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journal article·2025-06-24Open access

Selective Tracking of Charge Carrier Dynamics in CuInS2 Quantum Dots

Andrés Burgos-Caminal, Brener R. C. Vale, André F. V. Fonseca, Elisa P. P. Collet, Juan F. Hidalgo, Lázaro García, Luke Watson, Olivia Borrell-Grueiro, María E. Corrales, Tae-Kyu Choi, Tetsuo Katayama, Dongxiao Fan, Víctor Vega-Mayoral, Saül Garcia-Orrit, Shunsuke Nozawa, Thomas J. Penfold, Juan Cabanillas-González, Shin-Ichi Adachi, Luis Bañares, Ana Flávia Nogueira, Lázaro A. Padilha, Marco Antônio Schiavon, Wojciech Gawelda

ACS Nano· Volume 19· Issue 24
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Abstract

High Resolution Image Download MS PowerPoint Slide CuInS 2 quantum dots have been studied in a broad range of applications, but despite this, the fine details of their charge carrier dynamics remain a subject of intense debate. Two of the most relevant points of discussion are the hole dynamics and the influence of Cu:In synthesis stoichiometry. It has been proposed that Cu-deficiency leads to the formation of Cu 2+, affecting the localization of holes into Cu defects. Importantly, it is precisely these confined hole states that are used to explain the interesting photoluminescence properties of CuInS 2 quantum dots. We use static X-ray spectroscopy to show no evidence for a measurable amount of native Cu 2+ states in Cu-deficient samples (above 20%). Instead, the improved properties of these samples are explained by an increase of crystallinity, reducing the concentration of mid-gap states. Furthermore, to understand the charge carrier dynamics, herein, we employ ultrafast optical transient absorption and fluorescence up-conversion spectroscopies in combination with ultrafast X-ray absorption spectroscopy using a hard X-ray free electron laser. We demonstrate that in nonpassivated samples, holes are transferred from Cu atoms on subpicosecond time scales. Finally, we observe that Cu-deficient samples are more robust against photothermal effects at higher laser fluences. This is not the case for the Cu-rich sample, where heating effects on the structure are directly observed.
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Research context

OpenAlex topics: Chalcogenide Semiconductor Thin Films · Quantum Dots Synthesis And Properties · Copper-based nanomaterials and applications

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Madrid Institute for Advanced Studies in Nanoscience, IMDEA Nanociencia, Ciudad Universitaria de Cantoblanco, Calle Faraday 9, Madrid 28049, Spain

Departamento de Química, Universidad Autónoma de Madrid, Ciudad Universitaria de Cantoblanco, Calle Francisco Tomás y Valiente 7, Madrid 28049, Spain

Instituto de Física Gleb Wataghin

Universidade Estadual de Campinas - UNICAMP

Grupo de Pesquisa Química de Materiais, Departamento de Ciências Naturais

Universidade Federal de São João Del-Rei

Laboratório de Nanotecnologia e Energia Solar, Instituto de Química

Chemistry-School of Natural and Environmental Sciences

Newcastle University

Departamento de Química Física and Center for Ultrafast Lasers, Facultad de Ciencias Químicas

Universidad Complutense de Madrid

Departamento de Química Física Aplicada, Universidad Autónoma de Madrid, Ciudad Universitaria de Cantoblanco, Calle Francisco Tomás y Valiente 7, Madrid 28049, Spain

XFEL Division

Pohang Accelerator Laboratory, POSTECH

Japan Synchrotron Radiation Research Institute, Kouto 1-1-1, Sayo 679-5198, Hyogo, Japan

Institute of Materials Structure Science, High Energy Accelerator Research Organization (KEK), 1-1 Oho, Tsukuba 305-0801, Ibaraki, Japan

Faculty of Physics, Adam Mickiewicz University, ul. Uniwersytetu Poznańskiego 2, 61-614 Poznan, Poland

Funding

Funda????o de Amparo ?? Pesquisa do Estado de Minas Gerais · Comunidad de Madrid · Ministry of Science, Innovation and Universities · Ag??ncia Nacional do Petr??leo, G??s Natural e Biocombust??veis · Universidad Aut??noma de Madrid · Funda????o de Amparo ?? Pesquisa do Estado de S??o Paulo · European Commission · Shell

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