Time-resolved photoisomerization of 1,1′-di-tert-butylstilbene and 1,1′-dicyanostilbene

Dobryakov, A. L.; Quick, Martin; Lenoir, Dieter; Detert, Heiner; Érnsting, N. P.; Kovalenko, Sergey A.

doi:10.1016/j.cplett.2016.04.060

Chemical Physics Letters

2016

DOI: 10.1016/j.cplett.2016.04.060

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Time-resolved photoisomerization of 1,1′-di-tert-butylstilbene and 1,1′-dicyanostilbene

A. L. Dobryakov

Martin Quick

Dieter Lenoir

et al.

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Cited by 13 publications

(23 citation statements)

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“…Positive induced absorbance Δ A > 0 is caused by excited-state absorption (ESA) S 1 → S n , and negative contributions indicate bleach and stimulated emission (SE) S 1 → S 0 . Spectra have been measured repeatedly over several years; the result in Figure reproduces the one of ref but with improved accuracy. A global fit requires five exponential time functions, one oscillatory time function, and an offset.…”

supporting

confidence: 54%

“…As a consequence, significant population can now be accumulated at the perpendicular configuration even by excitation of the trans isomer. This opportunity is preserved in 1,1′-dicyano-stilbene where τ P = 27 ps; in addition, the absorption band of P is shifted to longer wavelengths around 370 nm . Separation from competitive kinetics and an electronic resonance closer to the visible range are helpful for femtosecond-stimulated Raman (FSR) spectroscopy. , …”

mentioning

confidence: 99%

“…For this reason, we study 1,1′-dicyano-stilbene, starting from the trans isomer in n -hexane. Transient absorption spectra are now described quantitatively. Quantum-chemical calculations provide initial structures and the likely direction of change after UV excitation.…”

mentioning

confidence: 99%

“…With the same time constant a new absorption band rises with a peak at 374 nm. By comparison with various stilbenes, , the 374 nm band is attributed to excited-state absorption from a perpendicular form P on the S 1 potential energy surface (denoted ESA(P) in the following, or “P band” for short). (c) On a slower time scale τ 3 = 1.0 ps the ESA(P) band continues to rise until 3 ps, while the red-shifted SE decays completely.…”

mentioning

confidence: 99%

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Perpendicular State of an Electronically Excited Stilbene: Observation by Femtosecond-Stimulated Raman Spectroscopy

Quick

Dobryakov

Ioffe

et al. 2016

J. Phys. Chem. Lett.

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In the photoisomerization path of stilbene, a perpendicular state P on the S potential energy surface is expected just before internal conversion through a conical intersection S/S. For decades the observation of P was thwarted by a short lifetime τ in combination with slow population flow over a barrier. But these limitations can be overcome by ethylenic substitution. Following optical excitation of trans-1,1'-dicyanostilbene, P is populated significantly (τ = 27 ps in n-hexane) and monitored by an exited-state absorption band at 370 nm. Here we report stimulated Raman lines of P. The strongest, at 1558 cm, is attributed to stretching vibrations of the phenyl rings. Transient electronic states, resonance conditions, and corresponding Raman signals are discussed.

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supporting

confidence: 54%

mentioning

confidence: 99%

mentioning

confidence: 99%

mentioning

confidence: 99%

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Perpendicular State of an Electronically Excited Stilbene: Observation by Femtosecond-Stimulated Raman Spectroscopy

Quick

Dobryakov

Ioffe

et al. 2016

J. Phys. Chem. Lett.

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“…data reports geometrical strain (Lenoir, 1989;Dobryakov et al, 2016). The reaction proceeds via a pinacol intermediate, the geometry of which is decisive for the configuration of the product.…”

mentioning

confidence: 98%

The rel-R,R-enantiomer of 7-[7-hydroxybicyclo[4.2.0]octa-1(6),2,4-trien-7-yl]bicyclo[4.2.0]octa-1(6),2,4-trien-7-ol

Detert

Schollmeyer

2018

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Multidimensional Vibrational Coherence Spectroscopy

Buckup

Léonard

2018

Top Curr Chem (Z)

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Multidimensional vibrational coherence spectroscopy has been part of laser spectroscopy since the 1990s and its role in several areas of science has continuously been increasing. In this contribution, after introducing the principals of vibrational coherence spectroscopy (VCS), we review the three most widespread experimental methods for multidimensional VCS (multi-VCS), namely femtosecond stimulated Raman spectroscopy, pump-impulsive vibrational spectroscopy, and pump-degenerate four wave-mixing. Focus is given to the generation and typical analysis of the respective signals in the time and spectral domains. Critical aspects of all multidimensional techniques are the challenges in the data interpretation due to the existence of several possible contributions to the observed signals or to optical interferences and how to overcome the corresponding difficulties by exploiting experimental parameters including higher-order nonlinear effects. We overview how multidimensional vibrational coherence spectroscopy can assist a chemist in understanding how molecular structural changes and eventually photochemical reactions take place. In order to illustrate the application of the techniques described in this chapter, two molecular systems are discussed in more detail in regard to the vibrational dynamics in the electronic excited states: (1) carotenoids as a non-reactive system and (2) stilbene derivatives as a reactive system.

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Time-resolved photoisomerization of 1,1′-di-tert-butylstilbene and 1,1′-dicyanostilbene

Cited by 13 publications

References 23 publications

Perpendicular State of an Electronically Excited Stilbene: Observation by Femtosecond-Stimulated Raman Spectroscopy

Perpendicular State of an Electronically Excited Stilbene: Observation by Femtosecond-Stimulated Raman Spectroscopy

The rel-R,R-enantiomer of 7-[7-hydroxybicyclo[4.2.0]octa-1(6),2,4-trien-7-yl]bicyclo[4.2.0]octa-1(6),2,4-trien-7-ol

Multidimensional Vibrational Coherence Spectroscopy

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