Excitons,bound electron–hole pairs,in two-dimensional hybrid organic inorganic perovskites(2D HOIPs)are capable of forming hybrid light-matter states known as exciton-polaritons(E–Ps)when the excitonic medium is con...Excitons,bound electron–hole pairs,in two-dimensional hybrid organic inorganic perovskites(2D HOIPs)are capable of forming hybrid light-matter states known as exciton-polaritons(E–Ps)when the excitonic medium is confined in an optical cavity.In the case of 2D HOIPs,they can self-hybridize into E–Ps at specific thicknesses of the HOIP crystals that form a resonant optical cavity with the excitons.However,the fundamental properties of these self-hybridized E–Ps in 2D HOIPs,including their role in ultrafast energy and/or charge transfer at interfaces,remain unclear.Here,we demonstrate that>0.5µm thick 2D HOIP crystals on Au substrates are capable of supporting multiple-orders of self-hybridized E–P modes.These E–Ps have high Q factors(>100)and modulate the optical dispersion for the crystal to enhance sub-gap absorption and emission.Through varying excitation energy and ultrafast measurements,we also confirm energy transfer from higher energy E–Ps to lower energy E–Ps.Finally,we also demonstrate that E–Ps are capable of charge transport and transfer at interfaces.Our findings provide new insights into charge and energy transfer in E–Ps opening new opportunities towards their manipulation for polaritonic devices.展开更多
基金support for this work by the Asian Office of Aerospace Research and Development of the Air Force Office of Scientific Research(AFOSR)FA2386-20-1-4074partial support from Office of Naval Research(ONR)Young Investigator Award(YIP)(N00014-23-1-203)+7 种基金S.B.A.gratefully acknowledges funding received from the Swiss National Science Foundation(SNSF)under the Early Postdoc Mobility grant(P2ELP2_187977)for this workC.M.is supported by an NSF-AFRL Intern Program.The experiments were carried out at the Singh Center for Nanotechnology at the University of Pennsylvania,which is supported by the National Science Foundation(N.S.F.)National Nanotechnology Coordinated Infrastructure Program grant NNCI-1542153D.J.and K.L.acknowledge the NSF REU SUNFEST program under Grant No.1950720,to support the stay of K.L.at the University of PennsylvaniaThe research performed by C.E.S.at the Air Force Research Laboratory was supported by contract award FA807518D0015J.R.H.acknowledges support from the Air Force Office of Scientific Research(Program Manager Dr.Gernot Pomrenke)under award number FA9550-20RYCOR059T.D.and P.J.S.gratefully acknowledge support from Programmable Quantum Materials,an Energy Frontier Research Center funded by the U.S.Department of Energy(DOE),Office of Science,Basic Energy Sciences(BES),under award DE-SC0019443H.H.acknowledges support from the Department of Energy(DE-SC0020101)A.D.M.acknowledges support from the Army Research Office(grant W911NF2210158).
文摘Excitons,bound electron–hole pairs,in two-dimensional hybrid organic inorganic perovskites(2D HOIPs)are capable of forming hybrid light-matter states known as exciton-polaritons(E–Ps)when the excitonic medium is confined in an optical cavity.In the case of 2D HOIPs,they can self-hybridize into E–Ps at specific thicknesses of the HOIP crystals that form a resonant optical cavity with the excitons.However,the fundamental properties of these self-hybridized E–Ps in 2D HOIPs,including their role in ultrafast energy and/or charge transfer at interfaces,remain unclear.Here,we demonstrate that>0.5µm thick 2D HOIP crystals on Au substrates are capable of supporting multiple-orders of self-hybridized E–P modes.These E–Ps have high Q factors(>100)and modulate the optical dispersion for the crystal to enhance sub-gap absorption and emission.Through varying excitation energy and ultrafast measurements,we also confirm energy transfer from higher energy E–Ps to lower energy E–Ps.Finally,we also demonstrate that E–Ps are capable of charge transport and transfer at interfaces.Our findings provide new insights into charge and energy transfer in E–Ps opening new opportunities towards their manipulation for polaritonic devices.
