Matthew P. Hautzinger, Shaham Quadir, Benjamin Feingold, Reilly Seban, Arianna J. Thornton, Nikita S. Dutta, Andrew G. Norman, Ian A. Leahy, Muhammad Rubaiat Hasan, Kirill A. Kovnir, Obadiah G. Reid, Bryon W. Larson, Joseph M. Luther, Matthew C. Beard, Sage R. Bauers
{"title":"光电用zintl相BaCd2P2量子点的合成与表征","authors":"Matthew P. Hautzinger, Shaham Quadir, Benjamin Feingold, Reilly Seban, Arianna J. Thornton, Nikita S. Dutta, Andrew G. Norman, Ian A. Leahy, Muhammad Rubaiat Hasan, Kirill A. Kovnir, Obadiah G. Reid, Bryon W. Larson, Joseph M. Luther, Matthew C. Beard, Sage R. Bauers","doi":"10.1021/acsnano.5c02271","DOIUrl":null,"url":null,"abstract":"We demonstrate the growth of size-controlled, high optical quality Zintl-phase BaCd<sub>2</sub>P<sub>2</sub> colloidal quantum dots (QDs), an emerging semiconductor absorbing/emitting in the red and predicted to have favorable defect chemistry. The QDs are grown via hot injection of a phosphorus precursor into a solution of solubilized Ba and Cd precursors. The absorbance and photoluminescence (PL) are tunable via growth temperature and show a bandgap ranging from 1.47 to 1.81 eV, depending on the size, which ranges from 3 to 9 nm based on electron microscopy. Selected area electron diffraction is used to determine that the BaCd<sub>2</sub>P<sub>2</sub> QDs crystallize in the <i>P</i>3̅<i>m</i>1 space group, same as the bulk material. Raman spectroscopy, powder X-ray diffraction, and X-ray fluorescence studies further confirm that BaCd<sub>2</sub>P<sub>2</sub> QDs match those of the crystalline phase bulk material. The high optoelectronic quality is assessed by quantification of long-lived photoexcited carriers (∼160 ns average weighting), as determined by time-resolved PL spectroscopy, and bright red visible emission (∼21% PL quantum yield) despite no complex surface passivation. Furthermore, a demonstration of thin-film fabrication is shown via a solid state ligand exchange protocol. This synthetic protocol enables researchers to explore and utilize BaCd<sub>2</sub>P<sub>2</sub> Zintl-phase QDs, as well as adjacent compositions, for a variety of optoelectronic applications enabled by their semiconducting properties.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"102 1","pages":""},"PeriodicalIF":16.0000,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Synthesis and Characterization of Zintl-Phase BaCd2P2 Quantum Dots for Optoelectronic Applications\",\"authors\":\"Matthew P. Hautzinger, Shaham Quadir, Benjamin Feingold, Reilly Seban, Arianna J. Thornton, Nikita S. Dutta, Andrew G. Norman, Ian A. Leahy, Muhammad Rubaiat Hasan, Kirill A. Kovnir, Obadiah G. Reid, Bryon W. Larson, Joseph M. Luther, Matthew C. Beard, Sage R. Bauers\",\"doi\":\"10.1021/acsnano.5c02271\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"We demonstrate the growth of size-controlled, high optical quality Zintl-phase BaCd<sub>2</sub>P<sub>2</sub> colloidal quantum dots (QDs), an emerging semiconductor absorbing/emitting in the red and predicted to have favorable defect chemistry. The QDs are grown via hot injection of a phosphorus precursor into a solution of solubilized Ba and Cd precursors. The absorbance and photoluminescence (PL) are tunable via growth temperature and show a bandgap ranging from 1.47 to 1.81 eV, depending on the size, which ranges from 3 to 9 nm based on electron microscopy. Selected area electron diffraction is used to determine that the BaCd<sub>2</sub>P<sub>2</sub> QDs crystallize in the <i>P</i>3̅<i>m</i>1 space group, same as the bulk material. Raman spectroscopy, powder X-ray diffraction, and X-ray fluorescence studies further confirm that BaCd<sub>2</sub>P<sub>2</sub> QDs match those of the crystalline phase bulk material. The high optoelectronic quality is assessed by quantification of long-lived photoexcited carriers (∼160 ns average weighting), as determined by time-resolved PL spectroscopy, and bright red visible emission (∼21% PL quantum yield) despite no complex surface passivation. Furthermore, a demonstration of thin-film fabrication is shown via a solid state ligand exchange protocol. This synthetic protocol enables researchers to explore and utilize BaCd<sub>2</sub>P<sub>2</sub> Zintl-phase QDs, as well as adjacent compositions, for a variety of optoelectronic applications enabled by their semiconducting properties.\",\"PeriodicalId\":21,\"journal\":{\"name\":\"ACS Nano\",\"volume\":\"102 1\",\"pages\":\"\"},\"PeriodicalIF\":16.0000,\"publicationDate\":\"2025-03-24\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Nano\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1021/acsnano.5c02271\",\"RegionNum\":1,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Nano","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1021/acsnano.5c02271","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Synthesis and Characterization of Zintl-Phase BaCd2P2 Quantum Dots for Optoelectronic Applications
We demonstrate the growth of size-controlled, high optical quality Zintl-phase BaCd2P2 colloidal quantum dots (QDs), an emerging semiconductor absorbing/emitting in the red and predicted to have favorable defect chemistry. The QDs are grown via hot injection of a phosphorus precursor into a solution of solubilized Ba and Cd precursors. The absorbance and photoluminescence (PL) are tunable via growth temperature and show a bandgap ranging from 1.47 to 1.81 eV, depending on the size, which ranges from 3 to 9 nm based on electron microscopy. Selected area electron diffraction is used to determine that the BaCd2P2 QDs crystallize in the P3̅m1 space group, same as the bulk material. Raman spectroscopy, powder X-ray diffraction, and X-ray fluorescence studies further confirm that BaCd2P2 QDs match those of the crystalline phase bulk material. The high optoelectronic quality is assessed by quantification of long-lived photoexcited carriers (∼160 ns average weighting), as determined by time-resolved PL spectroscopy, and bright red visible emission (∼21% PL quantum yield) despite no complex surface passivation. Furthermore, a demonstration of thin-film fabrication is shown via a solid state ligand exchange protocol. This synthetic protocol enables researchers to explore and utilize BaCd2P2 Zintl-phase QDs, as well as adjacent compositions, for a variety of optoelectronic applications enabled by their semiconducting properties.
期刊介绍:
ACS Nano, published monthly, serves as an international forum for comprehensive articles on nanoscience and nanotechnology research at the intersections of chemistry, biology, materials science, physics, and engineering. The journal fosters communication among scientists in these communities, facilitating collaboration, new research opportunities, and advancements through discoveries. ACS Nano covers synthesis, assembly, characterization, theory, and simulation of nanostructures, nanobiotechnology, nanofabrication, methods and tools for nanoscience and nanotechnology, and self- and directed-assembly. Alongside original research articles, it offers thorough reviews, perspectives on cutting-edge research, and discussions envisioning the future of nanoscience and nanotechnology.