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Title: Multicomponent Oxynitride Thin Films: Precise Growth Control and Excited State Dynamics

Abstract

Multicomponent oxynitrides significantly broadens the library of material design and promise wide applications for optoelectronics and solar energy conversion. Controlled growth of multicomponent oxynitrides with defined stoichiometry, uniformity, morphology and scalability has been challenging. In this work, we demonstrate wafer-scale growth of uniform, crystalline GaN:ZnO thin films with tunable stoichiometry, digitally-controlled film thickness and atomically smooth surface, at a process temperature as low as room temperature. In comparison to the particle form that is commonly encountered, the GaN:ZnO thin films studied here bypass the limitations imposed by surface or size implications and reveal the intrinsic nature of optical absorption in this system. The GaN:ZnO thin films demonstrate strong visible light absorption at the composition of (GaN) 0.67(ZnO) 0.33, and enables the first quantitative determination of bulk absorption coefficients in this system. Based on transient absorption spectroscopy measurements, photocarriers of GaN:ZnO thin films, excited by an ultraviolet or a visible pump, present nearly identical relaxation dynamics, indicating a direct gap origin of the visible light absorption. This is consistent with complimentary steady-state optical absorption measurements and first-principle calculations. The ability to precisely control the growth of functional oxynitrides across the multicomponent scale is critical to advance materials modeling and design formore » various applications.« less

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [1]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. Naval Research Lab. (NRL), Washington, DC (United States)
  3. Stony Brook Univ., NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1524552
Report Number(s):
BNL-211709-2019-JAAM
Journal ID: ISSN 0897-4756
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 31; Journal Issue: 9; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Zhang, Wenrui, Lyons, John L., Cen, Jiajie, Sfeir, Matthew Y., and Liu, Mingzhao. Multicomponent Oxynitride Thin Films: Precise Growth Control and Excited State Dynamics. United States: N. p., 2019. Web. doi:10.1021/acs.chemmater.9b00656.
Zhang, Wenrui, Lyons, John L., Cen, Jiajie, Sfeir, Matthew Y., & Liu, Mingzhao. Multicomponent Oxynitride Thin Films: Precise Growth Control and Excited State Dynamics. United States. doi:10.1021/acs.chemmater.9b00656.
Zhang, Wenrui, Lyons, John L., Cen, Jiajie, Sfeir, Matthew Y., and Liu, Mingzhao. Fri . "Multicomponent Oxynitride Thin Films: Precise Growth Control and Excited State Dynamics". United States. doi:10.1021/acs.chemmater.9b00656.
@article{osti_1524552,
title = {Multicomponent Oxynitride Thin Films: Precise Growth Control and Excited State Dynamics},
author = {Zhang, Wenrui and Lyons, John L. and Cen, Jiajie and Sfeir, Matthew Y. and Liu, Mingzhao},
abstractNote = {Multicomponent oxynitrides significantly broadens the library of material design and promise wide applications for optoelectronics and solar energy conversion. Controlled growth of multicomponent oxynitrides with defined stoichiometry, uniformity, morphology and scalability has been challenging. In this work, we demonstrate wafer-scale growth of uniform, crystalline GaN:ZnO thin films with tunable stoichiometry, digitally-controlled film thickness and atomically smooth surface, at a process temperature as low as room temperature. In comparison to the particle form that is commonly encountered, the GaN:ZnO thin films studied here bypass the limitations imposed by surface or size implications and reveal the intrinsic nature of optical absorption in this system. The GaN:ZnO thin films demonstrate strong visible light absorption at the composition of (GaN)0.67(ZnO)0.33, and enables the first quantitative determination of bulk absorption coefficients in this system. Based on transient absorption spectroscopy measurements, photocarriers of GaN:ZnO thin films, excited by an ultraviolet or a visible pump, present nearly identical relaxation dynamics, indicating a direct gap origin of the visible light absorption. This is consistent with complimentary steady-state optical absorption measurements and first-principle calculations. The ability to precisely control the growth of functional oxynitrides across the multicomponent scale is critical to advance materials modeling and design for various applications.},
doi = {10.1021/acs.chemmater.9b00656},
journal = {Chemistry of Materials},
number = 9,
volume = 31,
place = {United States},
year = {2019},
month = {4}
}

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