Quantum optical emulation of molecular vibronic spectroscopy using a trapped-ion deviceElectronic supplementary information (ESI) available: Trapped ion implementation of quantum optical operations, an experiment detection scheme, and experimental data error analysis. See DOI: 10.1039/c7sc04602b

Molecules are one of the most demanding quantum systems to be simulated by quantum computers due to their complexity and the emergent role of quantum nature. The recent theoretical proposal of Huh et al. (Nature Photon., 9, 615 (2015)) showed that a multi-photon network with a Gaussian input state can simulate a molecular spectroscopic process. Here, we present the first quantum device that generates a molecular spectroscopic signal with the phonons in a trapped ion system, using SO 2 as an example. In order to perform reliable Gaussian sampling, we develop the essential experimental technology with phonons, which includes the phase-coherent manipulation of displacement, squeezing, and rotation operations with multiple modes in a single realization. The required quantum optical operations are implemented through Raman laser beams. The molecular spectroscopic signal is reconstructed from the collective projection measurements for the two-phonon-mode. Our experimental demonstration will pave the way to large-scale molecular quantum simulations, which are classically intractable, but would be easily verifiable by real molecular spectroscopy. Here, we present the first quantum device that generates a molecular spectroscopic signal with the phonons in a trapped ion system, using SO 2 as an example.