Role of Missing Carotenoid in Reducing the Fluorescence of Single Monomeric Photosystem II Core Complexes
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1 Electronic Supplementry Mteril (ESI for Physicl Chemistry Chemicl Physics. This journl is the Owner Societies 017 Supporting Informtion Role of Missing Crotenoid in Reducing the Fluorescence of Single Monomeric Photosystem II Core Complexes Sepideh Sndry, Frn Müh, Imrn Ashrf, Mohmed Ibrhim, Michel Metzger, Athin Zouni, Alfred J. Meixner, nd Mrc Brecht,, IPTC nd LISA + Center, University of Tübingen, Tübingen, Germny, Institute of Theoreticl Physics, Johnnes Kepler University Linz, Linz, Austri, Institute of Biology, Humboldt University of Berlin, Berlin, Germny, nd Reutlingen University, Process Anlysis nd Technology, Reutlingen, Germny * E-mil: mrc.brecht@reutlingen-university.de * Phone: Fx:
2 S1 This lgorithm is used to determine the wvelength position of the most intense fluorescence emission nd its full width t hlf-mximum (fwhm. In ech dt set, constnt offset due to the CCD cmer is subtrcted, nd the wvelength position of the most intense contribution is determined. Strting from the mximum position, the width is determined where the intensity reches hlf of the mximum vlue. The results re shown s D scttering plot in Figure b in the min text. S Figure 5: Moleculr surfce of mpsiicc (PDB KZI. The view is on the dimeriztion surfce [1], which is in contct with the second monomer in dpsiicc nd thus prt of the monomer-monomer interfce. The β-cr pigments (yellow locted t this interfce re surfce-exposed in mpsiicc (i.e., exposed to the detergent phse nd despite being locted in binding niches my detch from the complex. Figure mde with VMD [].
3 S Figure 6: ( Energy level digrm illustrting the inetic model. 1 : excittion rte; 1 : fluorescence rte; : intersystem crossing rte; 1 = 1/: inverse triplet lifetime. (b Stedy-stte popultion of the singlet stte S 1 of the emitter ( 1 s function of the triplet lifetime for two different vlues of the rtio = 1 / 1 = 1 ( := / 1 = 1.8, 1/ 1 = 18 ns. Both rtes re in the sme order of mgnitude (i.e., is close to 1. The green rrow indictes the chnge in 1, when is doubled from 500 to 1000 ns while eeping 1 constnt (i.e., hs to be doubled s well. (c Sme s in Figure 6b, but with significntly lower excittion rte (i.e., significntly smller for the sme triplet lifetimes.
4 Kinetic model To find the popultions of the three sttes S 0 (singlet ground stte, S 1 (first singlet excited stte of the emitter nd T 1 (lowest triplet stte of the emitter, we hve to solve the set of differentil equtions relted to the inetic scheme depicted in Figure 6. With the bbrevitions S ; u S ; u T u ; we hve to solve A u& Au ( 1 1 with Determintion of the roots from the condition A I 0 yields 1 = 0 nd with 1, p 1 q 1 1 p p 4q u u u u With the resonble ssumption 1 > 1, it follows tht p 4q > 0, so tht ll roots re rel nd we hve: ui( t ie 1 t ( i 1,, Insertion of (6 into the system of differentil equtions yields for ech 1 ( ( We ssume tht the system is in the S 0 stte t t = 0. Then u 1 (0 = 1, u (0 = u (0 = 0, nd it follows from (6 tht Inserting (7 into (8 nd ting into ccount tht 1 = 0, yields three equtions for the three quntities ( = 1,,, from which it follows tht 1 (1 ( ( (4 (5 (6 (7 (8 4
5 1 1 1 q In the following, we use units of ns 1 for the rtes nd ssume := / 1 = 1.8 (corresponding to triplet yield of 64% for Chl in ether solution nd neglecting internl conversion [] s well s 1/ 1 = 18 ns [4]. Furthermore, we introduce the rtio := 1 / 1 nd the triplet lifetime = 1/ 1. We then hve: 1 1 p q ( q Of prticulr interest is the stedy-stte popultion (i.e., for t of S 1, which is given by 1 1 ( q We note tht similr model ws used by Avrm [5] tht lso includes the excited triplet stte T. The present three-stte model does not consider triplet-triplet bsorption, but cn be solved exctly. (9 (10 (11 References [1] M. Broser, A. Gbdulhov, J. Kern, A. Gusov, F. Müh, W. Senger, A. Zouni, Crystl Structure of Monomeric Photosystem II from Thermosynechococcus elongtus t.6 Å Resolution, J. Biol. Chem., 010, 85, [] W. Humphrey, A. Dle, K. Schulten, VMD: Visul Moleculr Dynmics. J. Mol. Grphics 1996, 14, -8. [] P. G. Bowers, G. Porter, Quntum Yields of Triplet Formtion in Solutions of Chlorophyll, Proc. Roy. Soc. Lond. A, 1967, 96, [4] T. Renger, M.E. Mdjet, F. Müh, I. Trostmnn, F.-J. Schmitt, C. Theiss, H. Pulsen, H.J. Eichler, A. Knorr, G. Renger, Thermlly Activted Superrdince nd Intersystem Crossing in the Wter- Soluble Chlorophyll Binding Protein, J. Phys. Chem. B, 009, 11, [5] R. Avrm, Fluorescence Detection of Triplet Stte Kinetics of Chlorophyll, Chem. Phys. Lett., 1977,
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