Size and Purity Control of HPHT Nanodiamonds down to 1 nm

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• 作者：Stepan Stehlik ; Marian Varga ; Martin Ledinsky ; Vit Jirasek ; Anna Artemenko ; Halyna Kozak ; Lukas Ondic ; Viera Skakalova ; Giacomo Argentero ; Timothy Pennycook ; Jannik C. Meyer ; Antonin Fejfar ; Alexander Kromka ; Bohuslav Rezek
• 刊名：Journal of Physical Chemistry C
• 出版年：2015
• 出版时间：December 10, 2015
• 年：2015
• 卷：119
• 期：49
• 页码：27708-27720
• 全文大小：694K
• ISSN：1932-7455

文摘

High-pressure high-temperature (HPHT) nanodiamonds originate from grinding of diamond microcrystals obtained by HPHT synthesis. Here we report on a simple two-step approach to obtain as small as 1.1 nm HPHT nanodiamonds of excellent purity and crystallinity, which are among the smallest artificially prepared nanodiamonds ever shown and characterized. Moreover we provide experimental evidence of diamond stability down to 1 nm. Controlled annealing at 450 掳C in air leads to efficient purification from the nondiamond carbon (shells and dots), as evidenced by X-ray photoelectron spectroscopy, Raman spectroscopy, photoluminescence spectroscopy, and scanning transmission electron microscopy. Annealing at 500 掳C promotes, besides of purification, also size reduction of nanodiamonds down to 鈭? nm. Comparably short (1 h) centrifugation of the nanodiamonds aqueous colloidal solution ensures separation of the sub-10 nm fraction. Calculations show that an asymmetry of Raman diamond peak of sub-10 nm HPHT nanodiamonds can be well explained by modified phonon confinement model when the actual particle size distribution is taken into account. In contrast, larger Raman peak asymmetry commonly observed in Raman spectra of detonation nanodiamonds is mainly attributed to defects rather than to the phonon confinement. Thus, the obtained characteristics reflect high material quality including nanoscale effects in sub-10 nm HPHT nanodiamonds prepared by the presented method.