arXiv subjects

Christian Gogolin

Publications and source records attributed to Christian Gogolin.

At least 19 recordsLinked to original sources

arXiv2026

Optimizing and Comparing Quantum Resources of Statistical Phase Estimation and Krylov Subspace Diagonalization

We develop a framework that enables direct and meaningful comparison of two early fault-tolerant methods for the computation of eigenenergies, namely \gls{qksd} and \gls{spe}, within which both methods use expectation values of Chebyshev polynomials of the Hamiltonian as input. For \gls{qksd} we propose methods for optimally distributing shots and ensuring sufficient non-linearity of states spanning the Krylov space. For \gls{spe} we improve rigorous error-bounds, achieving roughly a factor $2/3$ reduction of circuit depth. We provide insights into the scalability of and the practical realization of these methods by computing the maximum Chebyshev degree, linearly related to circuit depth, and the respective number of repetitions required for the simulation of molecules with active spaces up to 54 electrons in 36 orbitals by leveraging \gls{mps}/\gls{dmrg}.

quant-ph↗

arXiv2025

Molecular Properties from Quantum Krylov Subspace Diagonalization

Quantum Krylov subspace diagonalization is a prominent candidate for early fault tolerant quantum simulation of many-body and molecular systems, but so far the focus has been mainly on computing ground-state energies. We go beyond this by deriving analytical first-order derivatives for quantum Krylov methods and show how to obtain relaxed one and two particle reduced density matrices of the Krylov eigenstates. The direct approach to measuring these matrices requires a number of distinct measurement that scales quadratically with the Krylov dimension $D$. Here, we show how to reduce this scaling to a constant. This is done by leveraging quantum signal processing to prepare Krylov eigenstates, including exited states, in depth linear in $D$. We also compare several measurement schemes for efficiently obtaining the expectation value of an operator with states prepared using quantum signal processing. We validate our approach by computing the nuclear gradient of a small molecule and estimating its variance.

quant-ph↗

arXiv2024

Error mitigation and circuit division for early fault-tolerant quantum phase estimation

As fully fault-tolerant quantum computers capable of solving useful problems remain a distant goal, we anticipate an era of "early fault tolerance" where limited error correction is available. We propose a framework for designing early fault-tolerant algorithms by trading between error correction overhead and residual logical noise, and apply it to quantum phase estimation (QPE). We develop a quantum-Fourier-transform (QFT)-based QPE technique that is robust to global depolarising noise and outperforms the previous state of the art at low and moderate noise rates. We further introduce the Explicitly Unbiased Maximum Likelihood Estimation (EUMLE), a data processing technique that mitigates arbitrary errors in QFT-based QPE schemes. EUMLE provides consistent, asymptotically normal error-mitigated estimates, addressing the open problem of extending error mitigation beyond expectation value estimation. Applying this scheme to the ground state problem of the two-dimensional Hubbard model and various molecular Hamiltonians, we find we can roughly halve the number of physical qubits with a $\sim 10\times$ wall-clock time overhead, but further reduction causes a steep runtime increase. This work provides an end-to-end analysis of early fault-tolerance cost reductions and space-time trade-offs, and identifies which areas can be improved in the future.

quant-ph↗

arXiv2024

Simulating Chemistry with Fermionic Optical Superlattices

We show that quantum number preserving Ans\"{a}tze for variational optimization in quantum chemistry find an elegant mapping to ultracold fermions in optical superlattices. Using native Hubbard dynamics, trial ground states of molecular Hamiltonians can be prepared and their molecular energies measured in the lattice. The scheme requires local control over interactions and chemical potentials and global control over tunneling dynamics, but foregoes the need for optical tweezers, shuttling operations, or long-range interactions. We describe a complete compilation pipeline from the molecular Hamiltonian to the sequence of lattice operations, thus providing a concrete link between quantum simulation and chemistry. Our work enables the application of recent quantum algorithmic techniques, such as Double Factorization and quantum Tailored Coupled Cluster, to present-day fermionic optical lattice systems with significant improvements in the required number of experimental repetitions. We provide detailed quantum resource estimates for small non-trivial hardware experiments.

cond-mat.quant-gas↗

arXiv2023

Estimation of electrostatic interaction energies on a trapped-ion quantum computer

We present the first hardware implementation of electrostatic interaction energies using a trapped-ion quantum computer. As test system for our computation, we focus on the reduction of $\mathrm{NO}$ to $\mathrm{N}_2\mathrm{O}$ catalyzed by a nitric oxide reductase (NOR). The quantum computer is used to generate an approximate ground state within the NOR active space. To efficiently measure the necessary one-particle density matrices, we incorporate fermionic basis rotations into the quantum circuit without extending the circuit length, laying the groundwork for further efficient measurement routines using factorizations. Measurements in the computational basis are then used as inputs for computing the electrostatic interaction energies on a classical computer. Our experimental results strongly agree with classical noise-less simulations of the same circuits, finding electrostatic interaction energies within chemical accuracy despite hardware noise. This work shows that algorithms tailored to specific observables of interest, such as interaction energies, may require significantly fewer quantum resources than individual ground state energies would in the straightforward supermolecular approach.

quant-ph↗

arXiv2023

Tailored and Externally Corrected Coupled Cluster with Quantum Inputs

We propose to use wavefunction overlaps obtained from a quantum computer as inputs for the classical split-amplitude techniques, tailored and externally corrected coupled cluster, to achieve balanced treatment of static and dynamic correlation effects in molecular electronic structure simulations. By combining insights from statistical properties of matchgate shadows, which are used to measure quantum trial state overlaps, with classical correlation diagnostics, we are able to provide quantum resource estimates well into the classically no longer exactly solvable regime. We find that rather imperfect wavefunctions and remarkably low shot counts are sufficient to cure qualitative failures of plain coupled cluster singles doubles and to obtain chemically precise dynamic correlation energy corrections. We provide insights into which wavefunction preparation schemes have a chance of yielding quantum advantage, and we test our proposed method using overlaps measured on Google's Sycamore device.

quant-ph↗

arXiv2023

Quantum Simulation of Realistic Materials in First Quantization Using Non-local Pseudopotentials

This paper improves and demonstrates the usefulness of the first quantized plane-wave algorithms for the quantum simulation of electronic structure, developed by Babbush et al. and Su et al. We describe the first quantum algorithm for first quantized simulation that accurately includes pseudopotentials. We focus on the Goedecker-Tetter-Hutter (GTH) pseudopotential, which is among the most accurate and widely used norm-conserving pseudopotentials enabling the removal of core electrons from the simulation. The resultant screened nuclear potential regularizes cusps in the electronic wavefunction so that orders of magnitude fewer plane waves are required for a chemically accurate basis. Despite the complicated form of the GTH pseudopotential, we are able to block encode the associated operator without significantly increasing the overall cost of quantum simulation. This is surprising since simulating the nuclear potential is much simpler without pseudopotentials, yet is still the bottleneck. We also generalize prior methods to enable the simulation of materials with non-cubic unit cells, which requires nontrivial modifications. Finally, we combine these techniques to estimate the block-encoding costs for commercially relevant instances of heterogeneous catalysis (e.g. carbon monoxide adsorption on transition metals) and compare to the quantum resources needed to simulate materials in second quantization. We conclude that for computational cells with many particles, first quantization often requires meaningfully less spacetime volume.

quant-ph↗

arXiv2022

Accelerating Quantum Computations of Chemistry Through Regularized Compressed Double Factorization

We propose the regularized compressed double factorization (RC-DF) method to classically compute compressed representations of molecular Hamiltonians that enable efficient simulation with noisy intermediate scale (NISQ) and error corrected quantum algorithms. We find that already for small systems with 12 to 20 qubits, the resulting NISQ measurement scheme reduces the number of measurement bases by roughly a factor of three and the shot count to reach chemical accuracy by a factor of three to six compared to truncated double factorization (DF) and we see order of magnitude improvements over Pauli grouping schemes. We demonstrate the scalability of our approach by performing RC-DF on the CpdI species of cytochrome P450 with 58 orbitals and find that using the resulting compressed Hamiltonian cuts the run time of qubitization and truncated DF based error corrected algorithms almost in half and even outperforms the lambda parameters achievable with tensor hypercontraction (THC) while at the same time reducing the CCSD(T) energy error heuristic by an order of magnitude.

quant-ph↗

arXiv2022

PennyLane: Automatic differentiation of hybrid quantum-classical computations

PennyLane is a Python 3 software framework for differentiable programming of quantum computers. The library provides a unified architecture for near-term quantum computing devices, supporting both qubit and continuous-variable paradigms. PennyLane's core feature is the ability to compute gradients of variational quantum circuits in a way that is compatible with classical techniques such as backpropagation. PennyLane thus extends the automatic differentiation algorithms common in optimization and machine learning to include quantum and hybrid computations. A plugin system makes the framework compatible with any gate-based quantum simulator or hardware. We provide plugins for hardware providers including the Xanadu Cloud, Amazon Braket, and IBM Quantum, allowing PennyLane optimizations to be run on publicly accessible quantum devices. On the classical front, PennyLane interfaces with accelerated machine learning libraries such as TensorFlow, PyTorch, JAX, and Autograd. PennyLane can be used for the optimization of variational quantum eigensolvers, quantum approximate optimization, quantum machine learning models, and many other applications.

quant-ph↗

arXiv2022

Efficient Quantum Analytic Nuclear Gradients with Double Factorization

Efficient representations of the Hamiltonian such as double factorization drastically reduce circuit depth or number of repetitions in error corrected and noisy intermediate scale quantum (NISQ) algorithms for chemistry. We report a Lagrangian-based approach for evaluating relaxed one- and two-particle reduced density matrices from double factorized Hamiltonians, unlocking efficiency improvements in computing the nuclear gradient and related derivative properties. We demonstrate the accuracy and feasibility of our Lagrangian-based approach to recover all off-diagonal density matrix elements in classically-simulated examples with up to 327 quantum and 18470 total atoms in QM/MM simulations, with modest-sized quantum active spaces. We show this in the context of the variational quantum eigensolver (VQE) in case studies such as transition state optimization, ab initio molecular dynamics simulation and energy minimization of large molecular systems.

quant-ph↗

arXiv2021

Analytical Ground- and Excited-State Gradients for Molecular Electronic Structure Theory from Hybrid Quantum/Classical Methods

We develop analytical gradients of ground- and excited-state energies with respect to system parameters including the nuclear coordinates for the hybrid quantum/classical multistate contracted variational quantum eigensolver (MC-VQE) applied to fermionic systems. We show how the resulting response contributions to the gradient can be evaluated with a quantum effort similar to that of obtaining the VQE energy and independent of the total number of derivative parameters (e.g. number of nuclear coordinates) by adopting a Lagrangian formalism for the evaluation of the total derivative. We also demonstrate that large-step-size finite-difference treatment of directional derivatives in concert with the parameter shift rule can significantly mitigate the complexity of dealing with the quantum parameter Hessian when solving the quantum response equations. This enables the computation of analytical derivative properties of systems with hundreds of atoms, while solving an active space of their most strongly correlated orbitals on a quantum computer. We numerically demonstrate the exactness the analytical gradients and discuss the magnitude of the quantum response contributions.

quant-ph↗

arXiv2021

Local, Expressive, Quantum-Number-Preserving VQE Ansatze for Fermionic Systems

We propose VQE circuit fabrics with advantageous properties for the simulation of strongly correlated ground and excited states of molecules and materials under the Jordan-Wigner mapping that can be implemented linearly locally and preserve all relevant quantum numbers: the number of spin up ($α$) and down ($β$) electrons and the total spin squared. We demonstrate that our entangler circuits are expressive already at low depth and parameter count, appear to become universal, and may be trainable without having to cross regions of vanishing gradient, when the number of parameters becomes sufficiently large and when these parameters are suitably initialized. One particularly appealing construction achieves this with just orbital rotations and pair exchange gates. We derive optimal four-term parameter shift rules for and provide explicit decompositions of our quantum number preserving gates and perform numerical demonstrations on highly correlated molecules on up to 20 qubits.

quant-ph↗

arXiv2020

Constructions of k-uniform and absolutely maximally entangled states beyond maximum distance codes

Pure multipartite quantum states of n parties and local dimension q are called k-uniform if all reductions to k parties are maximally mixed. These states are relevant for our understanding of multipartite entanglement, quantum information protocols, and the construction of quantum error correction codes. To our knowledge, the only known systematic construction of these quantum states is based on classical error correction codes. We present a systematic method to construct other examples of k-uniform states and show that the states derived through our construction are not equivalent to any k-uniform state constructed from the so-called maximum distance separable error correction codes. Furthermore, we use our method to construct several examples of absolutely maximally entangled states whose existence was open so far.

quant-ph↗

arXiv2020

Simulating quantum chemistry in the seniority-zero space on qubit-based quantum computers

Accurate quantum chemistry simulations remain challenging on classical computers for problems of industrially relevant sizes and there is reason for hope that quantum computing may help push the boundaries of what is technically feasible. While variational quantum eigensolver (VQE) algorithms may already turn noisy intermediate scale quantum (NISQ) devices into useful machines, one has to make all efforts to use the scarce quantum resources as efficiently as possible. We combine the so-called seniority-zero, or paired-electron, approximation of computational quantum chemistry with techniques for simulating molecular chemistry on gate-based quantum computers and obtain a very resource efficient quantum simulation algorithm. While some accuracy is lost through the paired-electron approximation, we show that using the freed-up quantum resources for increasing the basis set can lead to more accurate results and reductions in the necessary number of quantum computing runs by several orders of magnitude, already for a simple system like lithium hydride. We also discuss an error mitigation scheme based on post-selection which shows an attractive scaling when the given Hamiltonian format is considered, increasing the viability of its NISQ implementation.

quant-ph↗

arXiv2020

Verifying the output of quantum optimizers with ground-state energy lower bounds

Solving optimisation problems encoded in the ground state of classical-spin systems is a focus area for quantum computing devices, providing upper bounds to the unknown solution. To certify these bounds, they are compared to those obtained by classical methods. However, even if the quantum bound beats them, this says little about how close it is to the unknown solution. We consider the use of relaxations to the ground-state problem as a benchmark for the output of quantum optimisers. These relaxations are radically more informative because they provide lower bounds to the ground-state energy. The chordal branch and bound algorithm we present provides a series of systematically improving confidence regions where the ground-state energy provably lies. Interestingly, each step in the process requires only an effort polynomial in the system size. Additionally, the algorithm exploits the locality and sparsity of relevant Ising spin models in a systematic way. This yields certified solutions for many of the problems that are currently addressed by heuristic optimisation algorithms more efficiently and for larger system sizes. We apply the method to verify the output of a D-Wave 2000Q device and identify instances where the annealer does not reach the ground-state energy and, more importantly, instances where it does, something impossible to do by means of standard variational approaches. Our work provides a flexible and scalable method for the verification of the outputs produced by quantum optimization devices.

quant-ph↗

arXiv2020

Locality of temperature and correlations in the presence of non-zero-temperature phase transitions

While temperature is well understood as an intensive quantity in standard thermodynamics, it is less clear whether the same holds in the presence of strong correlations, especially in the case of quantum systems, which may even display correlations with no classical analogue. The problem lies in the fact that, under the presence of strong correlations, subsystems of a system in thermal equilibrium are, in general, not described by a thermal state at the same temperature as the global system and thus one cannot simply assign a local temperature to them. However, there have been identified situations in which correlations in thermal states decay sufficiently fast so that the state of their subsystems can be very well approximated by the reduced states of equilibrium systems that are only slightly bigger than the subsystems themselves, hence allowing for a valid local definition of temperature. In this work, we address the question of whether temperature is locally well defined for a bosonic system with local interactions that undergoes a phase transition at non-zero temperature. We consider a three-dimensional bosonic model in the grand canonical state and verify that a certain form of locality of temperature holds regardless of the temperature, and despite the presence of infinite-range correlations at and below the critical temperature of the phase transition.

quant-ph↗

arXiv2020

Avoiding local minima in variational quantum eigensolvers with the natural gradient optimizer

We compare the BFGS optimizer, ADAM and Natural Gradient Descent (NatGrad) in the context of Variational Quantum Eigensolvers (VQEs). We systematically analyze their performance on the QAOA ansatz for the Transverse Field Ising Model (TFIM) as well as on overparametrized circuits with the ability to break the symmetry of the Hamiltonian. The BFGS algorithm is frequently unable to find a global minimum for systems beyond about 20 spins and ADAM easily gets trapped in local minima. On the other hand, NatGrad shows stable performance on all considered system sizes, albeit at a significantly higher cost per epoch. In sharp contrast to most classical gradient based learning, the performance of all optimizers is found to decrease upon seemingly benign overparametrization of the ansatz class, with BFGS and ADAM failing more often and more severely than NatGrad. Additional tests for the Heisenberg XXZ model corroborate the accuracy problems of BFGS in high dimensions, but they reveal some shortcomings of NatGrad as well. Our results suggest that great care needs to be taken in the choice of gradient based optimizers and the parametrization for VQEs.

quant-ph↗

arXiv2019

Automated discovery of characteristic features of phase transitions in many-body localization

We identify a new "order parameter" for the disorder driven many-body localization (MBL) transition by leveraging artificial intelligence. This allows us to pin down the transition, as the point at which the physics changes qualitatively, from vastly fewer disorder realizations and in an objective and cleaner way than is possible with the existing zoo of quantities. Contrary to previous studies, our method is almost entirely unsupervised. A game theoretic process between neural networks defines an adversarial setup with conflicting objectives to identify what characteristic features to base efficient predictions on. This reduces the numerical effort for mapping out the phase diagram by a factor of ~100x. This approach of automated discovery is applicable specifically to poorly understood phase transitions and exemplifies the potential of machine learning assisted research in physics.

quant-ph↗