Nonphotochemical hole burning of the reaction center of Rhodopseudomonas viridis

Reddy, N. R. S.; Kolaczkowski, Stephen V.; Small, Gerald J.

doi:10.1021/j100128a031

Cited by 73 publications

(98 citation statements)

References 7 publications

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“…We suggest that the approach with a lognormal spectral density describes the phonon lineshape more accurately, 25 although to reveal the difference between our approach and that of Hayes et al, 19 i.e., to compare our parameters with the previously published data, 8,9,28 we also show fits and parameters obtained with the G-L J(ω). On the basis of previous work, 8,9,28 only two profiles corresponding to peak frequencies ω ph and ω sp are required to simultaneously fit the P870 and P960 absorption bands and ω B -dependent photochemical (transient) HB spectra. Consistent with earlier assignment, we refer to ω ph as the mean (or rather peak) phonon frequency and ω sp as the special pair marker mode.…”

Section: A Calculation Of Hb Spectramentioning

confidence: 72%

“…19, along with many later works [7][8][9][10][11][12][13][14][15][16][17][18] ). Although such a profile does provide a reasonable approximation to the true form of l R (ω) at low temperatures when the Gaussian and Lorentzian components have similar widths, the approximation breaks down quite seriously when Γ G is much different from √ RΓ L (see below).…”

Section: Derivation Of Lineshape Formulasmentioning

confidence: 97%

“…(5) and (9) in this work) to produce a "hybrid" absorption expression involving finite-width profiles l R,P (±ω − Ω 0 + (R − 2P)ω m ) with Franck-Condon factors described (incorrectly) by Eq. (9). Such an expression might be used to model a system with a spectral density of the form…”

Section: Derivation Of Lineshape Formulasmentioning

confidence: 99%

“…This approach is compared below with the mean-phonon approximation used in earlier calculations, 8,9,28 where the spectral density was split into multiple effective phonon densities and the continuous weighting factor n(ω; T) was replaced by an effective factor n(ω k ; T) evaluated at a "mean" phonon frequency ω k near the peak of the kth phonon density; and where in place of numerical convolutions, multi-phonon transitions were described simply as increasingly broadened G-L profiles. We suggest that the approach with a lognormal spectral density describes the phonon lineshape more accurately, 25 although to reveal the difference between our approach and that of Hayes et al, 19 i.e., to compare our parameters with the previously published data, 8,9,28 we also show fits and parameters obtained with the G-L J(ω). On the basis of previous work, 8,9,28 only two profiles corresponding to peak frequencies ω ph and ω sp are required to simultaneously fit the P870 and P960 absorption bands and ω B -dependent photochemical (transient) HB spectra.…”

Section: A Calculation Of Hb Spectramentioning

confidence: 99%

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Comments on the optical lineshape function: Application to transient hole-burned spectra of bacterial reaction centers

Reppert

Kell

Pruitt

et al. 2015

The Journal of Chemical Physics

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The vibrational spectral density is an important physical parameter needed to describe both linear and non-linear spectra of multi-chromophore systems such as photosynthetic complexes. Low-temperature techniques such as hole burning (HB) and fluorescence line narrowing are commonly used to extract the spectral density for a given electronic transition from experimental data. We report here that the lineshape function formula reported by Hayes et al. [J. Phys. Chem. 98, 7337 (1994)] in the mean-phonon approximation and frequently applied to analyzing HB data contains inconsistencies in notation, leading to essentially incorrect expressions in cases of moderate and strong electron-phonon (el-ph) coupling strengths. A corrected lineshape function L(ω) is given that retains the computational and intuitive advantages of the expression of Hayes et al. [J. Phys. Chem. 98, 7337 (1994)]. Although the corrected lineshape function could be used in modeling studies of various optical spectra, we suggest that it is better to calculate the lineshape function numerically, without introducing the mean-phonon approximation. New theoretical fits of the P870 and P960 absorption bands and frequency-dependent resonant HB spectra of Rb. sphaeroides and Rps. viridis reaction centers are provided as examples to demonstrate the importance of correct lineshape expressions. Comparison with the previously determined el-ph coupling parameters [Johnson et al., J. Phys. Chem. 94, 5849 (1990); Lyle et al., ibid. 97, 6924 (1993); Reddy et al., ibid. 97, 6934 (1993)] is also provided. The new fits lead to modified el-ph coupling strengths and different frequencies of the special pair marker mode, ωsp, for Rb. sphaeroides that could be used in the future for more advanced calculations of absorption and HB spectra obtained for various bacterial reaction centers.

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Section: A Calculation Of Hb Spectramentioning

confidence: 72%

Section: Derivation Of Lineshape Formulasmentioning

confidence: 97%

Section: Derivation Of Lineshape Formulasmentioning

confidence: 99%

Section: A Calculation Of Hb Spectramentioning

confidence: 99%

See 2 more Smart Citations

Comments on the optical lineshape function: Application to transient hole-burned spectra of bacterial reaction centers

Reppert

Kell

Pruitt

et al. 2015

The Journal of Chemical Physics

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“…The low-energy exciton state of P (P Ϫ ) was excited at 880 nm, B A was excited at 796 nm, and a combination of B B and the high-energy exciton component of P (P ϩ ) was excited at 818 nm (27). However, given the relatively broad excitation pulses and partially overlapping absorbance bands of B A and B B , and given the possibility that B A and B B might be excitonically mixed (28), excitation in the B band will be only partial selective. In Fig.…”

Section: Resultsmentioning

confidence: 99%

Multiple pathways for ultrafast transduction of light energy in the photosynthetic reaction center of Rhodobacter sphaeroides

Brederode

Mourik

Stokkum

et al. 1999

Proc. Natl. Acad. Sci. U.S.A.

112

107

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A pathway of electron transfer is described that operates in the wild-type reaction center (RC) of the photosynthetic bacterium Rhodobacter sphaeroides. The pathway does not involve the excited state of the special pair dimer of bacteriochlorophylls (P*), but instead is driven by the excited state of the monomeric bacteriochlorophyll (B A *) present in the active branch of pigments along which electron transfer occurs. Pump-probe experiments were performed at 77 K on membrane-bound RCs by using different excitation wavelengths, to investigate the formation of the charge separated state P ؉ H A ؊ . In experiments in which P or B A was selectively excited at 880 nm or 796 nm, respectively, the formation of P ؉ H A ؊ was associated with similar time constants of 1.5 ps and 1.7 ps. However, the spectral changes associated with the two time constants are very different. Global analysis of the transient spectra shows that a mixture of P ؉ B A ؊ and P* is formed in parallel from B A * on a subpicosecond time scale. In contrast, excitation of the inactive branch monomeric bacteriochlorophyll (B B ) and the high exciton component of P (P ؉ ) resulted in electron transfer only after relaxation to P*. The multiple pathways for primary electron transfer in the bacterial RC are discussed with regard to the mechanism of charge separation in the RC of photosystem II from higher plants.

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Ultrafast Dynamics and Spectroscopy of Bacterial Photosynthetic Reaction Centers

Lin¹,

Chang²,

Liang³

et al. 2002

Advances in Chemical Physics

117

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Nonphotochemical hole burning of the reaction center of Rhodopseudomonas viridis

Cited by 73 publications

References 7 publications

Comments on the optical lineshape function: Application to transient hole-burned spectra of bacterial reaction centers

Comments on the optical lineshape function: Application to transient hole-burned spectra of bacterial reaction centers

Multiple pathways for ultrafast transduction of light energy in the photosynthetic reaction center of Rhodobacter sphaeroides

Ultrafast Dynamics and Spectroscopy of Bacterial Photosynthetic Reaction Centers

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