Picosecond time-resolved multiplex coherent anti-Stokes Raman scattering spectroscopy by using a streak camera: Isomerization dynamics of all-trans and 9-cis retinal in the lowest excited triplet state

Article abstract of DOI:10.1063/1.466561

A picosecond time-resolved multiplex coherent anti-Stokes Raman scattering (CARS) measuring system using a streak camera was constructed.Picosecond uv laser pulses (50 ps) were used for the photoexcitation and nanosecond laser pulses (7 ns) were used as ω₁ and ω₂ for CARS probing.The multiplex CARS signals were spectrally analyzed by a spectrograph, and time-resolved and detected by a streak camera.This system enabled us two-dimensional (the time and frequency domain) detection of CARS signals with picosecond time resolution.The cis-trans photoisomerization dynamics of all-trans and 9-cis retinal was investigated.In the case of all-trans retinal, the CARS signals due to the "all-trans-like" T₁ state appeared in accordance with the decay of the S₁ fluorescence.In contrast, the appearance of the all-trans-like T₁ signals was markedly delayed in the case of the 9-cis isomer.This indicates that there exists a T₁ state having "9-cis-like" conformation in the picosecond time region.The lifetime of this 9-cis-like T₁ state was obtained as 880 +/- 150 ps from the analysis of the rise of the all-trans-like T₁ state.The mechanism of retinal photoisomerization is discussed on the basis of the obtained picosecond time-resolved data.It is concluded that the conformational change from the 9-cis to the all-trans form in the triplet manifold proceeds from the thermalized (not vibrationally excited) 9-cis-like T₁ state.

Full text of DOI:10.1063/1.466561

Picosecond timeresolved multiplex coherent antiStokes Raman scattering
spectroscopy by using a streak camera: Isomerization dynamics of alltrans and 9
cis retinal in the lowest excited triplet state
Tahei Tahara, Bulat N. Toleutaev, and Hiroo Hamaguchi
Citation: The Journal of Chemical Physics 100, 786 (1994); doi: 10.1063/1.466561
View online: http://dx.doi.org/10.1063/1.466561
View Table of Contents: http://scitation.aip.org/content/aip/journal/jcp/100/2?ver=pdfcov
Published by the AIP Publishing
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