Search

Hummingbirds and insects achieve outstanding flight performance by adapting their flapping motion to the flight requirements. Their wing kinematics can change from smooth flapping to highly dynamic waveforms, generating unsteady aerodynamic phenomena such as leading-edge vortices (LEV), rotational circulation, wing wake capture, and added mass. This article uncovers the interactions of these mechanisms in the case of a rigid semi-elliptical wing undergoing aggressive kinematics in the hovering regime at $Re\sim \mathcal{O}(10^3)$. The flapping kinematics were parametrized using smoothed steps and triangular functions and the flow dynamics were simulated by combining the overset method with Large Eddy Simulations (LES). The analysis of the results identifies an initial acceleration phase and a cruising phase. During the former, the flow is mostly irrotational and governed by the added mass effect. The added mass was shown to be responsible for a lift first peak due to the strong flapping acceleration. The dynamic pitching and the wing wake interaction generate a second lift peak due to a downwash flow and a vortex system on the proximal and distal parts of the wing's pressure side. Conversely, aerodynamic forces in the cruising phase are mainly governed by the growth and the establishment of the LEV. Finally, the leading flow structures in each phase and their impact on the aerodynamic forces were isolated using the extended Proper Orthogonal Decomposition (POD).

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.

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., Comment: 11 pages, 3 figures, 1 table

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.

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 $O(\epsilon)$. In that case, we can estimate the expectation value of the entire operator within error $\epsilon$ using a number of quantum operations that scales as $O(1/\sqrt{\epsilon})$. 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., Comment: 23 pages, v2: additional explanations to clarify the assumptions and results

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.

Over the past decades, libraries of stellar spectra have been used in a large variety of science cases, including as sources of reference spectra for a given object or a given spectral type. Despite the existence of large libraries and the increasing number of projects of large-scale spectral surveys, there is to date only one very high-resolution spectral library offering spectra from a few hundred objects from the southern hemisphere (UVES-POP) . We aim to extend the sample, offering a finer coverage of effective temperatures and surface gravity with a uniform collection of spectra obtained in the northern hemisphere. Between 2010 and 2020, we acquired several thousand echelle spectra of bright stars with the Mercator-HERMES spectrograph located in the Roque de Los Muchachos Observatory in La Palma, whose pipeline offers high-quality data reduction products. We have also developed methods to correct for the instrumental response in order to approach the true shape of the spectral continuum. Additionally, we have devised a normalisation process to provide a homogeneous normalisation of the full spectral range for most of the objects. We present a new spectral library consisting of 3256 spectra covering 2043 stars. It combines high signal-to-noise and high spectral resolution over the entire range of effective temperatures and luminosity classes. The spectra are presented in four versions: raw, corrected from the instrumental response, with and without correction from the atmospheric molecular absorption, and normalised (including the telluric correction)., Comment: 17 pages, 18 figures Preview and access to the library: https://www.royer.se/melchiors.html

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 formalism, 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 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., Comment: 19 + 51 pages

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., Comment: 55 pages, 18 figures, 4 tables

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., Comment: 36 pages, 9 figures

In literature, the cost of a partitioned fluid-structure interaction scheme is typically assessed by the number of coupling iterations required per time step, while ignoring the internal iterations within the nonlinear subproblems. In this work, we demonstrate that these internal iterations have a significant influence on the computational cost of the coupled simulation. Particular attention is paid to how limiting the number of iterations within each solver call can shorten the overall run time, as it avoids polishing the subproblem solution using unconverged coupling data. Based on systematic parameter studies, we investigate the optimal number of subproblem iterations per coupling step. Lastly, this work proposes a new convergence criterion for coupled systems that is based on the residuals of the subproblems and therefore does not require any additional convergence tolerance for the coupling loop.

In this work, we test a recently developed method to enhance classical auxiliary-field quantum Monte Carlo (AFQMC) calculations with quantum computers against examples from chemistry and material science, representatives of classes of industry-relevant systems. As molecular test cases, we calculate the energy curve of H4 and relative energies of ozone and singlet molecular oxygen with respect to triplet molecular oxygen, which are industrially relevant in organic oxidation reactions. We find that trial wave functions beyond single Slater determinants improve the performance of AFQMC and allow to generate energies close to chemical accuracy compared to full configuration interaction (FCI) or experimental results. As a representative for material science we study a quasi-1D Fermi-Hubbard model derived from CuBr2, a compound displaying electronic structure properties analogous to cuprates. We find that trial wave functions with both, significantly larger fidelities and lower energies over a Hartree-Fock solution, do not necessarily lead to better AFQMC results.

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.

The computation of interaction energies on noisy intermediate-scale quantum (NISQ) computers appears to be challenging with straightforward application of existing quantum algorithms. For example, use of the standard supermolecular method with the variational quantum eigensolver (VQE) would require extremely precise resolution of the total energies of the fragments to provide for accurate subtraction to the interaction energy. Here we present a symmetry-adapted perturbation theory (SAPT) method that may provide interaction energies with high quantum resource efficiency. Of particular note, we present a quantum extended random-phase approximation (ERPA) treatment of the SAPT second-order induction and dispersion terms, including exchange counterparts. Together with previous work on first-order terms, this provides a recipe for complete SAPT(VQE) interaction energies up to second order. The SAPT interaction energy terms are computed as first-level observables with no subtraction of monomer energies invoked, and the only quantum observations needed are the the VQE one- and two-particle density matrices. We find empirically that SAPT(VQE) can provide accurate interaction energies even with coarsely optimized, low circuit depth wavefunctions from the quantum computer, simulated through ideal statevectors. The errors on the total interaction energy are orders of magnitude lower than the corresponding VQE total energy errors of the monomer wavefunctions., Comment: 38 pages, 6 primary figures

An accurate assessment of how quantum computers can be used for chemical simulation, especially their potential computational advantages, provides important context on how to deploy these future devices. In order to perform this assessment reliably, quantum resource estimates must be coupled with classical simulations attempting to answer relevant chemical questions and to define the classical simulation frontier. Herein, we explore the quantum and classical resources required to assess the electronic structure of cytochrome P450 enzymes (CYPs) and thus define a classical-quantum advantage boundary. This is accomplished by analyzing the convergence of DMRG+NEVPT2 and coupled cluster singles doubles with non-iterative triples (CCSD(T)) calculations for spin-gaps in models of the CYP catalytic cycle that indicate multireference character. The quantum resources required to perform phase estimation using qubitized quantum walks are calculated for the same systems. Compilation into the surface-code provides runtime estimates to compare directly to DMRG runtimes and to evaluate potential quantum advantage. Both classical and quantum resource estimates suggest that simulation of CYP models at scales large enough to balance dynamic and multiconfigurational electron correlation has the potential to be a quantum advantage problem and emphasizes the important interplay between classical simulations and quantum algorithms development for chemical simulation.

While most work on the quantum simulation of chemistry has focused on computing energy surfaces, a similarly important application requiring subtly different algorithms is the computation of energy derivatives. Almost all molecular properties can be expressed an energy derivative, including molecular forces, which are essential for applications such as molecular dynamics simulations. Here, we introduce new quantum algorithms for computing molecular energy derivatives with significantly lower complexity than prior methods. Under cost models appropriate for noisy-intermediate scale quantum devices we demonstrate how low rank factorizations and other tomography schemes can be optimized for energy derivative calculations. We perform numerics revealing that our techniques reduce the number of circuit repetitions required by many orders of magnitude for even modest systems. In the context of fault-tolerant algorithms, we develop new methods of estimating energy derivatives with Heisenberg limited scaling incorporating state-of-the-art techniques for block encoding fermionic operators. Our results suggest that the calculation of forces on a single nucleus may be of similar cost to estimating energies of chemical systems, but that further developments are needed for quantum computers to meaningfully assist with molecular dynamics simulations., Comment: 48 pages, 14 page appendix, 10 figures. v2 contains updated lambdas (rescaling factors) for sparse FT encodings and some NISQ methods, obtained by localizing orbitals

We explore the use of symmetry-adapted perturbation theory (SAPT) as a simple and efficient means to compute interaction energies between large molecular systems with a hybrid method combing NISQ-era quantum and classical computers. From the one- and two-particle reduced density matrices of the monomer wavefunctions obtained by the variational quantum eigensolver (VQE), we compute SAPT contributions to the interaction energy [SAPT(VQE)]. At first order, this energy yields the electrostatic and exchange contributions for non-covalently bound systems. We empirically find from ideal statevector simulations that the SAPT(VQE) interaction energy components display orders of magnitude lower absolute errors than the corresponding VQE total energies. Therefore, even with coarsely optimized low-depth VQE wavefunctions, we still obtain sub kcal/mol accuracy in the SAPT interaction energies. In SAPT(VQE), the quantum requirements, such as qubit count and circuit depth, are lowered by performing computations on the separate molecular systems. Furthermore, active spaces allow for large systems containing thousands of orbitals to be reduced to a small enough orbital set to perform the quantum portions of the computations. We benchmark SAPT(VQE) (with the VQE component simulated by ideal state-vector simulators) against a handful of small multi-reference dimer systems and the iron center containing human cancer-relevant protein lysine-specific demethylase 5 (KDM5A)., Comment: 16 pages, 4 figures, plus supplemental data

We present a review of the Unitary Coupled Cluster (UCC) ansatz and related ans\"atze which are used to variationally solve the electronic structure problem on quantum computers. A brief history of coupled cluster (CC) methods is provided, followed by a broad discussion of the formulation of CC theory. This includes touching on the merits and difficulties of the method and several variants, UCC among them, in the classical context, to motivate their applications on quantum computers. In the core of the text, the UCC ansatz and its implementation on a quantum computer are discussed at length, in addition to a discussion on several derived and related ans\"atze specific to quantum computing. The review concludes with a unified perspective on the discussed ans\"atze, attempting to bring them under a common framework, as well as with a reflection upon open problems within the field.

A universal fault-tolerant quantum computer that can solve efficiently problems such as integer factorization and unstructured database search requires millions of qubits with low error rates and long coherence times. While the experimental advancement towards realizing such devices will potentially take decades of research, noisy intermediate-scale quantum (NISQ) computers already exist. These computers are composed of hundreds of noisy qubits, i.e. qubits that are not error-corrected, and therefore perform imperfect operations in a limited coherence time. In the search for quantum advantage with these devices, algorithms have been proposed for applications in various disciplines spanning physics, machine learning, quantum chemistry and combinatorial optimization. The goal of such algorithms is to leverage the limited available resources to perform classically challenging tasks. In this review, we provide a thorough summary of NISQ computational paradigms and algorithms. We discuss the key structure of these algorithms, their limitations, and advantages. We additionally provide a comprehensive overview of various benchmarking and software tools useful for programming and testing NISQ devices., Comment: Added new content, Modified certain parts and the paper structure

Natural evolutionary strategies (NES) are a family of gradient-free black-box optimization algorithms. This study illustrates their use for the optimization of randomly-initialized parametrized quantum circuits (PQCs) in the region of vanishing gradients. We show that using the NES gradient estimator the exponential decrease in variance can be alleviated. We implement two specific approaches, the exponential and separable natural evolutionary strategies, for parameter optimization of PQCs and compare them against standard gradient descent. We apply them to two different problems of ground state energy estimation using variational quantum eigensolver (VQE) and state preparation with circuits of varying depth and length. We also introduce batch optimization for circuits with larger depth to extend the use of evolutionary strategies to a larger number of parameters. We achieve accuracy comparable to state-of-the-art optimization techniques in all the above cases with a lower number of circuit evaluations. Our empirical results indicate that one can use NES as a hybrid tool in tandem with other gradient-based methods for optimization of deep quantum circuits in regions with vanishing gradients.

Variational quantum algorithms are currently the most promising class of algorithms for deployment on near-term quantum computers. In contrast to classical algorithms, there are almost no standardized methods in quantum algorithmic development yet, and the field continues to evolve rapidly. As in classical computing, heuristics play a crucial role in the development of new quantum algorithms, resulting in high demand for flexible and reliable ways to implement, test, and share new ideas. Inspired by this demand, we introduce tequila, a development package for quantum algorithms in python, designed for fast and flexible implementation, prototyping, and deployment of novel quantum algorithms in electronic structure and other fields. Tequila operates with abstract expectation values which can be combined, transformed, differentiated, and optimized. On evaluation, the abstract data structures are compiled to run on state-of-the-art quantum simulators or interfaces.

A novel reduced order model (ROM) for incompressible flows is developed by performing a Galerkin projection based on a fully (space and time) discrete full order model (FOM) formulation. This 'discretize-then-project' approach requires no pressure stabilization technique (even though the pressure term is present in the ROM) nor a boundary control technique (to impose the boundary conditions at the ROM level). These are two main advantages compared to existing approaches. The fully discrete FOM is obtained by a finite volume discretization of the incompressible Navier-Stokes equations on a collocated grid, with a forward Euler time discretization. Two variants of the time discretization method, the inconsistent and consistent flux method, have been investigated. The latter leads to divergence-free velocity fields, also on the ROM level, whereas the velocity fields are only approximately divergence-free in the former method. For both methods, accurate results have been obtained for test cases with different types of boundary conditions: a lid-driven cavity and an open-cavity (with an inlet and outlet). The ROM obtained with the consistent flux method, having divergence-free velocity fields, is slightly more accurate but also slightly more expensive to solve compared to the inconsistent flux method. The speedup ratio of the ROM and FOM computation times is the highest for the open cavity test case with the inconsistent flux method., Comment: 36 pages, 22 figures, 1 table

The nuclear community has coupled several three-dimensional Computational Fluid Dynamics (CFD) solvers with one-dimensional system thermal-hydraulic (STH) codes. This work proposes to replace the CFD solver by a reduced order model (ROM) to reduce the computational cost. The system code RELAP5-MOD3.3 and a ROM of the finite volume CFD solver OpenFOAM are coupled by a partitioned domain decomposition coupling algorithm using an implicit coupling scheme. The velocity transported over a coupling boundary interface is imposed in the ROM using a penalty method. The coupled models are evaluated on open and closed pipe flow configurations. The results of the coupled simulations with the ROM are close to those with the CFD solver. Also for new parameter sets, the coupled RELAP5/ROM models are capable of predicting the coupled RELAP5/CFD results with good accuracy. Finally, coupling with the ROM is 3-5 times faster than coupling with the CFD solver., Comment: 39 pages, 33 figures

Adaptive construction of ansatz circuits offers a promising route towards applicable variational quantum eigensolvers on near-term quantum hardware. Those algorithms aim to build up optimal circuits for a certain problem and ansatz circuits are adaptively constructed by selecting and adding entanglers from a predefined pool. In this work, we propose a way to construct entangler pools with reduced size by leveraging classical algorithms. Our method uses mutual information between the qubits in classically approximated ground state to rank and screen the entanglers. The density matrix renormalization group method is employed for classical precomputation in this work. We corroborate our method numerically on small molecules. Our numerical experiments show that a reduced entangler pool with a small portion of the original entangler pool can achieve same numerical accuracy. We believe that our method paves a new way for adaptive construction of ansatz circuits for variational quantum algorithms., Comment: 10 pages, 13 figures

The potential advantage of machine learning in quantum computers is a topic of intense discussion in the literature. Theoretical, numerical and experimental explorations will most likely be required to understand its power. There has been different algorithms proposed to exploit the probabilistic nature of variational quantum circuits for generative modelling. In this paper, we employ a hybrid architecture for quantum generative adversarial networks (QGANs) and study their robustness in the presence of noise. We devise a simple way of adding different types of noise to the quantum generator circuit, and numerically simulate the noisy hybrid quantum generative adversarial networks (HQGANs) to learn continuous probability distributions, and show that the performance of HQGANs remain unaffected. We also investigate the effect of different parameters on the training time to reduce the computational scaling of the algorithm and simplify its deployment on a quantum computer. We then perform the training on Rigetti's Aspen-4-2Q-A quantum processing unit, and present the results from the training. Our results pave the way for experimental exploration of different quantum machine learning algorithms on noisy intermediate scale quantum devices.