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Bulletin of the American Physical Society

Motion and Photon Emission of Single Molecules in Space-Time

Joonhee Lee, Shawn M. Perdue, Alejandro Rodriguez Perez, Vartkess Ara Apkarian

Published Mar 1, 2012• 0 citations
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Quantum Photonic Devices•Oct 3, 2017•0 citations
In this paper, we study the influence of time-dependent phase delay on the emission of few photons from a single molecule in a solid matrix. The results demonstrate that a time-dependent phase of the pulses can be used to control the photon emission and strongly affects the spectrum of single molecules. The spectrum of the photon emission probabilities reflects the fast dynamics of the states of the system when the duration of the driven laser pulses is short. Also, it is shown that the coupling between the system and the rf field strongly affects the spectrum of the photon emission probabilities in space.
We consider the photon spontaneous emission of single molecules in a solid matrix with spectral diffusion. A general theoretical strategy for calculating the photon emission statistics in a solid matrix of single molecules is derived. In particular, the control photon emission from single molecules in a solid matrix driven simultaneously by a laser and an electric radiofrequency (rf) field is investigated. The photon emission of single molecules can be modulated by an rf field. The formulation also allows for the study of the average waiting time for the emission event of a single molecule.
Efficient quantum light sources and non-linear optical elements at the few photon level are the basic ingredients for most applications in nano and quantum technologies. On the other hand, a scalable platform for quantum ICT typically requires reliable light matter interfaces and on-chip integration. In this work we demonstrate the potential of a novel hybrid technology which combines single organic molecules as quantum emitters and dielectric chips [1]. Dibenzoterrylene molecules in anthracene crystals (DBT:Ac) are particularly suitable quantum systems for this task, since they exhibit long-term photostability in thin samples [2], easy fabrication methods and life-time limited emission at cryogenic temperatures [3]. We demonstrate at room temperature the emission of single photons from DBT molecules into ridge waveguides with a branching ratio up to 40%. The overall single-photon source efficiency, including emission into the guided mode, propagation losses, and emission into a quasi-gaussian mode in free space, is estimated around 16%. These results are competitive with state-of-the-art single photon emission into propagating guided modes from solid state systems [4], while offering a novel platform with unprecedented versatility. References [1] P. Lombardi et al., Arxiv: 1701.00459v1 (2017). [2] C. Toninelli et al., Opt. Express 18, 6577 (2010). [3] A. A. L. Nicolet et al., ChemPhysChem 8, 1929 (2007). [4] I. Zadeh et al., Nano Lett. 16, 2289 (2016); R. S. Daveau et al., Arxiv: 1610.08670v1 (2016). [5] J. Hwang et. al., New J. Phys. 13, 085009 (2011); H.-W. Lee et al., Phys. Rev. A 63, 012305 (2000).