Two-dimensional spectroscopy: Theory of nonstationary, time-dependent absorption and its application to femtosecond processes

Fain, Benjamin; Lin, Su; Hamer, N.D.

doi:10.1063/1.456786

Cited by 64 publications

(20 citation statements)

References 22 publications

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“…A zero time corresponds to the center of the pump pulse. Based on the density-matrix formalism and the transient linear susceptibility approach (Lin 1974;Fain et al 1989;Gu et al 1995), the incoherent time-dependent absorption of the ground state and the stimulated emission of the excited state can be written as…”

Section: Modelmentioning

confidence: 99%

Spectral exhibition of electron-vibrational relaxation in P* state of Rhodobacter sphaeroides reaction centers

Yakovlev

Shuvalov

2014

Photosynth Res

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Electron-vibrational relaxation in the excited state of the primary electron donor, bacteriochlorophyll dimer P, in the reaction centers (RCs) of purple photosynthetic bacteria Rhodobacter sphaeroides is modeled. A multimode model of three states (i.e., the ground state Pg, initially excited P1*, and relaxed excited P2*) is used to calculate the incoherent dynamics of the difference (ΔA) spectra on a femtosecond timescale for the YM210 W mutant RCs. The relaxation processes are described by the step-ladder model. The model shows that the electron-vibrational relaxation in the excited state of P is visualized by the transient red shift of the stimulated emission from P*. The dynamics of this shift is observed as a change in the ΔA spectrum shape in its red-most part, within a few hundreds of femtoseconds after excitation. As a result, an initial rise in the red-side ΔA kinetics is delayed with respect to the blue-side kinetics. The time constant of the P1* → P2* electronic relaxation (54 fs) and the Pg, P1*, and P2* vibrational relaxations (120 fs), used in the model, provided the best fit of the experimental time-resolved ΔA spectra and kinetics at 90 and 293 K. The possible nature of the P1* → P2* electronic relaxation is discussed.

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Section: Modelmentioning

confidence: 99%

Spectral exhibition of electron-vibrational relaxation in P* state of Rhodobacter sphaeroides reaction centers

Yakovlev

Shuvalov

2014

Photosynth Res

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“…We shall start with the definition of density matrix [82][83][84]. For this purpose, we consider a two-state system.…”

Section: Relaxation Dynamics Of a System In A Heat Bath A Densitmentioning

confidence: 99%

Ultrafast Dynamics and Spectroscopy of Bacterial Photosynthetic Reaction Centers

Lin¹,

Chang²,

Liang³

et al. 2002

Advances in Chemical Physics

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117

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“…The present work is organized as follows: the theoretical treatment on the basis of the perturbative density operator method [33,34] and the transient linear susceptibility theory [35][36][37] are briefly described in Section 2. The calculated FDSs are presented and compared with experimental spectra in Section 3.…”

Section: Introductionmentioning

confidence: 99%

Theoretical analysis of femtosecond fluorescence depletion spectra and vibrational relaxations of dye oxazine 750 and rhodamine 700 molecules in acetone solution

Dong

Niu

Cong

2006

Int J of Quantum Chemistry

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ABSTRACT:The fluorescence depletion spectra of oxazine 750 (OX750) and rhodamine 700 (LD700) molecules in acetone solution are calculated using the perturbative density operator method and the transient linear susceptibility theory. The calculated fluorescence depletion spectra of the dye OX750 and LD700 molecules agree well with the experimental results reported by Liu et al. The calculated decay time of the fluorescence depletion spectra due to the vibrational relaxation ranges from 300 to 450 fs, and the decay time resulting from the solvation effect is a few tens of picoseconds. The calculated vibrational relaxation rates are 4.3 and 4.9 ps Ϫ1 for the OX750 and LD700 molecules, respectively. The effects of temperature and probe pulse parameters on the fluorescence depletion spectra are also discussed.

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Two-dimensional spectroscopy: Theory of nonstationary, time-dependent absorption and its application to femtosecond processes

Cited by 64 publications

References 22 publications

Spectral exhibition of electron-vibrational relaxation in P* state of Rhodobacter sphaeroides reaction centers

Spectral exhibition of electron-vibrational relaxation in P* state of Rhodobacter sphaeroides reaction centers

Ultrafast Dynamics and Spectroscopy of Bacterial Photosynthetic Reaction Centers

Theoretical analysis of femtosecond fluorescence depletion spectra and vibrational relaxations of dye oxazine 750 and rhodamine 700 molecules in acetone solution

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