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Symmetry-protected topological phases have fundamentally changed our understanding of quantum matter. An archetypal example of such a quantum phase of matter is the Haldane phase, containing the spin-1 Heisenberg chain. The intrinsic quantum nature of such phases, however, often makes it challenging to study them using classical means. Here, we use trapped-ion qutrits to natively engineer spin-1 chains within the Haldane phase. Using a scalable, deterministic procedure to prepare the Affleck-Kennedy-Lieb-Tasaki (AKLT) state within the Haldane phase, we study the topological features of this system on a qudit quantum processor. Notably, we verify the long-range string order of the state, despite its short-range correlations, and observe spin fractionalization of the physical spin-1 particles into effective qubits at the chain edges, a defining feature of this system. The native realization of Haldane physics on a qudit quantum processor and the scalable preparation procedures open the door to the efficient exploration of a wide range of systems beyond spin-1/2, Comment: 12 pages, 6 figures

The interaction between a single emitter and a single photon is a fundamental aspect of quantum optics. This interaction allows for the study of various quantum processes, such as emitter-mediated single-photon scattering and effective photon-photon interactions. However, empirical observations of this scenario and its dynamics are rare, and in most cases, only partial approximations to the fully quantized case have been possible. Here, we demonstrate the resonant excitation of a solid-state quantum emitter using quantized input light. For this light-matter interaction, with both entities quantized, we observe single-photon interference introduced by the emitter in a coherent scattering process, photon-number-depended optical non-linearities, and stimulated emission processes involving only two photons. We theoretically reproduce our observations using a cascaded master equation model. Our findings demonstrate that a single photon is sufficient to change the state of a solid-state quantum emitter, and efficient emitter-mediated photon-photon interactions are feasible. These results suggest future possibilities ranging from enabling quantum information transfer in a quantum network to building deterministic entangling gates for photonic quantum computing., Comment: 13 pages, 8 figures

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.

Response theory has a successful history of connecting experimental observations with theoretical predictions. Of particular interest is the optical response of matter, from which spectroscopy experiments can be modelled. However, the calculation of response properties for quantum systems is often prohibitively expensive, especially for nonlinear spectroscopy, as it requires access to either the time evolution of the system or to excited states. In this work, we introduce a generalized quantum phase estimation framework designed for multi-variate phase estimation. This allows the treatment of general correlation functions enabling the recovery of response properties of arbitrary orders. The generalized quantum phase estimation circuit has an intuitive construction that is linked with a physical process of interest, and can directly sample frequencies from the distribution that would be obtained experimentally. In addition, we provide a single-ancilla modification of the new framework for early fault-tolerant quantum computers. Overall, our framework enables the efficient simulation of spectroscopy experiments beyond the linear regime, such as Raman spectroscopy. This opens up an exciting new field of applications for quantum computers with potential technological impact., Comment: 16 pages, 3 figures, 1 table

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., Comment: 18 pages, 4 figures, 2 tables

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.

We explore the practicality of early fault-tolerant quantum algorithms, focusing on ground-state energy estimation problems. Specifically, we address the computation of the cumulative distribution function (CDF) of the spectral measure of the Hamiltonian and the identification of its discontinuities. Scaling to bigger system sizes unveils three challenges: the smoothness of the CDF for large supports, the absence of tight lower bounds on the overlap with the actual ground state, and the complexity of preparing high-quality initial states. To tackle these challenges, we introduce a signal processing technique for identifying the inflection point of the CDF. We argue that this change of paradigm significantly simplifies the problem, making it more accessible while still being accurate. Hence, instead of trying to find the exact ground-state energy, we advocate improving on the classical estimate by aiming at the low-energy support of the initial state. Furthermore, we offer quantitative resource estimates for the maximum number of samples required to identify an increase in the CDF of a given size. Finally, we conduct numerical experiments on a 26-qubit fully-connected Heisenberg model using a truncated density-matrix renormalization group (DMRG) initial state of low bond dimension. Results show that the prediction obtained with the quantum algorithm aligns well with the DMRG-converged energy at large bond dimensions and requires several orders of magnitude fewer samples than predicted by the theory. Hence, we argue that CDF-based quantum algorithms are a viable, practical alternative to quantum phase estimation in resource-limited scenarios., Comment: 16 pages, 9 figures

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 $\tilde{\mathcal{O}}(d^{\,3/2}/\epsilon)$ 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 $\epsilon$-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.

Hamiltonian simulation is arguably the most fundamental application of quantum computers. The Magnus operator is a popular method for time-dependent Hamiltonian simulation in computational mathematics, yet its usage requires the implementation of exponentials of commutators, which has previously made it unappealing for quantum computing. The development of commutator-free quasi-Magnus operators (CFQMs) circumvents this obstacle, at the expense of a lack of provable global numeric error bounds. In this work, we establish one such error bound for CFQM-based time-dependent quantum Hamiltonian simulation by carefully estimating the error of each step involved in their definition. This allows us to compare its cost with the alternatives, and show that CFQMs are often the most efficient product-formula technique available by more than an order of magnitude. As a result, we find that CFQMs may be particularly useful to simulate time-dependent Hamiltonians on early fault-tolerant quantum computers., Comment: 22 pages, 7 figures

We analyze the implementation of high-fidelity, phonon-mediated gate operations and quantum simulation schemes for spin qubits associated with silicon vacancy centers in diamond. Specifically, we show how the application of continuous dynamical decoupling techniques can substantially boost the coherence of the qubit states while increasing at the same time the variety of effective spin models that can be implemented in this way. Based on realistic models and detailed numerical simulations, we demonstrate that this decoupling technique can suppress gate errors by more than two orders of magnitude and enable gate infidelities below $\sim 10^{-4}$ for experimentally relevant noise parameters. Therefore, when generalized to phononic lattices with arrays of implanted defect centers, this approach offers a realistic path toward moderate- and large-scale quantum devices with spins and phonons, at a level of control that is competitive with other leading quantum-technology platforms., Comment: 12+10 pages, 6+3 figures

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.

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., Comment: 9+21 pages

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.

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., Comment: 11 pages, 5 figures, 1 table

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., Comment: 22 pages, 10 figures. The following article has been submitted to the Journal of Chemical Physics. After it is published, it will be found at https://publishing.aip.org/resources/librarians/products/journals/

We use an electric-dipole laser-driven transition to precisely measure the cyclotron-frequency ratios of the pairs $^{42}$Ca$^+$-$^{40}$Ca$^+$, $^{44}$Ca$^+$-$^{40}$Ca$^+$ and $^{48}$Ca$^+$-$^{40}$Ca$^+$ in a 7-tesla Penning trap. A single laser-cooled ($T\approx 1$~mK) ion serves, together with photon-counting and/or photon-imaging units, as a radiofrequency detector covering a broad-band frequency spectrum, in the present case from kHz to a few MHz. Such detectors ($^{40,42,44,48}$Ca$^{\scriptsize{+}}$) allow measuring extremely small forces, with measured normalized sensitivities down to $7.4(3.5)$ yN$/\sqrt{\text{Hz}}$ and $24.9(9.9)$ yN$/\sqrt{\text{Hz}}$ in the MHz and kHz regime, respectively. The direct determination of the ions' amplitudes makes a cyclotron-frequency measurement process more robust against inhomogeneities of the magnetic field and/or deviations of the electric quadrupole field due to mechanical imperfections of the trap., Comment: 6 pages, 3 figures

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.

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., Comment: 34 pages, 12 figures

Robust qubit-qubit interactions mediated by bosonic modes are central to many quantum technologies. Existing proposals combining fast oscillator-mediated gates with dynamical decoupling require strong pulses or fast control over the qubit-boson coupling. Here, we present a method based on dynamical decoupling techniques that leads to faster-than-dispersive entanglement gates with low-intensity pulses. Our method is general, i.e., it is applicable to any quantum platform that has qubits interacting with bosonic mediators via longitudinal coupling. Moreover, the protocol provides robustness to fluctuations in qubit frequencies and control fields, while also being resistant to common errors such as frequency shifts and heating in the mediator as well as crosstalk effects. We illustrate our method with an implementation for trapped ions coupled via magnetic field gradients. With detailed numerical simulations, we show that entanglement gates with infidelities of $10^{-3}$ or $10^{-4}$ are possible with current or near-future experimental setups, respectively., Comment: 7+13 pages, 3+3 figures, 2 tables

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.

Sampling from a quantum distribution can be exponentially hard for classical computers and yet could be performed efficiently by a noisy intermediate-scale quantum device. A prime example of a distribution that is hard to sample is given by the output states of a linear interferometer traversed by $N$ identical boson particles. Here, we propose a scheme to implement such a boson sampling machine with ultracold atoms in a polarization-synthesized optical lattice. We experimentally demonstrate the basic building block of such a machine by revealing the Hong-Ou-Mandel interference of two bosonic atoms in a four-mode interferometer. To estimate the sampling rate for large $N$, we develop a theoretical model based on a master equation that accounts for particle losses, but not include technical errors. Our results show that atomic samplers have the potential to achieve quantum advantage over today's best supercomputers with $N \gtrsim 40$., Comment: 9 pages plus appendices and bibliography; 6 figures

We present the experimental implementation of a two-qubit phase gate, using a radio frequency (RF) controlled trapped-ion quantum processor. The RF-driven gate is generated by a pulsed dynamical decoupling sequence applied to the ions' carrier transitions only. It allows for a tunable phase shift with high-fidelity results, in particular a fringe contrast up to $99_{-2}^{+1}\%$ is observed in Ramsey-type measurements. We also prepare a Bell state using this laser-free gate. The phase gate is robust against common sources of error. We investigate the effect of the excitation of the center-of-mass (COM) mode, errors in the axial trap frequency, pulse area errors and errors in sequence timing. The contrast of the phase gate is not significantly reduced up to a COM mode excitation $<20$ phonons, trap frequency errors of +10%, and pulse area errors of -8%. The phase shift is not significantly affected up to $<10$ phonons and pulse area errors of -2%. Both, contrast and phase shift are robust to timing errors up to -30% and +15%. The gate implementation is resource efficient, since only a single driving field is required per ion. Furthermore, it holds the potential for fast gate speeds (gate times on the order of $100~\mu$s) by using two axial motional modes of a two-ion crystal through improved setups.

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 $\Omega(2^k / \varepsilon ^2)$ 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 $2^{O(p\kappa)}$, where $\kappa$ 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., Comment: 9 pages, 6 figures

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., Comment: 10 pages, 3 figures

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., Comment: 31 pages, 14 figures

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.

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., Comment: 44 pages; v3 - journal version

Universal gate sets for quantum computing have been known for decades, yet no universal gate set has been proposed for particle-conserving unitaries, which are the operations of interest in quantum chemistry. In this work, we show that controlled single-excitation gates in the form of Givens rotations are universal for particle-conserving unitaries. Single-excitation gates describe an arbitrary $U(2)$ rotation on the two-qubit subspace spanned by the states $|01\rangle, |10\rangle$, while leaving other states unchanged -- a transformation that is analogous to a single-qubit rotation on a dual-rail qubit. The proof is constructive, so our result also provides an explicit method for compiling arbitrary particle-conserving unitaries. Additionally, we describe a method for using controlled single-excitation gates to prepare an arbitrary state of a fixed number of particles. We derive analytical gradient formulas for Givens rotations as well as decompositions into single-qubit and CNOT gates. Our results offer a unifying framework for quantum computational chemistry where every algorithm is a unique recipe built from the same universal ingredients: Givens rotations., Comment: 11 pages, 12 figures

Classical algorithms for predicting the equilibrium geometry of strongly correlated molecules require expensive wave function methods that become impractical already for few-atom systems. In this work, we introduce a variational quantum algorithm for finding the most stable structure of a molecule by explicitly considering the parametric dependence of the electronic Hamiltonian on the nuclear coordinates. The equilibrium geometry of the molecule is obtained by minimizing a more general cost function that depends on both the quantum circuit and the Hamiltonian parameters, which are simultaneously optimized at each step. The algorithm is applied to find the equilibrium geometries of the $\mathrm{H}_2$, $\mathrm{H}_3^+$, $\mathrm{BeH}_2$ and $\mathrm{H}_2\mathrm{O}$ molecules. The quantum circuits used to prepare the electronic ground state for each molecule were designed using an adaptive algorithm where excitation gates in the form of Givens rotations are selected according to the norm of their gradient. All quantum simulations are performed using the PennyLane library for quantum differentiable programming. The optimized geometrical parameters for the simulated molecules show an excellent agreement with their counterparts computed using classical quantum chemistry methods., Comment: 7 pages, 4 figures, 1 codeblock