TY - JOUR
T1 - Infiltrated ainc oxide in poly(methyl methacrylate)
T2 - An atomic cycle growth study
AU - Ocola, Leonidas E.
AU - Connolly, Aine
AU - Gosztola, David J.
AU - Schaller, Richard D.
AU - Yanguas-Gil, Angel
N1 - Funding Information:
Use of the Center for Nanoscale Materials, an Office of Science user facility, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. This work was also supported by the University of Chicago Materials Research Center (MRSEC) IRG3-Engineering Quantum Materials and Interactions Contract #2-60700-95. The authors acknowledge the support of Alex Zinovev for access and training on the XPS tool for this work. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357, with the EXAFS data being collected at 9-BM-B.
Publisher Copyright:
© 2016 American Chemical Society.
PY - 2017/1/26
Y1 - 2017/1/26
N2 - 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.
AB - 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.
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U2 - 10.1021/acs.jpcc.6b08007
DO - 10.1021/acs.jpcc.6b08007
M3 - Article
AN - SCOPUS:85025446717
SN - 1932-7447
VL - 121
SP - 1893
EP - 1903
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
IS - 3
ER -