Reductive pathways in molten inorganic salts enable colloidal synthesis of III-V semiconductor nanocrystals

Justin C Ondry; Zirui Zhou; Kailai Lin; Aritrajit Gupta; Jun Hyuk Chang; Haoqi Wu; Ahhyun Jeong; Benjamin F Hammel; Di Wang; H Christopher Fry; Sadegh Yazdi; Gordana Dukovic; Richard D Schaller; Eran Rabani; Dmitri V Talapin

doi:10.1126/science.ado7088

Reductive pathways in molten inorganic salts enable colloidal synthesis of III-V semiconductor nanocrystals

Science. 2024 Oct 25;386(6720):401-407. doi: 10.1126/science.ado7088. Epub 2024 Oct 24.

Authors

Justin C Ondry¹, Zirui Zhou¹, Kailai Lin^{2

3}, Aritrajit Gupta¹, Jun Hyuk Chang¹, Haoqi Wu¹, Ahhyun Jeong¹, Benjamin F Hammel⁴, Di Wang¹, H Christopher Fry⁵, Sadegh Yazdi^{4

6}, Gordana Dukovic^{4

6

7}, Richard D Schaller^{5

8}, Eran Rabani^{2

3

9}, Dmitri V Talapin^{1

5

10}

Affiliations

¹ Department of Chemistry and James Franck Institute, University of Chicago, Chicago, IL 60637, USA.
² Department of Chemistry, University of California, Berkeley, CA 94720, USA.
³ Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.
⁴ Materials Science and Engineering, University of Colorado, Boulder, CO 80309, USA.
⁵ Center for Nanoscale Materials, Argonne National Laboratory, Argonne, IL 60439, USA.
⁶ Renewable and Sustainable Energy Institute, University of Colorado, Boulder, CO 80309, USA.
⁷ Department of Chemistry, University of Colorado, Boulder, CO 80309, USA.
⁸ Department of Chemistry, Northwestern University, Evanston, IL 60208, USA.
⁹ The Raymond and Beverly Sackler Center of Computational Molecular and Materials Science, Tel Aviv University, Tel Aviv 69978, Israel.
¹⁰ Pritzker School of Molecular Engineering, University of Chicago, Chicago, IL 60637, USA.

PMID: 39446954
DOI: 10.1126/science.ado7088

Abstract

Colloidal quantum dots, with their size-tunable optoelectronic properties and scalable synthesis, enable applications in which inexpensive high-performance semiconductors are needed. Synthesis science breakthroughs have been key to the realization of quantum dot technologies, but important group III-group V semiconductors, including colloidal gallium arsenide (GaAs), still cannot be synthesized with existing approaches. The high-temperature molten salt colloidal synthesis introduced in this work enables the preparation of previously intractable colloidal materials. We directly nucleated and grew colloidal quantum dots in molten inorganic salts by harnessing molten salt redox chemistry and using surfactant additives for nanocrystal shape control. Synthesis temperatures above 425°C are critical for realizing photoluminescent GaAs quantum dots, which emphasizes the importance of high temperatures enabled by molten salt solvents. We generalize the methodology and demonstrate nearly a dozen III-V solid-solution nanocrystal compositions that have not been previously reported.