Issue 35, 2023

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 whose cost 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, the number of required measurements depends on the desired spectral range and resolution, not molecular size. 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 SO2.

Graphical abstract: Predicting molecular vibronic spectra using time-domain analog quantum simulation

Article information

Article type
Edge Article
Submitted
13 May 2023
Accepted
09 Aug 2023
First published
10 Aug 2023
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY-NC license

Chem. Sci., 2023,14, 9439-9451

Predicting molecular vibronic spectra using time-domain analog quantum simulation

R. J. MacDonell, T. Navickas, T. F. Wohlers-Reichel, C. H. Valahu, A. D. Rao, M. J. Millican, M. A. Currington, M. J. Biercuk, T. R. Tan, C. Hempel and I. Kassal, Chem. Sci., 2023, 14, 9439 DOI: 10.1039/D3SC02453A

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