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Title: | Experimental measurement of the diamond nucleation landscape reveals classical and nonclassical features | Authors: | Gebbie, Matthew A. Ishiwata, Hitoshi McQuade, Patrick J. Petrak, Vaclav Taylor, Andrew FREIWALD, Christopher Dahl, Jeremy E. Carlson, Robert M. K. Fokin, Andrey A. Schreiner, Peter R. Shen, Zhi-Xun NESLADEK, Milos Melosha, Nicholas A. |
Issue Date: | 2018 | Publisher: | NATL ACAD SCIENCES | Source: | PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 115(33), p. 8284-8289 | Abstract: | Nucleation is a core scientific concept that describes the formation of new phases and materials. While classical nucleation theory is applied across wide-ranging fields, nucleation energy landscapes have never been directly measured at the atomic level, and experiments suggest that nucleation rates often greatly exceed the predictions of classical nucleation theory. Multistep nucleation via metastable states could explain unexpectedly rapid nucleation in many contexts, yet experimental energy landscapes supporting such mechanisms are scarce, particularly at nanoscale dimensions. In this work, we measured the nucleation energy landscape of diamond during chemical vapor deposition, using a series of diamondoid molecules as atomically defined protonuclei. We find that 26-carbon atom clusters, which do not contain a single bulk atom, are postcritical nuclei and measure the nucleation barrier to be more than four orders of magnitude smaller than prior bulk estimations. These data support both classical and nonclassical concepts for multistep nucleation and growth during the gas-phase synthesis of diamond and other semiconductors. More broadly, these measurements provide experimental evidence that agrees with recent conceptual proposals of multistep nucleation pathways with metastable molecular precursors in diverse processes, ranging from cloud formation to protein crystallization, and nanoparticle synthesis. | Notes: | [Gebbie, Matthew A.; McQuade, Patrick J.; Melosha, Nicholas A.] Stanford Univ, Dept Mat Sci & Engn, Stanford, CA 94305 USA. [Gebbie, Matthew A.; Ishiwata, Hitoshi; McQuade, Patrick J.; Dahl, Jeremy E.; Carlson, Robert M. K.; Shen, Zhi-Xun; Melosha, Nicholas A.] SLAC Natl Accelerator Lab, Stanford Inst Mat & Energy Sci, Menlo Pk, CA 94025 USA. [Ishiwata, Hitoshi] Tokyo Inst Technol, Dept Elect & Elect Engn, Meguro Ku, Tokyo 1528550, Japan. [Petrak, Vaclav; Taylor, Andrew] Czech Acad Sci, Inst Phys, CZ-18221 Prague, Czech Republic. [Freiwald, Christopher; Nesladek, Milos] Univ Hasselt, Inst Mat Res, B-3590 Diepenbeek, Belgium. [Freiwald, Christopher; Nesladek, Milos] Interuniv Microelect Ctr, Inst Mat Res Microelect, B-3590 Diepenbeek, Belgium. [Fokin, Andrey A.; Schreiner, Peter R.] Justus Liebig Univ, Inst Organ Chem, D-35392 Giessen, Germany. [Fokin, Andrey A.] Igor Sikorsky Kiev Polytech Inst, Dept Organ Chem, UA-03056 Kiev, Ukraine. [Shen, Zhi-Xun] Stanford Univ, Appl Phys, Stanford, CA 94305 USA. | Keywords: | nucleation; diamond; nanomaterials; thermodynamics; plasma synthesis;nucleation; diamond; nanomaterials; thermodynamics; plasma synthesis | Document URI: | http://hdl.handle.net/1942/28452 | ISSN: | 0027-8424 | e-ISSN: | 1091-6490 | DOI: | 10.1073/pnas.1803654115 | ISI #: | 000441638200042 | Category: | A1 | Type: | Journal Contribution | Validations: | ecoom 2019 |
Appears in Collections: | Research publications |
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