Transient Lens Spectroscopy in a Fast Timescale

Terazima, Masahide

doi:10.1002/ijch.199800016

Cited by 27 publications

(19 citation statements)

References 84 publications

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“…These originate from the solvent and (to a very small extent) from the windows of the quartz cuvette, for details see Section 4.1. Finally, two other lens effects must be mentioned, which however do not play a role in our case: 26 ''Molecular interaction lenses'' due to OKE contributions at high concentrations can be neglected, as shown by our concentration dependent experiments (Section 4.1.). Also lenses originating from a volume change of the solvent are not present in our case, because they require a fast and pronounced change of the solute geometry.…”

Section: Transient Lens Spectroscopymentioning

confidence: 90%

“…Lens phenomena have been known for a long time, and different types of lenses can occur: 26 On the nanosecond to millisecond time scale lenses are produced by heating (thermal lens) 27 or electrostriction (diffusion into the region of an intense laser field). On a much faster time scale (pico-to femtoseconds) the latter nonlocal effects are not important any more, and other types of lenses dominate.…”

Section: Transient Lens Spectroscopymentioning

confidence: 99%

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Ultrafast transient lens spectroscopy of various C40 carotenoids: lycopene, β-carotene, (3R,3′R)-zeaxanthin, (3R,3′R,6′R)-lutein, echinenone, canthaxanthin, and astaxanthin

Kopczynski

Lenzer

Oum

et al. 2005

Phys. Chem. Chem. Phys.

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The ultrafast internal conversion (IC) dynamics of seven C(40) carotenoids have been investigated at room temperature in a variety of solvents using two-color transient lens (TL) pump-probe spectroscopy. We provide comprehensive data sets for the carbonyl carotenoids canthaxanthin, astaxanthin, and-for the first time-echinenone, as well as new data for lycopene, beta-carotene, (3R,3'R)-zeaxanthin and (3R,3'R,6'R)-lutein in solvents which have not yet been investigated in the literature. Measurements were carried out to determine, how the IC processes are influenced by the conjugation length of the carotenoids, additional substituents and the polarity of the solvent. TL signals were recorded at 800 nm following excitation into the high energy edge of the carotenoid S2 band at 400 nm. For the S2 lifetime solvent-independent upper limits on the order of 100-200 fs are estimated for all carotenoids studied. The S1 lifetimes are in the picosecond range and increase systematically with decreasing conjugation length. For instance, in the sequence canthaxanthin/echinenone/beta-carotene (13/12/11 double bonds) one finds tau1 approximately 5, 7.7 and 9 ps for the S1-->S0 IC process, respectively. Hydroxyl groups not attached to the conjugated system have no apparent influence on tau1, as observed for canthaxanthin/astaxanthin (tau1 approximately 5 ps in both cases). For all carotenoids studied, tau1 is found to be insensitive to the solvent polarity. This is particularly interesting in the case of echinenone, canthaxanthin and astaxanthin, because earlier measurements for other carbonyl carotenoids like, e.g., peridinin partly showed dramatic differences. The likely presence of an intramolecular charge transfer state in the excited state manifold of C40 carbonyl carotenoids, which is stabilized in polar solvents, has obviously no influence on the measured tau1.

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Section: Transient Lens Spectroscopymentioning

confidence: 90%

Section: Transient Lens Spectroscopymentioning

confidence: 99%

Ultrafast transient lens spectroscopy of various C40 carotenoids: lycopene, β-carotene, (3R,3′R)-zeaxanthin, (3R,3′R,6′R)-lutein, echinenone, canthaxanthin, and astaxanthin

Kopczynski

Lenzer

Oum

et al. 2005

Phys. Chem. Chem. Phys.

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“…These effects, discussed below, include the optical Kerr effect, changes in concentrations of solutes, absorbance, and partial molal volume due to the induced photochemistry, and electrostriction. 64 In their traditional application, the time resolution of TL and PBD is determined by the mechanism of generation of the lens. To form the lens after a fast non-radiative relaxation, it takes a characteristic time for the medium to expand in response to the heat released.…”

Section: Photorefractive Techniquesmentioning

confidence: 99%

Time-resolved photothermal methods: accessing time-resolved thermodynamics of photoinduced processes in chemistry and biology

Gensch

Viappiani

2003

Photochem Photobiol Sci

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Photothermal methods are currently being employed in a variety of research areas, ranging from materials science to environmental monitoring. Despite the common term which they are collected under, the implementations of these techniques are as diverse as the fields of application. In this review, we concentrate on the recent applications of time-resolved methods in photochemistry and photobiology.

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“…The intensity of the TrL signal is proportional to the refractive index change induced by light excitation. 46 The origins of the TrL signal are described in more detail in the Supporting Information (SI-1(b)).…”

Section: Methodsmentioning

confidence: 99%

Time-resolved fluctuation during the photochemical reaction of a photoreceptor protein: phototropin1LOV2-linker

Kuroi

Sato

Nakasone

et al. 2016

Phys. Chem. Chem. Phys.

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Although the relationship between structural fluctuations and reactions is important for elucidating reaction mechanisms, experimental data describing such fluctuations of reaction intermediates are sparse. In order to investigate structural fluctuations during a protein reaction, the compressibilities of intermediate species after photoexcitation of a phot1LOV2-linker, which is a typical LOV domain protein with the C-terminal linker including the J-α helix and used recently for optogenetics, were measured in the time-domain by the transient grating and transient lens methods with a high pressure optical cell. The yield of covalent bond formation between the chromophore and a Cys residue (S state formation) relative to that at 0.1 MPa decreased very slightly with increasing pressure. The fraction of the reactive species that yields the T state (linker-unfolded state) decreased almost proportionally with pressure (0.1-200 MPa) to about 65%. Interestingly, the volume change associated with the reaction was much more pressure sensitive. By combining these data, the compressibility changes for the short lived intermediate (S state) and the final product (T state) formation were determined. The compressibility of the S state was found to increase compared with the dark (D) state, and the compressibility decreased during the transition from the S state to the T state. The compressibility change is discussed in terms of cavities inside the protein. By comparing the crystal structures of the phot1LOV2-linker at dark and light states, we concluded that the cavity volumes between the LOV domain and the linker domain increase in the S state, which explains the enhanced compressibility.

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Transient Lens Spectroscopy in a Fast Timescale

Cited by 27 publications

References 84 publications

Ultrafast transient lens spectroscopy of various C40 carotenoids: lycopene, β-carotene, (3R,3′R)-zeaxanthin, (3R,3′R,6′R)-lutein, echinenone, canthaxanthin, and astaxanthin

Ultrafast transient lens spectroscopy of various C40 carotenoids: lycopene, β-carotene, (3R,3′R)-zeaxanthin, (3R,3′R,6′R)-lutein, echinenone, canthaxanthin, and astaxanthin

Time-resolved photothermal methods: accessing time-resolved thermodynamics of photoinduced processes in chemistry and biology

Time-resolved fluctuation during the photochemical reaction of a photoreceptor protein: phototropin1LOV2-linker

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