Predicting molecular vibronic spectra using time-domain analog quantum simulation

Abstract

Spectroscopy is one of the most accurate probes of the molecular world. However, predicting molecular spectra accurately is computationally difficult because of the presence of entanglement between electronic and nuclear degrees of freedom. Although quantum computers promise to reduce this computational cost, existing quantum approaches rely on combining signals from individual eigenstates, an approach that is difficult to scale because the number of eigenstates grows exponentially with molecule size. Here, we introduce a method for scalable analog quantum simulation of molecular spectroscopy, by performing simulations in the time domain. Our approach can treat more complicated molecular models than previous ones, requires fewer approximations, and can be extended to open quantum systems with minimal overhead. We present a direct mapping of the underlying problem of time-domain simulation of molecular spectra to the degrees of freedom and control fields available in a trapped-ion quantum simulator. We experimentally demonstrate our algorithm on a trapped-ion device, exploiting both intrinsic electronic and motional degrees of freedom, showing excellent quantitative agreement for a single-mode vibronic photoelectron spectrum of SO${}_2$.

arXiv comment13 pages, 8 figures

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• Experimental Quantum Simulation of Chemical Dynamics
• Simulating open-system molecular dynamics on analog quantum computers
• Simulating Vibrational Dynamics on Bosonic Quantum Devices
• Benchmarking bosonic modes for quantum information with randomized displacements
• Spectral Signatures of Vibronic Coupling in Trapped Cold Ionic Rydberg Systems
• Simulating Non-Markovian Dynamics in Multidimensional Electronic Spectroscopy via Quantum Algorithm
• Refining resource estimation for the quantum computation of vibrational molecular spectra through Trotter error analysis
• Quantum Simulation of Charge and Exciton Transfer in Multi-mode Models using Engineered Reservoirs
• On the Noisy Road to Open Quantum Dynamics: The Place of Stochastic Hamiltonians
• Observation of synchronization between two quantum van der Pol oscillators in trapped ions