Long-range and fast transport of coherent excitons is important for the development of high-speed excitonic circuits and quantum computing applications.However,most of these coherent excitons have only been observed i...Long-range and fast transport of coherent excitons is important for the development of high-speed excitonic circuits and quantum computing applications.However,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 materials.Here,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 temperature.This value is one to several orders of magnitude higher than the values reported for other organic molecular aggregates and low-dimensional inorganic materials.Without 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 emission.The 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 films.In addition,the supertransport of excitons in monolayer pentacene samples showed highly anisotropic behaviour.Our results pave the way for the development of future high-speed excitonic circuits,fast OLEDs,and other optoelectronic devices.展开更多
基金funding support from ANU PhD student scholarship,China Scholarship Council,Australian Research Council(ARC,numbers DE140100805 and DP180103238)ARC Centre of Excellence in Future Low-Energy Electronics Technologies(project number CE170100039)ARC Centre of Excellence in Quantum Computation and Communication Technology(project number CE170100012).
文摘Long-range and fast transport of coherent excitons is important for the development of high-speed excitonic circuits and quantum computing applications.However,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 materials.Here,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 temperature.This value is one to several orders of magnitude higher than the values reported for other organic molecular aggregates and low-dimensional inorganic materials.Without 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 emission.The 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 films.In addition,the supertransport of excitons in monolayer pentacene samples showed highly anisotropic behaviour.Our results pave the way for the development of future high-speed excitonic circuits,fast OLEDs,and other optoelectronic devices.
