InAs colloidal quantum dots (CQDs) are a promising heavy-metal-free material for infrared optoelectronic devices. However, their synthesis is limited by their reagents: the acutely toxic and difficult to source tris(trimethylsilyl)arsine ((TMS)As), as well as the strong reducing agents (e.g., Super Hydride). A reducing agent is introduced based on hydrosilanes (Si-H) to address both challenges. A synthesis strategy with this agent is demonstrated, resulting in monodisperse InAs CQDs with a tunable first excitonic peak between 520 and 900 nm by hot injection, and between 900 and 1550 nm by continuous injection. Furthermore, by avoiding the use of carboxyl group-containing compounds, such as oleic acid or indium acetate, the synthesis minimizes surface oxidation during InAs CQDs formation. The synthesized InAs CQDs are of high optoelectronic quality, with a lower concentration of deep trap states, as evident by the remarkable characteristics of photodetectors fabricated from these CQDs: low dark current (≈150 nA cm), external quantum efficiency (32% at 900 nm), and a fast photoresponse time (≈4.4 µs). The elimination of (TMS)As in the synthesis overcomes a key practical barrier for exploiting and exploring the properties of large InAs CQDs in optoelectronic applications.
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http://dx.doi.org/10.1002/adma.202412105 | DOI Listing |
Adv Mater
December 2024
Center for Renewable Energy and Storage Technologies (CREST), Division of Physical Science and Engineering, King Abdullah University of Science and Technology, Thuwal, 23955-6900, Kingdom of Saudi Arabia.
J Am Chem Soc
October 2024
Center for Renewable Energy and Storage Technologies (CREST), Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Kingdom of Saudi Arabia.
J Am Chem Soc
September 2024
Department of Electrical and Computer Engineering, University of Toronto, 10 King's College Road, Toronto, ON M5S 3G4, Canada.
The synthesis of highly monodispersed InAs colloidal quantum dots (CQDs) is needed in InAs CQD-based optoelectronic devices. Because of the complexities of working with arsenic precursors such as tris-trimethylsilyl arsine ((TMSi)As) and tris-trimethylgermyl arsine ((TMGe)As), several attempts have been made to identify new candidates for synthesis; yet, to date, only the aforementioned two highly reactive precursors have led to excellent photodetector device performance. We begin the present study by investigating the mechanism, finding that the use of the cosurfactant dioctylamine plays a crucial role in producing monodispersed InAs populations.
View Article and Find Full Text PDFJACS Au
March 2024
Department of Energy Science (DOES) and Center for Artificial Atoms, Sungkyunkwan University (SKKU), Suwon, Gyeonggi-do 16419, South Korea.
Colloidal quantum dots (CQDs) have garnered significant attention in nanoscience and technology, with a particular emphasis on achieving high monodispersity in their synthesis. Recent advances in understanding the chemistry of reaction intermediates such as magic-sized nanoclusters (MSC) have paved the way for innovative synthetic strategies. Notably, monodisperse CQDs of various compositions, including indium phosphide, indium arsenide, and cadmium chalcogenide, have been successfully prepared using nanocluster intermediates as single-source precursors.
View Article and Find Full Text PDFAdv Sci (Weinh)
April 2024
Department of Chemical and Biological Engineering, Korea University, Seoul, 02841, Republic of Korea.
Solution-processed low-bandgap semiconductors are crucial to next-generation infrared (IR) detection for various applications, such as autonomous driving, virtual reality, recognitions, and quantum communications. In particular, III-V group colloidal quantum dots (CQDs) are interesting as nontoxic bandgap-tunable materials and suitable for IR absorbers; however, the device performance is still lower than that of Pb-based devices. Herein, a universal surface-passivation method of InAs CQDs enabled by intermediate phase transfer (IPT), a preliminary process that exchanges native ligands with aromatic ligands on the CQD surface is presented.
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