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Supertransport of excitons in atomically thin organic semiconductors at the 2D quantum limit

Light(Science & Applications) 2020年第1期9卷 907-919页

作者： Ankur Sharma Linglong Zhang jonathan o.tollerud Miheng Dong Yi Zhu Robert Halbich Tobias Vogl Kun Liang Hieu T.Nguyen Fan Wang Shilpa Sanwlani Stuart K.Earl Daniel Macdonald Ping Koy Lam Jeffrey A.Davis Yuerui Lu Research School of Electrical Energy and Materials EngineeringCollege of Engineering and Computer ScienceThe Australian National UniversityCanberraACT 2601Australia optical Sciences Centre Swinburne University of TechnologyHawthornVIC 3122Australia ARC Centre of Excellence for Future Low-Energy Electronics Technology Australia Centre for Quantum Computation and Communication Technology Department of Quantum ScienceResearch School of Physics and EngineeringThe Australian National UniversityActonACT 2601Australia School of Mechatronical Engineering Beijing Institute of TechnologyBeijing 100081China Institute for Biomedical Materials and Devices(IBMD) Faculty of ScienceUniversity of Technology SydneySydneyNSW 2007Australia

Long-range and fast transport of coherent excitons is important for the development of high-speed excitonic circuits and quantum computing ***,most of these coherent excitons have only been observed in some low-dimensional semiconductors when coupled with cavities,as there are large inhomogeneous broadening and dephasing effects on the transport of excitons in their native states in ***,by confining coherent excitons at the 2D quantum limit,we first observed molecular aggregation-enabled‘supertransport’of excitons in atomically thin two-dimensional(2D)organic semiconductors between coherent states,with a measured high effective exciton diffusion coefficient of ~346.9 cm^(2)/s at room *** value is one to several orders of magnitude higher than the values reported for other organic molecular aggregates and low-dimensional inorganic *** coupling to any optical cavities,the monolayer pentacene sample,a very clean 2D quantum system(~1.2 nm thick)with high crystallinity(J-type aggregation)and minimal interfacial states,showed superradiant emission from Frenkel excitons,which was experimentally confirmed by the temperature-dependent photoluminescence(PL)emission,highly enhanced radiative decay rate,significantly narrowed PL peak width and strongly directional in-plane *** coherence in monolayer pentacene samples was observed to be delocalised over~135 molecules,which is significantly larger than the values(a few molecules)observed for other organic thin *** addition,the supertransport of excitons in monolayer pentacene samples showed highly anisotropic *** results pave the way for the development of future high-speed excitonic circuits,fast oLEDs,and other optoelectronic devices.

关键词： transport quantum coherent

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Transient measurement of phononic states with covariance-based stochastic spectroscopy

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Light(Science & Applications) 2022年第3期11卷 68-75页

作者： Giorgia Sparapassi Stefano MCavaletto jonathan tollerud Angela Montanaro Filippo Glerean Alexandre Marciniak Fancesca Giusti Shaul Mukamel Daniele Fausti Physics Department University of TriesteTriesteItaly Elettra-Sincrotrone Trieste S.C.p.A. TriesteItaly Department of Chemistry and Department of Physics&Astronomy University of CaliforniaIrvineCAUSA optical Sciences Centre Swinburne UniversityMelbourneAustralia

We present a novel approach to transient Raman spectroscopy,which combines stochastic probe pulses and a covariance-based detection to measure stimulated Raman signals in alpha-quartz.A coherent broadband pump is used to simultaneously impulsively excite a range of different phonon modes,and the phase,amplitude,and energy of each mode are independently recovered as a function of the pump-probe delay by a noisy-probe and covariance-based *** experimental results and the associated theoretical description demonstrate the feasibility of 2D-Raman experiments based on the stochastic-probe schemes,with new capabilities not available in equivalent mean-value-based 2D-Raman *** work unlocks the gate for nonlinear spectroscopies to capitalize on the information hidden within the noise and overlooked by a mean-value analysis.

关键词： stochastic spectroscopy coherent

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