The relaxation process of the excitonic states in polydiacetylene studied by time- and wavenumber-resolved femtosecond coherent anti-Stokes Raman scattering

Chen, T.; Vierheilig, A.; Waltner, P.; Kiefer, W.; Materny, A.

doi:10.1016/s0009-2614(00)00683-7

Cited by 23 publications

(12 citation statements)

References 7 publications

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“…The experiments of this section were performed with the FBS side groups (d), although other side groups have been investigated in femtosecond CARS experiments as well [144].…”

Section: Methodsmentioning

confidence: 99%

“…The process is optimized in a feedback loop using the anti-Stokes Raman signal of a four-wave-mixing (FWM) process as feedback. Polydiacetylene (PDA) has been studied in detail with femtosecond time-and frequencyresolved coherent anti-Stokes Raman Scattering (fs-CARS) [143][144][145]. In those experiments, several normal modes were excited in a stimulated Raman process and the vibrational dynamics in the electronic ground and self-trapped exciton state were studied by analyzing the anti-Stokes signal.…”

Section: Introductionmentioning

confidence: 99%

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Evolutionary algorithms and their application to optimal control studies

et al. 2001

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“…The experiments of this section were performed with the FBS side groups (d), although other side groups have been investigated in femtosecond CARS experiments as well [144].…”

Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Evolutionary algorithms and their application to optimal control studies

et al. 2001

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“…In our CARS experiments, the chirp was estimated by measuring the time-and wavenumber-resolved nonresonant CARS signal of a thin glass plate (300 µm). 31 In this experiment, 2 was fixed and 1 was varied. The resulting three-dimensional plot [anti-Stokes intensity D f signal wavenumber, 1 )] was used to minimize the chirp for this experiment.…”

Section: Spectroscopy In the Time Domainmentioning

confidence: 99%

“…Additionally, owing to the pulse length of approximately 80 fs, the time resolution is at the limit for this experiment as the dynamics of the electronic excited PES are very fast. 31,128,129 In order to separate the chirp effect in this experiment, non-resonant femtosecond time-resolved CARS measurements are in preparation.…”

Section: Spectroscopy In the Time Domainmentioning

confidence: 99%

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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“…Femtosecond time-resolved CARS is a method for clarifying the origin of ultrafast dynamics associated with molecular motions in liquid [1] in the time domain since 1980s for some decades [2,3]. This technique has been widely used in different samples, such as polydiacetylene [4,5], porphyrin [6,7], toluene [8], methanol-water [9], flame [10][11][12], N 2 [13] and dipicolinic acid [14][15][16]. Recently, there have been some advances in femtosecond time-resolved CARS, such as single-shot [17], hybrid fs/ps [8,[18][19][20], single-beam [21][22][23], spectral focusing [24] and in situ heterodyne detection [25].…”

Section: Introductionmentioning

confidence: 99%