Abstract
Lead-free double perovskite nanocrystals(NCs)have emerged as a promising candidate in the optical field,owing to their non-toxic,good moist heat and chemical stability.However,their poor optical proper-ties limited their application.To improve the optical properties of lead-free double perovskite NCs,metal ion doping or alloying had been suggested as a promising strategy.Here,we prepared monodisperse,uniformly sized,cubic morphology of Cs2AgBiCl6 NCs with different Na+incorporation amounts via a simple hot-injection method.The Na+incorporation broke the parity-forbidden transition by reducing the inversion symmetry of the electron wave function at the Ag site,which changed the parity of the self-trapped exciton wave function and thus allowed radiative recombination.As a result,the photolumi-nescence quantum yield(PLQY)of Na+-alloyed Cs2AgBiCl6 NCs(12.1％)was higher than that of Cs2AgBiCl6 NCs(2.4％),and the exciton lifetime of Na+-alloyed Cs2AgBiCl6 NCs increased to 36.98 ns from 17.58 ns for Cs2AgBiCl6 NCs.By adjusting the amount of Na+incorporation,the band gap of Cs2AgBiCl6 NCs can be significantly tuned from～2.90 eV to～3.50 eV.Furthermore,the temperature-dependent photolu-minescence spectra indicated that the Na+-alloyed Cs2AgBiCl6 NCs possessed higher longitudinal optical phonon energy and exciton binding energy compared to Cs2AgBiCl6 NCs.This suggested that there were strong exciton-phonon interactions during exciton recombination,a reduced probability of non-radiative processes,and excellent thermal stability.It offers a promising strategy for improving the optical proper-ties of lead-free double perovskite NCs,and have the potential to replace traditional lead halide perovskite NCs in future optoelectronic applications.
基金项目
国家自然科学基金(21473051)
黑龙江省自然科学基金(LH2019B014)
Youth Science and Technology Innovation Team Project of Heilongjiang Province(2018-KYYWF-1593)
NETL
NSTL
万方数据