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Yvon Maday

Publications and source records attributed to Yvon Maday.

At least 19 recordsLinked to original sources

Mitigating Barren Plateaus via Domain Decomposition in Variational Quantum Algorithms for Nonlinear PDEs

Barren plateaus present a major challenge in the training of variational quantum algorithms (VQAs), particularly for large-scale discretizations of nonlinear partial differential equations. In this work, we introduce a domain decomposition framework to mitigate barren plateaus by localizing the cost functional. Our strategy is based on partitioning the spatial domain into overlapping subdomains, each associated with a localized parameterized quantum circuit and measurement operator. Numerical results for the time-independent Gross-Pitaevskii equation show that the domain-decomposed formulation, allowing subdomain iterations to be interleaved with optimization iterations, exhibits improved solution accuracy and stable optimization compared to the global VQA formulation.

math.NA

Nonlinear compressive reduced basis approximation : when Taylor meets Kolmogorov

This paper investigates model reduction methods for efficiently approximating the solution of parameter-dependent PDEs with a multi-parameter vector $\vecμ \in \mathbb{R}^p$. In cases where the Kolmogorov $N$-width decays fast enough, it is effective to approximate the solution as a sum of $N$ separable terms, each being the product of a parameter-dependent coefficient and a space-dependent function. This leads to reduced-order models with $N$ degrees of freedom and complexity of order ${\mathcal O}(N^3)$. However, when the $N$-width decays slowly, $N$ must be large to achieve acceptable accuracy, making cubic complexity prohibitive. The linear complexity measure in terms of Kolmogorov width must be replaced by the Gelfand width, with its associated sensing number. Recent nonlinear approaches based on this notion decompose the $N$ coordinates into two groups: $n$ free variables and $\overline{n}$ dependent variables, where the latter are nonlinear functions of the former ($N= n+\overline n$). Several works have focused on cases where these $\overline{n}$ functions are homogeneous quadratic forms of the $n$ variables, with optimization strategies for choosing $n$ given a target accuracy. A rigorous analysis of the local sensing number is carried out, showing that $n = p$ is optimal and appropriate, at least locally, around a reference point. In practical scenarios involving wide parameter ranges, the condition $p\le n \le p + k$ (with $k$ small) is valid and more robust from continuity arguments. Additionally, the assumption of a quadratic mapping, while justified in a local sense, becomes insufficient. More expressive nonlinear mappings-including those using machine learning-become necessary. This work contributes a theoretical foundation for such strategies and highlights the need for further investigations to push back the Kolmogorov Barrier.

math.NA

Analysis of the Single Reference Coupled Cluster Method for Electronic Structure Calculations: The Discrete Coupled Cluster Equations

Coupled cluster methods are widely regarded as the gold standard of computational quantum chemistry as they are perceived to offer the best compromise between computational cost and a high-accuracy resolution of the ground state eigenvalue of the electronic Hamiltonian -- an unbounded, self-adjoint operator acting on a Hilbert space of antisymmetric functions that describes electronic properties of molecular systems. The present contribution is the second in a series of two articles where we introduce a new numerical analysis of the single-reference coupled cluster method based on the invertibility of the coupled cluster Fréchet derivative. In this contribution, we study discretisations of the single-reference coupled cluster equations based on a prior mean-field (Hartree-Fock) calculation. We show that under some structural assumptions on the associated discretisation spaces and assuming that the discretisation is fine enough, the discrete coupled cluster equations are locally well-posed, and we derive a priori and residual-based a posteriori error estimates for the discrete coupled cluster solutions. Preliminary numerical experiments indicate that the structural assumptions that we impose for our analysis can be expected to hold for several small molecules and the theoretical constants that appear in our error estimates are an improvement over those obtained from earlier approaches.

math.NA

Pushing the Accuracy Limit of Foundation Neural Network Models with Quantum Monte Carlo Forces and Path Integrals

We propose an end-to-end integrated strategy to produce highly accurate quantum chemistry (QC) synthetic datasets (energies and forces) aimed at deriving Foundation Machine Learning models for molecular simulation. Starting from Density Functional Theory (DFT), a "Jacob's Ladder" approach leverages computationally-optimized layers of massively GPU-accelerated software with increasing accuracy. Thanks to Exascale, this is the first time that the computationally intensive calculation of Quantum Monte Carlo forces (QMC), and the combination of multi-determinant QMC energies and forces with selected-Configuration Interaction wavefunctions, are computed at such scale at the complete basis-set limit. To bridge the gap between accurate QC and condensed-phase Molecular Dynamics, we leverage transfer learning to improve the DFT-based FeNNix-Bio1 foundation model. The resulting approach is coupled to path integrals adaptive sampling quantum dynamics to perform nanosecond reactive simulations at unprecedented accuracy. These results demonstrate the promise of Exascale to deepen our understanding of the inner machinery of complex biosystems.

physics.chem-ph

Convergence analysis of a solver for the linear Poisson--Boltzmann model

This work investigates the convergence of a domain decomposition method for the Poisson-Boltzmann model that can be formulated as an interior-exterior transmission problem. To study its convergence, we introduce an interior-exterior constant providing an upper bound of the $L^2$ norm of any harmonic function in the interior, and establish a spectral equivalence for related Dirichlet-to-Neumann operators to estimate the spectrum of interior-exterior iteration operator. This analysis is nontrivial due to the unboundedness of the exterior subdomain, which distinguishes it from the classical analysis of the Schwarz alternating method with nonoverlapping bounded subdomains. It is proved that for the linear Poisson-Boltzmann solvent model in reality, the convergence of interior-exterior iteration is ensured when the relaxation parameter lies between 0 and 2. This convergence result interprets the good performance of ddLPB method developed in [SIAM Journal on Scientific Computing, 41 (2019), pp. B320-B350] where the relaxation parameter is set to 1. Numerical simulations are conducted to verify our convergence analysis and to investigate the optimal relaxation parameter for the interior-exterior iteration.

math.NA

On the relation between Galerkin approximations and canonical best-approximations of solutions to some non-linear Schrödinger equations

In this paper, we establish a superconvergence property of Galerkin approximations to some non-linear Schrödinger equations of Gross-Pitaevskii type. More precisely, denoting by $u^*\in X \subseteq H^1(Ω)$ the exact solution to such an equation, by $\{X_δ\}_{δ>0}$, a sequence of conforming subspaces of $X$ satisfying the approximation property, by $u_δ^*\in X_δ$ the Galerkin solution to the equation, and by $Π^X_δ u^*$, the $(\cdot, \cdot)_{X}$-best approximation in $X_δ$ of $u^*$, we show -- under some assumptions -- that $u_δ^*$ converges at a higher rate to $Π^X_δ u^*$ than to $u^*$ in both the $L^2$ norm and the canonical $H^1$ norm. Our results apply to conforming finite element discretisations as well as spectral Galerkin methods based on polynomials or Fourier (plane-wave) expansions.

math.NA

Greedy Gradient-free Adaptive Variational Quantum Algorithms on a Noisy Intermediate Scale Quantum Computer

Hybrid quantum-classical adaptive Variational Quantum Eigensolvers (VQE) hold the potential to outperform classical computing for simulating many-body quantum systems. However, practical implementations on current quantum processing units (QPUs) are challenging due to the noisy evaluation of a polynomially scaling number of observables, undertaken for operator selection and high-dimensional cost function optimization. We introduce an adaptive algorithm using analytic, gradient-free optimization, called Greedy Gradient-free Adaptive VQE (GGA-VQE). In addition to demonstrating the algorithm's improved resilience to statistical sampling noise in the computation of simple molecular ground states, we execute GGA-VQE on a 25-qubit error-mitigated QPU by computing the ground state of a 25-body Ising model. Although hardware noise on the QPU produces inaccurate energies, our implementation outputs a parameterized quantum circuit yielding a favorable ground-state approximation. We demonstrate this by retrieving the parameterized operators calculated on the QPU and evaluating the resulting ansatz wave-function via noiseless emulation (i.e., hybrid observable measurement).

quant-ph

Unsupervised detection and fitness estimation of emerging SARS-CoV-2 variants. Application to wastewater samples (ANRS0160)

Repeated waves of emerging variants during the SARS-CoV-2 pandemics have highlighted the urge of collecting longitudinal genomic data and developing statistical methods based on time series analyses for detecting new threatening lineages and estimating their fitness early in time. Most models study the evolution of the prevalence of particular lineages over time and require a prior classification of sequences into lineages. Such process is prone to induce delays and bias. More recently, few authors studied the evolution of the prevalence of mutations over time with alternative clustering approaches, avoiding specific lineage classification. Most of the aforementioned methods are however either non parametric or unsuited to pooled data characterizing, for instance, wastewater samples. In this context, we propose an alternative unsupervised method for clustering mutations according to their frequency trajectory over time and estimating group fitness from time series of pooled mutation prevalence data. Our model is a mixture of observed count data and latent group assignment and we use the expectation-maximization algorithm for model selection and parameter estimation. The application of our method to time series of SARS-CoV-2 sequencing data collected from wastewater treatment plants in France from October 2020 to April 2021 shows its ability to agnostically group mutations according to their probability of belonging to B.1.160, Alpha, Beta, B.1.177 variants with selection coefficient estimates per group in coherence with the viral dynamics in France reported by Nextstrain. Moreover, our method detected the Alpha variant as threatening as early as supervised methods (which track specific mutations over time) with the noticeable difference that, since unsupervised, it does not require any prior information on the set of mutations.

q-bio.QM

Shortcut to Chemically Accurate Quantum Computing via Density-based Basis-set Correction

Using GPU-accelerated state-vector emulation, we propose to embed a quantum computing ansatz into density-functional theory via density-based basis-set corrections (DBBSC) to obtain quantitative quantum-chemistry results on molecules that would otherwise require brute-force quantum calculations using hundreds of logical qubits. Indeed, accessing a quantitative description of chemical systems while minimizing quantum resources is an essential challenge given the limited qubit capabilities of current quantum processors. We provide a shortcut towards chemically accurate quantum computations by approaching the complete-basis-set limit through coupling the DBBSC approach, applied to any given variational ansatz, to an on-the-fly crafting of basis sets specifically adapted to a given system and user-defined qubit budget. The resulting approach self-consistently accelerates the basis-set convergence, improving electronic densities, ground-state energies, and first-order properties (e.g. dipole moments), but can also serve as a classical, a posteriori, energy correction to quantum hardware calculations with expected applications in drug design and materials science.

physics.chem-ph

Nonlinear compressive reduced basis approximation for multi-parameter elliptic problem

Reduced basis methods for approximating the solutions of parameter-dependant partial differential equations (PDEs) are based on learning the structure of the set of solutions - seen as a manifold ${\mathcal S}$ in some functional space - when the parameters vary. This involves investigating the manifold and, in particular, understanding whether it is close to a low-dimensional affine space. This leads to the notion of Kolmogorov $N$-width that consists of evaluating to which extent the best choice of a vectorial space of dimension $N$ approximates ${\mathcal S}$ well enough. If a good approximation of elements in ${\mathcal S}$ can be done with some well-chosen vectorial space of dimension $N$ -- provided $N$ is not too large -- then a ``reduced'' basis can be proposed that leads to a Galerkin type method for the approximation of any element in ${\mathcal S}$. In many cases, however, the Kolmogorov $N$-width is not so small, even if the parameter set lies in a space of small dimension yielding a manifold with small dimension. In terms of complexity reduction, this gap between the small dimension of the manifold and the large Kolmogorov $N$-width can be explained by the fact that the Kolmogorov $N$-width is linear while, in contrast, the dependency in the parameter is, most often, non-linear. There have been many contributions aiming at reconciling these two statements, either based on deterministic or AI approaches. We investigate here further a new paradigm that, in some sense, merges these two aspects: the nonlinear compressive reduced basisapproximation. We focus on a simple multiparameter problem and illustrate rigorously that the complexity associated with the approximation of the solution to the parameter dependant PDE is directly related to the number of parameters rather than the Kolmogorov $N$-width.

math.NA

An overview of a posteriori error estimation and post-processingmethods for nonlinear eigenvalue problems

In this article, we present an overview of different a posteriori error analysis and postprocessing methods proposed in the context of nonlinear eigenvalue problems, e.g. arising inelectronic structure calculations for the calculation of the ground state and compare them. Weprovide two equivalent error reconstructions based either on a second-order Taylor expansionof the minimized energy, or a first-order expansion of the nonlinear eigenvalue equation. Wethen show how several a posteriori error estimations as well as post-processing methods can beformulated as specific applications of the derived reconstructed errors, and we compare theirrange of applicability as well as numerical cost and precision.

math.NA

Overlap-ADAPT-VQE: Practical Quantum Chemistry on Quantum Computers via Overlap-Guided Compact Ansätze

ADAPT-VQE is a robust algorithm for hybrid quantum-classical simulations of quantum chemical systems on near-term quantum computers. While its iterative process systematically reaches the ground state energy, ADAPT-VQE is sensitive to local energy minima, leading to over-parameterized ansätze. We introduce the Overlap-ADAPT-VQE to grow wave-functions by maximizing their overlap with any intermediate target wave-function that already captures some electronic correlation. By avoiding building the ansatz in the energy landscape strewn with local minima, the Overlap-ADAPT-VQE produces ultra-compact ansätze suitable for high-accuracy initializations of a new ADAPT procedure. Spectacular advantages over ADAPT-VQE are observed for strongly correlated systems including massive savings in circuit depth. Since this compression strategy can also be initialized with accurate Selected-Configuration Interaction (SCI) classical target wave-functions, it paves the way for chemically accurate simulations of larger systems, and strengthens the promise of decisively surpassing classical quantum chemistry through the power of quantum computing.

quant-ph

Directed Message Passing Based on Attention for Prediction of Molecular Properties

Molecular representation learning (MRL) has long been crucial in the fields of drug discovery and materials science, and it has made significant progress due to the development of natural language processing (NLP) and graph neural networks (GNNs). NLP treats the molecules as one dimensional sequential tokens while GNNs treat them as two dimensional topology graphs. Based on different message passing algorithms, GNNs have various performance on detecting chemical environments and predicting molecular properties. Herein, we propose Directed Graph Attention Networks (D-GATs): the expressive GNNs with directed bonds. The key to the success of our strategy is to treat the molecular graph as directed graph and update the bond states and atom states by scaled dot-product attention mechanism. This allows the model to better capture the sub-structure of molecular graph, i.e., functional groups. Compared to other GNNs or Message Passing Neural Networks (MPNNs), D-GATs outperform the state-of-the-art on 13 out of 15 important molecular property prediction benchmarks.

cs.IT

Extension of the Trotterized Unitary Coupled Cluster to Triple Excitations

The Trotterized Unitary Coupled Cluster Single and Double (UCCSD) ansatz has recently attracted interest due to its use in Variation Quantum Eigensolver (VQE) molecular simulations on quantum computers. However, when the size of molecules increases, UCCSD becomes less interesting as it cannot achieve sufficient accuracy. Including higher-order excitations is therefore mandatory to recover the UCC's missing correlation effects. In this Letter, we extend the Trotterized UCC approach via the addition of (true) Triple T excitations introducing UCCSDT. We also include both spin and orbital symmetries. Indeed, in practice, these later help to reduce unnecessarily circuit excitations and thus accelerate the optimization process enabling to tackle larger molecules. Our initial numerical tests (12-14 qubits) show that UCCSDT improves the overall accuracy by at least two-orders of magnitudes with respect to standard UCCSD. Overall, the UCCSDT ansatz is shown to reach chemical accuracy and to be competitive with the CCSD(T) gold-standard classical method of quantum chemistry.

physics.chem-ph

Analysis of the Single Reference Coupled Cluster Method for Electronic Structure Calculations: The Full Coupled Cluster Equations

The central problem in electronic structure theory is the computation of the eigenvalues of the electronic Hamiltonian -- an unbounded, self-adjoint operator acting on a Hilbert space of antisymmetric functions. Coupled cluster (CC) methods, which are based on a non-linear parameterisation of the sought-after eigenfunction and result in non-linear systems of equations, are the method of choice for high accuracy quantum chemical simulations but their numerical analysis is underdeveloped. The existing numerical analysis relies on a local, strong monotonicity property of the CC function that is valid only in a perturbative regime, i.e., when the sought-after ground state CC solution is sufficiently close to zero. In this article, we introduce a new well-posedness analysis for the single reference coupled cluster method based on the invertibility of the CC derivative. Under the minimal assumption that the sought-after eigenfunction is intermediately normalisable and the associated eigenvalue is isolated and non-degenerate, we prove that the continuous (infinite-dimensional) CC equations are always locally well-posed. Under the same minimal assumptions and provided that the discretisation is fine enough, we prove that the discrete Full-CC equations are locally well-posed, and we derive residual-based error estimates with guaranteed positive constants. Preliminary numerical experiments indicate that the constants that appear in our estimates are a significant improvement over those obtained from the local monotonicity approach.

math.NA

Neural-Network-Augmented Projection-Based Model Order Reduction for Mitigating the Kolmogorov Barrier to Reducibility of CFD Models

Inspired by our previous work on mitigating the Kolmogorov barrier using a quadratic approximation manifold, we propose in this paper a computationally tractable approach for combining a projection-based reduced-order model (PROM) and an artificial neural network (ANN) for mitigating the Kolmogorov barrier to reducibility of convection-dominated flow problems. The main objective the PROM-ANN concept that we propose is to reduce the dimensionality of the online approximation of the solution beyond what is possible using affine and quadratic approximation manifolds. In contrast to previous approaches for constructing arbitrarily nonlinear manifold approximations for nonlinear model reduction that exploited one form or another of ANN, the training of the PROM-ANN we propose in this paper does not involve data whose dimension scales with that of the high-dimensional model; and this PROM-ANN is hyperreducible using any well-established hyperreduction method. Hence, unlike many other ANN-based approaches, the PROM-ANN concept we propose in this paper is practical for large-scale and industry-relevant CFD problems. Its potential is demonstrated here for a parametric, shock-dominated, benchmark problem.

cs.CE

Open Source Variational Quantum Eigensolver Extension of the Quantum Learning Machine (QLM) for Quantum Chemistry

Quantum Chemistry (QC) is one of the most promising applications of Quantum Computing. However, present quantum processing units (QPUs) are still subject to large errors. Therefore, noisy intermediate-scale quantum (NISQ) hardware is limited in terms of qubits counts and circuit depths. Specific algorithms such as Variational Quantum Eigensolvers (VQEs) can potentially overcome such issues. We introduce here a novel open-source QC package, denoted Open-VQE, providing tools for using and developing chemically-inspired adaptive methods derived from Unitary Coupled Cluster (UCC). It facilitates the development and testing of VQE algorithms. It is able to use the Atos Quantum Learning Machine (QLM), a general quantum programming framework enabling to write, optimize and simulate quantum computing programs. Along with Open-VQE, we introduce myQLM-Fermion, a new open-source module (that includes the key QLM ressources that are important for QC developments (fermionic second quantization tools etc...). The Open-VQE package extends therefore QLM to QC providing: (i) the functions to generate the different types of excitations beyond the commonly used UCCSD ans{ä}tz;(ii) a new implementation of the "adaptive derivative assembled pseudo-Trotter method" (ADAPT-VQE), written in simple class structure python codes. Interoperability with other major quantum programming frameworks is ensured thanks to myQLM, which allows users to easily build their own code and execute it on existing QPUs. The combined Open-VQE/myQLM-Fermion quantum simulator facilitates the implementation, tests and developments of variational quantum algorithms towards choosing the best compromise to run QC computations on present quantum computers while offering the possibility to test large molecules. We provide extensive benchmarks for several molecules associated to qubit counts ranging from 4 up to 24.

quant-ph

Error estimate of the Non-Intrusive Reduced Basis (NIRB) two-grid method with parabolic equations

Reduced Basis Methods (RBMs) are frequently proposed to approximate parametric problem solutions. They can be used to calculate solutions for a large number of parameter values (e.g. for parameter fitting) as well as to approximate a solution for a new parameter value (e.g. real time approximation with a very high accuracy). They intend to reduce the computational costs of High Fidelity (HF) codes. We will focus on the Non-Intrusive Reduced Basis (NIRB) two-grid method. Its main advantage is that it uses the HF code exclusively as a "black-box," as opposed to other so-called intrusive methods that require code modification. This is very convenient when the HF code is a commercial one that has been purchased, as is frequently the case in the industry. The effectiveness of this method relies on its decomposition into two stages, one offline (classical in most RBMs as presented above) and one online. The offline part is time-consuming but it is only performed once. On the contrary, the specificity of this NIRB approach is that, during the online part, it solves the parametric problem on a coarse mesh only and then improves its precision. As a result, it is significantly less expensive than a HF evaluation. This method has been originally developed for elliptic equations with finite elements and has since been extended to finite volume. In this paper, we extend the NIRB two-grid method to parabolic equations. We recover optimal estimates in $L^{\infty}(0,T;H^1(Ω))$ using as a model problem, the heat equation. Then, we present numerical results on the heat equation and on the Brusselator problem.

math.NA