Experimental and theoretical coherent anti-Stokes Raman scattering studies on triplet excited anthracene

Funk, J.-M.; Schmitt, Ulrich; Kiefer, W.; Materny, Arnulf

doi:10.1002/1097-4555(200008/09)31:8/9<743::aid-jrs591>3.0.co;2-b

Cited by 6 publications

(3 citation statements)

References 67 publications

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“…Similar experiments were performed by Funk et al on the nanosecond time-scale, where the CARS probe extracted spectral information about triplet states of polycyclic aromatic systems that were populated by pumping excited singlet states that undergo intersystem crossing. 32 A significant experiment for establishing third-order interactions as a probe mechanism of transient states in a pump-probe scheme was performed by Motzkus et al 33 In the experiment, degenerate four-wave mixing (DFWM) was used as a probe mechanism for probing the dissociation dynamics of sodium iodide in the gas phase. Here, the mechanism and state selectivity with which thirdorder interactions interrogate vibrational states in transient populations were established.…”

Section: Introductionmentioning

confidence: 99%

The role of specific normal modes during non‐Born–Oppenheimer dynamics: the S₁–S₀ internal conversion of β‐carotene interrogated on a femtosecond time‐scale with coherent anti‐Stokes Raman scattering

Siebert

Maksimenka

Materny

et al. 2002

J Raman Spectroscopy

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The population flow from the first excited singlet state (S 1 ) to the electronic ground state (S 0 ), facilitated through the S 1 -S 0 internal conversion, and the subsequent internal vibrational energy redistribution and vibrational cooling processes are monitored selectively with respect to the different forms of nuclear motion in all-trans-b-carotene. This is realized by exciting the molecule into the second excited singlet state (S 2 ) with an auxiliary pump laser pulse and interrogating the population recovery into the electronic ground state by means of a time-delayed, coherent anti-Stokes Raman (CARS) process. This spectroscopic scheme is referred to as a pump-CARS scheme in analogy to the classical pump-probe scheme in timeresolved spectroscopy. Here, the profound enhancement of the CARS signal intensity in the case of a Raman resonance to a specific vibrational mode is utilized as an intensity filter that amplifies the signal from the vibrational modes of interest, making the contributions from other vibrational modes negligible. This filter allows for the population flow in a specific vibrational mode to be monitored as the radiationless electronic transition between the S 1 and S 0 state takes place. This spectroscopic scheme opens up the possibility of identifying the vibrational motion with a large-amplitude motion in the C C double bond symmetric stretch as the primary acceptor of population from the S 1 state. A mechanism with which the other normal modes are populated is postulated.

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Section: Introductionmentioning

confidence: 99%

The role of specific normal modes during non‐Born–Oppenheimer dynamics: the S₁–S₀ internal conversion of β‐carotene interrogated on a femtosecond time‐scale with coherent anti‐Stokes Raman scattering

Siebert

Maksimenka

Materny

et al. 2002

J Raman Spectroscopy

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“…Recently the theory has been developed to relate [25] absorption spectra with the CARS susceptibility ) 3 ( F as well as femtosecond CARS with arbitrary pulsed laser excitations [26]. Results from the theory show good agreement with the sum-over states method [27,28] and experimental data [29].…”

Section: Femtosecond Coherent Anti-stokes Raman Introduction and Progmentioning

confidence: 83%

Femtosecond Coherent Anti-Stokes Raman Spectroscopy (CARS) As Next Generation Nonlinear LIDAR Spectroscopy and Microscopy

Ooi¹

2009

AIP Conference Proceedings

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Nonlinear spectroscopy using coherent anti-Stokes Raman scattering and femtosecond laser pulses has been successfully developed as powerful tools for chemical analysis and biological imaging. Recent developments show promising possibilities of incorporating CARS into LIDAR system for remote detection of molecular species in airborne particles. The corresponding theory is being developed to describe nonlinear scattering of a mesoscopic particle composed of complex molecules by laser pulses with arbitrary shape and spectral content. Microscopic many-body transform theory is used to compute the third order susceptibility for CARS in molecules with known absorption spectrum and vibrational modes. The theory is combined with an integral scattering formula and Mie-Lorentz formulae, giving a rigorous formalism which provides powerful numerical experimentation of CARS spectra, particularly on the variations with the laser parameters and the direction of detection.

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“…Such theory is available, called transform theory. [26] The theory relates [27] absorption spectra to the CARS susceptibilityχ (3) and has been shown to give good agreement with the sum-over states method [28,29] and experimental data. [30] Recently, the theory has been used to compute the time dependent polarization [31] under pulsed laser excitations.…”

Section: Introductionmentioning

confidence: 91%

Theory of coherent anti‐Stokes Raman scattering for mesoscopic particle with complex molecules: angular‐dependent spectrum

Ooi

2009

J Raman Spectroscopy

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We present a microscopic theory of nonlinear scattering of mesoscopic particle that may be composed of complex molecules. We predict that the spectrum of the scattered field depends on the angle of observation. Transform theory is used to compute the third-order susceptibility for coherent anti-Stokes Raman scattering (CARS) of molecules with known absorption spectrum and vibrational modes. By incorporating the theory into an integral scattering formula, we develop a rigorous theory which leads to powerful numerical experimentation of nonlinear optical process in mesoscopic systems composed of complex molecules and driven by laser pulses with arbitrary shape and spectral content. We obtain an expression for spectral dependent CARS field which includes multiple internal reflection and refraction of the incident fields via Mie theory. The theory is used to study the variations of the CARS spectra and intensity on laser parameters and direction of detection. High-resolution spectra computed for hybrid CARS scheme shows that the relative intensities of the characteristic peaks in the CARS spectrum depend on the direction of detection. This effect can be explained by the interference between the linear response (absorption and dispersion) and the four-wave mixing process in the mesoscopic medium. The theory is useful for nonlinear spectroscopy, microscopy and nanophotonics involving small particles.

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Experimental and theoretical coherent anti-Stokes Raman scattering studies on triplet excited anthracene

Cited by 6 publications

References 67 publications

The role of specific normal modes during non‐Born–Oppenheimer dynamics: the S₁–S₀ internal conversion of β‐carotene interrogated on a femtosecond time‐scale with coherent anti‐Stokes Raman scattering

The role of specific normal modes during non‐Born–Oppenheimer dynamics: the S₁–S₀ internal conversion of β‐carotene interrogated on a femtosecond time‐scale with coherent anti‐Stokes Raman scattering

Femtosecond Coherent Anti-Stokes Raman Spectroscopy (CARS) As Next Generation Nonlinear LIDAR Spectroscopy and Microscopy

Theory of coherent anti‐Stokes Raman scattering for mesoscopic particle with complex molecules: angular‐dependent spectrum

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Experimental and theoretical coherent anti-Stokes Raman scattering studies on triplet excited anthracene

Cited by 6 publications

References 67 publications

The role of specific normal modes during non‐Born–Oppenheimer dynamics: the S1–S0 internal conversion of β‐carotene interrogated on a femtosecond time‐scale with coherent anti‐Stokes Raman scattering

The role of specific normal modes during non‐Born–Oppenheimer dynamics: the S1–S0 internal conversion of β‐carotene interrogated on a femtosecond time‐scale with coherent anti‐Stokes Raman scattering

Femtosecond Coherent Anti-Stokes Raman Spectroscopy (CARS) As Next Generation Nonlinear LIDAR Spectroscopy and Microscopy

Theory of coherent anti‐Stokes Raman scattering for mesoscopic particle with complex molecules: angular‐dependent spectrum

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The role of specific normal modes during non‐Born–Oppenheimer dynamics: the S₁–S₀ internal conversion of β‐carotene interrogated on a femtosecond time‐scale with coherent anti‐Stokes Raman scattering

The role of specific normal modes during non‐Born–Oppenheimer dynamics: the S₁–S₀ internal conversion of β‐carotene interrogated on a femtosecond time‐scale with coherent anti‐Stokes Raman scattering