Simulating thermal-equilibrium properties at finite temperature plays a crucial role in studying the nature of quantum many-body systems. In particular, implementing a finite-temperature simulation on a quantum computer is expected to overcome the difficulty in simulating large-sized systems, for which the quantum Monte-Carlo technique on a classical computer suffers from the sign problem in general. While several methods suitable for fault-tolerant quantum computing (FTQC) devices are expected to be useful in studying large-scale quantum many-body systems, those proposed so far involve a large number of ancilla qubits and a deep quantum circuit with many basic gates, making them unsuitable for the early-FTQC era, i.e., the early stage of the FTQC era, at which only a limited number of qubits and quantum gates are available. In this paper, we propose a method suitable for quantum devices in this early stage to calculate the thermal-equilibrium expectation value of an observable at finite temperature. Our proposal, named the Markov-chain Monte Carlo with sampled-pairs of unitaries (MCMC-SPU) algorithm, is based on sampling simple quantum circuits and generating the corresponding statistical ensembles, and overcomes the difficulties in the resource requirements and the decay in probability associated with postselection of measurement outcomes on ancilla qubits. We demonstrate the validity of our proposal by performing a numerical simulation of the MCMC-SPU algorithm on the one-dimensional transverse-field Ising model as an illustrative example.

Simulation of quantum many-body systems is a promising application of quantum computers. However, implementing the time-evolution operator as a quantum circuit efficiently on near-term devices with limited resources is challenging. Standard approaches like Trotterization often require deep circuits, making them impractical. This paper proposes a hybrid quantum-classical algorithm called Local Subspace Variational Quantum Compilation (LSVQC) for compiling the time-evolution operator. The LSVQC uses variational optimization to reproduce the action of the target time-evolution operator within a physically reasonable subspace. Optimization is performed on small local subsystems based on the Lieb-Robinson bound, allowing for cost function evaluation using small-scale quantum devices or classical computers. Numerical simulations on a spin-lattice model and an ab initio effective model of strongly correlated material Sr2CuO3 demonstrate the algorithm's effectiveness. It is shown that the LSVQC achieves a 95% reduction in circuit depth compared to Trotterization while maintaining accuracy. The subspace restriction also reduces resource requirements and improves accuracy. Furthermore, we estimate the gate count needed to execute the quantum simulations using the LSVQC on near-term quantum computing architectures in the noisy intermediate-scale or early fault-tolerant quantum computing era. Our estimation suggests that the acceptable physical gate error rate for the LSVQC can be significantly larger than for Trotterization.

We present a quantum-classical hybrid algorithm for calculating the ground state and its energy of the quantum many-body Hamiltonian by proposing an adaptive construction of a quantum state for the quantum-selected configuration interaction (QSCI) method. QSCI allows us to select important electronic configurations in the system to perform CI calculation (subspace diagonalization of the Hamiltonian) by sampling measurement for a proper input quantum state on a quantum computer, but how we prepare a desirable input state has remained a challenge. We propose an adaptive construction of the input state for QSCI in which we run QSCI repeatedly to grow the input state iteratively. We numerically illustrate that our method, dubbed ADAPT-QSCI, can yield accurate ground-state energies for small molecules, including a noisy situation for eight qubits where error rates of two-qubit gates and the measurement are both as large as 1%. ADAPT-QSCI serves as a promising method to take advantage of current noisy quantum devices and pushes forward its application to quantum chemistry.

Quantum batteries are predicted to have the potential to outperform their classical counterparts and are therefore an important element in the development of quantum technologies. In this work we simulate the charging process and work extraction of many-body quantum batteries on noisy-intermediate scale quantum (NISQ) devices, and devise the Variational Quantum Ergotropy (VQErgo) algorithm which finds the optimal unitary operation that maximises work extraction from the battery. We test VQErgo by calculating the ergotropy of a quantum battery undergoing transverse field Ising dynamics. We investigate the battery for different system sizes and charging times and analyze the minimum required circuit depth of the variational optimization using both ideal and noisy simulators. Finally, we optimize part of the VQErgo algorithm and calculate the ergotropy on one of IBM's quantum devices.

Understanding and predicting the properties of solid-state materials from first-principles has been a great challenge for decades. Owing to the recent advances in quantum technologies, quantum computations offer a promising way to achieve this goal. Here, we demonstrate the first-principles calculation of a quasiparticle band structure on actual quantum computers. This is achieved by hybrid quantum-classical algorithms in conjunction with qubit-reduction and error-mitigation techniques. Our demonstration will pave the way to practical applications of quantum computers.

Computation of the Green's function is crucial to study the properties of quantum many-body systems such as strongly correlated systems. Although the high-precision calculation of the Green's function is a notoriously challenging task on classical computers, the development of quantum computers may enable us to compute the Green's function with high accuracy even for classically-intractable large-scale systems. Here, we propose an efficient method to compute the real-time Green's function based on the local variational quantum compilation (LVQC) algorithm, which simulates the time evolution of a large-scale quantum system using a low-depth quantum circuit constructed through optimization on a smaller-size subsystem. Our method requires shallow quantum circuits to calculate the Green's function and can be utilized on both near-term noisy intermediate-scale and long-term fault-tolerant quantum computers depending on the computational resources we have. We perform a numerical simulation of the Green's function for the one- and two-dimensional Fermi-Hubbard model up to 4×4 sites lattice (32 qubits) and demonstrate the validity of our protocol compared to a standard method based on the Trotter decomposition. We finally present a detailed estimation of the gate count for the large-scale Fermi-Hubbard model, which also illustrates the advantage of our method over the Trotter decomposition.

The analysis of a chemical reaction along the ground state potential energy surface in conjunction with an unknown spin state is challenging because electronic states must be separately computed several times using different spin multiplicities to find the lowest energy state. However, in principle, the ground state could be obtained with just a single calculation using a quantum computer without specifying the spin multiplicity in advance. In the present work, ground state potential energy curves for PtCO were calculated as a proof-of-concept using a variational quantum eigensolver (VQE) algorithm. This system exhibits a singlet-triplet crossover as a consequence of the interaction between Pt and CO. VQE calculations using a statevector simulator were found to converge to a singlet state in the bonding region, while a triplet state was obtained at the dissociation limit. Calculations performed using an actual quantum device provided potential energies within ±2 kcal/mol of the simulated energies after adopting error mitigation techniques. The spin multiplicities in the bonding and dissociation regions could be clearly distinguished even in the case of a small number of shots. The results of this study suggest that quantum computing can be a powerful tool for the analysis of the chemical reactions of systems for which the spin multiplicity of the ground state and variations in this parameter are not known in advance.

In this paper, we propose a cost-reduced method for finite-temperature molecular dynamics on a near-term quantum computer, Quantum Car-Parrinello molecular dynamics (QCPMD). One of the most promising applications of near-term quantum computers is quantum chemistry. It has been expected that simulations of molecules via molecular dynamics can be also efficiently performed on near-term quantum computers by applying a promising near-term quantum algorithm of the variational quantum eigensolver (VQE). However, this method may demand considerable computational costs to achieve a sufficient accuracy, and otherwise, statistical noise can significantly affect the results. To resolve these problems, we invent an efficient method for molecular time evolution inspired by Car-Parrinello method. In our method, parameters characterizing the quantum state evolve based on equations of motion instead of being optimized. Furthermore, by considering Langevin dynamics, we can make use of the intrinsic statistical noise. As an application of QCPMD, we propose an efficient method for vibrational frequency analysis of molecules in which we can use the results of the molecular dynamics calculated by QCPMD. Numerical experiments show that our method can precisely simulate the Langevin dynamics at the equilibrium state, and we can successfully predict a given molecule's eigen frequencies. Furthermore, in the numerical simulation, our method achieves a substantial cost reduction compared with molecular dynamics using the VQE. Our method achieves an efficient computation without using widely employed method of the VQE. In this sense, we open up a new possibility of molecular dynamics on near-term quantum computers. We expect our results inspire further invention of efficient near-term quantum algorithms for simulation of molecules.

We develop a quantum-classical hybrid algorithm to calculate the analytical second-order derivative of the energy for the orbital-optimized variational quantum eigensolver (OO-VQE), which is a method to calculate eigenenergies of a given molecular Hamiltonian by utilizing near-term quantum computers and classical computers. We show that all quantities required in the algorithm to calculate the derivative can be evaluated on quantum computers as standard quantum expectation values without using any ancillary qubits. We validate our formula by numerical simulations of quantum circuits for computing the polarizability of the water molecule, which is the second-order derivative of the energy with respect to the electric field. Moreover, the polarizabilities and refractive indices of thiophene and furan molecules are calculated as a testbed for possible industrial applications. We finally analyze the error-scaling of the estimated polarizabilities obtained by the proposed analytical derivative versus the numerical one obtained by the finite difference. Numerical calculations suggest that our analytical derivative may require fewer measurements (runs) on quantum computers than the numerical derivative to achieve the same fixed accuracy.

A non-adiabatic nuclear wavepacket dynamics simulation of the H₂O⁺ de-excitation process is performed based on electronic structure calculations using the variational quantum eigensolver. The adiabatic potential energy surfaces and non-adiabatic coupling vectors are computed with algorithms for noisy intermediate-scale quantum devices, and time propagation is simulated with conventional methods for classical computers. The results of non-adiabatic transition dynamics from the B^~ state to A^~ state reproduce the trend reported in previous studies, which suggests that this quantum-classical hybrid scheme may be a useful application for noisy intermediate-scale quantum devices.