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Type: Article × Subject: Inhomogeneous broadening ×

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Now showing 1 - 3 of 3
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    Static Disorder in Excitation Energies of the Fenna-Matthews-Olson Protein: Structure-Based Theory Meets Experiment
    (Washington, DC : ACS, 2020) Chaillet, Martin L.; Lengauer, Florian; Adolphs, Julian; Müh, Frank; Fokas, Alexander S.; Cole, Daniel J.; Chin, Alex W.; Renger, Thomas
    Inhomogeneous broadening of optical lines of the Fenna-Matthews-Olson (FMO) light-harvesting protein is investigated by combining a Monte Carlo sampling of low-energy conformational substates of the protein with a quantum chemical/electrostatic calculation of local transition energies (site energies) of the pigments. The good agreement between the optical spectra calculated for the inhomogeneous ensemble and the experimental data demonstrates that electrostatics is the dominant contributor to static disorder in site energies. Rotamers of polar amino acid side chains are found to cause bimodal distribution functions of site energy shifts, which can be probed by hole burning and single-molecule spectroscopy. When summing over the large number of contributions, the resulting distribution functions of the site energies become Gaussians, and the correlations in site energy fluctuations at different sites practically average to zero. These results demonstrate that static disorder in the FMO protein is in the realm of the central limit theorem of statistics. © 2020 American Chemical Society.
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    Vectorial nonlinear coherent response of a strongly confined exciton-biexciton system
    (Bristol : IOP, 2013) Kasprzak, J.; Portolan, S.; Rastelli, A.; Wang, L.; Plumhof, J.D.; Schmidt, O.G.; Langbein, W.
    The vectorial four-wave mixing response of an individual strongly confined exciton-biexciton system with fine-structure splitting in a GaAs/AlGaAs quantum dot is measured by dual-polarization heterodyne spectral interferometry. The results are compared with theoretical predictions based on the optical Bloch equations. The system is described by a four-level scheme, which is a model system of the nonlinear excitonic response in low-dimensional semiconductors. We measure its coherence properties and determine the underlying dephasing mechanisms. An impact of the inhomogeneous broadening by spectral wandering on the coherent response is investigated. We further discuss the different four-wave mixing pathways, polarization selection rules, the time-resolved polarization state, the vectorial response in two-dimensional four-wave mixing and ensemble properties.
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    Ultrafast vibrational dynamics of the DNA backbone at different hydration levels mapped by two-dimensional infrared spectroscopy
    (Melville, NY : AIP Publishing LLC, 2015) Guchhait, Biswajit; Liu, Yingliang; Siebert, Torsten; Elsaesser, Thomas
    DNA oligomers are studied at 0% and 92% relative humidity, corresponding to N < 2 and N > 20 water molecules per base pair. Two-dimensional (2D) infrared spectroscopy of DNA backbone modes between 920 and 1120 cm(-1) maps fluctuating interactions at the DNA surface. At both hydration levels, a frequency fluctuation correlation function with a 300 fs decay and a slow decay beyond 10 ps is derived from the 2D lineshapes. The fast component reflects motions of DNA helix, counterions, and water shell. Its higher amplitude at high hydration level reveals a significant contribution of water to the fluctuating forces. The slow component reflects disorder-induced inhomogeneous broadening.