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New Journal of Physics

Detuning dependent Rabi oscillations of a single molecule

Mohammad Rezai, Jörg Wrachtrup, Ilja Gerhardt

Published Mar 25, 2019• 22 citations

Abstract

Abstract 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 was well described and had 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 spectrally 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 20–50 ms. After approx. 1 h of repetitive laser detunings a full anti-bunching curve is reconstructed for each spectral position. An alternative technique with 100 ns laser pulses allows us to acquire a set of comparable data. Our study is derived from a single dibenzanthanthrene molecule with a natural linewidth of 2π×16 MHz. It emits under resonant excitation more than 380.000 photons per second. Under spectral detuning, Rabi-oscillations are observed up to Ω Rabi = 2π×160 MHz.

DOI: 10.1088/1367-2630/ab130e

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Abstract 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 was well described and had 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 spectrally 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 20–50 ms. After approx. 1 h of repetitive laser detunings a full anti-bunching curve is reconstructed for each spectral position. An alternative technique with 100 ns laser pulses allows us to acquire a set of comparable data. Our study is derived from a single dibenzanthanthrene molecule with a natural linewidth of 2π×16 MHz. It emits under resonant excitation more than 380.000 photons per second. Under spectral detuning, Rabi-oscillations are observed up to Ω Rabi = 2π×160 MHz.

A single-photon source is an essential tool for the emerging field of quantum technologies. Ideally, it should be spectrally compatible with other photonic devices while providing a high flux of narrow-band photons. The single organic dye molecule dibenzanthanthrene under cryogenic conditions possesses the given characteristics and therefore constitutes a prominent single-photon source. Nevertheless, the implementation of such a single-photon source requires a complex experimental setup involving a cryostat with a confocal microscope for the effective collection of the molecular emission. In the approach presented here we use a single emitter coupled directly to the end facet of an optical fiber. This has the potential to transfer a single-photon source based on a quantum emitter from a proof-of-principle type of setup to a scalable ``plug-and-play'' device. We present successful coupling of a single organic molecule to an optical fiber and record the excitation spectrum, measure the saturation curve, and analyze the contributions of Raman background fluorescence. The single-photon nature is proven by an antibunched autocorrelation recording, which reveals coherent Rabi oscillations.

We study the two-time correlation function and the resonance fluorescence spectrum of a semiconductor quantum dot excited by a strong off-resonant laser pulse. The obtained analytical expressions exhibit a specific detuning-dependent damping of Rabi oscillations of the dressed quantum dot as well as a detuning-dependent width of Mollow-triplet lines. In the absence of pure dephasing, the central peak of the triplet is broadened, upon increasing detuning, but the blue and red side peaks are narrowed. We demonstrate that pure dephasing processes can invert these dependences. A crossover between the regimes of detuning-dependent narrowing and broadening of the side and central peaks is identified. The predicted effects are consistent with resent experimental results and numerical calculations.

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 $\ensuremath{\pi}$-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.

Fluorescence photons emitted by a single molecule trapped in a solid at low temperature are correlated in time. A simple theory of the correlation pattern is presented, including in the same formalism photon antibunching from coherent Rabi oscillations and photon bunching due to incoherent quantum transitions between electronic levels. The correlation method is applied to single pentacene molecules in a para-terphenyl crystal. A clear photon bunching allows us to determine the ISC rates for each molecule. We attribute the scatter of our results for the transition rate between excited singlet and triplet states, and the difference with the average value taken from the literature, to molecular distortions induced by crystal defects in our small sample. We conclude that the correlation method associated to single molecule spectroscopy has a great potential to study dynamical processes on intermediate time scales in condensed matter.

We study the two-time correlation function and the resonance fluorescence spectrum of a semi-conductor quantum dot excited by a strong off-resonant laser pulse. The obtained analytic expressions exhibit a specific detuning-dependent damping of Rabi oscillations of the dressed quantum dot as well as a detuning-dependent width of Mollow triplet lines. In the absence of pure dephasing, the central peak of the triplet is broadened upon increasing detuning, but the blue- and red-side peaks are narrowed. We demonstrate that the pure dephasing processes can invert these dependences. A crossover between the regimes of detuning-dependent narrowing and broadening of the side and central peaks is identified. The predicted effects are consistent with recent experimental results and numerical calculations.

Antibunching is a quantum effect demonstrating clearly the quantum nature of the radiation field. Its detection through measurements of the second order correlation function is a direct proof of the presence of single molecule or single nano particle. In this paper we present the experimental setup of the Hanbury Brown - Twiss interferometer and the measurement results of the antibunching effect from single Rhodamine B dye molecules and single CdTe quantum dots in dilute solution. By fitting the second order correlation data, we derive a fluorescence lifetime of approximately 2 ns for Rhodamine B and 45 ns for CdTe quantum dots. Our results demonstrate an alternative way for determining the fluorescence lifetime using the antibunching effect.