Line Narrowing of Excited-State Transitions in Nonlinear Polarization Spectroscopy: Application to Water-Soluble Chlorophyll-Binding Protein

Schoth, Mario; Richter, Marten; Knorr, Andreas; Renger, Thomas

doi:10.1103/physrevlett.108.178104

Cited by 7 publications

(5 citation statements)

References 25 publications

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“…Besides structure prediction , and the development of theory, WSCP has been an important model system for the study of intersystem crossing in Chl a and Chl b . It has also been used for a theoretical demonstration of the capability of nonlinear polarization spectroscopy in the frequency domain to reveal the homogeneous broadening and thereby the lifetime of the upper exciton state . In the present work, we show that this lifetime is also accessible from HB spectra for resonant excitation of the upper exciton state.…”

Section: Introductionmentioning

confidence: 59%

Hole-Burning Spectroscopy on Excitonically Coupled Pigments in Proteins: Theory Meets Experiment

2016

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A theory for the calculation of resonant and nonresonant hole-burning (HB) spectra of pigment–protein complexes is presented and applied to the water-soluble chlorophyll-binding protein (WSCP) from cauliflower. The theory is based on a non-Markovian line shape theory (RengerMarcusRengerMarcusJ. Chem. Phys.20021169997) and includes exciton delocalization, vibrational sidebands, and lifetime broadening. An earlier approach by Reppert (J. Phys. Chem. Lett.201122716) is found to describe nonresonant HB spectra only. Here we present a theory that can be used for a quantitative description of HB data for both nonresonant and resonant burning conditions. We find that it is important to take into account the excess energy of the excitation in the HB process. Whereas excitation of the zero-phonon transition of the lowest exciton state, that is, resonant burning allows the protein to access only its conformational substates in the neighborhood of the preburn state, any higher excitation gives the protein full access to all conformations present in the original inhomogeneous ensemble. Application of the theory to recombinant WSCP from cauliflower, reconstituted with chlorophyll a or chlorophyll b, gives excellent agreement with experimental data by Pieper et al. (21417356J. Phys. Chem. B20111154053) and allows us to obtain an upper bound of the lifetime of the upper exciton state directly from the HB experiments in agreement with lifetimes measured recently in time domain 2D experiments by Alster et al. (24627983J. Phys. Chem. B20141183524).

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Section: Introductionmentioning

confidence: 59%

Hole-Burning Spectroscopy on Excitonically Coupled Pigments in Proteins: Theory Meets Experiment

2016

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“…). Systems like this can be found in coupled chromophores in photosynthetic complexes , coupled semiconductor quantum dots , coupled metal nanostructures , hybrid structures , etc.…”

Section: Unrevealing Signatures Not Visible In Far Fieldmentioning

confidence: 99%

Spatially localized spectroscopy for examining the internal structure of coupled nanostructures

Richter

2013

Phys. Status Solidi B

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Recent experimental progress in localized excitation with nanofields and localized detection for various observables (light intensities, photo electrons, etc.) at nanometer scales, suggest to rethink conventional spectroscopic schemes in terms of localized excitation and detection. In this paper, a systematic overview will be given, how the observables and Hamilton operators in case of localized excitation and detection need to be modified. The implications of localized excitation and detection are also illustrated using linear optics and pump probe spectroscopy.

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“…Complex (hybrid) nanostructures are often formed by combining different individual nanostructures such as metal nanoparticles, semiconductor quantum dots (QDs), pigments embedded in proteins, such as in light harvesting complexes and J-aggregates [1][2][3][4][5][6][7][8][9][10]. Couplings (such as Coulomb couplings) between the individual emitters lead to the formation of new quantum states delocalized over the individual nanostructure.…”

Section: Introductionmentioning

confidence: 99%

Using localized double-quantum-coherence spectroscopy to reconstruct the two-exciton wave function of coupled quantum emitters

et al. 2013

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Coherent multidimensional spectroscopy allows us to inspect the energies and the coupling of quantum systems. Coupled quantum systems-such as a coupled semiconductor quantum dot or pigments in photosynthesis-form delocalized exciton and two-exciton states. A technique is presented to decompose these delocalized wave functions into the basis of individual quantum emitters. This quantum state tomography protocol is illustrated for three coupled InAs quantum dots. To achieve the decomposition of the wavefunction, we combine the double-quantum-coherence spectroscopy with spatiotemporal control, which allows us to localize optical excitations at a specific quantum dot. Recently, a protocol was proposed for single exciton states (Richter et al 2012 Phys . Rev. B 86 085308). In this paper, we extend the method presented by Richter et al with respect to: the reconstruction of two-exciton states, a detailed analysis process of reconstruction and the effect of filtering to enhance the quality of the reconstructed wave function.

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Line Narrowing of Excited-State Transitions in Nonlinear Polarization Spectroscopy: Application to Water-Soluble Chlorophyll-Binding Protein

Cited by 7 publications

References 25 publications

Hole-Burning Spectroscopy on Excitonically Coupled Pigments in Proteins: Theory Meets Experiment

Hole-Burning Spectroscopy on Excitonically Coupled Pigments in Proteins: Theory Meets Experiment

Spatially localized spectroscopy for examining the internal structure of coupled nanostructures

Using localized double-quantum-coherence spectroscopy to reconstruct the two-exciton wave function of coupled quantum emitters

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