Coherent heteroepitaxial growth of I-III-VI2 Ag(In,Ga)S2 colloidal nanocrystals with near-unity quantum yield for use in luminescent solar concentrators

Hak June Lee, Seongbin Im, Dongju Jung, Kyuri Kim, Jong Ah Chae, Jaemin Lim, Jeong Woo Park, Doyoon Shin, Kookheon Char, Byeong Guk Jeong, Ji-Sang Park, Euyheon Hwang, Doh C. Lee, Young-Shin Park, Hyung-Jun Song (), Jun Hyuk Chang () and Wan Ki Bae ()
Additional contact information
Hak June Lee: Sungkyunkwan University (SKKU)
Seongbin Im: Sungkyunkwan University (SKKU)
Dongju Jung: Sungkyunkwan University (SKKU)
Kyuri Kim: Sungkyunkwan University (SKKU)
Jong Ah Chae: Sungkyunkwan University (SKKU)
Jaemin Lim: Sungkyunkwan University (SKKU)
Jeong Woo Park: Sungkyunkwan University (SKKU)
Doyoon Shin: Sungkyunkwan University (SKKU)
Kookheon Char: Seoul National University
Byeong Guk Jeong: Pusan National University
Ji-Sang Park: Sungkyunkwan University (SKKU)
Euyheon Hwang: Sungkyunkwan University (SKKU)
Doh C. Lee: KAIST Institute for the Nanocentury, Korea Advanced Institute of Science and Technology (KAIST)
Young-Shin Park: Chemistry Division, Los Alamos National Laboratory
Hyung-Jun Song: Seoul National University of Science and Technology
Jun Hyuk Chang: University of Chicago
Wan Ki Bae: Sungkyunkwan University (SKKU)

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract Colloidal Ag(In,Ga)S2 nanocrystals (AIGS NCs) with the band gap tunability by their size and composition within visible range have garnered surging interest. High absorption cross-section and narrow emission linewidth of AIGS NCs make them ideally suited to address the challenges of Cd-free NCs in wide-ranging photonic applications. However, AIGS NCs have shown relatively underwhelming photoluminescence quantum yield (PL QY) to date, primarily because coherent heteroepitaxy has not been realized. Here, we report the heteroepitaxy for AIGS-AgGaS2 (AIGS-AGS) core-shell NCs bearing near-unity PL QYs in almost full visible range (460 to 620 nm) and enhanced photochemical stability. Key to the successful growth of AIGS-AGS NCs is the use of the Ag-S-Ga(OA)2 complex, which complements the reactivities among cations for both homogeneous AIGS cores in various compositions and uniform AGS shell growth. The heteroepitaxy between AIGS and AGS results in the Type I heterojunction that effectively confines charge carriers within the emissive core without optically active interfacial defects. AIGS-AGS NCs show higher extinction coefficient and narrower spectral linewidth compared to state-of-the-art heavy metal-free NCs, prompting their immediate use in practicable applications including displays and luminescent solar concentrators (LSCs).

Date: 2023
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DOI: 10.1038/s41467-023-39509-y

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