Naif S. Alharthi, Salim A. Thomas, Reed J. Petersen, Kenneth J. Anderson, Todd A. Pringle, Dmitri Kilin, Erik K. Hobbie
{"title":"表面钝化二维层状碳化硅纳米晶体的温度依赖性光致发光","authors":"Naif S. Alharthi, Salim A. Thomas, Reed J. Petersen, Kenneth J. Anderson, Todd A. Pringle, Dmitri Kilin, Erik K. Hobbie","doi":"10.1021/acs.jpcc.5c01576","DOIUrl":null,"url":null,"abstract":"Ligand-passivated 2D-layered SiC nanocrystals (NCs) are suspended in a cross-linked polymer to measure their cryogenic photoluminescence (PL). Three scenarios are queried based on surface chemistry as dictated by sample history. Samples exposed to oxygen during processing are dominated by nonradiative recombination despite full passivation, showing broad PL and relatively low (10–20%) quantum yields (QYs) that increase only modestly with cooling. In contrast, both fully and partially passivated samples shielded from oxygen show much stronger radiative recombination with bright narrow blue PL and higher QYs that increase markedly under cryogenic conditions. We compare these results to room-temperature radiative rates measured for size-purified fractions derived from analogous colloidal parents. From the multipeak PL structure exhibited by the shielded nanocomposites under cryogenic conditions, we invoke a Franck–Condon argument to link the bright narrow emission to surface SiCH<sub><i>x</i></sub>, while the weak PL in exposed samples is linked to surface bridging oxygen. The results have important implications for visible light emission from all forms of nanostructured SiC.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"5 1","pages":""},"PeriodicalIF":3.2000,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Temperature-Dependent Photoluminescence of Surface-Passivated 2D-Layered Silicon Carbide Nanocrystals\",\"authors\":\"Naif S. Alharthi, Salim A. Thomas, Reed J. Petersen, Kenneth J. Anderson, Todd A. Pringle, Dmitri Kilin, Erik K. Hobbie\",\"doi\":\"10.1021/acs.jpcc.5c01576\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Ligand-passivated 2D-layered SiC nanocrystals (NCs) are suspended in a cross-linked polymer to measure their cryogenic photoluminescence (PL). Three scenarios are queried based on surface chemistry as dictated by sample history. Samples exposed to oxygen during processing are dominated by nonradiative recombination despite full passivation, showing broad PL and relatively low (10–20%) quantum yields (QYs) that increase only modestly with cooling. In contrast, both fully and partially passivated samples shielded from oxygen show much stronger radiative recombination with bright narrow blue PL and higher QYs that increase markedly under cryogenic conditions. We compare these results to room-temperature radiative rates measured for size-purified fractions derived from analogous colloidal parents. From the multipeak PL structure exhibited by the shielded nanocomposites under cryogenic conditions, we invoke a Franck–Condon argument to link the bright narrow emission to surface SiCH<sub><i>x</i></sub>, while the weak PL in exposed samples is linked to surface bridging oxygen. The results have important implications for visible light emission from all forms of nanostructured SiC.\",\"PeriodicalId\":61,\"journal\":{\"name\":\"The Journal of Physical Chemistry C\",\"volume\":\"5 1\",\"pages\":\"\"},\"PeriodicalIF\":3.2000,\"publicationDate\":\"2025-05-27\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"The Journal of Physical Chemistry C\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.jpcc.5c01576\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"The Journal of Physical Chemistry C","FirstCategoryId":"1","ListUrlMain":"https://doi.org/10.1021/acs.jpcc.5c01576","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Temperature-Dependent Photoluminescence of Surface-Passivated 2D-Layered Silicon Carbide Nanocrystals
Ligand-passivated 2D-layered SiC nanocrystals (NCs) are suspended in a cross-linked polymer to measure their cryogenic photoluminescence (PL). Three scenarios are queried based on surface chemistry as dictated by sample history. Samples exposed to oxygen during processing are dominated by nonradiative recombination despite full passivation, showing broad PL and relatively low (10–20%) quantum yields (QYs) that increase only modestly with cooling. In contrast, both fully and partially passivated samples shielded from oxygen show much stronger radiative recombination with bright narrow blue PL and higher QYs that increase markedly under cryogenic conditions. We compare these results to room-temperature radiative rates measured for size-purified fractions derived from analogous colloidal parents. From the multipeak PL structure exhibited by the shielded nanocomposites under cryogenic conditions, we invoke a Franck–Condon argument to link the bright narrow emission to surface SiCHx, while the weak PL in exposed samples is linked to surface bridging oxygen. The results have important implications for visible light emission from all forms of nanostructured SiC.
期刊介绍:
The Journal of Physical Chemistry A/B/C is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.