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Hybridized electronic states between CdSe nanoparticles and conjugated organic ligands： A theoretical and ultrafast photo-excited carrier dynamics study

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Nano Research 2018年第1期11卷 142-150页

作者： Tersilla Virgili Arrigo Calzolarit Inma Suarez Lopez alice ruini Alessandra Catellani1 Barbara Vercelli Francesco Tassone IFN -CNR c o Dipartimento di Fisica Politecnico di Milano 20132 Milano Italy Istituto Nanoscienze CNR-NANO-S3 Via Campi 213/A I-41125 Modena Italy Dipartimento di Scienze Fisiche Informatiche e Matematiche Universit# di Modena e Reggio Emilia Via Campi 213/a I-41125 Modena Italy Istituto di Chimica della Materia Condensata e di Tecnologie per I'Energia ICMATE-CNR SS di Milano Via Cozzi 53 20125 Milano Italy Center for Nano Science and Technology @Polimi Istituto Italiano di Tecnologia Via Pascoli 70/3 20133 Milano Italy

Formation of densely packed thin films of semiconductor nanocrystals is advantageous for the exploitation of their unique optoelectronic properties for real-world applications. Here we investigate the fundamental role of the structure of the bridging ligand on the optoelectronic properties of the resulting hybrid film. In particular, we considered hybrid films formed using the same CdSe nanocrystals and two organic ligands that have the same bidentate dithiocarbamate bInding moiety, but differ in their bridging structures, one bridged by ethylene, the other by phenylene that exhibits conjugation. Based on the results of photo- excited carrier dynamics experiments combined with theoretical calculations on the electronic states of bridged CdSe layers, we show that only the phenylene- based ligand presents a strong hybridization of the molecular HOMO state with CdSe layers, that is a marker of formation of an effective bridge. We argue that this hybridization spread favors the hopping of photo-excited carriers between nanocrystals, which may explain the reported larger photo-currents in phenylene-based hybrid films than those observed in ethylene-based ones.

关键词： hybrid layer-by-layer film ultrafast spectroscopy CdSe nanoparticles molecular orbitals density functional theory

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