Journal ArticleDOI
ULTRA: A Unique Instrument for Time-Resolved Spectroscopy.
Gregory M. Greetham,Pierre Burgos,Qian Cao,Ian P. Clark,Peter S. Codd,Richard C. Farrow,Michael W. George,Moschos Kogimtzis,Pavel Matousek,Anthony W. Parker,Mark R. Pollard,David Robinson,Zhi-Jun Xin,Michael Towrie +13 more
TLDR
A high-sensitivity time-resolved infrared and Raman spectrometer with exceptional experimental flexibility based on a 10-kHz synchronized dual-arm femtosecond and picosecond laser system is reported.Abstract:
We report the development of a high-sensitivity time-resolved infrared and Raman spectrometer with exceptional experimental flexibility based on a 10-kHz synchronized dual-arm femtosecond and picosecond laser system. Ultrafast high-average-power titanium sapphire lasers and optical parametric amplifiers provide wavelength tuning from the ultraviolet (UV) to the mid-infrared region. Customized silicon, indium gallium arsenide, and mercury cadmium telluride linear array detectors are provided to monitor the probe laser intensity in the UV to mid-infrared wavelength range capable of measuring changes in sample absorbance of ΔOD ~ 10(-5) in 1 second. The system performance is demonstrated for the time-resolved infrared, two-dimensional (2D) infrared, and femtosecond stimulated Raman spectroscopy techniques with organometallic intermediates, organic excited states, and the dynamics of the tertiary structure of DNA.read more
Citations
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Journal ArticleDOI
Femtosecond Stimulated Raman Spectroscopy
D. Dietze,Richard A. Mathies +1 more
TL;DR: The historic overview and discusses the theoretical and experimental concepts behind FSRS, and emphasis is put on the current state-of-the-art experimental realization and several variations of FSRS that have been developed.
Journal ArticleDOI
Toward control of electron transfer in donor-acceptor molecules by bond-specific infrared excitation.
Milan Delor,Paul A. Scattergood,Igor V. Sazanovich,Igor V. Sazanovich,Anthony W. Parker,Gregory M. Greetham,Anthony J. H. M. Meijer,Michael Towrie,Julia A. Weinstein +8 more
TL;DR: It is demonstrated how the outcome of light-induced ET can be radically altered by mode-specific infrared (IR) excitation of vibrations that are coupled to the ET pathway, effectively switching a charge separation pathway off.
Journal Article
Ultrafast 2D IR vibrational echo chemical exchange spectroscopy
Junrong Zheng,Michael D. Fayer +1 more
TL;DR: In this article, the authors describe 2D IR vibrational echo chemical exchange experiments and apply them to several types of molecular systems, including the formation and dissociation of organic solute-solvent complexes.
Journal ArticleDOI
Direct observation of ultrafast long-range charge separation at polymer-fullerene heterojunctions.
Françoise Provencher,Nicolas Bérubé,Anthony W. Parker,Gregory M. Greetham,Michael Towrie,Christoph Hellmann,Michel Côté,Natalie Stingelin,Carlos Silva,Sophia C. Hayes +9 more
TL;DR: In this paper, the authors investigated polaron photogeneration dynamics at polymer:fullerene heterojunctions by monitoring its time-resolved resonance-Raman spectrum following ultrafast photoexcitation.
Journal ArticleDOI
On the mechanism of vibrational control of light-induced charge transfer in donor–bridge–acceptor assemblies
Milan Delor,Theo Keane,Paul A. Scattergood,Igor V. Sazanovich,Gregory M. Greetham,Michael Towrie,Anthony J. H. M. Meijer,Julia A. Weinstein +7 more
TL;DR: The experiments reveal a complex combination of vibronic mechanisms responsible for the observed changes in electron transfer rates and pathways, and raise new fundamental questions about the function of vibrational processes immediately following charge transfer photoexcitation.
References
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Journal ArticleDOI
A library of IR bands of nucleic acids in solution.
TL;DR: This review presents a compilation and discussion of infrared (IR) bands characteristic of nucleic acids in various conformations, aimed at highlighting specific features that are useful for following major changes in nucleic acid structures.
Journal ArticleDOI
Mapping GFP structure evolution during proton transfer with femtosecond Raman spectroscopy
TL;DR: It is shown that femtosecond stimulated Raman spectroscopy provides sufficiently detailed and time-resolved vibrational spectra of the electronically excited chromophore of GFP to reveal skeletal motions involved in the proton transfer that produces the fluorescent form of the protein.
Journal ArticleDOI
Effective Rejection of Fluorescence Interference in Raman Spectroscopy Using a Shifted Excitation Difference Technique
TL;DR: In this article, the wavelength of the excitation laser was tuned into resonance with an electronic absorption band of only one molecular species, and the vibrational Raman scattering from this species can be selectively enhanced.
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ULTRAFAST CHEMISTRY: Using Time-Resolved Vibrational Spectroscopy for Interrogation of Structural Dynamics
TL;DR: Time-resolved infrared (IR) and Raman spectroscopy elucidates molecular structure evolution during ultrafast chemical reactions through transient frequency shifts of IR-active vibrations and through nonequilibrium populations as deduced by Raman resonances.
Journal ArticleDOI
Efficient Rejection of Fluorescence from Raman Spectra Using Picosecond Kerr Gating
TL;DR: In this article, an efficient method for the rejection of fluorescence from picosecond time-resolved resonance Raman (ps-TR3) spectra, applicable also to ground-state Raman spectroscopy, has been demonstrated.