Structure of Colloidal Quantum Dots from Dynamic Nuclear Polarization Surface Enhanced NMR Spectroscopy

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• 作者：Laura Piveteau ; Ta-Chung Ong ; Aaron J. Rossini ; Lyndon Emsley ; Christophe Cop茅ret ; Maksym V. Kovalenko
• 刊名：Journal of the American Chemical Society
• 出版年：2015
• 出版时间：November 4, 2015
• 年：2015
• 卷：137
• 期：43
• 页码：13964-13971
• 全文大小：436K
• ISSN：1520-5126

文摘

Understanding the chemistry of colloidal quantum dots (QDs) is primarily hampered by the lack of analytical methods to selectively and discriminately probe the QD core, QD surface and capping ligands. Here, we present a general concept for studying a broad range of QDs such as CdSe, CdTe, InP, PbSe, PbTe, CsPbBr₃, etc., capped with both organic and inorganic surface capping ligands, through dynamic nuclear polarization (DNP) surface enhanced NMR spectroscopy. DNP can enhance NMR signals by factors of 10鈥?00, thereby reducing the measurement times by 2鈥? orders of magnitude. 1D DNP enhanced spectra acquired in this way are shown to clearly distinguish QD surface atoms from those of the QD core, and environmental effects such as oxidation. Furthermore, 2D NMR correlation experiments, which were previously inconceivable for QD surfaces, are demonstrated to be readily performed with DNP and provide the bonding motifs between the QD surfaces and the capping ligands.