دورية أكاديمية

Navigating the Potential Energy Surface of CdSe Magic-Sized Clusters: Synthesis and Interconversion of Atomically Precise Nanocrystal Polymorphs.

التفاصيل البيبلوغرافية
العنوان: Navigating the Potential Energy Surface of CdSe Magic-Sized Clusters: Synthesis and Interconversion of Atomically Precise Nanocrystal Polymorphs.
المؤلفون: Ripberger HH; Department of Chemistry, University of Washington, Seattle, Washington 98195-1700, United States., Schnitzenbaumer KJ; Division of Natural Sciences and Mathematics, Transylvania University, Lexington, Kentucky 40508-1797, United States., Nguyen LK; Department of Chemistry, University of Washington, Seattle, Washington 98195-1700, United States., Ladd DM; Materials Science and Engineering Program, University of Colorado, Boulder, Colorado 80309, United States., Levine KR; Materials Science and Engineering Program, University of Colorado, Boulder, Colorado 80309, United States., Dayton DG; Materials Science and Engineering Program, University of Colorado, Boulder, Colorado 80309, United States., Toney MF; Materials Science and Engineering Program, University of Colorado, Boulder, Colorado 80309, United States.; Department of Chemical and Biological Engineering, Renewable and Sustainable Energy Institute, University of Colorado, Boulder, Colorado 80309, United States., Cossairt BM; Department of Chemistry, University of Washington, Seattle, Washington 98195-1700, United States.
المصدر: Journal of the American Chemical Society [J Am Chem Soc] 2023 Dec 20; Vol. 145 (50), pp. 27480-27492. Date of Electronic Publication: 2023 Dec 07.
نوع المنشور: Journal Article
اللغة: English
بيانات الدورية: Publisher: American Chemical Society Country of Publication: United States NLM ID: 7503056 Publication Model: Print-Electronic Cited Medium: Internet ISSN: 1520-5126 (Electronic) Linking ISSN: 00027863 NLM ISO Abbreviation: J Am Chem Soc Subsets: PubMed not MEDLINE; MEDLINE
أسماء مطبوعة: Publication: Washington, DC : American Chemical Society
Original Publication: Easton, Pa. [etc.]
مستخلص: Magic-sized clusters (MSCs) are kinetically stable, atomically precise intermediates along the quantum dot (QD) reaction potential energy surface. Literature precedent establishes two classes of cadmium selenide MSCs with QD-like inorganic cores: one class is proposed to be cation-rich with a zincblende crystal structure, while the other is proposed to be stoichiometric with a "wurtzite-like" core. However, the wide range of synthetic protocols used to access MSCs has made direct comparisons of their structure and surface chemistry difficult. Furthermore, the physical and chemical relationships between MSC polymorphs are yet to be established. Here, we demonstrate that both cation-rich and stoichiometric CdSe MSCs can be synthesized from identical reagents and can be interconverted through the addition of either excess cadmium or selenium precursor. The structural and compositional differences between these two polymorphs are contrasted using a combination of 1 H NMR spectroscopy, X-ray diffraction (XRD), pair distribution function (PDF) analysis, inductively coupled plasma optical emission spectroscopy, and UV-vis transient absorption spectroscopy. The subsequent polymorph interconversion reactions are monitored by UV-vis absorption spectroscopy, with evidence for an altered cluster atomic structure observed by powder XRD and PDF analysis. This work helps to simplify the complex picture of the CdSe nanocrystal landscape and provides a method to explore structure-property relationships in colloidal semiconductors through atomically precise synthesis.
تواريخ الأحداث: Date Created: 20231207 Latest Revision: 20231220
رمز التحديث: 20231220
DOI: 10.1021/jacs.3c08897
PMID: 38061033
قاعدة البيانات: MEDLINE
الوصف
تدمد:1520-5126
DOI:10.1021/jacs.3c08897