Coherent State Preparation and Observation of Rabi Oscillations in a Single Molecule

TL;DR

This paper demonstrates the coherent control of a single molecule's electronic states using laser pulses, achieving Rabi oscillations with minimal photon numbers, advancing quantum manipulation techniques.

Contribution

It presents the first observation of Rabi oscillations in a single molecule with few-photon excitation, showing potential for quantum control at the molecular level.

Findings

Pi-pulse excitation with 500 photons

Observation of 5 Rabi cycles

Agreement with theoretical models

Abstract

We report on the excitation of single molecules via narrow zero-phonon transitions using short laser pulses. By monitoring the Stokes-shifted fluorescence, we studied the excited state population as a function of the delay time, laser intensity, and frequency detuning. A pi-pulse excitation was demonstrated with merely 500 photons, and 5 Rabi cycles were achieved at higher excitation powers. Our findings are in good agreement with theoretical calculations and provide a first step toward coherent manipulation of the electronic states of single molecules with few photons.