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Juan Miguel Arrazola

Publications and source records attributed to Juan Miguel Arrazola.

At least 37 records · Page 2Linked to original sources
arXiv2024

A differentiable quantum phase estimation algorithm

The simulation of electronic properties is a pivotal issue in modern electronic structure theory, driving significant efforts over the past decades to develop protocols for computing energy derivatives. In this work, we address this problem by developing a strategy to integrate the quantum phase estimation algorithm within a fully differentiable framework. This is accomplished by devising a smooth estimator able to tackle arbitrary initial states. We provide analytical expressions to characterize the statistics and algorithmic cost of this estimator. Furthermore, we provide numerical evidence that the estimation accuracy is retained when an arbitrary state is considered and that it exceeds the one of standard majority rule. We explicitly use this procedure to estimate chemically relevant quantities, demonstrating our approach through ground-state and triplet excited state geometry optimization with simulations involving up to 19 qubits. This work paves the way for new quantum algorithms that combine interference methods and quantum differentiable programming.

quant-ph↗
arXiv2024

Simulating optically-active spin defects with a quantum computer

There is a pressing need for more accurate computational simulations of the opto-electronic properties of defects in materials to aid in the development of quantum sensing platforms. In this work, we explore how quantum computers could be effectively utilized for this purpose. Specifically, we develop fault-tolerant quantum algorithms to simulate optically active defect states and their radiative emission rates. We employ quantum defect embedding theory to translate the Hamiltonian of a defect-containing supercell into a smaller, effective Hamiltonian that accounts for dielectric screening effects. Our approach integrates block-encoding of the dipole operator with quantum phase estimation to selectively sample the optically active excited states that exhibit the largest dipole transition amplitudes. We also provide estimates of the quantum resources required to simulate a negatively-charged boron vacancy in a hexagonal boron nitride cluster. We conclude by offering a forward-looking perspective on the potential of quantum computers to enhance quantum sensor capabilities and identify specific scenarios where quantum computing can resolve problems traditionally challenging for classical computers.

quant-ph↗
arXiv2024

Simulating X-ray absorption spectroscopy of battery materials on a quantum computer

X-ray absorption spectroscopy is a crucial experimental technique for elucidating the mechanisms of structural degradation in battery materials. However, extracting information from the measured spectrum is challenging without high-quality simulations. In this work, we propose simulating near-edge X-ray absorption spectra as a promising application for quantum computing. It is attractive due to the ultralocal nature of X-ray absorption that significantly reduces the sizes of problems to be simulated, and because of the classical hardness of simulating spectra. We describe three quantum algorithms to compute the X-ray absorption spectrum and provide their asymptotic cost. One of these is a Monte-Carlo based time-domain algorithm, which is cost-friendly to early fault-tolerant quantum computers. We then apply the framework to an industrially relevant example, a CAS(22e,18o) active space for an O-Mn cluster in a Li-excess battery cathode, showing that practically useful simulations could be obtained with much fewer qubits and gates than ground-state energy estimation of the same material.

quant-ph↗
arXiv2024

Ground State Preparation via Dynamical Cooling

Quantum algorithms for probing ground-state properties of quantum systems require good initial states. Projection-based methods such as eigenvalue filtering rely on inputs that have a significant overlap with the low-energy subspace, which can be challenging for large, strongly-correlated systems. This issue has motivated the study of physically-inspired dynamical approaches such as thermodynamic cooling. In this work, we introduce a ground-state preparation algorithm based on the simulation of quantum dynamics. Our main insight is to transform the Hamiltonian by a shifted sign function via quantum signal processing, effectively mapping eigenvalues into positive and negative subspaces separated by a large gap. This automatically ensures that all states within each subspace conserve energy with respect to the transformed Hamiltonian. Subsequent time-evolution with a perturbed Hamiltonian induces transitions to lower-energy states while preventing unwanted jumps to higher energy states. The approach does not rely on a priori knowledge of energy gaps and requires no additional qubits to model a bath. Furthermore, it makes $\tilde{\mathcal{O}}(d^{\,3/2}/ε)$ queries to the time-evolution operator of the system and $\tilde{\mathcal{O}}(d^{\,3/2})$ queries to a block-encoding of the perturbation, for $d$ cooling steps and an $ε$-accurate energy resolution. Our results provide a framework for combining quantum signal processing and Hamiltonian simulation to design heuristic quantum algorithms for ground-state preparation.

quant-ph↗
arXiv2024

Better bounds for low-energy product formulas

Product formulas are one of the main approaches for quantum simulation of the Hamiltonian dynamics of a quantum system. Their implementation cost is computed based on error bounds which are often pessimistic, resulting in overestimating the total runtime. In this work, we rigorously consider the error induced by product formulas when the state undergoing time evolution lies in the low-energy sector with respect to the Hamiltonian of the system. We show that in such a setting, the usual error bounds based on the operator norm of nested commutators can be replaced by those restricted to suitably chosen low-energy subspaces, yielding tighter error bounds. Furthermore, under some locality and positivity assumptions, we show that the simulation of generic product formulas acting on low-energy states can be done asymptotically more efficiently when compared with previous results.

quant-ph↗
arXiv2024

Initial state preparation for quantum chemistry on quantum computers

Quantum algorithms for ground-state energy estimation of chemical systems require a high-quality initial state. However, initial state preparation is commonly either neglected entirely, or assumed to be solved by a simple product state like Hartree-Fock. Even if a nontrivial state is prepared, strong correlations render ground state overlap inadequate for quality assessment. In this work, we address the initial state preparation problem with an end-to-end algorithm that prepares and quantifies the quality of initial states, accomplishing the latter with a new metric -- the energy distribution. To be able to prepare more complicated initial states, we introduce an implementation technique for states in the form of a sum of Slater determinants that exhibits significantly better scaling than all prior approaches. We also propose low-precision quantum phase estimation (QPE) for further state quality refinement. The complete algorithm is capable of generating high-quality states for energy estimation, and is shown in select cases to lower the overall estimation cost by several orders of magnitude when compared with the best single product state ansatz. More broadly, the energy distribution picture suggests that the goal of QPE should be reinterpreted as generating improvements compared to the energy of the initial state and other classical estimates, which can still be achieved even if QPE does not project directly onto the ground state. Finally, we show how the energy distribution can help in identifying potential quantum advantage.

quant-ph↗
arXiv2023

The hardness of quantum spin dynamics

Recent experiments demonstrated quantum computational advantage in random circuit sampling and Gaussian boson sampling. However, it is unclear whether these experiments can lead to practical applications even after considerable research effort. On the other hand, simulating the quantum coherent dynamics of interacting spins has been considered as a potential first useful application of quantum computers, providing a possible quantum advantage. Despite evidence that simulating the dynamics of hundreds of interacting spins is challenging for classical computers, concrete proof is yet to emerge. We address this problem by proving that sampling from the output distribution generated by a wide class of quantum spin Hamiltonians is a hard problem for classical computers. Our proof is based on the Taylor series of the output probability, which contains the permanent of a matrix as a coefficient when bipartite spin interactions are considered. We devise a classical algorithm that extracts the coefficient using an oracle estimating the output probability. Since calculating the permanent is #P-hard, such an oracle does not exist unless the polynomial hierarchy collapses. With an anticoncentration conjecture, the hardness of the sampling task is also proven. Based on our proof, we estimate that an instance involving about 200 spins will be challenging for classical devices but feasible for intermediate-scale quantum computers with fault-tolerant qubits.

quant-ph↗
arXiv2023

Grad DFT: a software library for machine learning enhanced density functional theory

Density functional theory (DFT) stands as a cornerstone method in computational quantum chemistry and materials science due to its remarkable versatility and scalability. Yet, it suffers from limitations in accuracy, particularly when dealing with strongly correlated systems. To address these shortcomings, recent work has begun to explore how machine learning can expand the capabilities of DFT; an endeavor with many open questions and technical challenges. In this work, we present Grad DFT: a fully differentiable JAX-based DFT library, enabling quick prototyping and experimentation with machine learning-enhanced exchange-correlation energy functionals. Grad DFT employs a pioneering parametrization of exchange-correlation functionals constructed using a weighted sum of energy densities, where the weights are determined using neural networks. Moreover, Grad DFT encompasses a comprehensive suite of auxiliary functions, notably featuring a just-in-time compilable and fully differentiable self-consistent iterative procedure. To support training and benchmarking efforts, we additionally compile a curated dataset of experimental dissociation energies of dimers, half of which contain transition metal atoms characterized by strong electronic correlations. The software library is tested against experimental results to study the generalization capabilities of a neural functional across potential energy surfaces and atomic species, as well as the effect of training data noise on the resulting model accuracy.

physics.chem-ph↗
arXiv2023

Autoregressive Neural Quantum States with Quantum Number Symmetries

Neural quantum states have established themselves as a powerful and versatile family of ansatzes for variational Monte Carlo simulations of quantum many-body systems. Of particular prominence are autoregressive neural quantum states (ANQS), which enjoy the expressibility of deep neural networks, and are equipped with a procedure for fast and unbiased sampling. Yet, the non-selective nature of autoregressive sampling makes incorporating quantum number symmetries challenging. In this work, we develop a general framework to make the autoregressive sampling compliant with an arbitrary number of quantum number symmetries. We showcase its advantages by running electronic structure calculations for a range of molecules with multiple symmetries of this kind. We reach the level of accuracy reported in previous works with more than an order of magnitude speedup and achieve chemical accuracy for all studied molecules, which is a milestone unreported so far. Combined with the existing effort to incorporate space symmetries, our approach expands the symmetry toolbox essential for any variational ansatz and brings the ANQS closer to being a competitive choice for studying challenging quantum many-body systems.

quant-ph↗
arXiv2023

Quantum simulation of battery materials using ionic pseudopotentials

Ionic pseudopotentials are widely used in classical simulations of materials to model the effective potential due to the nucleus and the core electrons. Modeling fewer electrons explicitly results in a reduction in the number of plane waves needed to accurately represent the states of a system. In this work, we introduce a quantum algorithm that uses pseudopotentials to reduce the cost of simulating periodic materials on a quantum computer. We use a qubitization-based quantum phase estimation algorithm that employs a first-quantization representation of the Hamiltonian in a plane-wave basis. We address the challenge of incorporating the complexity of pseudopotentials into quantum simulations by developing highly-optimized compilation strategies for the qubitization of the Hamiltonian. This includes a linear combination of unitaries decomposition that leverages the form of separable pseudopotentials. Our strategies make use of quantum read-only memory subroutines as a more efficient alternative to quantum arithmetic. We estimate the computational cost of applying our algorithm to simulating lithium-excess cathode materials for batteries, where more accurate simulations are needed to inform strategies for gaining reversible access to the excess capacity they offer. We estimate the number of qubits and Toffoli gates required to perform sufficiently accurate simulations with our algorithm for three materials: lithium manganese oxide, lithium nickel-manganese oxide, and lithium manganese oxyfluoride. Our optimized compilation strategies result in a pseudopotential-based quantum algorithm with a total Toffoli cost four orders of magnitude lower than the previous state of the art for a fixed target accuracy.

quant-ph↗
arXiv2023

Fast quantum circuit cutting with randomized measurements

We propose a new method to extend the size of a quantum computation beyond the number of physical qubits available on a single device. This is accomplished by randomly inserting measure-and-prepare channels to express the output state of a large circuit as a separable state across distinct devices. Our method employs randomized measurements, resulting in a sample overhead that is $\widetilde{O}(4^k / \varepsilon ^2)$, where $\varepsilon $ is the accuracy of the computation and $k$ the number of parallel wires that are "cut" to obtain smaller sub-circuits. We also show an information-theoretic lower bound of $Ω(2^k / \varepsilon ^2)$ for any comparable procedure. We use our techniques to show that circuits in the Quantum Approximate Optimization Algorithm (QAOA) with $p$ entangling layers can be simulated by circuits on a fraction of the original number of qubits with an overhead that is roughly $2^{O(pκ)}$, where $κ$ is the size of a known balanced vertex separator of the graph which encodes the optimization problem. We obtain numerical evidence of practical speedups using our method applied to the QAOA, compared to prior work. Finally, we investigate the practical feasibility of applying the circuit cutting procedure to large-scale QAOA problems on clustered graphs by using a $30$-qubit simulator to evaluate the variational energy of a $129$-qubit problem as well as carry out a $62$-qubit optimization.

quant-ph↗
arXiv2023

Simulating key properties of lithium-ion batteries with a fault-tolerant quantum computer

There is a pressing need to develop new rechargeable battery technologies that can offer higher energy storage, faster charging, and lower costs. Despite the success of existing methods for the simulation of battery materials, they can sometimes fall short of delivering accurate and reliable results. Quantum computing has been discussed as an avenue to overcome these issues, but only limited work has been done to outline how they may impact battery simulations. In this work, we provide a detailed answer to the following question: how can a quantum computer be used to simulate key properties of a lithium-ion battery? Based on recently-introduced first-quantization techniques, we lay out an end-to-end quantum algorithm for calculating equilibrium cell voltages, ionic mobility, and thermal stability. These can be obtained from ground-state energies of materials, which is the core calculation executed by the quantum computer using qubitization-based quantum phase estimation. The algorithm includes explicit methods for preparing approximate ground states of periodic materials in first quantization. We bring these insights together to perform the first estimation of the resources required to implement a quantum algorithm for simulating a realistic cathode material, dilithium iron silicate.

quant-ph↗
arXiv2023

Differentiable quantum computational chemistry with PennyLane

This work describes the theoretical foundation for all quantum chemistry functionality in PennyLane, a quantum computing software library specializing in quantum differentiable programming. We provide an overview of fundamental concepts in quantum chemistry, including the basic principles of the Hartree-Fock method. A flagship feature in PennyLane is the differentiable Hartree-Fock solver, allowing users to compute exact gradients of molecular Hamiltonians with respect to nuclear coordinates and basis set parameters. PennyLane provides specialized operations for quantum chemistry, including excitation gates as Givens rotations and templates for quantum chemistry circuits. Moreover, built-in simulators exploit sparse matrix techniques for representing molecular Hamiltonians that lead to fast simulation for quantum chemistry applications. In combination with PennyLane's existing methods for constructing, optimizing, and executing circuits, these methods allow users to implement a wide range of quantum algorithms for quantum chemistry. We discuss how PennyLane can be used to implement variational algorithms for calculating ground-state energies, excited-state energies, and energy derivatives, all of which can be differentiated with respect to both circuit and Hamiltonian parameters. We provide an example workflow describing how to jointly optimize circuit parameters, nuclear coordinates, and basis set parameters for quantum chemistry algorithms. We discuss a functionality for reducing the number of qubits by using symmetries and explain how PennyLane can be used to estimate quantum resources needed to implement several quantum algorithms. By combining insights from quantum computing, computational chemistry, and machine learning, PennyLane is the first library for differentiable quantum computational chemistry.

quant-ph↗
arXiv2023

Generating Approximate Ground States of Molecules Using Quantum Machine Learning

The potential energy surface (PES) of molecules with respect to their nuclear positions is a primary tool in understanding chemical reactions from first principles. However, obtaining this information is complicated by the fact that sampling a large number of ground states over a high-dimensional PES can require a vast number of state preparations. In this work, we propose using a generative quantum machine learning model to prepare quantum states at arbitrary points on the PES. The model is trained using quantum data consisting of ground-state wavefunctions associated with different classical nuclear coordinates. Our approach uses a classical neural network to convert the nuclear coordinates of a molecule into quantum parameters of a variational quantum circuit. The model is trained using a fidelity loss function to optimize the neural network parameters. We show that gradient evaluation is efficient and numerically demonstrate our method's ability to prepare wavefunctions on the PES of hydrogen chains, water, and beryllium hydride. In all cases, we find that a small number of training points are needed to achieve very high overlap with the groundstates in practice. From a theoretical perspective, we further prove limitations on these protocols by showing that if we were able to learn across an avoided crossing using a small number of samples, then we would be able to violate Grover's lower bound. Additionally, we prove lower bounds on the amount of quantum data needed to learn a locally optimal neural network function using arguments from quantum Fisher information. This work further identifies that quantum chemistry can be an important use case for quantum machine learning.

quant-ph↗
arXiv2022

The Complexity of Bipartite Gaussian Boson Sampling

Gaussian boson sampling is a model of photonic quantum computing that has attracted attention as a platform for building quantum devices capable of performing tasks that are out of reach for classical devices. There is therefore significant interest, from the perspective of computational complexity theory, in solidifying the mathematical foundation for the hardness of simulating these devices. We show that, under the standard Anti-Concentration and Permanent-of-Gaussians conjectures, there is no efficient classical algorithm to sample from ideal Gaussian boson sampling distributions (even approximately) unless the polynomial hierarchy collapses. The hardness proof holds in the regime where the number of modes scales quadratically with the number of photons, a setting in which hardness was widely believed to hold but that nevertheless had no definitive proof. Crucial to the proof is a new method for programming a Gaussian boson sampling device so that the output probabilities are proportional to the permanents of submatrices of an arbitrary matrix. This technique is a generalization of Scattershot BosonSampling that we call BipartiteGBS. We also make progress towards the goal of proving hardness in the regime where there are fewer than quadratically more modes than photons (i.e., the high-collision regime) by showing that the ability to approximate permanents of matrices with repeated rows/columns confers the ability to approximate permanents of matrices with no repetitions. The reduction suffices to prove that GBS is hard in the constant-collision regime.

quant-ph↗
arXiv2022

A practical overview of image classification with variational tensor-network quantum circuits

Circuit design for quantum machine learning remains a formidable challenge. Inspired by the applications of tensor networks across different fields and their novel presence in the classical machine learning context, one proposed method to design variational circuits is to base the circuit architecture on tensor networks. Here, we comprehensively describe tensor-network quantum circuits and how to implement them in simulations. This includes leveraging circuit cutting, a technique used to evaluate circuits with more qubits than those available on current quantum devices. We then illustrate the computational requirements and possible applications by simulating various tensor-network quantum circuits with PennyLane, an open-source python library for differential programming of quantum computers. Finally, we demonstrate how to apply these circuits to increasingly complex image processing tasks, completing this overview of a flexible method to design circuits that can be applied to industrially-relevant machine learning tasks.

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

Tailgating quantum circuits for high-order energy derivatives

To understand the chemical properties of molecules, it is often important to study derivatives of energies with respect to nuclear coordinates or external fields. Quantum algorithms for computing energy derivatives have been proposed, but only limited work has been done to address the specific challenges that arise in this context, where calculations are more complicated and involve more stringent requirements on accuracy compared to single-point energy calculations. In this work, we introduce a technique to improve the performance of variational quantum circuits calculating energy derivatives. The method, which we refer to as tailgating, is an adaptive procedure that selects gates based on their gradient with respect to the expectation value of Hamiltonian derivatives. These gates are then added at the end of a quantum circuit originally designed to calculate ground- or excited-state energies. A distinguishing feature of this approach is that the appended gates do not need to be optimized: their parameters can be set to zero and varied only for the purpose of computing energy derivatives, via calculating derivatives with respect to circuit parameters. We support the validity of this method by establishing sufficient conditions for a circuit to compute accurate energy gradients. This is achieved through a connection between energy derivatives and eigenstates of Taylor approximations of the Hamiltonian. We illustrate the advantages of the tailgating approach by performing simulations calculating the vibrational modes of beryllium hydride and water: quantities that depend on second-order energy derivatives.

quant-ph↗