Vibrational polarization beats in femtosecond coherent anti-Stokes Raman spectroscopy: A signature of dissociative pump–dump–pump wave packet dynamics

Faeder, James R.; Pinkas, Iddo; Knopp, G.; Prior, Yehiam; Tannor, David J.

doi:10.1063/1.1412253

Cited by 53 publications

(53 citation statements)

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“…Consequently, in calculating the third order susceptibility, one has to both sum over bound state and integrate over continuum contributions. Faeder et al 10 did a thorough study of the situation when probing both above and below this threshold. These authors showed how anomalous peaks in the frequency spectrum found only when probing above the dissociation threshold could be assigned as polarization beats.…”

Section: ͑4͒mentioning

confidence: 99%

“…The CARS process involves the interaction of three laser fields, generating a third order polarization whose associated emitted field is measured in a phasematched direction. As discussed by Faeder et al, 10 the expression for the third order polarization includes all possible time orderings of the three interactions. The spectroscopic pathways producing the third order polarization may be depicted using double-sided Feynman diagrams, as shown, for example, in Fig.…”

Section: Introductionmentioning

confidence: 99%

“…10 can contribute to the femtosecond time-resolved CARS signal, depending on the delays. Defining the pump/Stokes pulse pair overlap as t =0, the situation where the delayed pump pulse arrives before ͑after͒ t = 0 thus corresponds to negative ͑positive͒ delays.…”

Section: Introductionmentioning

confidence: 99%

“…The selec-tion mechanisms which apply to hot molecules have been discussed by Faeder et al: 10 There are two complementary factors which can lead to suppression of diagram B. First, if the detuning between the Stokes and pump pulses, ͑E v − E 0 = p − S ͒, is large compared with the vibrational level spacing and k B T, diagram B will be suppressed since there will be no population in the vibrationally excited state, E v , from which the Stokes photon can be absorbed.…”

Section: Introductionmentioning

confidence: 99%

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Time- and frequency-resolved coherent anti-Stokes Raman scattering spectroscopy with sub-25fs laser pulses

Lausten

Smirnova

Sussman

et al. 2008

The Journal of Chemical Physics

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/npsi/ctrl?lang=en http://nparc.cisti-icist.nrc-cnrc.gc.ca/npsi/ctrl?lang=fr READ THESE TERMS AND CONDITIONS CAREFULLY BEFORE USING THIS WEBSITE.http://nparc.cisti-icist.nrc-cnrc.gc.ca/npsi/jsp/nparc_cp.jsp?lang=en Vous avez des questions? Nous pouvons vous aider. Pour communiquer directement avec un auteur, consultez la première page de la revue dans laquelle son article a été publié afin de trouver ses coordonnées. Si vous n'arrivez pas à les repérer, communiquez avec nous à PublicationsArchive-ArchivesPublications@nrc-cnrc.gc.ca. Questions?Contact the NRC Publications Archive team at PublicationsArchive-ArchivesPublications@nrc-cnrc.gc.ca. If you wish to email the authors directly, please see the first page of the publication for their contact information. NRC Publications Archive Archives des publications du CNRCThis publication could be one of several versions: author's original, accepted manuscript or the publisher's version. / La version de cette publication peut être l'une des suivantes : la version prépublication de l'auteur, la version acceptée du manuscrit ou la version de l'éditeur. For the publisher's version, please access the DOI link below./ Pour consulter la version de l'éditeur, utilisez le lien DOI ci-dessous.http://doi.org/10.1063/1.2932101 Journal of Chemical Physics, 128Time-and frequency-resolved coherent anti-Stokes Raman scattering spectroscopy with sub-25 fs laser pulses In general, many different diagrams can contribute to the signal measured in broadband four-wave mixing experiments. Care must therefore be taken when designing an experiment to be sensitive to only the desired diagram by taking advantage of phase matching, pulse timing, sequence, and the wavelengths employed. We use sub-25 fs pulses to create and monitor vibrational wavepackets in gaseous iodine, bromine, and iodine bromide through time-and frequency-resolved femtosecond coherent anti-Stokes Raman scattering ͑CARS͒ spectroscopy. We experimentally illustrate this using iodine, where the broad bandwidths of our pulses, and Boltzmann population in the lower three vibrational levels conspire to make a single diagram dominant in one spectral region of the signal spectrum. In another spectral region, however, the signal is the sum of two almost equally contributing diagrams, making it difficult to directly extract information about the molecular dynamics. We derive simple analytical expressions for the time-and frequency-resolved CARS signal to study the interplay of different diagrams. Expressions are given for all five diagrams which can contribute to the CARS signal in our case.

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Section: ͑4͒mentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Time- and frequency-resolved coherent anti-Stokes Raman scattering spectroscopy with sub-25fs laser pulses

Lausten

Smirnova

Sussman

et al. 2008

The Journal of Chemical Physics

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“…Coherent optical response in gas has been revealed by using the Fourier transform of two-dimensional spectroscopic measurements [21,22]. A time-dependent perturbation theory has been adopted to understand various FWM processes [23][24][25]. Density matrix formalism [26] has proved to be an important tool to interpret molecular coherent processes observed in femtosecond experiments [27,28].…”

Section: Introductionmentioning

confidence: 99%

Tracking molecular wave packets in cesium dimers by coherent Raman scattering

et al. 2012

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We explore wave-packet dynamics in the ground X 1 + g and excited B 1 u states of cesium dimers (Cs 2 ). In particular, we study the dependence of the wave-packet dynamics on the relative timing between femtosecond pump, Stokes, and probe pulses in a nondegenerate BOXCARS beam geometry, which are commonly used for coherent anti-Stokes Raman scattering (CARS) spectroscopy. The experimental results are elucidated by theoretical calculations, which are based on the Liouville equations for the density matrix for the molecular states. We observe oscillations in CARS signals as functions of both Stokes and probe pulse delays with respect to the pump pulse. The oscillation period relates to the wave-packet motion cycle in either the ground or excited state of Cs 2 molecules, depending on the sequence of the input laser pulses in time. The performed analysis can be applied to study and/or manipulate wave-packet dynamics in a variety of molecules. It also provides an excellent test platform for theoretical models of molecular systems.

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Ground state vibrational wave‐packet and recovery dynamics studied by time‐resolved CARS and pump‐CARS spectroscopy

Siebert

Schmitt

Gräfe

et al. 2006

J Raman Spectroscopy

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Recent experiments on gaseous iodine and b-carotene are analyzed within a wave-packet description of femtosecond-time resolved four-wave mixing spectroscopy. Employing the same formalism, two different experimental setups, both established in the Kiefer group, are treated. In a transient four-wave-mixing (FWM) experiment, where two pulses interact simultaneously with the system, the interaction with a third time-delayed pulse leads to light emission reflecting ground state vibrational dynamics in I 2 . On the other hand, delaying a FWM-pulse sequence with respect to a single pump pulse interacting with b-carotene yields a signal that is directly proportional to the population of a selected nuclear eigenstate in the electronic ground state. Thus, within this setup, it is possible to monitor ground-state re-population dynamics mode specifically.

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Vibrational polarization beats in femtosecond coherent anti-Stokes Raman spectroscopy: A signature of dissociative pump–dump–pump wave packet dynamics

Abstract: Articles you may be interested inAnalysis of time resolved femtosecond and femtosecond/picosecond coherent anti-Stokes Raman spectroscopy: Application to toluene and Rhodamine 6G

Cited by 53 publications

References 77 publications

Time- and frequency-resolved coherent anti-Stokes Raman scattering spectroscopy with sub-25fs laser pulses

Time- and frequency-resolved coherent anti-Stokes Raman scattering spectroscopy with sub-25fs laser pulses

Tracking molecular wave packets in cesium dimers by coherent Raman scattering

Ground state vibrational wave‐packet and recovery dynamics studied by time‐resolved CARS and pump‐CARS spectroscopy

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