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Implementation of Time-Resolved Step-Scan Fourier Transform Infrared (FT-IR) Spectroscopy Using a kHz Repetition Rate Pump Laser

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Abstract:

Time-resolved step-scan Fourier transform infrared (FT-IR) spectroscopy has been shown to be invaluable for studying excited-state structures and dynamics in both biological and inorganic systems. Despite the established utility of this method, technical challenges continue to limit the data quality and more wide ranging applications. A critical problem has been the low laser repetition rate and interferometer stepping rate (both are typically 10 Hz) used for data acquisition. Here we demonstrate significant improvement in the quality of time-resolved spectra through the use of a kHz repetition rate laser to achieve kHz excitation and data collection rates while stepping the spectrometer at 200 Hz. We have studied the metal-to-ligand charge transfer excited state of Ru(bipyridine)3Cl2 in deuterated acetonitrile to test and optimize high repetition rate data collection. Comparison of different interferometer stepping rates reveals an optimum rate of 200 Hz due to minimization of long-term baseline drift. With the improved collection efficiency and signal-to-noise ratio, better assignments of the MLCT excited-state bands can be made. Using optimized parameters, carbonmonoxy myoglobin in deuterated buffer is also studied by observing the infrared signatures of carbon monoxide photolysis upon excitation of the heme. We conclude from these studies that a substantial increase in performance of ss-FT-IR instrumentation is achieved by coupling commercial infrared benches with kHz repetition rate lasers.

Keywords: FT-IR SPECTROSCOPY; INFRARED SPECTROSCOPY; NANOSECOND PHENOMENA; SPECTROSCOPIC INSTRUMENTATION; TIME-RESOLVED SPECTROSCOPY; TIME-RESOLVED STEP-SCAN FOURIER TRANSFORM INFRARED SPECTROSCOPY

Document Type: Research Article

DOI: http://dx.doi.org/10.1366/10-06179

Affiliations: 1: Department of Chemistry, Emory University, Atlanta, Georgia 300322, USA 2: Materials Physics and Applications Division, Center for Integrated Nanotechnologies (MPA-CINT), Los Alamos National Laboratory, Los Alamos, New Mexico 87545, USA

Publication date: May 1, 2011

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