arXiv subjects

Raffaele Santagati

Publications and source records attributed to Raffaele Santagati.

At least 19 recordsLinked to original sources

arXiv2026

Faster quantum chemistry simulations on a quantum computer with improved tensor factorization and active volume compilation

Electronic structure calculations of molecular systems are among the most promising applications for fault-tolerant quantum computing (FTQC) in quantum chemistry and drug design. However, while recent algorithmic advancements such as qubitization and Tensor Hypercontraction (THC) have significantly reduced the complexity of such calculations, they do not yet achieve computational runtimes short enough to be practical for industrially relevant use cases. In this work, we introduce several advances to electronic structure calculation for molecular systems, resulting in a two-orders-of-magnitude speedup of estimated runtimes over prior-art algorithms run on comparable quantum devices. One of these advances is a novel framework for block-invariant symmetry-shifted Tensor Hypercontraction (BLISS-THC), with which we achieve the tightest Hamiltonian factorizations reported to date. We compile our algorithm for an Active Volume (AV) architecture, a technical layout that has recently been proposed for fusion-based photonic quantum hardware. AV compilation contributes towards a lower runtime of our computation by eliminating overheads stemming from connectivity issues in the underlying surface code. We present a detailed benchmark of our approach, focusing primarily on the computationally challenging benchmark molecule P450. Leveraging a number of hardware tradeoffs in interleaving-based photonic FTQC, we estimate runtimes for the electronic structure calculation of P450 as a function of the device footprint.

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arXiv2026

Fullqubit alchemist: Quantum algorithm for alchemical free energy calculations

Accurately computing the free energies of biological processes is a cornerstone of computer-aided drug design, but it is a daunting task. The need to sample vast conformational spaces and account for entropic contributions makes the estimation of binding free energies very expensive. While classical methods, such as thermodynamic integration and alchemical free energy calculations, have significantly contributed to reducing computational costs, they still face limitations in terms of efficiency and scalability. We tackle this through a quantum algorithm for the estimation of free energy differences by adapting the existing Liouvillian approach and introducing several key algorithmic improvements. We directly implement the Liouvillian operator and provide an efficient description of electronic forces acting on both nuclear and electronic particles on the quantum ground state potential energy surface. This leads to super-polynomial runtime scaling improvements in the precision of our Liouvillian simulation approach and quadratic improvements in the scaling with the number of particles relative to prior quantum algorithms. Second, our algorithm calculates free energy differences via a fully quantum implementation of thermodynamic integration and alchemy, thereby foregoing expensive entropy estimation subroutines used in prior works. Our results open new avenues towards the application of quantum computers in drug discovery.

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arXiv2026

Observation of associative-memory retrieval and spin-glass phases on a photonic quantum simulator

Models of interacting complex systems provide the fundamental statistical physics reference frame for the study and the understanding of associative memories, machine learning, and the dynamics of neural networks. On the other hand, simulating complex multi-synaptic interactions on a classical hardware is computationally demanding due to the super-linear scaling of the system complexity. Photonic quantum technologies provide a promising solution to these limitations by leveraging on their inherent speed and parallel processing ability in order to simulate complex networks. Recently, a connection between multiphoton processes and generalized $p$-body Hopfield models has been theoretically established. Here, we design and demonstrate an experimental platform that exploits single photons distributed across a set of optical modes, in which controlled arrays of binary phase shifters act as Ising-like neurons. We focus specifically on a fully connected Hopfield Hamiltonian with four-body local interaction terms, realized via two-photon processes. Through quantum simulations on programmable photonic processors, the study identifies three distinct regimes: a memory retrieval phase, a spin-glass memory "black-out" phase, and a paramagnetic phase. Experimental results confirm successful memory retrieval at low storage capacities and temperatures, where the system consistently relaxes to fixed points with high memory overlap, effectively reconstructing the stored patterns. Future research will extend the platform design to investigate networks with local or dilute interactions, while advances in the realization of scalable photonic circuits will enable architectures that encompass very large numbers of interacting spins.

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arXiv2026

Improved precision scaling for simulating coupled quantum-classical dynamics

We present a super-polynomial improvement in the precision scaling of quantum simulations for coupled classical-quantum systems in this paper. Such systems are found, for example, in molecular dynamics simulations within the Born-Oppenheimer approximation. By employing a framework based on the Koopman-von Neumann formulation of classical mechanics, we express the Liouville equation of motion as unitary dynamics and utilize phase kickback from a dynamical quantum simulation to calculate the quantum forces acting on classical particles. This approach allows us to simulate the dynamics of these classical particles without the overheads associated with measuring gradients and solving the equations of motion on a classical computer, resulting in a super-polynomial advantage at the price of increased space complexity. We demonstrate that these simulations can be performed in both microcanonical and canonical ensembles, enabling the estimation of thermodynamic properties from the prepared probability density.

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arXiv2025

Classical optimisation of reduced density matrix estimations with classical shadows using N-representability conditions under shot noise considerations

Classical shadow tomography has become a powerful tool in learning about quantum states prepared on a quantum computer. Recent works have used classical shadows to variationally enforce N-representability conditions on the 2-particle reduced density matrix. In this paper, we build upon previous research by choice of an improved estimator within classical shadow tomography and rephrasing the optimisation constraints, resulting in an overall enhancement in performance under comparable measurement shot budgets. We further explore the specific regimes where these methods outperform the unbiased estimator of the standalone classical shadow protocol and quantify the potential savings in numerical studies.

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arXiv2025

Multiphoton quantum simulation of the generalized Hopfield memory model

In the present work, we introduce, develop, and investigate a connection between multiphoton quantum interference, a core element of emerging photonic quantum technologies, and Hopfieldlike Hamiltonians of classical neural networks, the paradigmatic models for associative memory and machine learning in systems of artificial intelligence. Specifically, we show that combining a system composed of Nph indistinguishable photons in superposition over M field modes, a controlled array of M binary phase-shifters, and a linear-optical interferometer, yields output photon statistics described by means of a p-body Hopfield Hamiltonian of M Ising-like neurons +-1, with p = 2Nph. We investigate in detail the generalized 4-body Hopfield model obtained through this procedure and show that it realizes a transition from a memory retrieval to a memory black-out regime, i.e. a spin-glass phase, as the amount of stored memory increases. The mapping enables novel routes to the realization and investigation of disordered and complex classical systems via efficient photonic quantum simulators, as well as the description of aspects of structured photonic systems in terms of classical spin Hamiltonians.

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arXiv2025

Improving the runtime of quantum phase estimation for chemistry through basis set optimization

Quantum phase estimation (QPE) is a promising quantum algorithm for obtaining molecular ground-state energies with chemical accuracy. However, its computational cost, dominated by the Hamiltonian 1-norm $λ$ and the cost of the block encoding, scales at least quadratically with the number of molecular orbitals, making it challenging to incorporate dynamic correlation by enlarging the active space. In this work, we investigate two strategies to mitigate this cost through the optimization of the basis set. First, we investigate whether adjusting the coefficients of Gaussian basis functions can minimize the 1-norm while preserving the accuracy of the ground state energy. Although this method leads to a reduction in the 1-norm up to 10%, this reduction is system-dependent and diminishes with increasing molecular size. Second, we demonstrate that employing a large-basis-set frozen natural orbital (FNO) strategy results in a substantial reduction in QPE resources without compromising accuracy. We study a dataset of 58 small organic molecules and the dissociation curve of N2, and demonstrate that an active space constructed from orbitals derived from larger basis sets captures correlation effects more effectively. This approach yields up to an 80% reduction in the 1-norm $λ$ and also leads to a 55% reduction in the number of orbitals. Our results highlight that improving the quality, not just the size, of the orbital basis is a viable strategy for extending QPE to include dynamical correlation, making progress toward scalable and chemically accurate quantum simulations with tractable resource requirements.

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arXiv2025

Calibration of Quantum Devices via Robust Statistical Methods

Bayesian inference is a widely used technique for real-time characterization of quantum systems. It excels in experimental characterization in the low data regime, and when the measurements have degrees of freedom. A decisive factor for its performance is the numerical representation of the Bayesian probability distributions. In this work, we explore advanced statistical methods for this purpose, and numerically analyze their performance against the state-of-the-art in quantum parameter learning. In particular, we consider sequential importance resampling, tempered likelihood estimation, Markov Chain Monte Carlo, random walk Metropolis (RWM), Hamiltonian Monte Carlo (HMC) and variants (stochastic gradients with and without friction, energy conserving subsampling), block pseudo-marginal Metropolis-Hastings with subsampling, hybrid HMC-RWM approaches, and Gaussian rejection filtering. We demonstrate advantages of these approaches over existing ones, namely robustness under multi-modality and high dimensionality. We apply these algorithms to the calibration of superconducting qubits from IBMQ, surpassing the standard quantum limit and achieving better results than Qiskit's default tools. In Hahn echo and Ramsey experiments, we reduce the uncertainty by factors of 10 and 3 respectively, without increasing the number of measurements; conversely, we match the performance of Qiskit's methods while using up to to 99.5% less experimental data. We additionally investigate the roles of adaptivity, dataset ordering and heuristics in quantum characterization. Our findings have applications in challenging quantum characterization tasks, namely learning the dynamics of open quantum systems.

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arXiv2025

Dividing and Conquering the Van Vleck Catastrophe

The quantum-computational cost of determining ground state energies through quantum phase estimation depends on the overlap between an easily preparable initial state and the targeted ground state. The Van Vleck orthogonality catastrophe has frequently been invoked to suggest that quantum computers may not be able to efficiently prepare ground states of large systems because the overlap with the initial state tends to decrease exponentially with the system size, even for non-interacting systems. We show that this intuition is not necessarily true. Specifically, we introduce a divide-and-conquer strategy that repeatedly uses phase estimation to merge ground states of increasingly larger subsystems. We provide rigorous bounds for this approach and show that if the minimum success probability of each merge is lower bounded by a constant, then the query complexity of preparing the ground state of $N$ interacting systems is in $O(N^{\log\log(N)} {\rm poly}(N))$, which is quasi-polynomial in $N$, in contrast to the exponential scaling anticipated by the Van Vleck catastrophe. We also discuss sufficient conditions on the Hamiltonian that ensure a quasi-polynomial running time.

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arXiv2024

Assessing the query complexity limits of quantum phase estimation using symmetry aware spectral bounds

The computational cost of quantum algorithms for physics and chemistry is closely linked to the spectrum of the Hamiltonian, a property that manifests in the necessary rescaling of its eigenvalues. The typical approach of using the 1-norm as an upper bound to the spectral norm to rescale the Hamiltonian suits the most general case of bounded Hermitian operators but neglects the influence of symmetries commonly found in chemical systems. In this work, we introduce a hierarchy of symmetry-aware spectral bounds that provide a unified understanding of the performance of quantum phase estimation algorithms using block-encoded electronic structure Hamiltonians. We present a variational and numerically tractable method for computing these bounds, based on orbital optimization, to demonstrate that the computed bounds are smaller than conventional spectral bounds for a variety of molecular benchmark systems. We also highlight the unique analytical and numerical scaling behavior of these bounds in the thermodynamic and complete basis set limits. Our work shows that there is room for improvement in reducing the 1-norm, not yet achieved through methods like double factorization and tensor hypercontraction, but highlights potential challenges in improving the performance of current quantum algorithms beyond small constant factors through 1-norm reduction techniques alone.

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arXiv2024

Enhancing initial state overlap through orbital optimization for faster molecular electronic ground-state energy estimation

The quantum phase estimation algorithm stands as the primary method for determining the ground state energy of a molecular electronic Hamiltonian on a quantum computer. In this context, the ability to initialize a classically tractable state that has a strong overlap with the desired ground state is critical as it directly affects the runtime of the algorithm. However, several numerical studies have shown that this overlap decays exponentially with system size. In this work, we demonstrate that this decay can be alleviated by optimizing the molecular orbital basis, for an initial state constructed from a single Slater determinant. We propose a practical method to achieve this optimization without knowledge of the true molecular ground state and test this method numerically. By comparing the resulting optimized orbitals to the natural orbitals, we find improved overlap. Specifically, for four iron-sulfur molecules, which are known to suffer from the mentioned decay, we show that our method yields one to two orders of magnitude improvement compared to localized molecular orbitals.

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arXiv2024

Reducing the runtime of fault-tolerant quantum simulations in chemistry through symmetry-compressed double factorization

Quantum phase estimation based on qubitization is the state-of-the-art fault-tolerant quantum algorithm for computing ground-state energies in chemical applications. In this context, the 1-norm of the Hamiltonian plays a fundamental role in determining the total number of required iterations and also the overall computational cost. In this work, we introduce the symmetry-compressed double factorization (SCDF) approach, which combines a compressed double factorization of the Hamiltonian with the symmetry shift technique, significantly reducing the 1-norm value. The effectiveness of this approach is demonstrated numerically by considering various benchmark systems, including the FeMoco molecule, cytochrome P450, and hydrogen chains of different sizes. To compare the efficiency of SCDF to other methods in absolute terms, we estimate Toffoli gate requirements, which dominate the execution time on fault-tolerant quantum computers. For the systems considered here, SCDF leads to a sizeable reduction of the Toffoli gate count in comparison to other variants of double factorization or even tensor hypercontraction, which is usually regarded as the most efficient approach for qubitization.

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arXiv2024

Amplified Amplitude Estimation: Exploiting Prior Knowledge to Improve Estimates of Expectation Values

We provide a method for estimating the expectation value of an operator that can utilize prior knowledge to accelerate the learning process on a quantum computer. Specifically, suppose we have an operator that can be expressed as a concise sum of projectors whose expectation values we know a priori to be $O(ε)$. In that case, we can estimate the expectation value of the entire operator within error $ε$ using a number of quantum operations that scales as $O(1/\sqrtε)$. We then show how this can be used to reduce the cost of learning a potential energy surface in quantum chemistry applications by exploiting information gained from the energy at nearby points. Furthermore, we show, using Newton-Cotes methods, how these ideas can be exploited to learn the energy via integration of derivatives that we can estimate using a priori knowledge. This allows us to reduce the cost of energy estimation if the block-encodings of directional derivative operators have a smaller normalization constant than the Hamiltonian of the system.

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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.

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arXiv2023

Fault-tolerant quantum computation of molecular observables

Over the past three decades significant reductions have been made to the cost of estimating ground-state energies of molecular Hamiltonians with quantum computers. However, comparatively little attention has been paid to estimating the expectation values of other observables with respect to said ground states, which is important for many industrial applications. In this work we present a novel expectation value estimation (EVE) quantum algorithm which can be applied to estimate the expectation values of arbitrary observables with respect to any of the system's eigenstates. In particular, we consider two variants of EVE: std-EVE, based on standard quantum phase estimation, and QSP-EVE, which utilizes quantum signal processing (QSP) techniques. We provide rigorous error analysis for both both variants and minimize the number of individual phase factors for QSPEVE. These error analyses enable us to produce constant-factor quantum resource estimates for both std-EVE and QSP-EVE across a variety of molecular systems and observables. For the systems considered, we show that QSP-EVE reduces (Toffoli) gate counts by up to three orders of magnitude and reduces qubit width by up to 25% compared to std-EVE. While estimated resource counts remain far too high for the first generations of fault-tolerant quantum computers, our estimates mark a first of their kind for both the application of expectation value estimation and modern QSP-based techniques.

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arXiv2023

Fault-tolerant quantum algorithm for symmetry-adapted perturbation theory

The efficient computation of observables beyond the total energy is a key challenge and opportunity for fault-tolerant quantum computing approaches in quantum chemistry. Here we consider the symmetry-adapted perturbation theory (SAPT) components of the interaction energy as a prototypical example of such an observable. We provide a guide for calculating this observable on a fault-tolerant quantum computer while optimizing the required computational resources. Specifically, we present a quantum algorithm that estimates interaction energies at the first-order SAPT level with a Heisenberg-limited scaling. To this end, we exploit a high-order tensor factorization and block encoding technique that efficiently represents each SAPT observable. To quantify the computational cost of our methodology, we provide resource estimates in terms of the required number of logical qubits and Toffoli gates to execute our algorithm for a range of benchmark molecules, also taking into account the cost of the eigenstate preparation and the cost of block encoding the SAPT observables. Finally, we perform the resource estimation for a heme and artemisinin complex as a representative large-scale system encountered in drug design, highlighting our algorithm's performance in this new benchmark study and discussing possible bottlenecks that may be improved in future work.

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arXiv2023

Learning Quantum Systems

The future development of quantum technologies relies on creating and manipulating quantum systems of increasing complexity, with key applications in computation, simulation and sensing. This poses severe challenges in the efficient control, calibration and validation of quantum states and their dynamics. Although the full simulation of large-scale quantum systems may only be possible on a quantum computer, classical characterization and optimization methods still play an important role. Here, we review different approaches that use classical post-processing techniques, possibly combined with adaptive optimization, to learn quantum systems, their correlation properties, dynamics and interaction with the environment. We discuss theoretical proposals and successful implementations across different multiple-qubit architectures such as spin qubits, trapped ions, photonic and atomic systems, and superconducting circuits. This Review provides a brief background of key concepts recurring across many of these approaches with special emphasis on the Bayesian formalism and neural networks.

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arXiv2023

Drug design on quantum computers

Quantum computers promise to impact industrial applications, for which quantum chemical calculations are required, by virtue of their high accuracy. This perspective explores the challenges and opportunities of applying quantum computers to drug design, discusses where they could transform industrial research and elaborates on what is needed to reach this goal.

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