CCD broadband detection technique for the spectral characterization of the inhomogeneous signal in femtosecond time‐resolved four‐wave mixing spectroscopy

Siebert, Thorsten; Schmitt, Michael; Michelis, T.; Materny, A.; Kiefer, W.

doi:10.1002/(sici)1097-4555(199909)30:9<807::aid-jrs452>3.0.co;2-#

Cited by 19 publications

(13 citation statements)

References 28 publications

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“…If we generate the vibrational motion of a molecule by the pump-dump process using two ultrashort laser pulses, the driving forces are determined by the time-dependent phases of the two laser pulses. With femtosecond time-and wavenumber-resolved CARS 70 we can not only generate the vibrational coherent motion of PDAs in their electronic ground state but also distinguish in the antiStokes signal contributions from different modes. 30 -32,34,35 In our review we will discuss the application of femtosecond time-resolved coherent anti-Stokes Raman scattering (CARS) 71 which enabled us to excite selectively ground-state vibrations and also detect the time response of these modes and neighboring modes.…”

Section: Introductionmentioning

confidence: 86%

A review on linear and non‐linear resonance Raman spectroscopy of the conjugated system polydiacetylene

Materny

Chen

Vierheilig

et al. 2001

J Raman Spectroscopy

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We review resonance Raman investigations of the linear conjugated p-electron system of polydiacetylenes embedded in single-crystalline monomer matrices. Absorption, luminescence, resonance Raman and resonance CARS spectroscopy were used to investigate vibronic properties of the polymers. As an example, we discuss the theoretical model applied for the simulation of the resonance Raman line and excitation profiles obtained from the polymer chains in FBS, TS/FBS and TS6 diacetylene single crystals. The theory is based on a Franck-Condon model, which considers a chain length dependence. The electronic transition energies and matrix elements were calculated by means of an LCAO MO (linear combination of atomic orbitals molecular orbital) calculation in the Hückel approach. An interaction between ensemble and intramolecular properties due to defects can be shown. Besides the well known polymer absorption, the partially polymerized single crystals of the diacetylenes under investigation show blue-shifted absorption bands in sharply separated crystal areas. The spectroscopic investigations of this chromism revealed that most probably growth defects in f111g crystal growth sectors influence the side-group geometry of the polymer chains. Using femtosecond time-resolved CARS spectroscopy, the dynamics of the vibrational excitation in the electronic ground and excited states can be investigated. Here, we report the controlled selective excitation of the polymers. We used a CARS scheme where the difference of pump and Stokes laser wavelengths is chosen to achieve resonance with several chain modes of the polydiacetylenes. By varying the timing and the phases of the femtosecond laser pulses, the timing and the intensity of these modes can be strongly influenced.

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Section: Introductionmentioning

confidence: 86%

A review on linear and non‐linear resonance Raman spectroscopy of the conjugated system polydiacetylene

Materny

Chen

Vierheilig

et al. 2001

J Raman Spectroscopy

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“…cess can be used to study both ground and excited state dynamics in I 2 by detection at a particular wavelength, 16,35 or by dispersed broadband detection. 8,36 We therefore summarize only briefly. Defining the overlap of pump/Stokes pulses to be t = 0, we introduce a delay ⌬t of the second pump interaction with respect to this.…”

Section: Methodsmentioning

confidence: 99%

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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“…The experimental setup of our fs-CARS spectrometer is similar to that described previously 11,12,27 and is only briefly discussed here. Pulses of about 90 fs duration centered at 800 nm from a Ti:sapphire oscillator (Mira, Coherent) are used as seed pulses for a regenerative amplifier (CPA-1000, Clark MXR) with a repetition rate of 1 kHz.…”

Section: Methodsmentioning

confidence: 99%

“…It is given by the amplitude of the probe pulse and its temporal pulse envelope and oscillates with ω Pr C 2 cQ j . Using Eqn (12) it is in principle possible to perform a numerical fit of the decay behavior at every wavenumber position Q CARS , where one might extract the vibrational dephasing times T 2j and also the amplitudes Q j of all excited vibrational modes.…”

Section: Vibrational Dephasingmentioning

confidence: 99%

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Two‐dimensional probing of ground‐state vibrational dynamics in porphyrin molecules by fs‐CARS

Heid

Schlücker

Schmitt

et al. 2001

J Raman Spectroscopy

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We report on spectrally dispersed femtosecond time-resolved coherent anti-Stokes Raman scattering (CARS) for the investigation of the electronic ground-state vibrational dynamics of porphyrin molecules in solution. The two-dimensional experimental data obtained in our measurements provide a detailed mapping of the large number of molecular vibrations in these systems, excited by broadband ultrashort laser pulses, and make a thorough interpretation of the complex signal structure possible. In particular, an analysis of the data by applying Fourier transform methods to the time domain signal allows a clear identification of the excited porphyrin normal modes when compared with results on the mode structure from spectrally resolved (cw) spectroscopy. Altogether the method is capable of yielding detailed information on the dephasing behavior and on the relative spectral positions of the excited vibrations at the same time. Three porphyrin systems, dissolved in dichloromethane, were investigated: magnesium octaethylporphyrin, magnesium tetraphenylporphyrin and the free-base porphyrin octaethylporphyrin. The measurements were performed in the spectral region of the ring vibrations of the porphyrin macrocycle. We also provide a discussion of the expected signals on a theoretical basis by deriving the CARS third-order non-linear polarization for these experiments.

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CCD broadband detection technique for the spectral characterization of the inhomogeneous signal in femtosecond time‐resolved four‐wave mixing spectroscopy

Cited by 19 publications

References 28 publications

A review on linear and non‐linear resonance Raman spectroscopy of the conjugated system polydiacetylene

A review on linear and non‐linear resonance Raman spectroscopy of the conjugated system polydiacetylene

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

Two‐dimensional probing of ground‐state vibrational dynamics in porphyrin molecules by fs‐CARS

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