期刊
NANO LETTERS
卷 17, 期 8, 页码 4624-4633出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.7b01047
关键词
Crystallization by particle attachment; nanoparticle building blocks; pulsed laser deposition; molecular dynamics simulation
类别
资金
- U.S. Department of Energy, Office of Science, Basic Energy Sciences (BES), Materials Sciences and Engineering Division
- Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]
Nonequilibrium growth pathways for crystalline nano structures with metastable phases are demonstrated through the gas-phase formation, attachment, and crystallization of ultrasmall amorphous nanoparticles as building blocks in pulsed laser deposition (PLD). Temporally and spatially resolved gated-intensified charge couple device (ICCD) imaging and ion probe measurements are employed as in situ diagnostics to understand and control the plume expansion conditions for the synthesis of nearly pure fluxes of ultrasmall (similar to 3 nm) amorphous TiO2 nanoparticles in background gases and their selective delivery to substrates. These amorphous nanoparticles assemble into loose, mesoporous assemblies on substrates at room temperature but dynamically crystallize by sequential particle attachment at higher substrate temperatures to grow nanostructures with different phases and morphologies. Molecular dynamics calculations are used to simulate and understand the crystallization dynamics. This work demonstrates that nonequilibrium crystallization by particle attachment of metastable ultrasmall nanoscale building blocks provides a versatile approach for exploring and controlling the growth of nanoarchitectures with desirable crystalline phases and morphologies.
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