TY - JOUR
T1 - Phonon-Induced Optical Dephasing in Single Organic Molecules
AU - Clear, Chloe
AU - Schofield, Ross
AU - Major, Kyle D
AU - Iles-Smith, Jake
AU - Clark, Alex S
AU - Mccutcheon, Dara P S
PY - 2020/4/15
Y1 - 2020/4/15
N2 - We present a joint experiment-theory analysis of the temperature-dependent emission spectra, zero-phonon linewidth, and second-order correlation function of light emitted from a single organic molecule. We observe spectra with a zero-phonon line together with several additional sharp peaks, broad phonon sidebands, and a strongly temperature dependent homogeneous broadening. Our model includes both localized vibrational modes of the molecule and a thermal phonon bath, which we include nonperturbatively, and is able to capture all observed features. For resonant driving we measure Rabi oscillations that become increasingly damped with temperature, which our model naturally reproduces. Our results constitute an essential characterization of the photon coherence of molecules, paving the way to their use in future quantum information applications.
AB - We present a joint experiment-theory analysis of the temperature-dependent emission spectra, zero-phonon linewidth, and second-order correlation function of light emitted from a single organic molecule. We observe spectra with a zero-phonon line together with several additional sharp peaks, broad phonon sidebands, and a strongly temperature dependent homogeneous broadening. Our model includes both localized vibrational modes of the molecule and a thermal phonon bath, which we include nonperturbatively, and is able to capture all observed features. For resonant driving we measure Rabi oscillations that become increasingly damped with temperature, which our model naturally reproduces. Our results constitute an essential characterization of the photon coherence of molecules, paving the way to their use in future quantum information applications.
U2 - 10.1103/PhysRevLett.124.153602
DO - 10.1103/PhysRevLett.124.153602
M3 - Letter (Academic Journal)
C2 - 32357066
VL - 124
JO - Physical Review Letters
JF - Physical Review Letters
SN - 0031-9007
M1 - 153602
ER -