Polarization effects in time resolved incoherent anti-Stokes Raman spectroscopy

Hofmann, M.; Zürl, R.; Graener, H.

doi:10.1063/1.472473

Cited by 16 publications

(11 citation statements)

References 17 publications

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“…Vibrational relaxation data are normally described in terms of rate equations, which include the orientational motion via angle dependencies . It will turn out that the reorientation of chloroform is much faster than the vibrational relaxation; therefore, it can be neglected for the following discussion of the long-time evolution vibrational relaxation. Upon an excess population Δ n i 0 being produced at t = 0, the time dependence of the excess population of the i th vibrational state Δ n i (t) is described by …”

Section: Interpretation and Discussionmentioning

confidence: 99%

“…Therefore, only limited information about the relaxation pathways was available. Recently the anti-Stokes spectroscopy after strong vibrational excitation via resonant absorption was rediscovered. − By the help of high-sensitive multichannel detection setups, the time evolution of complete anti-Stokes spectra can be observed and analyzed. In the following section, a rather complete data set will be presented: after excitation of the CH stretching vibration of chloroform, time dependent changes of the anti-Stokes Raman scattering of all fundamental vibrational transitions were simultaneously observed.…”

Section: Introductionmentioning

confidence: 99%

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Vibrational Relaxation of Liquid Chloroform

1997

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The state of information about vibrational population relaxation in the liquid state is still rather scarce. By using incoherent anti-Stokes scattering after strong infrared excitation, it is now possible to obtain rather complete information about these relaxation processes. In this paper we will report a study on the chloroform molecule. As all vibrations of this molecule are Raman active, they can be investigated by this experimental approach. Population lifetimes between 23 and several hundred ps are found. This is, to our knowledge, the first measurement displaying simultaneously the time evolution of all fundamentals of a molecule after direct population of a vibrational state.

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Section: Interpretation and Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Vibrational Relaxation of Liquid Chloroform

1997

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“…Hofmann et al have experimentally shown that time-dependent Raman signals can decrease by more than B50% due to rotational diffusion. 60 For a molecule the size of NBA dissolved in acetonitrile rotational diffusion times in the range of the measured bleach recovery (B10 ps) are to be expected. 61 So vibrational cooling and rotational diffusion might contribute to the B10 ps bleach recovery.…”

Section: Fsrs Experimentsmentioning

confidence: 96%

The ketene intermediate in the photochemistry of ortho-nitrobenzaldehyde

Laimgruber

Schmierer

Gilch

et al. 2008

Phys. Chem. Chem. Phys.

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The first intermediate of the photochemical transformation of ortho-nitrobenzaldehyde to ortho-nitrosobenzoic acid in acetonitrile solvent has been characterized by femtosecond spectroscopy and time-dependent density functional theory (TDDFT) calculations. Femtosecond stimulated Raman spectroscopy (FSRS) indicates that this intermediate adopts a ketene structure. This assignment is supported by the TDDFT results. A kinetic analysis of FSRS and transient absorption data points to two channels for the formation of the ketene. For the predominating first channel the formation takes 0.4 ps. For the second channel it is much slower and takes 220 ps. We assign the first channel to a reaction via an excited singlet state. The second one might involve a triplet state.

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“…The same authors also studied intermolecular vibrational energy transfer between alcohols and nitromethane. 24 Recently, Graener and co-workers used a 50 Hz Nd : YLF system with 1.5 ps resolution to study VER in dichloromethane 25 (CH 2 Cl 2 ) and chloroform 26 (CHCl 3 ) after C-H stretch excitation. The latter work 26 is especially notable for being the first where every one of the vibrations of a particular polyatomic molecule was monitored during a VER process.…”

Section: Introductionmentioning

confidence: 99%

Ultrafast infrared-Raman studies of vibrational energy redistribution in polyatomic liquids

Deàk

Iwaki

Rhea

et al. 2000

J. Raman Spectrosc.

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Vibrational energy relaxation and vibrational cooling of polyatomic liquids were studied with the ultrafast infrared-Raman (IR-Raman) technique. In the IR-Raman technique, a type of two-dimensional vibrational spectroscopy, a vibrational transition is pumped with a mid-infrared pulse and the instantaneous populations of all Raman-active transitions are simultaneously probed via incoherent anti-Stokes Raman scattering of a time-delayed visible pulse. The theoretical framework for these measurements, including force-force correlation function methods and perturbative techniques, is reviewed. Experimental aspects of the IR-Raman technique are discussed, including laser instrumentation, experimental set-up, the nature of the pumping and probing processes, detection sensitivity and optical background, and the interpretation of results including spectroscopic artifacts. Then examples are provided from recent research by our group, focusing on timely problems such as the pseudo-vibrational cascade, the dynamics of doorway vibrations, dynamics of overtones with Fermi resonance, multiple vibrational excitations via combination band pumping and spectral evolution in associated liquids.

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Polarization effects in time resolved incoherent anti-Stokes Raman spectroscopy

Cited by 16 publications

References 17 publications

Vibrational Relaxation of Liquid Chloroform

Vibrational Relaxation of Liquid Chloroform

The ketene intermediate in the photochemistry of ortho-nitrobenzaldehyde

Ultrafast infrared-Raman studies of vibrational energy redistribution in polyatomic liquids

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