Fluorescence-line-narrowing spectroscopy of nile blue in glass and polymer at 5 K: Determination of a single-site line shape function

Zhang, Yiping; Hartmann, S. R.; Moshary, Fred

doi:10.1063/1.471188

Cited by 11 publications

(17 citation statements)

References 16 publications

(22 reference statements)

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“…For input we use the same functions ͑Ϫ 00 ͒ and g͑ 00 Ϫ 00 0 ͒ as were used in our FLN study. 12 The function ͑Ϫ 00 ͒ is shown in Fig. 10͑a͒.…”

Section: Broadband Excitationmentioning

confidence: 99%

“…This basis rests on the single-site line shape analysis which we successfully applied to our FLN experiments on nile blue in ethanol. 12 It requires the existence and knowledge of the site independent single-site absorption response ͑Ϫ 00 ͒ and its associated inhomogeneous distribution function g͑ 00 Ϫ 00 0 ͒. Here 00 is the frequency of the electronic transition in the absence of vibronic excitation and 00 0 is the central frequency of this distribution.…”

Section: Introductionmentioning

confidence: 99%

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Incoherent four-wave-mixing on nile blue and cresyl violet in glass and polymer at 5 K: Single-site line shape analysis

Zhang

Hartmann

Moshary

1996

The Journal of Chemical Physics

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An analysis of the radiation line shape from a multiple quantum well structure in fourwavemixing AIP Conf. Proc. 328, 361 (1995); 10.1063/1.47474 Studies of resonant and preresonant femtosecond degenerate fourwave mixing in unoriented conducting polymersTime-delayed-four-wave-mixing ͑TDFWM͒ experiments performed on nile blue and cresyl violet at 5 K using incoherent laser radiation yield a response which depends dramatically on excitation conditions. Fast ͑femtosecond͒ and slow ͑picosecond͒ processes, variable peak shifts, and type I and II quantum beats are all observed according to the laser frequency L and bandwidth ⌬ L . We model the TDFWM response on the basis of a site-independent molecular response and an associated inhomogeneous distribution function. These functions are constructed by combining information from TDFWM and fluorescence-line-narrowing ͑FLN͒ experiments.

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“…For input we use the same functions ͑Ϫ 00 ͒ and g͑ 00 Ϫ 00 0 ͒ as were used in our FLN study. 12 The function ͑Ϫ 00 ͒ is shown in Fig. 10͑a͒.…”

Section: Broadband Excitationmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Incoherent four-wave-mixing on nile blue and cresyl violet in glass and polymer at 5 K: Single-site line shape analysis

Zhang

Hartmann

Moshary

1996

The Journal of Chemical Physics

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“…We therefore attribute the clear synchronized spectral motion to local modes acting independently on the seven BChl a chromophores to produce synchronized motions for the distinct excitons. For reference, the same treatment was applied to a Nile Blue A standard, confirming that it produces its own expected power spectral densities, [35][36][37][38] which are distinct from those in FMO.…”

Section: Resultsmentioning

confidence: 99%

Correlated Protein Environments Drive Quantum Coherence Lifetimes in Photosynthetic Pigment-Protein Complexes

Rolczynski

Zheng

Singh

et al. 2018

Chem

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Energy transfer in photosynthesis occurs as electronic excitations of coupled chromophores interact with their environment. The microscopic nature of these motions can enable novel energy-transfer mechanisms if the motions are not random. This study reveals synchronized and correlated fluctuations of the states within a photosynthetic pigment-protein complex, which explains prior observations of long-lived quantum coherence. SUMMARYEarly reports of long-lived quantum beating signals in photosynthetic pigmentprotein complexes were interpreted to suggest that electronic coherence benefits from protection by the protein, but many subsequent studies have suggested instead that vibrational or vibronic contributions are responsible for the observed signals. Here, we devised two 2D-spectroscopy methods to observe how each exciton is perturbed by its nuclear environment in a photosynthetic complex. The first approach simultaneously monitors each exciton's energy fluctuations over time to obtain its time-dependent electronic-nuclear interactions. The second method isolates evidence of coupled interexcitonic environmental motions. The techniques are validated with Nile Blue A and subsequently used on the Fenna-Matthews-Olson (FMO) complex. The FMO data reveal that each exciton experiences nearly identical spectral motion after excitation and that spectral motion of one excited exciton induces similar motion on unpopulated neighboring excitonic states. These synchronized and correlated spectral dynamics prolong coherences in the FMO complex after femtosecond excitation.

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“…62 Incoherent four-wave-mixing and fluorescence-line-narrowing measurements obtained an inhomogeneous broadening of 600 cm -1 at fwhm in ethanol glass and in poly(vinyl alcohol). 70,71 Our simulation resulted in λ B ) 80 cm -1 and ∆ in ) 500 cm -1 which seems to be not a bad approximation.…”

Section: Comparison With Other Photon Echo Experimentsmentioning

confidence: 88%

Two-Dimensional Analysis of Integrated Three-Pulse Photon Echo Signals of Nile Blue Doped in PMMA

et al. 2003

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The integrated three-pulse photon echo signal of Nile blue doped in poly(methyl methacrylate) (PMMA) was measured two-dimensionally by varying the first coherence period and the subsequent population period. The electronic dephasing time was in the femtosecond time range even at low temperatures, whereas rephasing and echo formation were still possible even when the population period was extended to >100 ps. Oscillation was present in the echo signal even when population period was extended to longer values than the dephasing time of the vibrational coherence. Echo peak shift measurement indicated a presence of small spectral diffusion in the picosecond time range. A computer simulation was carried out from a model spectral density. The phonon mode of PMMA was represented by a Brownian oscillator centered at ∼116 cm -1 , and it reproduced the temperature dependence of the echo signal surprisingly well.

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Fluorescence-line-narrowing spectroscopy of nile blue in glass and polymer at 5 K: Determination of a single-site line shape function

Cited by 11 publications

References 16 publications

Incoherent four-wave-mixing on nile blue and cresyl violet in glass and polymer at 5 K: Single-site line shape analysis

Incoherent four-wave-mixing on nile blue and cresyl violet in glass and polymer at 5 K: Single-site line shape analysis

Correlated Protein Environments Drive Quantum Coherence Lifetimes in Photosynthetic Pigment-Protein Complexes

Two-Dimensional Analysis of Integrated Three-Pulse Photon Echo Signals of Nile Blue Doped in PMMA

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