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http://hdl.handle.net/1942/28452
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DC Field | Value | Language |
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dc.contributor.author | Gebbie, Matthew A. | - |
dc.contributor.author | Ishiwata, Hitoshi | - |
dc.contributor.author | McQuade, Patrick J. | - |
dc.contributor.author | Petrak, Vaclav | - |
dc.contributor.author | Taylor, Andrew | - |
dc.contributor.author | FREIWALD, Christopher | - |
dc.contributor.author | Dahl, Jeremy E. | - |
dc.contributor.author | Carlson, Robert M. K. | - |
dc.contributor.author | Fokin, Andrey A. | - |
dc.contributor.author | Schreiner, Peter R. | - |
dc.contributor.author | Shen, Zhi-Xun | - |
dc.contributor.author | NESLADEK, Milos | - |
dc.contributor.author | Melosha, Nicholas A. | - |
dc.date.accessioned | 2019-06-18T11:20:19Z | - |
dc.date.available | 2019-06-18T11:20:19Z | - |
dc.date.issued | 2018 | - |
dc.identifier.citation | PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 115(33), p. 8284-8289 | - |
dc.identifier.issn | 0027-8424 | - |
dc.identifier.uri | http://hdl.handle.net/1942/28452 | - |
dc.description.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. | - |
dc.description.sponsorship | This work was supported by the Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering, under Contract DE-AC02-76SF00515. M.A.G. acknowledges the funding provided by the Geballe Laboratory for Advanced Materials Postdoctoral Fellowship program at Stanford University. C.F. and M.N. acknowledge support of the Flemish Funds for Scientific Research (FWO), Project G0E7417N (Single-Atom Diamond Quantum Probe: Proof-of-Principle Molecular Engineering Methodology and ERANET Project Nanobit). Part of this work was performed at the Stanford Nano Shared Facilities, supported by the National Science Foundation under Award ECCS-1542152. | - |
dc.language.iso | en | - |
dc.publisher | NATL ACAD SCIENCES | - |
dc.subject.other | nucleation; diamond; nanomaterials; thermodynamics; plasma synthesis | - |
dc.subject.other | nucleation; diamond; nanomaterials; thermodynamics; plasma synthesis | - |
dc.title | Experimental measurement of the diamond nucleation landscape reveals classical and nonclassical features | - |
dc.type | Journal Contribution | - |
dc.identifier.epage | 8289 | - |
dc.identifier.issue | 33 | - |
dc.identifier.spage | 8284 | - |
dc.identifier.volume | 115 | - |
local.format.pages | 6 | - |
local.bibliographicCitation.jcat | A1 | - |
dc.description.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. | - |
local.publisher.place | WASHINGTON | - |
local.type.refereed | Refereed | - |
local.type.specified | Article | - |
dc.identifier.doi | 10.1073/pnas.1803654115 | - |
dc.identifier.isi | 000441638200042 | - |
item.contributor | Gebbie, Matthew A. | - |
item.contributor | Ishiwata, Hitoshi | - |
item.contributor | McQuade, Patrick J. | - |
item.contributor | Petrak, Vaclav | - |
item.contributor | Taylor, Andrew | - |
item.contributor | FREIWALD, Christopher | - |
item.contributor | Dahl, Jeremy E. | - |
item.contributor | Carlson, Robert M. K. | - |
item.contributor | Fokin, Andrey A. | - |
item.contributor | Schreiner, Peter R. | - |
item.contributor | Shen, Zhi-Xun | - |
item.contributor | NESLADEK, Milos | - |
item.contributor | Melosha, Nicholas A. | - |
item.fullcitation | 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. (2018) Experimental measurement of the diamond nucleation landscape reveals classical and nonclassical features. In: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 115(33), p. 8284-8289. | - |
item.accessRights | Restricted Access | - |
item.fulltext | With Fulltext | - |
item.validation | ecoom 2019 | - |
crisitem.journal.issn | 0027-8424 | - |
crisitem.journal.eissn | 1091-6490 | - |
Appears in Collections: | Research publications |
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8284.full.pdf Restricted Access | Published version | 942.44 kB | Adobe PDF | View/Open Request a copy |
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