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Physical Review A

Molecular emission tomography of anharmonic vibrations

Leon J. Waxer, Ian A. Walmsley, W. Vogel

Published Oct 1, 1997• 18 citations
Publisher

Abstract

We describe a method for the determination of the quantum state of molecular vibrations in a regime where the anharmonicities are significant. The method is based on the direct analysis of the observed time-resolved spectrum of resonance fluorescence of the molecular sample.
DOI
10.1103/physreva.56.r2491

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Using a photonic quantum computer for boson sampling has demonstrated a tremendous advantage over classical supercomputers. It is highly desirable to develop boson sampling algorithms for realistic scientific problems. In this work, we propose a hybrid quantum-classical sampling (HQCS) algorithm to calculate the optical spectrum for complex molecules considering Duschinsky rotation effects and anharmonicity. The classical sum-over-states method for this problem has a computational complexity that exponentially increases with system size. The HQCS algorithm creates an intermediate harmonic potential energy surface (PES) to bridge the initial and final PESs. The magnitude and sign of the overlap between the initial and the intermediate state are estimated by boson sampling and classical algorithms, respectively. The overlap between the intermediate and the final state is efficiently evaluated by classical algorithms. The feasibility of HQCS is demonstrated in calculations of the emission spectrum of a Morse model as well as the pyridine molecule.