed much further, and when used in conjunction with theoretical constructs it is possible to measure virtually any observable of interest in a wide range of systems. We focus on how to measure quantum entanglement in large interacting quantum systems. In particular, we show that quantum gas microscopes can be used to measure the entanglement of interacting boson systems exactly, where previously it had been thought this was only possible for non-interacting systems. We consider algorithms that can work for large experimental data sets which are similar to theoretical variational Monte Carlo techniques, and more data limited sets using properties of correlation functions.

cond-mat.str-el↗

arXiv2016

Theory of Finite Size Effects for Electronic Quantum Monte Carlo Calculations of Liquids and Solids

Concentrating on zero temperature Quantum Monte Carlo calculations of electronic systems, we give a general description of the theory of finite size extrapolations of energies to the thermodynamic limit based on one and two-body correlation functions. We introduce new effective procedures, such as using the potential and wavefunction split-up into long and short range functions to simplify the method and we discuss how to treat backflow wavefunctions. Then we explicitly test the accuracy of our method to correct finite size errors on example hydrogen and helium many-body systems and show that the finite size bias can be drastically reduced for even small systems.

physics.comp-ph↗

arXiv2016

A deterministic alternative to the full configuration interaction quantum Monte Carlo method

Development of exponentially scaling methods has seen great progress in tackling larger systems than previously thought possible. One such technique, full configuration interaction quantum Monte Carlo, is a useful algorithm that allows exact diagonalization through stochastically sampling determinants. The method derives its utility from the information in the matrix elements of the Hamiltonian, along with a stochastic projected wave function, to find the important parts of Hilbert space. However, the stochastic representation of the wave function is not required to search Hilbert space efficiently, and here we describe a highly efficient deterministic method to achieve chemical accuracy for a wide range of systems, including the difficult Cr$_{2}$ dimer. In addition our method also allows efficient calculation of excited state energies, for which we illustrate with benchmark results for the excited states of C$_{2}$.

cond-mat.str-el↗

arXiv2016

Charge density waves in disordered media circumventing the Imry-Ma argument

Two powerful theoretical predictions, Anderson localization and the Imry-Ma argument, impose significant restrictions on the phases of matter that can exist in the presence of even the smallest amount of disorder in one-dimensional systems. These predictions forbid conducting states and ordered states respectively. It was thus remarkable that a mechanism to circumvent Anderson localization relying on the presence of correlated disorder was found, that is also realized in certain biomolecular systems. In a similar manner, we show that the Imry-Ma argument can be circumvented resulting in the formation of stable ordered states with discrete broken symmetries in disordered one dimensional systems. Specifically, we simulate a family of Hamiltonians of spinless fermions with correlated disorder and interactions, where we find that a charge density wave is stable up to a finite critical disorder strength. Having circumvented the Imry-Ma mechanism, we then investigate other mechanisms by which disorder can destroy an ordered state.

cond-mat.dis-nn↗

arXiv2015

Phase diagram of the $Z_3$ Parafermionic Chain with Chiral Interactions

Parafermions are exotic quasiparticles with non-Abelian fractional statistics that can be realized and stabilized in 1-dimensional models that are generalizations of the Kitaev p-wave wire. We study the simplest generalization, i.e. the $Z_3$ parafermionic chain. Using a Jordan-Wigner transform we focus on the equivalent three-state chiral clock model, and study its rich phase diagram using the density matrix renormalization group technique. We perform our analyses using quantum entanglement diagnostics which allow us to determine phase boundaries, and the nature of the phase transitions. In particular, we study the transition between the topological and trivial phases, as well as to an intervening incommensurate phase which appears in a wide region of the phase diagram. The phase diagram is predicted to contain a Lifshitz type transition which we confirm using entanglement measures. We also attempt to locate and characterize a putative tricritical point in the phase diagram where the three above mentioned phases meet at a single point.

cond-mat.str-el↗

arXiv2014

Quantum dissection of a covalent bond with the entanglement spectrum

We propose that spatial density matrices, which are singularly important in the study of quantum entanglement, encode the electronic fluctuations and correlations responsible for covalent bonding. From these density matrices, we develop tools that allow us to analyse how many body wave functions can be broken up into real space pieces. We apply these tools to the first row dimers, and in particular, we address the conflicting evidence in the literature about the presence of an inverted fourth bond and anti-ferromagnetic correlations in the $\text{C}_2$ molecule. Our results show that many body effects enhance anti-ferromagnetic fluctuations but are not related to the formation of an inverted fourth bond. We identify two inverted bonds in the $\text{C}_2$ molecule and establish their correspondence to the bonds in the $\text{Be}_2$ molecule. Additionally, we provide a new interpretation of the Mayer index, introduce partial bonds to fix deficiencies in molecular orbital theory, and prove the Hartree-Fock wave function for C$_{2}$ is not a triple bond. Our results suggest that entanglement-based methods can lead to a more realistic treatment of molecular and extended systems than possible before.

cond-mat.str-el↗