We propose an orbital optimized method for unitary coupled cluster theory (OO-UCC) within the variational quantum eigensolver (VQE) framework for quantum computers. OO-UCC variationally determines the coupled cluster amplitudes and also molecular orbital coefficients. Owing to its fully variational nature, first-order properties are readily available. This feature allows the optimization of molecular structures in VQE without solving any additional equations. Furthermore, the method requires smaller active space and shallower quantum circuit than UCC to achieve the same accuracy. We present numerical examples of OO-UCC using quantum simulators, which include the geometry optimization of the water molecule.

The Green's function plays a crucial role when studying the nature of quantum many-body systems, especially strongly-correlated systems. Although the development of quantum computers in the near future may enable us to compute energy spectra of classically-intractable systems, methods to simulate the Green's function with near-term quantum algorithms have not been proposed yet. Here, we propose two methods to calculate the Green's function of a given Hamiltonian on near-term quantum computers. The first one makes use of a variational dynamics simulation of quantum systems and computes the dynamics of the Green's function in real time directly. The second one utilizes the Lehmann representation of the Green's function and a method which calculates excited states of the Hamiltonian. Both methods require shallow quantum circuits and are compatible with near-term quantum computers. We numerically simulated the Green's function of the Fermi-Hubbard model and demonstrated the validity of our proposals.

We propose a quantum-classical hybrid algorithm to simulate the non-equilibrium steady state of an open quantum many-body system, named the dissipative-system Variational Quantum Eigensolver (dVQE). To employ the variational optimization technique for a unitary quantum circuit, we map a mixed state into a pure state with a doubled number of qubits and design the unitary quantum circuit to fulfill the requirements for a density matrix. This allows us to define a cost function that consists of the time evolution generator of the quantum master equation. Evaluation of physical observables is, in turn, carried out by a quantum circuit with the original number of qubits. We demonstrate our dVQE scheme by both numerical simulation on a classical computer and actual quantum simulation that makes use of the device provided in Rigetti Quantum Cloud Service.

Quantum simulation is one of the key applications of quantum computing, which can accelerate research and development in chemistry, material science, etc. Here, we propose an efficient method to simulate the time evolution driven by a static Hamiltonian, named subspace variational quantum simulator (SVQS). SVQS employs the subspace-search variational eigensolver (SSVQE) to find a low-energy subspace and further extends it to simulate dynamics within the low-energy subspace. More precisely, using a parameterized quantum circuit, the low-energy subspace of interest is encoded into a computational subspace spanned by a set of computational basis, where information processing can be easily done. After the information processing, the computational subspace is decoded to the original low-energy subspace. This allows us to simulate the dynamics of low-energy subspace with lower overhead compared to existing schemes. While the dimension is restricted for feasibility on near-term quantum devices, the idea is similar to quantum phase estimation and its applications such as quantum linear system solver and quantum metropolis sampling. Because of this simplicity, we can successfully demonstrate the proposed method on the actual quantum device using Regetti Quantum Cloud Service. Furthermore, we propose a variational initial state preparation for SVQS, where the initial states are searched from the simulatable eigensubspace. Finally, we demonstrate SVQS on Rigetti Quantum Cloud Service.

We propose a sequential minimal optimization method for quantum-classical hybrid algorithms, which converges faster, robust against statistical error, and hyperparameter-free. Specifically, the optimization problem of the parameterized quantum circuits is divided into solvable subproblems by considering only a subset of the parameters. In fact, if we choose a single parameter, the cost function becomes a simple sine curve with period 2π, and hence we can exactly minimize with respect to the chosen parameter. Furthermore, even in general cases, the cost function is given by a simple sum of trigonometric functions with certain periods and hence can be minimized by using a classical computer. By repeatedly performing this procedure, we can optimize the parameterized quantum circuits so that the cost function becomes as small as possible. We perform numerical simulations and compare the proposed method with existing gradient-free and gradient-based optimization algorithms. We find that the proposed method substantially outperforms the existing optimization algorithms and converges to a solution almost independent of the initial choice of the parameters. This accelerates almost all quantum-classical hybrid algorithms readily and would be a key tool for harnessing near-term quantum devices.

The variational quantum eigensolver (VQE) and its variants, which is a method for finding eigenstates and eigenenergies of a given Hamiltonian, are appealing applications of near-term quantum computers. Although the eigenenergies are certainly important quantities which determines properties of a given system, their derivatives with respect to parameters of the system, such as positions of nuclei if we target a quantum chemistry problem, are also crucial to analyze the system. Here, we describe methods to evaluate analytical derivatives of the eigenenergy of a given Hamiltonian, including the excited state energy as well as the ground state energy, with respect to the system parameters in the framework of the VQE. We give explicit, low-depth quantum circuits which can measure essential quantities to evaluate energy derivatives, incorporating with proof-of-principle numerical simulations. This work extends the theory of the variational quantum eigensolver, by enabling it to measure more physical properties of a quantum system than before and to perform the geometry optimization of a molecule.