Optimization strategies in WAHTOR algorithm for quantum computing empirical ansatz: a comparative study

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 combining 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−1 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 statevector simulators) against a handful of small multi-reference dimer systems and the iron center containing human cancer-relevant protein lysine-specific demethylase 5 (KDM5A).

The variational quantum eigensolver (VQE) is a promising algorithm to demonstrate quantum advantage on near-term noisy-intermediate-scale quantum (NISQ) computers. One central problem of VQE is the effect of noise, especially physical noise, on realistic quantum computers. We systematically study the effect of noise for the VQE algorithm by performing numerical simulations with various local noise models, including amplitude damping, dephasing, and depolarizing noise. We show that the ground state energy will deviate from the exact value as the noise probability increase, and typically, the noise will accumulate as the circuit depth increase. The results suggest that the noisy quantum system can remain entanglement at the noise level of NISQ devices by comparing the VQE solution with the mean-field solution for the many-body ground state problem. We build a noise model to capture the noise in a real quantum computer, and the corresponding numerical simulation is consistent with experimental results on IBM Quantum computers through cloud. Our work sheds new light on the practical research of noisy VQE, and the deep understanding of the noise effect of VQE will also help develop error mitigation techniques on near-term quantum computers.

The variational quantum eigensolver is a promising way to solve the Schrödinger equation on a noisy intermediate-scale quantum (NISQ) computer, while its success relies on a well-designed wave function ansatz. Inspired by the quantum neural network, we propose a new hardware heuristic ansatz where its expressibility can be improved by increasing either the depth or the width of the circuit. Such a character makes this ansatz adaptable to different hardware environments. More importantly, it provides a general framework to improve the efficiency of the quantum resource utilization. For example, on a superconducting quantum computer where circuit depth is usually the bottleneck and the qubits thus cannot be fully used, circuit depth can be significantly reduced by introducing ancilla qubits. Ancilla qubits also make the circuit less sensitive to noises in practical application. These results open a new avenue to develop practical applications of quantum computation in the NISQ era.

Materials simulations involving strongly correlated electrons pose fundamental challenges to state‐of‐the‐art electronic structure methods but are hypothesized to be the ideal use case for quantum computing algorithms. To date, no quantum computer has simulated a molecule of a size and complexity relevant to real‐world applications, despite the fact that the variational quantum eigensolver (VQE) algorithm can predict chemically accurate total energies. Nevertheless, because of the many applications of moderately sized, strongly correlated systems, such as molecular catalysts, the successful use of the VQE stands as an important waypoint in the advancement toward useful chemical modeling on near‐term quantum processors. In this paper, we take a significant step in this direction. We lay out the steps, write, and run parallel code for an (emulated) quantum computer to compute the bond dissociation curves of the TiH, LiH, NaH, and KH diatomic hydride molecules using the VQE. TiH was chosen as a relatively simple chemical system that incorporates d orbitals and strong electron correlation. Because current VQE implementations on existing quantum hardware are limited by qubit error rates, the number of qubits available, and the allowable gate depth, recent studies using it have focused on chemical systems involving s and p block elements. Through VQE + UCCSD calculations of TiH, we evaluate the near‐term feasibility of modeling a molecule with d‐orbitals on real quantum hardware. We demonstrate that the inclusion of d‐orbitals and the use of the UCCSD ansatz, which are both necessary to capture the correct TiH physics, dramatically increase the cost of this problem. We estimate the approximate error rates necessary to model TiH on current quantum computing hardware using VQE + UCCSD and show them to likely be prohibitive until significant improvements in hardware and error correction algorithms are available.

The Variational Quantum Eigensolver (VQE) is a method of choice to solve the electronic structure problem for molecules on near-term gate-based quantum computers. However, the circuit depth is expected to grow significantly with problem size. Increased depth can both degrade the accuracy of the results and reduce trainability. In this work, we propose a novel approach to reduce ansatz circuit depth. Our approach, called PermVQE, adds an additional optimization loop to VQE that permutes qubits in order to solve for the qubit Hamiltonian that minimizes long-range correlations in the ground state. The choice of permutations is based on mutual information, which is a measure of interaction between electrons in spin-orbitals. Encoding strongly interacting spin-orbitals into proximal qubits on a quantum chip naturally reduces the circuit depth needed to prepare the ground state. For representative molecular systems, LiH, H$_2$, (H$_2$)$_2$, H$_4$, and H$_3^+$, we demonstrate for linear qubit connectivity that placing entangled qubits in close proximity leads to shallower depth circuits required to reach a given eigenvalue-eigenvector accuracy. This approach can be extended to any qubit connectivity and can significantly reduce the depth required to reach a desired accuracy in VQE. Moreover, our approach can be applied to other variational quantum algorithms beyond VQE.

The variational quantum eigensolver (VQE) stands as a prominent quantum-classical hybrid algorithm for near-term quantum computers to obtain the ground states of molecular Hamiltonians in quantum chemistry. However, due to the noncommutativity of the Pauli operators in the Hamiltonian, the number of measurements required on quantum computers increases significantly as the system size grows, which may hinder practical applications of VQE. In this work, we present a protocol termed (JBM-VQE) to reduce the number of measurements and speed up the VQE algorithm. Our method employs joint Bell measurements, enabling the simultaneous measurement of the absolute values of all expectation values of Pauli operators present in the Hamiltonian. In the course of the optimization, JBM-VQE estimates the absolute values of the expectation values of the Pauli operators for each iteration by the joint Bell measurement, while the signs of them are measured less frequently by the conventional method to measure the expectation values. Our approach is based on the empirical observation that the signs do not often change during optimization. We illustrate the speed-up of JBM-VQE compared to conventional VQE by numerical simulations for finding the ground states of molecular Hamiltonians of small molecules, and the speed-up of JBM-VQE at the early stage of the optimization becomes increasingly pronounced in larger systems. Our approach based on the joint Bell measurement is not limited to VQE and can be utilized in various quantum algorithms whose cost functions are expectation values of many Pauli operators. Published by the American Physical Society 2024

The possibility of adopting quantum computing in the field of financial services can bring a new breakthrough in portfolio management since the optimization of this method requires large numbers for the solution that exceed the capabilities of classical computing algorithms. This study focuses on using a hybrid quantum-classical computational method known as the Variational Quantum Eigensolver (VQE) in optimizing portfolio selection. The VQE aims at finding the best allocation of the portfolio; the best weights that correspond to minimum risk and maximum return as predicted by the modern portfolio theory. The study assesses the suitability and speed of VQE in solving matters involving portfolio management tasks such as handling vast data and nonlinear constraints which are hard to solve through other optimization methods. Thus, under the theoretical framework of quantum computing, the study seeks to address some of the following challenges: computational time and scalability in portfolio optimization. The VQE algorithm work on different portfolio configurations; their performance in comparison with classical techniques; special attention is paid to the rate of convergence and the achievement of the optimal solution. Based on the results of this work we can conclude that there is a considerable literature on quantum finance and that this field can benefit from utilization of quantum algorithms as a tool to improve decision-making in the financial market. That is why the study proves that quantum optimization techniques, to wit VQE, can provide better solutions when it comes to portfolio management within the sphere of finance.

The variational quantum eigensolver (VQE) algorithm, designed to calculate the energy of molecular ground states on near‐term quantum computers, requires specification of symmetries that describe the system, for example, spin state and number of electrons. This opens the possibility of using VQE to obtain excited states as the lowest‐energy solutions of a given set of symmetries. In this paper, the performances of various unitary coupled cluster (UCC) ansätze applied to VQE calculations on excited states are investigated using quantum circuits designed to represent single reference and multireference wavefunctions to calculate energy curves with respect to variations in the molecular geometry. These ansätze include standard Unitary Coupled Cluster Singles and Doubles (UCCSD), as well as modified versions of Unitary Coupled Cluster Generalized Singles and Doubles (UCCGSD) and k‐UpCCGSD, which are engineered to tackle excited states without undesired spin symmetry crossover to lower states during VQE optimization. These studies are carried out on a range of systems, including H2, H3, H4, NH, OH+, CH2, and , covering examples of spin singlet, doublet, and triplet molecular ground states with single and multireference excited states. In most cases, our calculations are in excellent agreement with results from full‐configuration interaction calculations on classical machines, thus showing that the VQE algorithm is capable of calculating the lowest excited state at a certain symmetry, including multireference closed‐ and open‐shell states, by setting appropriate restrictions on the excitations considered in the cluster operator and appropriate constraints in the qubit register encoding the starting mean field state.

Quantum chemistry is one of the most promising near-term applications of quantum computers. Quantum algorithms such as variational quantum eigen solver (VQE) and variational quantum deflation (VQD) algorithms have been mainly applied for molecular systems and there is a need to implement such methods for periodic solids. Using Wannier tight-binding Hamiltonian (WTBH) approaches, we demonstrate the application of VQE and VQD to accurately predict both electronic and phonon bandstructure properties of several elemental as well as multi-component solid-state materials. We apply VQE–VQD calculations for 307 spin–orbit coupling based electronic WTBHs and 933 finite-difference based phonon WTBHs. Also, we discuss a workflow for using VQD with lattice Green’s function that can be used for solving dynamical mean-field theory problems. The WTBH model solvers can be used for testing other quantum algorithms and models also.

We propose a modification of the Variational Quantum Eigensolver algorithm for electronic structure optimization using quantum computers, named nonunitary Variational Quantum Eigensolver (nu-VQE), in which a nonunitary operator is combined with the original system Hamiltonian leading to a new variational problem with a simplified wave function ansatz. In the present work, as nonunitary operator, we use the Jastrow factor, inspired from classical Quantum Monte Carlo techniques for simulation of strongly correlated electrons. The method is applied to prototypical molecular Hamiltonians for which we obtain accurate ground-state energies with shallower circuits, at the cost of an increased number of measurements. Finally, we also show that this method achieves an important error mitigation effect that drastically improves the quality of the results for VQE optimizations on today's noisy quantum computers. The absolute error in the calculated energy within our scheme is 1 order of magnitude smaller than the corresponding result using traditional VQE methods, with the same circuit depth.

Thanks to the rise of quantum computers, many variations of the variational quantum eigensolver (VQE) have been proposed in recent times. This is a promising development for real quantum algorithms, as the VQE is a promising algorithm that runs on current quantum hardware. However, the popular method of comparing your algorithm versus a classical baseline in a small basis set is not meaningful in the big picture. Moreover, many papers use a different molecular representation or a different quantum computer to test their algorithms such that the used baselines are different between different papers. Thus, it is almost impossible to compare the different algorithms to each other. As a solution, we have built a benchmarking framework to standardize the VQE performance metrics, such that they can be analyzed more easily. Using our framework, any researcher working on the VQE can easily test their own algorithms against previous ones on the leaderboard without the need to reproduce previous work themselves.

Materials design stands to be one of the most promising applications of quantum computing. However, the presence of noise in near-term quantum devices restricts quantum simulations of materials to shallow circuits. In this work, we present circuit-efficient variational quantum eigensolver (VQE) simulations of periodic materials using qubit-encoded wave functions based on Adaptive Derivative-Assembled Pseudo-Trotter (ADAPT) VQE. To iteratively construct accurate wave functions for periodic systems, we introduce operator pools comprising a complete set of anti-Hermitian one- and two-body qubit excitation/flipping operators. Numerical results demonstrate that these qubit-encoded algorithms can accurately predict the ground-state energy of periodic systems while significantly reducing circuit depth compared to Fermion-encoded algorithms. Additionally, we integrate the variance extrapolation technique with ADAPT-VQE algorithms to enhance the accuracy of ground-state energy estimations. This strategy further reduces the required circuit depth, enabling scalable and precise simulations of periodic systems.

Quantum computers offer significant potential for complex system analysis, yet their application in large systems is hindered by limitations such as qubit availability and quantum hardware noise. While the variational quantum eigensolver (VQE) was proposed to address these issues, its scalability remains limited. Many efforts, including new ansätze and Hamiltonian modifications, have been made to overcome these challenges. In this work, we introduced the novel Fragment Molecular Orbital/Variational Quantum Eigensolver (FMO/VQE) algorithm. This method combines the fragment molecular orbital (FMO) approach with VQE and efficiently utilizes qubits for quantum chemistry simulations. Employing the UCCSD ansatz, the FMO/VQE achieved an absolute error of just 0.053 mHa with 8 qubits in a H24\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${{\ ext{H}}}_{24}$$\\end{document} system using the STO-3G basis set, and an error of 1.376 mHa with 16 qubits in a H20\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${{\ ext{H}}}_{20}$$\\end{document} system with the 6-31G basis set. These results indicated a significant advancement in scalability over conventional VQE, maintaining accuracy with fewer qubits. Therefore, our FMO/VQE method exemplifies how integrating fragment-based quantum chemistry with quantum algorithms can enhance scalability, facilitating more complex molecular simulations and aligning with quantum computing advancements.

Currently available quantum processors are noisy intermediate-scale quantum (NISQ) devices. The variational quantum eigensolver (VQE) is an algorithm that is closer to near-term applicability due to lower quantum hardware requirements. In VQE, trial states with variational parameters are prepared by quantum computers, and the optimal parameters are determined by a classical optimizer. This optimization is known to be an NP-hard problem. In this work, we make a comparison between various gradient-free optimizers in terms of approximation ratio and function evaluations. As a result, we find that COBYLA method is the best to find the approximated solution with a lower number of executions of quantum computers.

Finding and probing the ground states of spin lattices, such as the antiferromagnetic Heisenberg model on the kagome lattice (KAFH), is a very challenging problem on classical computers and only possible for relatively small systems. We propose using the variational quantum eigensolver (VQE) to find the ground state of the KAFH on a quantum computer. We find efficient ansatz circuits and show how physically interesting observables can be measured efficiently. To investigate the expressiveness and scaling of our ansatz circuits we used classical, exact simulations of VQE for the KAFH for different lattices ranging from 8 to 24 qubits. We find that the fidelity with the ground state approaches one exponentially in the circuit depth for all lattices considered, except for a 24-qubit lattice with an almost degenerate ground state. We conclude that VQE circuits that are able to represent the ground state of the KAFH on lattices inaccessible to exact diagonalization techniques may be achievable on near-term quantum hardware. However, for large systems, circuits with many variational parameters are needed to achieve high fidelity with the ground state.