Up-conversion photoluminescence(UCPL)refers to the elementary process where low-energy photons are converted into high-energy ones via consecutive interactions inside a medium.When additional energy is provided by int...Up-conversion photoluminescence(UCPL)refers to the elementary process where low-energy photons are converted into high-energy ones via consecutive interactions inside a medium.When additional energy is provided by intermnal thermal energy in the form of lttice vibrations(phonons),the process is called phonon-assisted UCPL.Here,we report the exceptionally large phonon-assisted energy gain of up to^8kgT(kg is Boltzmann constant,T is temperature)on all-inorganic lead halide perovskite semiconductor colloidal nanocrystals that goes beyond the maximum capabilty of only harvesting optical phonon modes.By systematic optical study in combination with a statistical probability model,we explained the nontrivial phonon-assisted UCPL process in perovskites nanocrystals,where in addition to the strong electron-phonon(light-matter)coupling,other nonlinear processes such as phonon-phonon(matter-matter)interaction also effectively boost the up-conversion efficiency.展开更多
基金the Singapore National Research Foundation through the NRF Investigatorship Award(No.NRF-NRFI2015-03)the Singapore Ministry of Education via AcRF Tier 3 Programme(No.MOE2018-T3-1-002),Tier 2 grant(No.MOE2018-T2-2-068)and Tier 1 grants(Nos.RG103/15 and RG113/16)A.G.D.A.gratefully acknowledges the financial support of the Presidential Postdoctoral Fellowship program of the Nanyang Technological University
文摘Up-conversion photoluminescence(UCPL)refers to the elementary process where low-energy photons are converted into high-energy ones via consecutive interactions inside a medium.When additional energy is provided by intermnal thermal energy in the form of lttice vibrations(phonons),the process is called phonon-assisted UCPL.Here,we report the exceptionally large phonon-assisted energy gain of up to^8kgT(kg is Boltzmann constant,T is temperature)on all-inorganic lead halide perovskite semiconductor colloidal nanocrystals that goes beyond the maximum capabilty of only harvesting optical phonon modes.By systematic optical study in combination with a statistical probability model,we explained the nontrivial phonon-assisted UCPL process in perovskites nanocrystals,where in addition to the strong electron-phonon(light-matter)coupling,other nonlinear processes such as phonon-phonon(matter-matter)interaction also effectively boost the up-conversion efficiency.