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Title: Intrinsic and Extrinsic Exciton Recombination Pathways in AgInS 2 Colloidal Nanocrystals

Journal Article · · Energy Material Advances
ORCiD logo [1]; ORCiD logo [1];  [2];  [3];  [4];  [5];  [5]; ORCiD logo [1];  [5];  [3]; ORCiD logo [6];  [7]; ORCiD logo [1]
  1. Dipartimento di Scienza dei Materiali, Università degli studi di Milano-Bicocca, via Roberto Cozzi 55, 20125 Milano, Italy
  2. Dipartimento di Energia, Politecnico di Milano, Via Ponzio 34/3, 20133 Milano, Italy
  3. Istituto Italiano di Tecnologia, Via Morego 30, 16163 Genova, Italy
  4. Dipartimento di Scienza dei Materiali, Università degli studi di Milano-Bicocca, via Roberto Cozzi 55, 20125 Milano, Italy, Glass to Power SpA, Via Fortunato Zeni 8, 38068 RoveretoItaly
  5. Beijing Key Laboratory of Construction-Tailorable Advanced Functional Materials and Green Applications, School of Materials Science &, Engineering, Beijing Institute of Technology, Beijing 100081, China
  6. Dipartimento di Energia, Politecnico di Milano, Via Ponzio 34/3, 20133 Milano, Italy, IFN-CNR, Piazza Leonardo da Vinci 32, 20133 MilanoItaly
  7. National High Magnetic Field Laboratory, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, USA
+ Show Author Affiliations

Ternary I-III-VI 2 nanocrystals (NCs), such as AgInS 2 and CuInS 2 , are garnering interest as heavy-metal-free materials for photovoltaics, luminescent solar concentrators, LEDs, and bioimaging. The origin of the emission and absorption properties in this class of NCs is still a subject of debate. Recent theoretical and experimental studies revealed that the characteristic Stokes-shifted and long-lived luminescence of stoichiometric CuInS 2 NCs arises from the detailed structure of the valence band featuring two sublevels with different parity. The same valence band substructure is predicted to occur in AgInS 2 NCs, yet no experimental confirmation is available to date. Here, we use complementary spectroscopic, spectro-electrochemical, and magneto-optical investigations as a function of temperature to investigate the band structure and the excitonic recombination mechanisms in stoichiometric AgInS 2 NCs. Transient transmission measurements reveal the signatures of two subbands with opposite parity, and photoluminescence studies at cryogenic temperatures evidence a dark state emission due to enhanced exchange interaction, consistent with the behavior of stoichiometric CuInS 2 NCs. Lowering the temperature as well as applying reducing electrochemical potentials further suppress electron trapping, which represents the main nonradiative channel for exciton decay, leading to nearly 100% emission efficiency.

Research Organization:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA); National Science Foundation (NSF); Italian Ministry of Education, University and Research (MIUR); National Natural Science Foundation of China (NSFC)
Grant/Contract Number:
89233218CNA000001; DMR-1644779; 2015WTW7J3; 51872030; 51631001
OSTI ID:
1909317
Alternate ID(s):
OSTI ID: 1804374
Report Number(s):
LA-UR-21-21348; 2021/1959321
Journal Information:
Energy Material Advances, Journal Name: Energy Material Advances Vol. 2021; ISSN 2692-7640
Publisher:
American Association for the Advancement of Science (AAAS)Copyright Statement
Country of Publication:
United States
Language:
English

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36 MATERIALS SCIENCE
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