Principles and Applications of Broadband Impulsive Vibrational Spectroscopy

We present an experimental setup for recording vibrational coherences and thereby Raman spectra of molecules in their ground and excited electronic states over the 50-3000 cm(-1) spectral range using broadband impulsive vibrational spectroscopy. Our approach relies on the combination of a andlt;10 f...

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Main Authors: Liebel, M, Schnedermann, C, Wende, T, Kukura, P
Format: Journal article
Language:English
Published: American Chemical Society 2015
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author Liebel, M
Schnedermann, C
Wende, T
Kukura, P
author_facet Liebel, M
Schnedermann, C
Wende, T
Kukura, P
author_sort Liebel, M
collection OXFORD
description We present an experimental setup for recording vibrational coherences and thereby Raman spectra of molecules in their ground and excited electronic states over the 50-3000 cm(-1) spectral range using broadband impulsive vibrational spectroscopy. Our approach relies on the combination of a andlt;10 fs excitation pulse with an uncompressed white light continuum probe, which drastically reduces experimental complexity compared to frequency domain based techniques. We discuss the parameters determining vibrational coherence amplitudes, outline how to optimize the experimental setup including approaches aimed at conclusively assigning vibrational coherences to specific electronic states, and provide a clear comparison with existing techniques. To demonstrate the applicability of our spectroscopic approach we conclude with several examples revealing the evolution of vibrational coherence in rhodopsin and β-carotene.
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spelling oxford-uuid:ed46185e-38e1-4c93-aacf-45ef5d5600aa2022-03-27T11:23:40ZPrinciples and Applications of Broadband Impulsive Vibrational SpectroscopyJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:ed46185e-38e1-4c93-aacf-45ef5d5600aaEnglishSymplectic Elements at OxfordAmerican Chemical Society2015Liebel, MSchnedermann, CWende, TKukura, PWe present an experimental setup for recording vibrational coherences and thereby Raman spectra of molecules in their ground and excited electronic states over the 50-3000 cm(-1) spectral range using broadband impulsive vibrational spectroscopy. Our approach relies on the combination of a andlt;10 fs excitation pulse with an uncompressed white light continuum probe, which drastically reduces experimental complexity compared to frequency domain based techniques. We discuss the parameters determining vibrational coherence amplitudes, outline how to optimize the experimental setup including approaches aimed at conclusively assigning vibrational coherences to specific electronic states, and provide a clear comparison with existing techniques. To demonstrate the applicability of our spectroscopic approach we conclude with several examples revealing the evolution of vibrational coherence in rhodopsin and β-carotene.
spellingShingle Liebel, M
Schnedermann, C
Wende, T
Kukura, P
Principles and Applications of Broadband Impulsive Vibrational Spectroscopy
title Principles and Applications of Broadband Impulsive Vibrational Spectroscopy
title_full Principles and Applications of Broadband Impulsive Vibrational Spectroscopy
title_fullStr Principles and Applications of Broadband Impulsive Vibrational Spectroscopy
title_full_unstemmed Principles and Applications of Broadband Impulsive Vibrational Spectroscopy
title_short Principles and Applications of Broadband Impulsive Vibrational Spectroscopy
title_sort principles and applications of broadband impulsive vibrational spectroscopy
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AT schnedermannc principlesandapplicationsofbroadbandimpulsivevibrationalspectroscopy
AT wendet principlesandapplicationsofbroadbandimpulsivevibrationalspectroscopy
AT kukurap principlesandapplicationsofbroadbandimpulsivevibrationalspectroscopy