Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 139, Issue 6, Pages 2456-2463Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.6b12709
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Funding
- Northwestern University Institute for Catalysis in Energy Processes (ICEP)
- U.S. Department of Energy, Office of Basic Energy Sciences [DE-FG02-03ER15457]
- National Science Foundation Graduate Fellowship Research Program [DGE-0824162]
- MRSEC program (NSF) at the Materials Research Center [DMR-1121262]
- International Institute for Nanotechnology (IIN)
- State of Illinois through the IIN
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Operando surface-enhanced Raman spectroscopy (SERS) was used to successfully ickntify hitherto unknown dimeric methylalumina surface species during atomic layer deposition (ALD) on a silver surface. Vibrational modes associated with the bridging moieties of both trimethylaluminum (TMA) and dimethylaluminum chloride (DMACl) surface species were found during ALD. The appropriate monomer vibrational modes were:found to be absent as a result of the selective nature of SERS. Density functional theory (DFT) calculations were also performed to locate and identify the expected vibrational modes. An operando localized surface plasmon resonance (LSPR) spectrometer was utilized to account for changes in SER signal as a function of the number of ALD cycles. DMACI surface species were unable to be measured after multiple ALD cycles as a result of a loss in SERS enhancement and shift in LSPR This work highlights how operando optical spectroscopy by SERS and LSPR scattering are useful for prObing the identity and structure of the surface species involved in ALP and,, ultimately, catalytic reactions on these support materials.
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