Scalable Quantum Monte Carlo with Direct-Product Trial Wave Functions.

The computational demand posed by applying multi-Slater determinant trials in phaseless auxiliary-field quantum Monte Carlo methods (MSD-AFQMC) is particularly significant for molecules exhibiting strong correlations. Here, we propose using direct-product wave functions as trials for MSD-AFQMC, aiming to reduce computational overhead by leveraging the compactness of multi-Slater determinant trials in direct-product form (DP-MSD). This efficiency arises when the active space can be divided into noncoupling subspaces, a condition we term "decomposable active space". By employing localized-active space self-consistent field wave functions as an example of such trials, we demonstrate our proposed approach across a range of molecular systems, each exhibiting varying degrees of complexity in their electronic structures. Our findings indicate that the compact DP-MSD trials can reduce computational costs substantially, by up to 36 times for the C2H6N4 molecule where the two double bonds between nitrogen N=N are clearly separated by a C-C single bond, while maintaining accuracy when active spaces are decomposable. In the case of larger systems such as the benzene dimer, characterized by weak coupling between the two monomers, we observed a decrease in computational cost compared to using a complete active space trial, yet we retained the same level of accuracy. However, for systems where these active subspaces strongly couple, a scenario we refer to as "strong subspace coupling", the method's accuracy decreases compared to that achieved with a complete active space approach. We anticipate that our method will be beneficial for systems with noncoupling to weakly coupling subspaces that require local multireference treatments.

A Nonstochastic Optimization Algorithm for Neural-Network Quantum States.

Neural-network quantum states (NQS) employ artificial neural networks to encode many-body wave functions in a second quantization through variational Monte Carlo (VMC). They have recently been applied to accurately describe electronic wave functions of molecules and have shown the challenges in efficiency compared with traditional quantum chemistry methods. Here, we introduce a general nonstochastic optimization algorithm for NQS in chemical systems, which deterministically generates a selected set of important configurations simultaneously with energy evaluation of NQS. This method bypasses the need for Markov-chain Monte Carlo within the VMC framework, thereby accelerating the entire optimization process. Furthermore, this newly developed nonstochastic optimization algorithm for NQS offers comparable or superior accuracy compared to its stochastic counterpart and ensures more stable convergence. The application of this model to test molecules exhibiting strong electron correlations provides further insight into the performance of NQS in chemical systems and opens avenues for future enhancements.

Circuit-Depth Reduction of Unitary-Coupled-Cluster Ansatz by Energy Sorting.

Quantum computation represents a revolutionary approach to solving problems in quantum chemistry. However, due to the limited quantum resources in the current noisy intermediate-scale quantum (NISQ) devices, quantum algorithms for large chemical systems remain a major task. In this work, we demonstrate that the circuit depth of the unitary coupled cluster (UCC) and UCC-based ansatzes in the algorithm of the variational quantum eigensolver can be significantly reduced by an energy-sorting strategy. Specifically, subsets of excitation operators are first prescreened from the operator pool according to its contribution to the total energy. The quantum circuit ansatz is then iteratively constructed until convergence of the final energy to a typical accuracy. For demonstration, this method has been successfully applied to molecular and periodic systems. Particularly, a reduction of 50%-98% in the number of operators is observed while retaining the accuracy of the original UCCSD operator pools. This method can be straightforwardly extended to general parametric variational ansatzes.

Efficient Quantum Imaginary Time Evolution by Drifting Real-Time Evolution: An Approach with Low Gate and Measurement Complexity.

Quantum imaginary time evolution (QITE) is one of the promising candidates for finding the eigenvalues and eigenstates of a Hamiltonian on a quantum computer. However, the original proposal suffers from large circuit depth and measurements due to the size of the Pauli operator pool and Trotterization. To alleviate the requirement for deep circuits, we propose a time-dependent drifting scheme inspired by the qDRIFT algorithm [Campbell, E. Phys. Rev. Lett. 2019, 123, 070503]. We show that this drifting scheme removes the depth dependency on the size of the operator pool and converges inversely with respect to the number of steps. We further propose a deterministic algorithm that selects the dominant Pauli term to reduce the fluctuation for the ground state preparation. We also introduce an efficient measurement reduction scheme across Trotter steps that removes its cost dependence on the number of iterations. We analyze the main source of error for our scheme both theoretically and numerically. We numerically test the validity of depth reduction, convergence performance of our algorithms, and the faithfulness of the approximation for our measurement reduction scheme on several benchmark molecules. In particular, the results on the LiH molecule give circuit depths comparable to that of the advanced adaptive variational quantum eigensolver (VQE) methods while requiring much fewer measurements.

Toward practical quantum embedding simulation of realistic chemical systems on near-term quantum computers.

Quantum computing has recently exhibited great potential in predicting chemical properties for various applications in drug discovery, material design, and catalyst optimization. Progress has been made in simulating small molecules, such as LiH and hydrogen chains of up to 12 qubits, by using quantum algorithms such as variational quantum eigensolver (VQE). Yet, originating from the limitations of the size and the fidelity of near-term quantum hardware, the accurate simulation of large realistic molecules remains a challenge. Here, integrating an adaptive energy sorting strategy and a classical computational method-the density matrix embedding theory, which respectively reduces the circuit depth and the problem size, we present a means to circumvent the limitations and demonstrate the potential of near-term quantum computers toward solving real chemical problems. We numerically test the method for the hydrogenation reaction of C6H8 and the equilibrium geometry of the C18 molecule, using basis sets up to cc-pVDZ (at most 144 qubits). The simulation results show accuracies comparable to those of advanced quantum chemistry methods such as coupled-cluster or even full configuration interaction, while the number of qubits required is reduced by an order of magnitude (from 144 qubits to 16 qubits for the C18 molecule) compared to conventional VQE. Our work implies the possibility of solving industrial chemical problems on near-term quantum devices.

NOON States of Nine Quantized Vibrations in Two Radial Modes of a Trapped Ion.

We develop a deterministic method to generate and verify arbitrarily high NOON states of quantized vibrations (phonons), through the coupling to the internal state. We experimentally create the entangled states up to N=9 phonons in two vibrational modes of a single trapped ^{171}Yb^{+} ion. We observe an increasing phase sensitivity of the generated NOON state as the number of phonons N increases and obtain the fidelity from the contrast of the phase interference and the population of the phonon states through the two-mode projective measurement, which are significantly above the classical bound. We also measure the quantum Fisher information of the generated state and observe Heisenberg scaling in the lower bounds of phase sensitivity as N increases. Our scheme is generic and applicable to other photonic or phononic systems such as circuit QED systems or nanomechanical oscillators, which have Jaynes-Cummings-type of interactions.

Shortcuts to adiabaticity by counterdiabatic driving for trapped-ion displacement in phase space.

The application of adiabatic protocols in quantum technologies is severely limited by environmental sources of noise and decoherence. Shortcuts to adiabaticity by counterdiabatic driving constitute a powerful alternative that speed up time-evolution while mimicking adiabatic dynamics. Here we report the experimental implementation of counterdiabatic driving in a continuous variable system, a shortcut to the adiabatic transport of a trapped ion in phase space. The resulting dynamics is equivalent to a 'fast-motion video' of the adiabatic trajectory. The robustness of this protocol is shown to surpass that of competing schemes based on classical local controls and Fourier optimization methods. Our results demonstrate that shortcuts to adiabaticity provide a robust speedup of quantum protocols of wide applicability in quantum technologies.

Phonon arithmetic in a trapped ion system.

Single-quantum level operations are important tools to manipulate a quantum state. Annihilation or creation of single particles translates a quantum state to another by adding or subtracting a particle, depending on how many are already in the given state. The operations are probabilistic and the success rate has yet been low in their experimental realization. Here we experimentally demonstrate (near) deterministic addition and subtraction of a bosonic particle, in particular a phonon of ionic motion in a harmonic potential. We realize the operations by coupling phonons to an auxiliary two-level system and applying transitionless adiabatic passage. We show handy repetition of the operations on various initial states and demonstrate by the reconstruction of the density matrices that the operations preserve coherences. We observe the transformation of a classical state to a highly non-classical one and a Gaussian state to a non-Gaussian one by applying a sequence of operations deterministically.

Testing nonclassicality and non-gaussianity in phase space.

We theoretically propose and experimentally demonstrate a nonclassicality test of a single-mode field in phase space, which has an analogy with the nonlocality test proposed by Banaszek and Wódkiewicz [Phys. Rev. Lett. 82, 2009 (1999)]. Our approach to deriving the classical bound draws on the fact that the Wigner function of a coherent state is a product of two independent distributions as if the orthogonal quadratures (position and momentum) in phase space behave as local realistic variables. Our method detects every pure nonclassical Gaussian state, which can also be extended to mixed states. Furthermore, it sets a bound for all Gaussian states and their mixtures, thereby providing a criterion to detect a genuine quantum non-Gaussian state. Remarkably, our phase-space approach with invariance under Gaussian unitary operations leads to an optimized test for a given non-Gaussian state. We experimentally show how this enhanced method can manifest quantum non-Gaussianity of a state by simply choosing phase-space points appropriately, which is essentially equivalent to implementing a squeezing operation on a given state.