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Optical Signatures of Transiently Disordered Semiconductor Nanocrystals.
ACS Nano ; 12(10): 10008-10015, 2018 Oct 23.
Artigo em Inglês | MEDLINE | ID: mdl-30226751
ABSTRACT
The optoelectronic properties of semiconductor nanocrystals (NCs) have led to efforts to integrate them as the active material in light-emitting diodes, solid-state lighting, and lasers. Understanding related high carrier injection conditions is therefore critical as resultant thermal effects can impact optical properties. The physical integrity of NCs is indeed questionable as recent transient X-ray diffraction studies have suggested that nanoscopic particles reversibly lose crystalline order, or melt, under high fluence photoexcitation. Informed by such studies, here, we examine CdSe NCs under elevated fluences to determine the impact of lattice disordering on optical properties. To this end, we implement intensity-dependent transient absorption using both one- and two-pump methods where the latter effectively subtracts out the NC optical signatures associated with lower fluence photoexcitation, especially band-edge features. At elevated fluences, we observe a long-lived induced absorption at a lower energy than the crystalline-NC bandgap across a wide range of sizes that follows power-dependent trends and kinetics consistent with the prior transient X-ray measurements. NC photoluminescence studies provide further evidence that melting influences optical properties. These methods of characterizing bandgap narrowing caused by lattice disordering could facilitate routes to improved optical amplification and band-edge emission at high excitation density.

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Texto completo: Disponível Coleções: Bases de dados internacionais Base de dados: MEDLINE Idioma: Inglês Revista: ACS Nano Ano de publicação: 2018 Tipo de documento: Artigo País de afiliação: Estados Unidos