Nonequilibrium Synthesis of TiO2 Nanoparticle “Building Blocks” for Crystal Growth by Sequential Attachment in Pulsed Laser Deposition

Mahjouri-Samani, Masoud; Tian, Mengkun; Puretzky, Alexander A.; Chi, Miaofang; Wang, Kai; Duscher, Gerd; Rouleau, Christopher M.; Eres, Gyula; Yoon, Mina; Lasseter, John C.; Xiao, Kai; Geohegan, David B.

doi:10.1021/acs.nanolett.7b01047

Nonequilibrium Synthesis of TiO₂ Nanoparticle “Building Blocks” for Crystal Growth by Sequential Attachment in Pulsed Laser Deposition

Journal Article · Mon Jul 10 00:00:00 EDT 2017 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.7b01047· OSTI ID:1484731

^[1]; ^[2]; ^[1]; ^[1]; Wang, Kai ^[1]; Duscher, Gerd ^[3]; ^[1]; ^[4]; ^[1]; Lasseter, John C. ^[1]; ^[1]; ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering
Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division

Nonequilibrium growth pathways for crystalline nanostructures 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 (~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. Our report highlights 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.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-05CH11231; AC05-00OR22725

OSTI ID:: 1484731

Alternate ID(s):: OSTI ID: 3010642

Journal Information:: Nano Letters, Journal Name: Nano Letters Journal Issue: 8 Vol. 17; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

77 NANOSCIENCE AND NANOTECHNOLOGY
Crystallization by particle attachment
molecular dynamics simulation
nanoparticle building blocks
pulsed laser deposition