Quantum chemistry simulation of ground- and excited-state properties of the sulfonium cation on a superconducting quantum processor

Abstract

The computational description of correlated electronic structure, and particularly of excited states of many-electron systems, is an anticipated application for quantum devices. An important ramification is to determine the dominant molecular fragmentation pathways in photo-dissociation experiments of light-sensitive compounds, like sulfonium-based photo-acid generators used in photolithography. Here we simulate the static and dynamic electronic structure of the H${}_3$S${}^{+}$ molecule, taken as a minimal model of a triply-bonded sulfur cation, on a superconducting quantum processor of the IBM Falcon architecture. To this end, we generalize a qubit reduction technique termed entanglement forging or EF [A. Eddins et al., Phys. Rev. X Quantum, 3, 010309 (2022)], currently restricted to the evaluation of ground-state energies, to the treatment of molecular properties. While, in a conventional quantum simulation, a qubit represents a spin-orbital, within EF a qubit represents a spatial orbital, reducing the number of required qubits by half. We combine the generalized EF with quantum subspace expansion [W. Colless et al, Phys. Rev. X 8, 011021 (2018)], a technique used to project the time-independent Schrodinger equation for ground and excited states in a subspace. To enable experimental demonstration of this algorithmic workflow, we deploy a sequence of error-mitigation techniques. We compute dipole structure factors and partial atomic charges along the ground- and excited-state potential energy curves, revealing the occurrence of homo- and heterolytic fragmentation. This study is an important step toward the computational description of photo-dissociation on near-term quantum devices, as it can be generalized to other photodissociation processes and naturally extended in different ways to achieve more realistic simulations.

13 pages, 7 figures

References in corpus (13)

• A Grand Unification of Quantum Algorithms
• Scalable mitigation of measurement errors on quantum computers
• Doubling the size of quantum simulators by entanglement forging
• Quantum Solver of Contracted Eigenvalue Equations for Scalable Molecular Simulations on Quantum Computing Devices
• Generalized quantum subspace expansion
• Quantum Filter Diagonalization with Double-Factorized Hamiltonians
• Variational Quantum Computation of Molecular Linear Response Properties on a Superconducting Quantum Processor
• Quantum-Classical Hybrid Algorithm for the Simulation of All-Electron Correlation
• N-electron valence perturbation theory with reference wavefunctions from quantum computing: application to the relative stability of hydroxide anion and hydroxyl radical
• Quantum simulation of molecules in solution
• Spectral Functions from Auxiliary-Field Quantum Monte Carlo without Analytic Continuation: The Extended Koopmans' Theorem Approach
• Entanglement Forging with generative neural network models
• Say NO to Optimization: A Non-Orthogonal Quantum Eigensolver

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