TY - JOUR

T1 - Detuning Dependent Rabi Oscillations of a Single Molecule

AU - Rezai, Mohammad

AU - Wrachtrup, Jörg

AU - Gerhardt, Ilja

N1 - Publisher Copyright: © 2019 The Author(s). Published by IOP Publishing Ltd on behalf of the Institute of Physics and Deutsche Physikalische Gesellschaft.

PY - 2019/4/26

Y1 - 2019/4/26

N2 - A single organic dye molecule at cryogenic conditions is resonantly excited in a confocal microscope. Under strong laser illumination it undergoes Rabi oscillations. Mathematically, this is well described and it has been experimentally implemented. These oscillations can be measured as side-bands on their resonance fluorescence, e.g. in the Mollow-Triplet. An alternative method is to research this effect by an analysis of the single molecule anti-bunched photon statistics. This has been performed in this work. Here we research on the detuning dependence of this signal -- it is experimentally demanding since the utilized laser might drift or single emitters are not necessarily spectral stable enough, such that the spectrum can be measured indefinitely. We therefore apply a measurement technique in which the photon correlation signal is acquired in detuning dependent steps. This is performed by continuous laser sweeps over the single molecule excitation spectrum. A single recording of the anti-bunched photons takes 20 to 50 ms. After approx. 1 hour of repetitive laser detunings a full anti-bunching curve is reconstructed for each spectral position. An alternative technique with 100 ns laser pulses allows to acquire a set of comparable data. Our study is derived from a single dibenzanthanthrene molecule. It emits under resonant excitation more than 380.000 photons per second. Under spectral detuning, Rabi-oscillations are observed up to Rabi=2 Pi 160 MHz.

AB - A single organic dye molecule at cryogenic conditions is resonantly excited in a confocal microscope. Under strong laser illumination it undergoes Rabi oscillations. Mathematically, this is well described and it has been experimentally implemented. These oscillations can be measured as side-bands on their resonance fluorescence, e.g. in the Mollow-Triplet. An alternative method is to research this effect by an analysis of the single molecule anti-bunched photon statistics. This has been performed in this work. Here we research on the detuning dependence of this signal -- it is experimentally demanding since the utilized laser might drift or single emitters are not necessarily spectral stable enough, such that the spectrum can be measured indefinitely. We therefore apply a measurement technique in which the photon correlation signal is acquired in detuning dependent steps. This is performed by continuous laser sweeps over the single molecule excitation spectrum. A single recording of the anti-bunched photons takes 20 to 50 ms. After approx. 1 hour of repetitive laser detunings a full anti-bunching curve is reconstructed for each spectral position. An alternative technique with 100 ns laser pulses allows to acquire a set of comparable data. Our study is derived from a single dibenzanthanthrene molecule. It emits under resonant excitation more than 380.000 photons per second. Under spectral detuning, Rabi-oscillations are observed up to Rabi=2 Pi 160 MHz.

KW - Single Molecules

KW - Rabi Oscillations

KW - Coherent Control

KW - Single Photons

KW - Quantum information processing

KW - Quantum optics

KW - single photons

KW - Rabi oscillations

KW - coherent spectroscopy

KW - anti-bunching

KW - single molecules

UR - http://www.scopus.com/inward/record.url?scp=85067595905&partnerID=8YFLogxK

U2 - 10.1088/1367-2630/ab130e

DO - 10.1088/1367-2630/ab130e

M3 - Article

VL - 21

JO - New journal of physics

JF - New journal of physics

SN - 1367-2630

IS - 4

M1 - 045005

ER -