1998
DOI: 10.1021/jp973197z
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Ultrashort Processes of Native Phytochrome:  Femtosecond Kinetics of the Far-Red-Absorbing Form Pfr

Abstract: The biologically active far-red-absorbing form of the plant photoreceptor phytochrome, Pfr, was studied by femtosecond spectroscopy. The transient absorption changes that occurred upon excitation of Pfr at 730 nm with laser pulses of 150 fs were measured as a function of time at selected probe wavelengths. Immediately after excitation, bleaching of the ground-state absorption bands in the red and blue spectral region was observed. Bleaching was accompanied by an absorption increase at wavelengths between 775 a… Show more

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Cited by 21 publications
(22 citation statements)
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“…The difference in the early-time dynamics between the lactam and lactim tautomers of PCB is reminiscent of that in the excitedstate chemistry of phytochromes, revealing that the Pfr-to-Pr back reaction occurs in % 700 fs and is clearly faster than the Pr-to-Pfr forward reaction. [19,20,22,29] It is therefore suggested that the chromophore in the Pfr-form of phytochrome could adopt a lactim-like structure, which is responsible for the red shift in the long-wavelength absorption and in particular for the extremely fast primary reaction time. Interactions with the protein moiety in the native chromoprotein are expected to assist the stabilization of the lactim-like structure and to control the specific photochemistry.…”
Section: Discussionmentioning
confidence: 99%
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“…The difference in the early-time dynamics between the lactam and lactim tautomers of PCB is reminiscent of that in the excitedstate chemistry of phytochromes, revealing that the Pfr-to-Pr back reaction occurs in % 700 fs and is clearly faster than the Pr-to-Pfr forward reaction. [19,20,22,29] It is therefore suggested that the chromophore in the Pfr-form of phytochrome could adopt a lactim-like structure, which is responsible for the red shift in the long-wavelength absorption and in particular for the extremely fast primary reaction time. Interactions with the protein moiety in the native chromoprotein are expected to assist the stabilization of the lactim-like structure and to control the specific photochemistry.…”
Section: Discussionmentioning
confidence: 99%
“…The difference in the early-time dynamics between the lactam and lactim tautomers of PCB is reminiscent of that in the excitedstate chemistry of phytochromes, revealing that the Pfr-to-Pr back reaction occurs in % 700 fs and is clearly faster than the Pr-to-Pfr forward reaction. [19,20,22,29] It is therefore suggested Table 1. Geometrical parameters defining the planarity of the minimum energy structures in the different lactam/lactim tautomers of PCB (1)- (6).…”
Section: Discussionmentioning
confidence: 99%
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“…The constants are used in a simulation procedure to fit the experimental data. Such an approach differs from the standard fittings, such as the scanning procedure or a global scanning fit (see Bischoff et al . (1998) and applies also in Appenroth et al .…”
Section: Methodsmentioning
confidence: 99%
“…The constants are used in a simulation procedure to fit the experimental data. Such an approach differs from the standard fittings, such as the scanning procedure or a global scanning fit (see Bischoff et al (1998) and applies also in Appenroth et al (2000), which utilizes the analytic expressions of solutions to the simplified model equations as a basis for the fitting procedure. The proposed method can be successfully applied in such cases when exact solutions to the model equations cannot be obtained.…”
Section: S F T K Ttmentioning
confidence: 99%