Basis Set Generation and Optimization in the NISQ Era with Quiqbox.jl.

In the noisy intermediate-scale quantum era, ab initio computation of electronic structure problems has become one of the major benchmarks for identifying the boundary between classical and quantum computational power. Basis sets play a key role in the electronic structure methods implemented on both classical and quantum devices. To investigate the consequences of single-particle basis sets, we propose a framework for more customizable basis set generation and optimization. This framework allows composite basis sets to go beyond typical basis set frameworks, such as atomic basis sets, by introducing the concept of mixed-contracted Gaussian-type orbitals. These basis set generations set the stage for more flexible variational optimization of basis set parameters. To realize this framework, we have developed an open-source software package named "Quiqbox" in the Julia programming language. We demonstrate various examples of using Quiqbox for basis set optimization and generation, ranging from optimizing atomic basis sets on the Hartree-Fock level, preparing the initial state for variational quantum eigensolver computation, and constructing basis sets with completely delocalized orbitals. We also include various benchmarks of Quiqbox for basis set optimization and ab initial electronic structure computation.

Solver for the Electronic V-Representation Problem of Time-Dependent Density Functional Theory.

One route to numerically propagating quantum systems is time-dependent density functional theory (TDDFT). The application of TDDFT to a particular system's time evolution is predicated on V-representability, which we have analyzed in a previous publication. Here, we describe a newly developed solver for the scalar time-dependent Kohn-Sham potential. We present and interpret the force-balance equation central to our numerical method, describe details of its implementation, and present illustrative numerical results for one- and two-electron systems in both one-dimensional and three-dimensional grids. Innovations of our numerical implementation include the use of preconditioning when inverting the force-balance matrix and an improved propagation method obtaining the Kohn-Sham potential self-consistently at each step of the propagation. A new characterization of V-representability for one-electron systems is also included, along with possible improvements and future directions.

Reducing Qubit Requirements for Quantum Simulations Using Molecular Point Group Symmetries.

Simulating molecules is believed to be one of the early stage applications for quantum computers. Current state-of-the-art quantum computers are limited in size and coherence; therefore, optimizing resources to execute quantum algorithms is crucial. In this work, we develop the second quantization representation of spatial symmetries, which are then transformed to their qubit operator representation. These qubit operator representations are used to reduce the number of qubits required for simulating molecules. We present our results for various molecules and elucidate a formal connection of this work with a previous technique that analyzed generic Z2 Pauli symmetries.

Bravyi-Kitaev Superfast simulation of electronic structure on a quantum computer.

Present quantum computers often work with distinguishable qubits as their computational units. In order to simulate indistinguishable fermionic particles, it is first required to map the fermionic state to the state of the qubits. The Bravyi-Kitaev Superfast (BKSF) algorithm can be used to accomplish this mapping. The BKSF mapping has connections to quantum error correction and opens the door to new ways of understanding fermionic simulation in a topological context. Here, we present the first detailed exposition of the BKSF algorithm for molecular simulation. We provide the BKSF transformed qubit operators and report on our implementation of the BKSF fermion-to-qubits transform in OpenFermion. In this initial study of a hydrogen molecule we have compared BKSF, Jordan-Wigner, and Bravyi-Kitaev transforms under the Trotter approximation. The gate count to implement BKSF is lower than Jordan-Wigner but higher than Bravyi-Kitaev. We considered different orderings of the exponentiated terms and found lower Trotter errors than the previously reported for Jordan-Wigner and Bravyi-Kitaev algorithms. These results open the door to the further study of the BKSF algorithm for quantum simulation.

Quantum Simulation of Helium Hydride Cation in a Solid-State Spin Register.

Ab initio computation of molecular properties is one of the most promising applications of quantum computing. While this problem is widely believed to be intractable for classical computers, efficient quantum algorithms exist which have the potential to vastly accelerate research throughput in fields ranging from material science to drug discovery. Using a solid-state quantum register realized in a nitrogen-vacancy (NV) defect in diamond, we compute the bond dissociation curve of the minimal basis helium hydride cation, HeH(+). Moreover, we report an energy uncertainty (given our model basis) of the order of 10(-14) hartree, which is 10 orders of magnitude below the desired chemical precision. As NV centers in diamond provide a robust and straightforward platform for quantum information processing, our work provides an important step toward a fully scalable solid-state implementation of a quantum chemistry simulator.

Quantum transport enhancement by time-reversal symmetry breaking.

Quantum mechanics still provides new unexpected effects when considering the transport of energy and information. Models of continuous time quantum walks, which implicitly use time-reversal symmetric Hamiltonians, have been intensely used to investigate the effectiveness of transport. Here we show how breaking time-reversal symmetry of the unitary dynamics in this model can enable directional control, enhancement, and suppression of quantum transport. Examples ranging from exciton transport to complex networks are presented. This opens new prospects for more efficient methods to transport energy and information.

Solving quantum ground-state problems with nuclear magnetic resonance.

Quantum ground-state problems are computationally hard problems for general many-body Hamiltonians; there is no classical or quantum algorithm known to be able to solve them efficiently. Nevertheless, if a trial wavefunction approximating the ground state is available, as often happens for many problems in physics and chemistry, a quantum computer could employ this trial wavefunction to project the ground state by means of the phase estimation algorithm (PEA). We performed an experimental realization of this idea by implementing a variational-wavefunction approach to solve the ground-state problem of the Heisenberg spin model with an NMR quantum simulator. Our iterative phase estimation procedure yields a high accuracy for the eigenenergies (to the 10⁻5 decimal digit). The ground-state fidelity was distilled to be more than 80%, and the singlet-to-triplet switching near the critical field is reliably captured. This result shows that quantum simulators can better leverage classical trial wave functions than classical computers.

Simulating chemistry using quantum computers.

The difficulty of simulating quantum systems, well known to quantum chemists, prompted the idea of quantum computation. One can avoid the steep scaling associated with the exact simulation of increasingly large quantum systems on conventional computers, by mapping the quantum system to another, more controllable one. In this review, we discuss to what extent the ideas in quantum computation, now a well-established field, have been applied to chemical problems. We describe algorithms that achieve significant advantages for the electronic-structure problem, the simulation of chemical dynamics, protein folding, and other tasks. Although theory is still ahead of experiment, we outline recent advances that have led to the first chemical calculations on small quantum information processors.