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Project B7

Ultrafast dynamics and structural studies of prokaryotic and plant phytochromes

Principal Investigators: Prof. Dr. Karsten Heyne (FU), Prof. Dr. Jon Hughes (JLU)

Using X-ray crystallography together with state-of-the-art ultrafast Vis and IR spectroscopic methods, we propose to determine and interpret phytochrome structures and track ultrafast changes in hydrogen bonding networks, proton donor and acceptor groups and electrostatic interactions following photon absorption. We will focus on Cph1 and plant phytochromes, although studies on rhodopsins are also included. Comparison of related structures and dynamics will allow us to make general conclusions regarding structure/functional regulation via protonation dynamics and other processes.

Publications

2017 - 2020

Kraskov, A., Nguyen, A.D., Goerling, J., Buhrke, D., Velazquez Escobar, F., Fernandez Lopez, M., Michael, N., Sauthof, L., Schmidt, A., Piwowarski, P., Yang, Y., Stensitzki, T., Adam, S., Bartl, F., Schapiro, I., Heyne, K., Siebert, F., Scheerer, P., Mroginski, M.A., and Hildebrandt, P. (2020). Intramolecular proton transfer controls protein structural changes in phytochrome. Biochemistry 59, 1023-1037; doi: 10.1021/acs.biochem.0c00053

Nass Kovacs, G., Colletier, J.-P., Grünbein, M. L., Yang, Y., Stensitzki, T., Batyuk, A., Carbajo, S., Doak, R. B., Ehrenberg, D., Foucar, L., Gasper, R., Gorel, A., Hilpert, M., Kloos, M., Koglin, J. E., Reinstein, J., Roome, C. M., Schlesinger, R., Seaberg, M., Shoeman, R. L., Stricker, M., Boutet, S., Haacke, S., Heberle, J., Heyne, K., Domratcheva, T., Barends, T. R. M., and Schlichting, I.(2019). Three-dimensional view of ultrafast dynamics in photoexcited bacteriorhodopsin. Nature Communications 10, Article Number 3177. doi: 10.1038/s41467-019-10758

Stensitzki, T., Adam, S., Schlesinger, R., Schapiro, I., and Heyne, K. (2020). Ultrafast backbone protonation in Channelrhodopsin-1 captured by polarization resolved fs vis-pump-IR-probe spectroscopy and computational methods. Molecules 25, pii: E848; doi: 10.3390/molecules25040848

Stensitzki, T., Yang, Y., Wölke, A.L., Knapp, E.-W., Hughes, J., Mroginski, M. A., and Heyne, K. (2017). Influence of Heterogeneity on the Ultrafast Photoisomerization Dynamics of Pfr in Cph1 Phytochrome. Photochemistry and Photobiology 93, 703-712; doi: 10.1111/php.12743

2013 - 2016

Linke, M., Yang, Y., Zienicke, B., Hammam, M.A.S., von Haimberger, T., Zacarias, A., Inomata, K., Lamparter, T., and Heyne, K. (2013). Electronic transitions and heterogeneity of the bacteriophytochrome Pr absorption band: An angle balanced polarization resolved femtosecond VIS pump-IR probe study. Biophysical Journal 105, 1756-1766.

Stensitzki, T., Muders, V., Schlesinger, R., Heberle, J., and Heyne, K. (2015). The primary photoreaction of channelrhodopsin-1: Wavelength dependent photoreactions induced by ground-state heterogeneity. Frontiers in Molecular Biosciences 2, 41.

Stensitzki, T., Yang, Y., Berg, A., Mahammed, A., Gross, Z., and Heyne, K. (2016). Ultrafast electronic and vibrational dynamics in brominated aluminum corroles: Energy relaxation and triplet formation. Structural Dynamics 3, 043210.

Stensitzki, T., Yang, Y., Muders, V., Schlesinger, R., Heberle, J., and Heyne, K. (2016). Femtosecond infrared spectroscopy of channelrhodopsin-1 chromophore isomerization. Structural Dynamics 3, 043208.

Velazquez Escobar, F., von Stetten, D., Günther-Lütkens, M., Keidel, A., Michael, N., Lamparter, T., Essen, L.-O., Hughes, J., Gärtner, W., Yang, Y., Heyne, K., Mroginski, M.A., and Hildebrandt, P. (2015). Conformational heterogeneity of the Pfr chromophore in plant and cyanobacterial phytochromes. Frontiers in Molecular Biosciences 2, 37.

Yang, Y., Heyne, K., Mathies, R.A., and Dasgupta, J. (2016). Non-Bonded Interactions Drive the Sub-Picosecond Bilin Photoisomerization in the Pfr State of Phytochrome Cph1. ChemPhysChem 17, 369-374.

Yang, Y., Linke, M., von Haimberger, T., Matute, R., González, L., Schmieder, P., and Heyne, K. (2014). Active and silent chromophore isoforms for phytochrome Pr photoisomerization: An alternative evolutionary strategy to optimize photoreaction quantum yields. Structural Dynamics 1, 014701.