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Title: Fully automated dual-frequency three-pulse-echo 2DIR spectrometer accessing spectral range from 800 to 4000 wavenumbers

Abstract

A novel dual-frequency two-dimensional infrared instrument is designed and built that permits three-pulse heterodyned echo measurements of any cross-peak within a spectral range from 800 to 4000 cm{sup −1} to be performed in a fully automated fashion. The superior sensitivity of the instrument is achieved by a combination of spectral interferometry, phase cycling, and closed-loop phase stabilization accurate to ∼70 as. The anharmonicity of smaller than 10{sup −4} cm{sup −1} was recorded for strong carbonyl stretching modes using 800 laser shot accumulations. The novel design of the phase stabilization scheme permits tuning polarizations of the mid-infrared (m-IR) pulses, thus supporting measurements of the angles between vibrational transition dipoles. The automatic frequency tuning is achieved by implementing beam direction stabilization schemes for each m-IR beam, providing better than 50 μrad beam stability, and novel scheme for setting the phase-matching geometry for the m-IR beams at the sample. The errors in the cross-peak amplitudes associated with imperfect phase matching conditions and alignment are found to be at the level of 20%. The instrument can be used by non-specialists in ultrafast spectroscopy.

Authors:
; ; ; ; ; ; ; ; ;  [1];  [2]
  1. Department of Chemistry, Tulane University, New Orleans, Louisiana 70118 (United States)
  2. Institute for Nuclear Research of the Russian Academy of Sciences, Moscow 117312 (Russian Federation)
Publication Date:
OSTI Identifier:
22314652
Resource Type:
Journal Article
Resource Relation:
Journal Name: Review of Scientific Instruments; Journal Volume: 85; Journal Issue: 8; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND TECHNOLOGY; ALIGNMENT; AMPLITUDES; BEAMS; DESIGN; DIPOLES; ERRORS; GEOMETRY; INFRARED SPECTRA; INFRARED SPECTROMETERS; INTERFEROMETRY; PEAKS; POLARIZATION; PULSES; SENSITIVITY; SPECTROSCOPY; STABILIZATION

Citation Formats

Leger, Joel D., Nyby, Clara M., Varner, Clyde, Tang, Jianan, Rubtsova, Natalia I., Yue, Yuankai, Kireev, Victor V., Burtsev, Viacheslav D., Qasim, Layla N., Rubtsov, Igor V., E-mail: irubtsov@tulane.edu, and Rubtsov, Grigory I. Fully automated dual-frequency three-pulse-echo 2DIR spectrometer accessing spectral range from 800 to 4000 wavenumbers. United States: N. p., 2014. Web. doi:10.1063/1.4892480.
Leger, Joel D., Nyby, Clara M., Varner, Clyde, Tang, Jianan, Rubtsova, Natalia I., Yue, Yuankai, Kireev, Victor V., Burtsev, Viacheslav D., Qasim, Layla N., Rubtsov, Igor V., E-mail: irubtsov@tulane.edu, & Rubtsov, Grigory I. Fully automated dual-frequency three-pulse-echo 2DIR spectrometer accessing spectral range from 800 to 4000 wavenumbers. United States. doi:10.1063/1.4892480.
Leger, Joel D., Nyby, Clara M., Varner, Clyde, Tang, Jianan, Rubtsova, Natalia I., Yue, Yuankai, Kireev, Victor V., Burtsev, Viacheslav D., Qasim, Layla N., Rubtsov, Igor V., E-mail: irubtsov@tulane.edu, and Rubtsov, Grigory I. Fri . "Fully automated dual-frequency three-pulse-echo 2DIR spectrometer accessing spectral range from 800 to 4000 wavenumbers". United States. doi:10.1063/1.4892480.
@article{osti_22314652,
title = {Fully automated dual-frequency three-pulse-echo 2DIR spectrometer accessing spectral range from 800 to 4000 wavenumbers},
author = {Leger, Joel D. and Nyby, Clara M. and Varner, Clyde and Tang, Jianan and Rubtsova, Natalia I. and Yue, Yuankai and Kireev, Victor V. and Burtsev, Viacheslav D. and Qasim, Layla N. and Rubtsov, Igor V., E-mail: irubtsov@tulane.edu and Rubtsov, Grigory I.},
abstractNote = {A novel dual-frequency two-dimensional infrared instrument is designed and built that permits three-pulse heterodyned echo measurements of any cross-peak within a spectral range from 800 to 4000 cm{sup −1} to be performed in a fully automated fashion. The superior sensitivity of the instrument is achieved by a combination of spectral interferometry, phase cycling, and closed-loop phase stabilization accurate to ∼70 as. The anharmonicity of smaller than 10{sup −4} cm{sup −1} was recorded for strong carbonyl stretching modes using 800 laser shot accumulations. The novel design of the phase stabilization scheme permits tuning polarizations of the mid-infrared (m-IR) pulses, thus supporting measurements of the angles between vibrational transition dipoles. The automatic frequency tuning is achieved by implementing beam direction stabilization schemes for each m-IR beam, providing better than 50 μrad beam stability, and novel scheme for setting the phase-matching geometry for the m-IR beams at the sample. The errors in the cross-peak amplitudes associated with imperfect phase matching conditions and alignment are found to be at the level of 20%. The instrument can be used by non-specialists in ultrafast spectroscopy.},
doi = {10.1063/1.4892480},
journal = {Review of Scientific Instruments},
number = 8,
volume = 85,
place = {United States},
year = {Fri Aug 15 00:00:00 EDT 2014},
month = {Fri Aug 15 00:00:00 EDT 2014}
}