4.8 Article

Ligand Exchange at a Covalent Surface Enables Balanced Stoichiometry in III-V Colloidal Quantum Dots

Journal

NANO LETTERS
Volume 21, Issue 14, Pages 6057-6063

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.1c01286

Keywords

III-V colloidal quantum dots; covalent surface; ligand exchange; stoichiometry; photodetector

Funding

  1. NSERC Discovery Grant
  2. Canada Research Chair
  3. National Research Foundation of Korea (NRF) - Government of Korea (MSIT) [2021R1A4A3024237]
  4. National Research Foundation of Korea [2021R1A4A3024237] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)

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The study demonstrates stoichiometric reconstruction in InAs CQDs by ligand exchange, replacing indium-carboxylate ligands with anionic ligands like thiols to produce balanced-stoichiometry CQDs inks. This approach enables the use of InAs CQD solids as the active layer in photodiode detectors with high external quantum efficiency and fast photoresponse time, outperforming reference PbS CQD devices by a factor of 4.
III-V colloidal quantum dots (CQDs) are promising semiconducting materials for optoelectronic applications; however, their strong covalent character requires a distinct approach to surface management compared with widely investigated II-VI and IV-VI CQDs-dots, which by contrast are characterized by an ionic nature. Here we show stoichiometric reconstruction in InAs CQDs by ligand exchange. In particular, we find that indium-carboxylate ligands, which passivate assynthesized InAs CQDs and are responsible for In-rich surfaces, can be replaced by anionic ligands such as thiols. This enables the production of inks consisting of balanced-stoichiomety CQDs; this is distinct from what is observed in II-VI and IV-VI CQDs, in which thiols replace carboxylates. The approach enables the implementation of InAs CQD solids as the active layer in photodiode detectors that exhibit an external quantum efficiency of 36% at 930 nm and a photoresponse time of 65 ns, which is 4 times shorter than that of reference PbS CQD devices.

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