Extending GPU-accelerated Gaussian integrals in the TeraChem software package to f type orbitals: Implementation and applications.

The increasing availability of graphics processing units (GPUs) for scientific computing has prompted interest in accelerating quantum chemical calculations through their use. However, the complexity of integral kernels for high angular momentum basis functions often limits the utility of GPU implementations with large basis sets or for metal containing systems. In this work, we report the implementation of f function support in the GPU-accelerated TeraChem software package through the development of efficient kernels for the evaluation of Hamiltonian integrals.

Graph-|⟩⟨|: A Quantum Algorithm with Reduced Quantum Circuit Depth for Electronic Structure.

The accurate determination of chemical properties is known to have a critical impact on multiple fundamental chemical problems but is deeply hindered by the steep algebraic scaling of electron correlation calculations and the exponential scaling of quantum nuclear dynamics. With the advent of new quantum computing hardware and associated developments in creating new paradigms for quantum software, this avenue has been recognized as perhaps one way to address exponentially complex challenges in quantum chemistry and molecular dynamics. In this paper, we discuss a new approach to drastically reduce the quantum circuit depth (by several orders of magnitude) and help improve the accuracy in the quantum computation of electron correlation energies for large molecular systems.

Graph-|⟩⟨|, a Graph-Based Quantum/Classical Algorithm for Efficient Electronic Structure on Hybrid Quantum/Classical Hardware Systems: Improved Quantum Circuit Depth Performance.

We present a procedure to reduce the depth of quantum circuits and improve the accuracy of results in computing post-Hartree-Fock electronic structure energies in large molecular systems. The method is based on molecular fragmentation where a molecular system is divided into overlapping fragments through a graph-theoretic procedure. This allows us to create a set of projection operators that decompose the unitary evolution of the full system into separate sets of processes, some of which can be treated on quantum hardware and others on classical hardware.

Weighted-Graph-Theoretic Methods for Many-Body Corrections within ONIOM: Smooth AIMD and the Role of High-Order Many-Body Terms.

We present a weighted-graph-theoretic approach to adaptively compute contributions from many-body approximations for smooth and accurate post-Hartree-Fock (pHF) molecular dynamics (AIMD) of highly fluxional chemical systems. This approach is ONIOM-like, where the full system is treated at a computationally feasible quality of treatment (density functional theory (DFT) for the size of systems considered in this publication), which is then improved through a perturbative correction that captures local many-body interactions up to a certain order within a higher level of theory (post-Hartree-Fock in this publication) described through graph-theoretic techniques. Due to the fluxional and dynamical nature of the systems studied here, these graphical representations evolve during dynamics.