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Title: Development of nanosecond time-resolved infrared detection at the LEAF pulse radiolysis facility

Abstract

When coupled with transient absorption spectroscopy, pulse radiolysis, which utilizes high-energy electron pulses from an accelerator, is a powerful tool for investigating the kinetics and thermodynamics of a wide range of radiation-induced redox and electron transfer processes. The majority of these investigations detect transient species in the UV, visible, or near-IR spectral regions. Unfortunately, the often-broad and featureless absorption bands in these regions can make the definitive identification of intermediates difficult. Time-resolved vibrational spectroscopy would offer much improved structural characterization, but has received only limited application in pulse radiolysis. In this paper, we describe in detail the development of a unique nanosecond time-resolved infrared (TRIR) detection capability for condensed-phase pulse radiolysis on a new beam line at the LEAF facility of Brookhaven National Laboratory. The system makes use of a suite of high-power, continuous wave external-cavity quantum cascade lasers as the IR probe source, with coverage from 2330-1051 cm⁻¹. The response time of the TRIR detection setup is ~40 ns, with a typical sensitivity of ~100 µOD after 4-8 signal averages using a dual-beam probe/reference normalization detection scheme. As a result, this new detection method has enabled mechanistic investigations of a range of radiation-induced chemical processes, some of which aremore » highlighted here.« less

Authors:
 [1];  [2];  [1];  [1]; ORCiD logo [3]; ORCiD logo [1]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States); Sydor Instruments, LLC, Rochester, NY (United States)
  3. Dowling College, Shirley, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1183835
Report Number(s):
BNL-107866-2015-JA
Journal ID: ISSN 0034-6748; RSINAK; R&D Project: CO-004; KC0304030
Grant/Contract Number:
SC00112704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Review of Scientific Instruments
Additional Journal Information:
Journal Volume: 86; Journal Issue: 4; Journal ID: ISSN 0034-6748
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; infrared detectors; particle beam detectors; solvents; mirrors; time resolved spectroscopy

Citation Formats

Grills, David C., Farrington, Jaime A., Layne, Bobby H., Preses, Jack M., Bernstein, Herbert J., and Wishart, James F. Development of nanosecond time-resolved infrared detection at the LEAF pulse radiolysis facility. United States: N. p., 2015. Web. doi:10.1063/1.4918728.
Grills, David C., Farrington, Jaime A., Layne, Bobby H., Preses, Jack M., Bernstein, Herbert J., & Wishart, James F. Development of nanosecond time-resolved infrared detection at the LEAF pulse radiolysis facility. United States. doi:10.1063/1.4918728.
Grills, David C., Farrington, Jaime A., Layne, Bobby H., Preses, Jack M., Bernstein, Herbert J., and Wishart, James F. Mon . "Development of nanosecond time-resolved infrared detection at the LEAF pulse radiolysis facility". United States. doi:10.1063/1.4918728. https://www.osti.gov/servlets/purl/1183835.
@article{osti_1183835,
title = {Development of nanosecond time-resolved infrared detection at the LEAF pulse radiolysis facility},
author = {Grills, David C. and Farrington, Jaime A. and Layne, Bobby H. and Preses, Jack M. and Bernstein, Herbert J. and Wishart, James F.},
abstractNote = {When coupled with transient absorption spectroscopy, pulse radiolysis, which utilizes high-energy electron pulses from an accelerator, is a powerful tool for investigating the kinetics and thermodynamics of a wide range of radiation-induced redox and electron transfer processes. The majority of these investigations detect transient species in the UV, visible, or near-IR spectral regions. Unfortunately, the often-broad and featureless absorption bands in these regions can make the definitive identification of intermediates difficult. Time-resolved vibrational spectroscopy would offer much improved structural characterization, but has received only limited application in pulse radiolysis. In this paper, we describe in detail the development of a unique nanosecond time-resolved infrared (TRIR) detection capability for condensed-phase pulse radiolysis on a new beam line at the LEAF facility of Brookhaven National Laboratory. The system makes use of a suite of high-power, continuous wave external-cavity quantum cascade lasers as the IR probe source, with coverage from 2330-1051 cm⁻¹. The response time of the TRIR detection setup is ~40 ns, with a typical sensitivity of ~100 µOD after 4-8 signal averages using a dual-beam probe/reference normalization detection scheme. As a result, this new detection method has enabled mechanistic investigations of a range of radiation-induced chemical processes, some of which are highlighted here.},
doi = {10.1063/1.4918728},
journal = {Review of Scientific Instruments},
number = 4,
volume = 86,
place = {United States},
year = {Mon Apr 27 00:00:00 EDT 2015},
month = {Mon Apr 27 00:00:00 EDT 2015}
}

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