Transient Hole Burning and Solvation Dynamics of Chlorophyll <i>b</i> Monomers in Various Solvent Environments

Oksanen, J. A. I.; Martinsson, Peter; Åkesson, Eva; Hynninen, Paavo H.; Sundström, Villy

doi:10.1021/jp980252a

Cited by 26 publications

(32 citation statements)

References 33 publications

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“…The results provide direct information as to which wavelengths are best for monitoring energy transfer and at which wavelengths the transient absorption signal, and concomitantly the transient absorption anisotropy, are strongly influenced by excited state absorption. Similar information has previously been reported for chlorophyll a [18] and chlorophyll b [19] in pyridine.…”

Section: Introductionsupporting

confidence: 89%

An ultrafast time‐resolved anisotropy study of bacteriochlorophyll a in pyridine

2000

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The transient absorption anisotropy spectrum of bacteriochlorophyll a (BChl a) in pyridine was measured in the wavelength interval 550^850 nm, 1 ps after optical excitation with a 792-nm femtosecond light pulse. In the wavelength region of Q y absorption and stimulated emission (775^825 nm), the anisotropy was found to be close to the theoretically expected value (0.4) for a two-level system. In the wavelength region 6507 50 nm, where the transient absorption signal is dominated by excited state absorption, the anisotropy is reduced to V V0.18. Anisotropy kinetics were measured at several wavelengths and found to be constant within the time window 0^5 ps, showing that no internal dynamics of the BChl a molecule change the anisotropy on the time scale of tens of picoseconds.z 2000 Federation of European Biochemical Societies.

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Section: Introductionsupporting

confidence: 89%

An ultrafast time‐resolved anisotropy study of bacteriochlorophyll a in pyridine

2000

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“…Early time DAS spectra at 490 nm excitation (Fig. 6Sa in ESM) show positive amplitudes (rise of ESA) around 652 nm most (Oksanen et al 1998;Martinsson et al 1999). Around 680 nm positive amplitudes (rise of Chl a bleach/stimulated emission, SE) appear at early times but turn into negative amplitudes at later times (decay of Chl a bleach/SE).…”

Section: Nm Excitationmentioning

confidence: 96%

Excitation energy transfer in the LHC-II trimer: from carotenoids to chlorophylls in space and time

et al. 2011

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Exciton model for description of experimentally determined excitation energy transfer from carotenoids to chlorophylls in the LHC-II trimer of spinach is presented. Such an approach allows connecting the excitonic states to the spatial structure of the complex and hence descriptions of advancements of the initially created excitations in space and time. Carotenoids were excited at 490 nm and at 500 nm and induced absorbance changes probed in the Chl Q(y) region to provide kinetic data that were interpreted by using the results from exciton calculations. Calculations included the 42 chlorophylls and the 12 carotenoids of the complex, Soret, Q(x) and Q(y) states of the chlorophylls, and the main absorbing S(2) state of the carotenoids. According to the calculations excitation at 500 nm populates mostly a mixed Lut S(2) Chl a Soret state, from where excitation is transferred to the Q(x) and Q(y) states of the Chl a's on the stromal side. Internal conversion of the mixed state to a mixed Lut S(1) and Chl a Q(y) state provides a channel for Lut S(1) to Chl a Q(y) energy transfer. The results from the calculations support a picture where excitation at 490 nm populates primarily a mixed neoxanthin S(2) Chl b Soret state. From this state excitation from neoxanthin is transferred to iso-energetic Chl b Soret states or via internal conversion to S(1) Chl b Q(y) states. From the Soret states excitation proceeds via internal conversion to Q(y) states of Chl b's mostly on the lumenal side. A rapid Chl b to Chl a transfer and subsequent transfer to the stromal side Chl a's and to the final state completes the process after 490 nm excitation. The interpretation is further supported by the fact that excitation energy transfer kinetics after excitation of neoxanthin at 490 nm and the Chl b Q(y) band at 647 nm (Linnanto et al., Photosynth Res 87:267-279, 2006) are very similar.

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“…It was found that the sensitivity of the Q y band to hydrogen bond donors is larger than that of the Q x band. [106,118] The oscillator strengths of chlorophyll pigments also depend on the solvent. For example, for Chl a a range of the extinction coefficient from 6.14 10 À4 mol À1 cm À1 in cyclohexane to 8.52…”

mentioning

confidence: 99%

“…[119,120] Depending on the scheme, there are quite large differences in the extrapolated vacuum value. [120] Other possible solvent effects which might influence the absorption spectra of chlorophylls are self-aggregate breaking [118] or aggregate formation induced by the solvent molecules (see ref. [93] and references therein).…”

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confidence: 99%

Quantum Chemical Description of Absorption Properties and Excited‐State Processes in Photosynthetic Systems

2011

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The theoretical description of the initial steps in photosynthesis has gained increasing importance over the past few years. This is caused by more and more structural data becoming available for light-harvesting complexes and reaction centers which form the basis for atomistic calculations and by the progress made in the development of first-principles methods for excited electronic states of large molecules. In this Review, we discuss the advantages and pitfalls of theoretical methods applicable to photosynthetic pigments. Besides methodological aspects of excited-state electronic-structure methods, studies on chlorophyll-type and carotenoid-like molecules are discussed. We also address the concepts of exciton coupling and excitation-energy transfer (EET) and compare the different theoretical methods for the calculation of EET coupling constants. Applications to photosynthetic light-harvesting complexes and reaction centers based on such models are also analyzed.

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Transient Hole Burning and Solvation Dynamics of Chlorophyll b Monomers in Various Solvent Environments

Cited by 26 publications

References 33 publications

An ultrafast time‐resolved anisotropy study of bacteriochlorophyll a in pyridine

An ultrafast time‐resolved anisotropy study of bacteriochlorophyll a in pyridine

Excitation energy transfer in the LHC-II trimer: from carotenoids to chlorophylls in space and time

Quantum Chemical Description of Absorption Properties and Excited‐State Processes in Photosynthetic Systems

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