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Title: Energy transfer networks: Quasicontinuum photoluminescence linked to high densities of defects

Abstract

In a series of studies related to laser-induced damage of optical materials and deposition of plastics, we discovered a broadly emitting photoluminescence with fast lifetimes that we termed quasicontinuum photoluminescence (QC-PL). Here in this paper, we suggest that a high density of optically active defects leads to QC-PL, where interactions between defects affect the temporal and spectral characteristics of both excitation and emission. We develop a model that predicts the temporal characteristics of QC-PL, based on energy transfer interactions between high densities of defects. Our model does not explain all spectral broadening and redshifts found in QC-PL, since we do not model spectral changes in defects due to proximity to other defects. However, we do provide an example of a well-defined system that exhibits the QC-PL characteristics of a distribution in shortened lifetimes and broadened, redshifted energy levels: an organic chromophore (fluorescein) that has been dried rapidly on a fused silica surface. Recently, we showed that regions of fused silica exposed to up to 1 billion high-fluence laser shots at 351 rm nm at subdamage fluences exhibit significant transmission losses at the surface. Here, we find that these laser-exposed regions also exhibit QC-PL. Increases in the density of induced defectsmore » on these laser-exposed surfaces, as measured by the local transmission loss, lead to decreases in the observed lifetime and redshifts in the spectrum of the QC-PL, consistent with our explanation for QC-PL. In conclusion, we have found QC-PL in an increasing variety of situations and materials, and we believe it is a phenomenon commonly found on surfaces and nanostructured materials.« less

Authors:
 [1];  [1];  [1];  [1];  [1];  [1]
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Materials Science Division
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1409993
Alternate Identifier(s):
OSTI ID: 1407446
Report Number(s):
LLNL-JRNL-733134
Journal ID: ISSN 2475-9953; PRMHAR; TRN: US1702965
Grant/Contract Number:  
AC52-07NA27344
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 1; Journal Issue: 6; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS

Citation Formats

Laurence, Ted A., Ly, Sonny, Bude, Jeff D., Baxamusa, Salmaan H., Lepró, Xavier, and Ehrmann, Paul. Energy transfer networks: Quasicontinuum photoluminescence linked to high densities of defects. United States: N. p., 2017. Web. doi:10.1103/PhysRevMaterials.1.065201.
Laurence, Ted A., Ly, Sonny, Bude, Jeff D., Baxamusa, Salmaan H., Lepró, Xavier, & Ehrmann, Paul. Energy transfer networks: Quasicontinuum photoluminescence linked to high densities of defects. United States. doi:10.1103/PhysRevMaterials.1.065201.
Laurence, Ted A., Ly, Sonny, Bude, Jeff D., Baxamusa, Salmaan H., Lepró, Xavier, and Ehrmann, Paul. Mon . "Energy transfer networks: Quasicontinuum photoluminescence linked to high densities of defects". United States. doi:10.1103/PhysRevMaterials.1.065201.
@article{osti_1409993,
title = {Energy transfer networks: Quasicontinuum photoluminescence linked to high densities of defects},
author = {Laurence, Ted A. and Ly, Sonny and Bude, Jeff D. and Baxamusa, Salmaan H. and Lepró, Xavier and Ehrmann, Paul},
abstractNote = {In a series of studies related to laser-induced damage of optical materials and deposition of plastics, we discovered a broadly emitting photoluminescence with fast lifetimes that we termed quasicontinuum photoluminescence (QC-PL). Here in this paper, we suggest that a high density of optically active defects leads to QC-PL, where interactions between defects affect the temporal and spectral characteristics of both excitation and emission. We develop a model that predicts the temporal characteristics of QC-PL, based on energy transfer interactions between high densities of defects. Our model does not explain all spectral broadening and redshifts found in QC-PL, since we do not model spectral changes in defects due to proximity to other defects. However, we do provide an example of a well-defined system that exhibits the QC-PL characteristics of a distribution in shortened lifetimes and broadened, redshifted energy levels: an organic chromophore (fluorescein) that has been dried rapidly on a fused silica surface. Recently, we showed that regions of fused silica exposed to up to 1 billion high-fluence laser shots at 351 rm nm at subdamage fluences exhibit significant transmission losses at the surface. Here, we find that these laser-exposed regions also exhibit QC-PL. Increases in the density of induced defects on these laser-exposed surfaces, as measured by the local transmission loss, lead to decreases in the observed lifetime and redshifts in the spectrum of the QC-PL, consistent with our explanation for QC-PL. In conclusion, we have found QC-PL in an increasing variety of situations and materials, and we believe it is a phenomenon commonly found on surfaces and nanostructured materials.},
doi = {10.1103/PhysRevMaterials.1.065201},
journal = {Physical Review Materials},
number = 6,
volume = 1,
place = {United States},
year = {Mon Nov 06 00:00:00 EST 2017},
month = {Mon Nov 06 00:00:00 EST 2017}
}

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Works referenced in this record:

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journal, May 1953

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Adsorption and surface-enhanced Raman of dyes on silver and gold sols
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