Coherent heteroepitaxial growth of I-III-VI2 Ag(In,Ga)S2 colloidal nanocrystals with near-unity quantum yield for use in luminescent solar concentrators
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...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2023-06-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-023-39509-y |
| _version_ | 1797795614777409536 |
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| author | 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 Wan Ki Bae |
| author_facet | 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 Wan Ki Bae |
| author_sort | Hak June Lee |
| collection | DOAJ |
| description | 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). |
| first_indexed | 2024-03-13T03:20:39Z |
| format | Article |
| id | doaj.art-e22faa9bc3f8472e86aee1a9feeee9aa |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-13T03:20:39Z |
| publishDate | 2023-06-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-e22faa9bc3f8472e86aee1a9feeee9aa2023-06-25T11:22:05ZengNature PortfolioNature Communications2041-17232023-06-0114111110.1038/s41467-023-39509-yCoherent heteroepitaxial growth of I-III-VI2 Ag(In,Ga)S2 colloidal nanocrystals with near-unity quantum yield for use in luminescent solar concentratorsHak June Lee0Seongbin Im1Dongju Jung2Kyuri Kim3Jong Ah Chae4Jaemin Lim5Jeong Woo Park6Doyoon Shin7Kookheon Char8Byeong Guk Jeong9Ji-Sang Park10Euyheon Hwang11Doh C. Lee12Young-Shin Park13Hyung-Jun Song14Jun Hyuk Chang15Wan Ki Bae16SKKU Advanced Institute of Nanotechnology (SAINT), Sungkyunkwan University (SKKU)SKKU Advanced Institute of Nanotechnology (SAINT), Sungkyunkwan University (SKKU)SKKU Advanced Institute of Nanotechnology (SAINT), Sungkyunkwan University (SKKU)SKKU Advanced Institute of Nanotechnology (SAINT), Sungkyunkwan University (SKKU)SKKU Advanced Institute of Nanotechnology (SAINT), Sungkyunkwan University (SKKU)SKKU Advanced Institute of Nanotechnology (SAINT), Sungkyunkwan University (SKKU)SKKU Advanced Institute of Nanotechnology (SAINT), Sungkyunkwan University (SKKU)SKKU Advanced Institute of Nanotechnology (SAINT), Sungkyunkwan University (SKKU)School of Chemical and Biological Engineering, Seoul National UniversitySchool of Chemical and Biomolecular Engineering, Pusan National UniversitySKKU Advanced Institute of Nanotechnology (SAINT), Sungkyunkwan University (SKKU)SKKU Advanced Institute of Nanotechnology (SAINT), Sungkyunkwan University (SKKU)Department of Chemical and Biomolecular Engineering, KAIST Institute for the Nanocentury, Korea Advanced Institute of Science and Technology (KAIST)Chemistry Division, Los Alamos National LaboratoryDepartment of Safety Engineering, Seoul National University of Science and TechnologyDepartment of Chemistry, James Franck Institute, and Pritzker School of Molecular Engineering, University of ChicagoSKKU Advanced Institute of Nanotechnology (SAINT), Sungkyunkwan University (SKKU)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).https://doi.org/10.1038/s41467-023-39509-y |
| spellingShingle | 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 Wan Ki Bae Coherent heteroepitaxial growth of I-III-VI2 Ag(In,Ga)S2 colloidal nanocrystals with near-unity quantum yield for use in luminescent solar concentrators Nature Communications |
| title | Coherent heteroepitaxial growth of I-III-VI2 Ag(In,Ga)S2 colloidal nanocrystals with near-unity quantum yield for use in luminescent solar concentrators |
| title_full | Coherent heteroepitaxial growth of I-III-VI2 Ag(In,Ga)S2 colloidal nanocrystals with near-unity quantum yield for use in luminescent solar concentrators |
| title_fullStr | Coherent heteroepitaxial growth of I-III-VI2 Ag(In,Ga)S2 colloidal nanocrystals with near-unity quantum yield for use in luminescent solar concentrators |
| title_full_unstemmed | Coherent heteroepitaxial growth of I-III-VI2 Ag(In,Ga)S2 colloidal nanocrystals with near-unity quantum yield for use in luminescent solar concentrators |
| title_short | Coherent heteroepitaxial growth of I-III-VI2 Ag(In,Ga)S2 colloidal nanocrystals with near-unity quantum yield for use in luminescent solar concentrators |
| title_sort | coherent heteroepitaxial growth of i iii vi2 ag in ga s2 colloidal nanocrystals with near unity quantum yield for use in luminescent solar concentrators |
| url | https://doi.org/10.1038/s41467-023-39509-y |
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