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Title: Infiltrated Zinc Oxide in Poly(methyl methacrylate): An Atomic Cycle Growth Study

Abstract

We have investigated the growth of zinc oxide in a polymer matrix by sequential infiltration synthesis (SiS). The atomic cycle-by-cycle self-terminating reaction growth investigation was done using photoluminescence (PL), Raman, and X-ray photoemission spectroscopy (XPS). Results show clear differences between Zn atom configurations at the initial stages of growth. Mono Zn atoms (O-Zn and O-Zn-O) exhibit pure UV emission with little evidence of deep level oxygen vacancy states (VO). Dimer Zn atoms (O-Zn-O-Zn and O-Zn-O-Zn-O) show strong UV and visible PL emission from VO states 20 times greater than that from the mono Zn atom configuration. After three precursor cycles, the PL emission intensity drops significantly exhibiting first evidence of crystal formation as observed with Raman spectroscopy via the presence of longitudinal optical phonons. We also report a first confirmation of energy transfer between polymer and ZnO where the polymer absorbs light at 241 nm and emits at 360 nm, which coincides with the ZnO UV emission peak. Our work shows that ZnO dimers are unique ZnO configurations with high PL intensity, unique O1s oxidation states, and sub-10 ps absorption and decay, which are interesting properties for novel quantum material applications.

Authors:
ORCiD logo [1];  [2];  [1];  [1];  [1]
  1. Argonne National Laboratory, 9700 South Cass Avenue, Argonne, Illinois 60439, United States
  2. Vassar College, 124 Raymond Avenure, Poughkeepsie, New York 12604, United States
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE U.S. Department of Energy; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); University of Chicago - Materials Research Science & Engineering Center (MRSEC)
OSTI Identifier:
1433052
DOE Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 121; Journal Issue: 3; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
Raman spectroscopy; XPS; Zinc oxide; infiltration; photoluminescence; polymethyl methacrylate

Citation Formats

Ocola, Leonidas E., Connolly, Aine, Gosztola, David J., Schaller, Richard D., and Yanguas-Gil, Angel. Infiltrated Zinc Oxide in Poly(methyl methacrylate): An Atomic Cycle Growth Study. United States: N. p., 2016. Web. doi:10.1021/acs.jpcc.6b08007.
Ocola, Leonidas E., Connolly, Aine, Gosztola, David J., Schaller, Richard D., & Yanguas-Gil, Angel. Infiltrated Zinc Oxide in Poly(methyl methacrylate): An Atomic Cycle Growth Study. United States. doi:10.1021/acs.jpcc.6b08007.
Ocola, Leonidas E., Connolly, Aine, Gosztola, David J., Schaller, Richard D., and Yanguas-Gil, Angel. Fri . "Infiltrated Zinc Oxide in Poly(methyl methacrylate): An Atomic Cycle Growth Study". United States. doi:10.1021/acs.jpcc.6b08007.
@article{osti_1433052,
title = {Infiltrated Zinc Oxide in Poly(methyl methacrylate): An Atomic Cycle Growth Study},
author = {Ocola, Leonidas E. and Connolly, Aine and Gosztola, David J. and Schaller, Richard D. and Yanguas-Gil, Angel},
abstractNote = {We have investigated the growth of zinc oxide in a polymer matrix by sequential infiltration synthesis (SiS). The atomic cycle-by-cycle self-terminating reaction growth investigation was done using photoluminescence (PL), Raman, and X-ray photoemission spectroscopy (XPS). Results show clear differences between Zn atom configurations at the initial stages of growth. Mono Zn atoms (O-Zn and O-Zn-O) exhibit pure UV emission with little evidence of deep level oxygen vacancy states (VO). Dimer Zn atoms (O-Zn-O-Zn and O-Zn-O-Zn-O) show strong UV and visible PL emission from VO states 20 times greater than that from the mono Zn atom configuration. After three precursor cycles, the PL emission intensity drops significantly exhibiting first evidence of crystal formation as observed with Raman spectroscopy via the presence of longitudinal optical phonons. We also report a first confirmation of energy transfer between polymer and ZnO where the polymer absorbs light at 241 nm and emits at 360 nm, which coincides with the ZnO UV emission peak. Our work shows that ZnO dimers are unique ZnO configurations with high PL intensity, unique O1s oxidation states, and sub-10 ps absorption and decay, which are interesting properties for novel quantum material applications.},
doi = {10.1021/acs.jpcc.6b08007},
journal = {Journal of Physical Chemistry. C},
issn = {1932-7447},
number = 3,
volume = 121,
place = {United States},
year = {2016},
month = {12}
}