arXiv subjects

James K. Freericks

Publications and source records attributed to James K. Freericks.

At least 37 records · Page 2Linked to original sources

arXiv2022

Operator relationship between conventional coupled cluster and unitary coupled cluster

The chemistry community has long sought the exact relationship between the conventional and the unitary coupled cluster ansatz for a single-reference system, especially given the interest in performing quantum chemistry on quantum computers. In this work, we show how one can use the operator manipulations given by the exponential disentangling identity and the Hadamard lemma to relate the factorized form of the unitary coupled-cluster approximation to a factorized form of the conventional coupled cluster approximation (the factorized form is required, because some amplitudes are operator-valued and do not commute with other terms). By employing the Trotter product formula, one can then relate the factorized form to the standard form of the unitary coupled cluster ansatz. The operator dependence of the factorized form of the coupled cluster approximation can also be removed at the expense of requiring even more higher-rank operators, finally yielding the conventional coupled cluster. The algebraic manipulations of this approach are daunting to carry out by hand, but can be automated on a computer for small enough systems.

quant-ph↗

arXiv2022

Cartesian operator factorization method for Hydrogen

We generalize Schroedinger's factorization method for Hydrogen from the conventional separation into angular and radial coordinates to a Cartesian-based factorization. Unique to this approach, is the fact that the Hamiltonian is represented as a sum over factorizations in terms of coupled operators that depend on the coordinates and momenta in each Cartesian direction. We determine the eigenstates and energies, the wavefunctions in both coordinate and momentum space, and we also illustrate how this technique can be employed to develop the conventional confluent hypergeometric equation approach. The methodology developed here could potentially be employed for other Hamiltonians that can be represented as the sum over coupled Schroedinger factorizations.

quant-ph↗

arXiv2021

Low-Depth Unitary Coupled Cluster Theory for Quantum Computation

The unitary coupled cluster (UCC) approximation is one of the more promising wave-function ansätze for electronic structure calculations on quantum computers via the variational quantum eigensolver algorithm. However, for large systems with many orbitals, the required number of UCC factors still leads to very deep quantum circuits, which can be challenging to implement. Based on the observation that most UCC amplitudes are small for weakly correlated molecules, we devise an algorithm that employs a Taylor expansion in the small amplitudes, trading off circuit depth for extra measurements. Strong correlations can be taken into account by performing the expansion about a small set of UCC factors, which are treated exactly. Near equilibrium, the Taylor series expansion often works well without the need to include any exact factors; as the molecule is stretched and correlations increase, we find only a small number of factors need to be treated exactly.

quant-ph↗

arXiv2021

Algebraic Compression of Quantum Circuits for Hamiltonian Evolution

Unitary evolution under a time dependent Hamiltonian is a key component of simulation on quantum hardware. Synthesizing the corresponding quantum circuit is typically done by breaking the evolution into small time steps, also known as Trotterization, which leads to circuits whose depth scales with the number of steps. When the circuit elements are limited to a subset of SU(4) -- or equivalently, when the Hamiltonian may be mapped onto free fermionic models -- several identities exist that combine and simplify the circuit. Based on this, we present an algorithm that compresses the Trotter steps into a single block of quantum gates. This results in a fixed depth time evolution for certain classes of Hamiltonians. We explicitly show how this algorithm works for several spin models, and demonstrate its use for adiabatic state preparation of the transverse field Ising model.

quant-ph↗

arXiv2021

Real-time evolution of static electron-phonon models in time-dependent electric fields

We present an exact Monte Carlo method to simulate the nonequilibrium dynamics of electron-phonon models in the adiabatic limit of zero phonon frequency. The classical nature of the phonons allows us to sample the equilibrium phonon distribution and efficiently evolve the electronic subsystem in a time-dependent electromagnetic field for each phonon configuration. We demonstrate that our approach is particularly useful for charge-density-wave systems experiencing pulsed electric fields, as they appear in pump-probe experiments. For the half-filled Holstein model in one and two dimensions, we calculate the out-of-equilibrium response of the current and the energy after a pulse is applied as well as the photoemission spectrum before and after the pump. Finite-size effects are under control for chains of $162$ sites (in one dimension) or $16\times 16$ square lattices (in two dimensions).

cond-mat.str-el↗

arXiv2021

Bridging the Gap Between the Transient and the Steady State of a Nonequilibrium Quantum System

Many-body quantum systems in nonequilibrium remain one of the frontiers of many-body physics. While there has been significant advances in describing the short-time evolution of these systems using a variety of different numerical algorithms, it has been quite difficult to evolve a system from an equilibrium state prior to the application of a driving field, to the long-time steady (or periodically oscillating) state. These dynamics are complex: the retarded quantities tend to approach their long-time limit much faster than the lesser (or greater) quantities. Recent work on strongly correlated electrons in DC electric fields illustrated that the system may evolve through successive quasi-thermal states obeying an effective fluctuation-dissipation theorem in time. We demonstrate an extrapolation scheme that uses the short-time transient calculation to obtain the retarded quantities and to extract how the lesser/greater quantities vary with time and then extend the numerical solutions all the way to the steady state, with minimal additional computational cost. Our approach focuses on extrapolating the electronic self-energy and then employing that to determine the Green's function and various experimentally relevant expectation values.

quant-ph↗

arXiv2020

Sparse-Hamiltonian approach to the time evolution of molecules on quantum computers

Quantum chemistry has been viewed as one of the potential early applications of quantum computing. Two techniques have been proposed for electronic structure calculations: (i) the variational quantum eigensolver and (ii) the phase-estimation algorithm. In both cases, the complexity of the problem increases for basis sets where either the Hamiltonian is not sparse, or it is sparse, but many orbitals are required to accurately describe the molecule of interest. In this work, we explore the possibility of mapping the molecular problem onto a sparse Hubbard-like Hamiltonian, which allows a Green's-function-based approach to electronic structure via a hybrid quantum-classical algorithm. We illustrate the time-evolution aspect of this methodology with a simple four-site hydrogen ring.

quant-ph↗

arXiv2020

Schrodinger's original quantum-mechanical solution for hydrogen

In 1926, Erwin Schrodinger wrote a series of papers that invented wave mechanics and set the foundation for much of the single-particle quantum mechanics that we teach today. In his first paper, he solved the Schrodinger equation using the Laplace method, which is a technique that is quite powerful, but rarely taught. This is unfortunate, because it opens the door to examining quantum mechanics from a complex-analysis perspective. Gaining this experience with complex analysis is a useful notion to consider when teaching quantum mechanics, as these techniques can be widely used outside of quantum mechanics, unlike the standard Frobenius summation method, which is normally taught, but rarely used elsewhere. The Laplace method strategy is subtle and no one has carefully gone through the arguments that Schrodinger did in this first paper, instead it is often just stated that the solution was adopted from Schlesinger's famous differential equation textbook. In this work, we show how the Laplace method can be used to solve for the quantum-mechanical energy eigenfunctions of the hydrogen atom, following Schrodinger's original solution, with all the necessary details, and illustrate how it can be taught in advanced instruction; it does require familiarity with intermediate-level complex analysis, which we also briefly review.

quant-ph↗

arXiv2020

Characterizing the Nonequilibrium Dynamics of Field-Driven Correlated Quantum Systems

Recent experimental advances in ultrafast phenomena have triggered renewed interest in the dynamics of correlated quantum systems away from equilibrium. We review nonequilibrium dynamical mean-field theory studies of both the transient and the steady states of a DC field-driven correlated quantum system. In particular, we focus on the nonequilibrium behavior and how it relates to the fluctuation-dissipation theorem. The fluctuation-dissipation theorem emerges as an indicator for how the system thermalizes and for how it reaches a steady state. When the system thermalizes in an infinite temperature steady state it can pass through a succession of quasi-thermal states that approximately obey the fluctuation-dissipation theorem. We also discuss the Wigner distribution and what its evolution tells us about the nonequilibrium many-body problem.

cond-mat.str-el↗

arXiv2019

Theory for Time-Resolved Resonant Inelastic X-ray Scattering

Time-resolved measurements of materials provide a wealth of information on quasiparticle dynamics, and have been the focus of optical studies for decades. In this paper, we develop a theory for explicitly evaluating time-resolved resonant inelastic X-ray scattering (tr-RIXS). We apply the theory to a non-interacting electronic system and reveal the particle-hole spectrum and its evolution during the pump pulse. With a high-frequency pump, the frequency and amplitude dependence analysis of the spectra agrees well with the steady-state assumptions and Floquet excitations. When the pump frequency is low, the spectrum extracts real-time dynamics of the particle-hole continuum in momentum space. These results verify the correctness of our theory and demonstrate the breadth of physical problems that tr-RIXS could shed light on.

cond-mat.str-el↗

arXiv2019

Proving the existence of bound states for attractive potentials in 1-d and 2-d without calculus

Schroedinger developed an operator method for solving quantum mechanics. While this technique is overshadowed by his more familiar differential equation approach, it has found wide application as an illustration of supersymmetric quantum mechanics. One reason for the reticence in its usage for conventional quantum instruction is that the approach for simple problems like the particle-in-a-box is much more complicated than the differential equation approach, making it appear to be less useful for pedagogy. We argue that the approach is still quite attractive because it employs only algebraic methods, and thereby has a much lower level of math background needed to use it. We show how Schroedinger's operator method can be streamlined for these particle-in-a-box problems greatly reducing the complexity of the solution and making it much more accessible. As an application, we illustrate how this approach can be used to prove an important result, the existence of bound states for one- and two-dimensional attractive potentials, using only algebraic methods. The approach developed here can be employed in undergraduate classes and possibly even high school classes because it employs only algebra and requires essentially no calculus.

physics.gen-ph↗

arXiv2018

Minimal Effective Gibbs Ansatz (MEGA): A simple protocol for extracting an accurate thermal representation for quantum simulation

Quantum Gibbs state sampling algorithms generally suffer from either scaling exponentially with system size or requiring specific knowledge of spectral properties \textit{a priori}. Also, these algorithms require a large overhead of bath or scratch/ancilla qubits. We propose a method, termed the minimal effective Gibbs ansatz (MEGA), which uses a quantum computer to determine a minimal ensemble of pure states that accurately reproduce thermal averages of typical observables. This technique employs properties of correlation functions that can be split into a lesser and greater part; here, we primarily focus on single-particle Green's functions. When properly measured, these correlation functions provide a simple test to indicate how close a given pure state or ensemble of pure states are to providing accurate thermal expectation values. Further, we show that when properties such as the eigenstate thermalization hypothesis hold, this approach leads to accurate results with a sparse ensemble of pure states; sometimes only one suffices. We illustrate the ansatz using exact diagonalization simulations on small clusters for the Fermi-Hubbard and Hubbard-like models. Even if MEGA becomes as computationally complex as other Gibbs state samplers, it still gains an advantage due to its ease of implementation without any \textit{a priori} information about the Hamiltonian and in the efficient allocation of available qubits by eliminating bath qubits and using a minimal number of ancilla.

quant-ph↗

arXiv2018

Positivity of the spectral densities of retarded Floquet Green functions

Periodically driven nonequilibrium many-body systems are interesting because they have a quasi-energy spectra, which can be tailored by controlling the external driving fields. We derive the general spectral representation of retarded Green functions in the Floquet regime, thereby generalizing the well-known Lehmann representation from equilibrium many-body physics. The derived spectral Floquet representation allows us to prove the nonnegativity of spectral densities and to determine exact spectral sum rules, which can be employed to benchmark the accuracy of approximations to the exact Floquet many-body Green functions.

cond-mat.str-el↗

arXiv2016

Zone-center phonons of bulk, few-layer, and monolayer 1T-TaS$_2$: Detection of the commensurate charge density wave phase through Raman scattering

We present first-principles calculations of the vibrational properties of the transition metal dichalcogenide 1T-TaS$_2$ for various thicknesses in the high-temperature (undistorted) phase and the low-temperature commensurate charge density wave (CDW) phase. We also present measurements of the Raman spectra for bulk, few-layer, and monolayer samples at temperatures well below that of the bulk transition to the commensurate phase. Through our calculations, we identify the low-frequency folded-back acoustic modes as a convenient signature of the commensurate CDW wave structure in vibrational spectra. In our measured Raman spectra, this signature is clearly evident in all of the samples, indicating that the commensurate phase remains the ground state as the material is thinned, even down to a single layer. This is in contrast to some previous studies which suggest a suppression of the commensurate CDW transition in thin flakes. We also use polarized Raman spectroscopy to probe c-axis orbital texture in the low-T phase, which has recently been suggested as playing a role in the metal-insulator transition that accompanies the structural transition to the commensurate CDW phase.

cond-mat.mtrl-sci↗

arXiv2013

Examining electron-boson coupling using time-resolved spectroscopy

Nonequilibrium pump-probe time domain spectroscopies can become an important tool to disentangle degrees of freedom whose coupling leads to broad structures in the frequency domain. Here, using the time-resolved solution of a model photoexcited electron-phonon system we show that the relaxational dynamics are directly governed by the equilibrium self-energy so that the phonon frequency sets a window for "slow" versus "fast" recovery. The overall temporal structure of this relaxation spectroscopy allows for a reliable and quantitative extraction of the electron-phonon coupling strength without requiring an effective temperature model or making strong assumptions about the underlying bare electronic band dispersion.

cond-mat.other↗

arXiv2012

Spectroscopy and Thermometry of Drumhead Modes in a Mesoscopic Trapped-Ion Crystal using Entanglement

We demonstrate spectroscopy and thermometry of individual motional modes in a mesoscopic 2D ion array using entanglement-induced decoherence as a method of transduction. Our system is a $\sim$400 $μ$m-diameter planar crystal of several hundred $^9$Be$^+$ ions exhibiting complex drumhead modes in the confining potential of a Penning trap. Exploiting precise control over the $^9$Be$^+$ valence electron spins, we apply a homogeneous spin-dependent optical dipole force to excite arbitrary transverse modes with an effective wavelength approaching the interparticle spacing ($\sim$20 \nolinebreak$μ$m). Center-of-mass displacements below 1 nm are detected via entanglement of spin and motional degrees of freedom.

quant-ph↗

arXiv2012

Engineered 2D Ising interactions on a trapped-ion quantum simulator with hundreds of spins

The presence of long-range quantum spin correlations underlies a variety of physical phenomena in condensed matter systems, potentially including high-temperature superconductivity. However, many properties of exotic strongly correlated spin systems (e.g., spin liquids) have proved difficult to study, in part because calculations involving N-body entanglement become intractable for as few as N~30 particles. Feynman divined that a quantum simulator - a special-purpose "analog" processor built using quantum particles (qubits) - would be inherently adept at such problems. In the context of quantum magnetism, a number of experiments have demonstrated the feasibility of this approach. However, simulations of quantum magnetism allowing controlled, tunable interactions between spins localized on 2D and 3D lattices of more than a few 10's of qubits have yet to be demonstrated, owing in part to the technical challenge of realizing large-scale qubit arrays. Here we demonstrate a variable-range Ising-type spin-spin interaction J_ij on a naturally occurring 2D triangular crystal lattice of hundreds of spin-1/2 particles (9Be+ ions stored in a Penning trap), a computationally relevant scale more than an order of magnitude larger than existing experiments. We show that a spin-dependent optical dipole force can produce an antiferromagnetic interaction J_ij ~ 1/d_ij^a, where a is tunable over 0<a<3; d_ij is the distance between spin pairs. These power-laws correspond physically to infinite-range (a=0), Coulomb-like (a=1), monopole-dipole (a=2) and dipole-dipole (a=3) couplings. Experimentally, we demonstrate excellent agreement with theory for 0.05<a<1.4. This demonstration coupled with the high spin-count, excellent quantum control and low technical complexity of the Penning trap brings within reach simulation of interesting and otherwise computationally intractable problems in quantum magnetism.

quant-ph↗

arXiv2011

Lanczos-based Low-Rank Correction Method for Solving the Dyson Equation in Inhomogenous Dynamical Mean-Field Theory

Inhomogeneous dynamical mean-field theory has been employed to solve many interesting strongly interacting problems from transport in multilayered devices to the properties of ultracold atoms in a trap. The main computational step, especially for large systems, is the problem of calculating the inverse of a large sparse matrix to solve Dyson's equation and determine the local Green's function at each lattice site from the corresponding local self-energy. We present a new efficient algorithm, the Lanczos-based low-rank algorithm, for the calculation of the inverse of a large sparse matrix which yields this local (imaginary time) Green's function. The Lanczos-based low-rank algorithm is based on a domain decomposition viewpoint, but avoids explicit calculation of Schur complements and relies instead on low-rank matrix approximations derived from the Lanczos algorithm, for solving the Dyson equation. We report at least a 25-fold improvement of performance compared to explicit decomposition (such as sparse LU) of the matrix inverse. We also report that scaling relative to matrix sizes, of the low-rank correction method on the one hand and domain decomposition methods on the other, are comparable.

cond-mat.str-el↗