Bode, W.

Huber, R.

Scheer, Hugo

Schirmer, T.

Schneider, S.

English

Universität München: Elektronischen Publikationen

High-resolution crystal structure of C-Phycocyanin and polarized optical spectra of single crystals

Open Access LMU

Photosynthetic Light-Harvesting Systems Organization and Function Proceedings of an International Workshop October 12-16,1987 Freising, Fed Rep. of Germany Editors Hugo Scheer · Siegfried Schneider W DE G Walter de Gruyter · Berlin · New York 1988 CONTENTS L i s t of P a r t i c i p a n t s X I I I SECTION I . ORGANIZATION: BIOCHEMICAL METHODS I n t r o d u c t i o n : The Biochemistry of Light-Harvesting Complexes by R.J. Cogdell 1 Phycobilisome-Thylakoid I n t e r a c t i o n : The Nature of High Molecular Weight Polypeptides by E. Gantt C.A. L i p s c h u l t z and F.X. Cunningham Jr 11 On the S t r u c t u r e of Photosystem II-Phycobilisome Complexes of Cyanobacteria by E. Mörschel and G.-H. Schatz 21 Stru c t u r e of Cryptophyte Photosynthetic Membranes by W. Wehrmeyer 35 S t r u c t u r a l and Phylogenetic Relationships of Phycoerythrins from Cyanobacteria, Red Algae and Cryptophyceae by W. S i d l e r and H. Zuber 49 I s o l a t i o n and C h a r a c t e r i z a t i o n of the Components of the Phycobilisome from Mastigocladus laminosus and Cross-l i n k i n g Experiments by R. Rümbeli and H. Zuber 61 C-Phycocyanin from Mastigocladus laminosus: Chromophore Assignment i n Higher Aggregates by Cystein M o d i f i c a t i o n by R. Fischer, S. Siebzehnrlibl and H. Scheer 71 Photochromic Prope r t i e s of C-Phycocyanin by G. Schmidt, S. Siebzehnrübl, R. Fischer and H. Scheer 77 Concerning the Relat i o n s h i p of L i g h t Harvesting B i l i -p r o t e i n s t o Phycochromes i n Cyanobacteria by W. Kufer 89 Subunit S t r u c t u r e and Reassembly of the Light-Harvesting Complex from Rhodospiri Hum rubrum G9+ by R. Ghosh, ThT~Rosatzin ancTR. Baclofen 93 Primary S t r u c t u r e Analyses of B a c t e r i a l Antenna Polypeptides - C o r r e l a t i o n of Aromatic Amino Acids w i t h Spectral Properties - S t r u c t u r a l S i m i l a r i t i e s w i t h Reaction Center Polypeptides by R.A. Brunisholz and H. Zuber 103 VIII The S t r u c t u r e o f the "Core1* of the Purple B a c t e r i a l Photo-s y n t h e t i c Unit by D.J. Dawkins, L.A. Ferguson and R.J. Cogdell 115 A Comparison o f the Ba c t e r i o c h l o r o p h y l 1 C--Binding Proteins of Chlorobium and Chloroflexus by P.D. Gerola, P. Hpjrup and J.M. Olson 129 I n t e r a c t i o n s between B a c t e r i o c h l o r o p h y l 1 c Molecules i n Oligomers and i n Chlorosomes of Green Photosynthetic Bacteria by D.C. Brune, G.H. King and R.E. Blankenship 141 Ligh t - H a r v e s t i n g Complexes of Chlorophyll c-Containing Algae by A.W.D. Larkum and R.G. H i l l e r 153 I s o l a t i o n and C h a r a c t e r i z a t i o n of a Chloro p h y l l a/c-Hetero-xanthin/Diadinoxanthin Light-Harvesting Complex from P l e u r o c h l o r i s meiringensis (Xanthophyceae) by C. Wilhelm, C. Bliche I and B. Rousseau 167 The Antenna Components of Photosystem I I w i t h Emphasis on the Major Pigment-Protein, LHC l i b by G.F. Peter and P. Thornber 175 SECTION I I : ORGANIZATION: MOLECULAR GENETICS AND CRYSTALLOGRAPHY Molecular Biology of Antennas by G. Drews 187 High-Resolution C r y s t a l S t r u c t u r e of C-Phycocyanin and Polarized O p t i c a l Spectra of Single C r y s t a l s by T. Schirmer, W. Bode and R. Huber 195 C r y s t a l l i z a t i o n and Spectroscopic I n v e s t i g a t i o n of Purple B a c t e r i a l B800-850 and RC-B875 Complexes by W. Welte, Τ. Wacker and A. Becker 201 S t r u c t u r e of the Light-Harvesting Chlorophyll a/b-Protein Complex from Chloroplast Membranes by W. Kühlbrandt 211 PhycobiIi somes of Synchechococcus Sp. PCC 7002, Pseudanabaena Sp. PCC 7409, and Cyanopnora paracioxa: An "Analysis by" HoTecular Genetics by D.A. Bryant 217 Organization and Assembly of B a c t e r i a l Antenna Complexes by G. Drews 233 IX The Use of Mutants t o Inv e s t i g a t e the Organization of the Photosynthetic Apparatus of Rhodobacter sphaeroides by C.N. Hunter and R. van Grondel l e 77.77 247 Mechanisms of P l a s t i d and Nuclear Gene Expression During Thylakoid Membrane Biogenesis i n Higher Plants by P. Westhoff, Η. Grüne, Η. Schrubar, Α. Oswald, Μ. Streubel, U. Ljungberg and R.G. Herrmann 261 SECTION I I I : ORGANIZATION: SPECIAL SPECTROSCOPY TECHNIQUES AND MODELS Assigment o f Spectral Forms i n the Photosynthetic Antennas to Chemically Defined Chromophores by A. Scherz 277 Linear Dichroism and Or i e n t a t i o n of Pigments i n Phycobilisomes and t h e i r Subunits by L. Juszcak, N.E. Geacintov, B.A. Z i l i n s k a s and J. Breton 281 Low Temperature Spectroscopy of Cyanobacteria! Antenna Pigments by W. Köhler, J. F r i e d r i c h , R. Fischer and H. Scheer 293 Chromophore Conformations i n Phycocyanin and Allophycocyanin as Studied by Resonance Raman Spectroscopy by B. S z a l o n t a i , V. Csizmadia, Z. Gombos, K. Csatorday and M. Lutz 307 Coherent Anti-Stokes Raman Spectroscopy of Phycobi1isomes, Phycocyanin and Allophycocyanin from Mastigocladus laminosus by S. Schneider, F. Baumann, W. Steiner, R. Fischer, S. Siebzehnrlibl and H. Scheer 317 Op t i c a l Absorption and C i r c u l a r Dichroism of Bacteriochlorophyl1 Oligomers i n T r i t o n X-100 and i n the Light-Harvesting-Complex B850; A Comparative Study by V. Rozenbach-Belkin, P. Braun, P. Kovatch and A.Scherz 323 Absorption Detected Magnetic Resonance i n Zero Magnetic F i e l d on Antenna Complexes from Rps. acidophila 7050 - The Temperature Dependence of tfie CarotenoTiTTrTpTet State Prop e r t i e s by J. U l l r i c h , J.U. v. Schütz and H.C. Wolf 339 E f f e c t o f Li t h i u m Dodecyl S u l f a t e on Β 800-850 Antenna Complexes from Rhodopseudomonas acidophila: A Resonance Raman Study by B. Robert and H. Frank 349 χ B a c t e r i o c h l o r o p h y l 1 a/b i n Antenna Complexes of Purple Bacteria by Β. Robert, A. Vermeglio, R. Steiner, Η. Scheer and Μ. Lutz 355 B a c t e r i o c h l o r o p h y l l c Aggregates i n Carbon T e t r a c h l o r i d e as Models f o r Chlo r o p h y l l Organization i n Green Photo-s y n t h e t i c B acteria by J.M. Olson and J.P. Pedersen 365 O r i e n t a t i o n o f t he Pigments i n the Reaction Center and the Core Antenna o f Photosystem I I by J. Breton, J. Duranton and K. Satoh 375 Non-Linear Absorption Spectroscopy of Antenna Chlorophyll a in Higher Plants by D. Leupold, H. S t i e l and P. Hoffmann 387 SECTION IV: FUNCTION: ELECTRONIC EXCITATION AND ENERGY TRANSFER E x c i t a t i o n Energy Transfer i n Photosynthesis by R. van Grondelle and V. Sundström 403 Fluorescence Spectroscopy of Allophycocyanin Complexes from Synechococcus 6301 S t r a i n AN112 by P.Maxson, KTTauer and A.N. Glazer 439 Picosecond Energy Transfer K i n e t i c s i n Allophycocyanin Aggregates from Mastigocladus laminosus by E. Bittersmann, W. Reuter, W. Wehrmeyer and A.R. Holzwarth 451 Picosecond Time-Resolved Energy Transfer K i n e t i c s w i t h i n C-Phycocyanin and Allophycocyanin Aggregates by T. G i l l b r o , A. Sandström, V. Sundström, R. Fischer and H. Scheer 457 Energy Transfer i n "Native" and Chemically Modified C-Phyco-cyanin Trimers and the Constituent Subunits by S. Schneider, P. Gei s e l h a r t , F. Baumann, S. Siebzehnrübl, R. Fischer and Η. Scheer 469 E f f e c t of P r o t e i n Environment and Exc i t o n i c Coupling on the Excited-State Pro p e r t i e s of the Bilinchromophores i n C-Phycocyanin by S. Schneider, Ch. Scharnagl, M. Dürring, T. Schirmer and W. Bode 483 E x c i t a t i o n Energy M i g r a t i o n i n C-Phycocyanin Aggregates I s o l a t e d from Phormidium luridum: P r e d i c t i o n s from the Förster's I n d u c t i v e Resonance Theory by J. Grabowski and G.S. Björn 491 XI Energy Tra n s f e r Calculations f o r two C-Phycocyanins Based on Refined X-Ray Crystal S t r u c t u r e Coordinates of Chromophores by K. Sauer and H. Scheer 507 Energy Transfer i n Light-Harvesting Antenna o f Purple B a c t e r i a Studied by Picosecond Spectroscopy by V. Sundström, H. Bergström, Τ. G i l l b r o , R. van Grondelle, W. Westerhuis, R.A. Niederman and R.J. Cogdell 513 E x c i t a t i o n Energy Transfer i n the Light-Harvesting Antenna o f Photosynthetic Purple B a c t e r i a : The Role of the Long-Wave-Length Absorbing Pigment B896 by R. van Grondelle, H. Bergström, V. Sundström, R.J. van Dorssen, M. Vos and C.N. Hunter 519 The Function o f Chlorosomes i n Energy Transfer in Green Photo-s y n t h e t i c Bacteria by R.J. van Dorssen, M. Vos and J. Amesz 531 Energy Transfer i n Chloroflexus aurantiacus: E f f e c t s of Temperature and TSaerobic^onönHons by B.P. Wittmershaus, D.C. Brune and R.E. Blankenship 543 I n t e r p r e t a t i o n o f Optical Spectra of Bacteriochlorophyl 1 Antenna Complexes by R.M. P e a r l s t e i n 555 Time Resolution and K i n e t i c s o f "F680" a t Low Temperatures i n Spinach Chloroplasts by R. Knox and S. L i n 567 Picosecond Studies of Fluorescence and Absorbance Changes i n Photosystem I I P a r t i c l e s from Synechococcus Sp. by A.R. Holzwarth, G.H. Schatz and H. Brock 579 Analysis of E x c i t a t i o n Energy Transfer i n Thylakoid Membranes by the Time-Resolved Fluorescence Spectra by M. Mimuro 589 V. CONCLUDING REMARKS Future Problems on Antenna Systems and Summary Remarks by E. Gantt 601 Author Index 605 Subject Index 609 HIGH-RESOLUTION CRYSTAL STRUCTURE OF C-PHYCOCYANIN AND POLARIZED OPTICAL SPECTRA OF SINGLE CRYSTALS Τ.Schirmer*), W.Bode, R.Huber M a x - P l a n c k - I n s t i t u t für B i o c h e m i e , Am K l o p f e r s p i t z , D-8033 M a r t i n s r i e d , F.R.G. S e v e r a l b i l i p r o t e i n c r y s t a l s a r e composed o f o l i g o m e r i c a g g r e g a t e s w h i c h most p r o b a b l y c l o s e l y r e s e m b l e t h e t r i m e r i c and h e x a m e r i c d i s c s of n a t i v e p h y c o b i l i s o m e s ( 1 - 3 ) . T h e r e f o r e , X - r a y a n a l y s i s o f t h e s e c r y s t a l s y i e l d s n ot o n l y i n f o r m a t i o n about t h e monomeric s t r u c t u r e , but about t h e i n t e r a c t i o n of t h e monomers and r e l a t i v e geometry of t h e i r chromophores as w e l l . P a r t i c u l a r l y , t h e s t r u c t u r e o f C - p h y c o c y a n i n (C-PC) hexamers from Agmenellum quadruplicatum (2, 4) shows t h a t t h e r e i s a m u l t i t u d e o f p a t h s f o r i n t r a - h e x a m e r i c e n e r g y t r a n s f e r . Chromophore (X84 and ß84 o f t h e n e i g h b o u r i n g monomer (same t r i m e r ) have t h e most f a v o u r a b l e r e l a t i v e p o s i t i o n , whereas (X84 - 0C84 and ßl55 - ßl55 seem t o r e p r e s e n t t h e main p a t h s f o r i n t e r - t r i m e r i c e n e r g y t r a n s f e r . E n e r g y t r a n s f e r a c r o s s t h e i n t e r f a c e o f hexamers i n t h e p h y c o b i l i s o m e r o d s most p r o b a b l y p r o c e e d s from ß84 t o ß84. The c r y s t a l s t r u c t u r e o f C-PC from Mastigocladus laminosus has r e c e n t l y been r e f i n e d ( 4 ) . The h i g h r e s o l u t i o n (2.1 A) of t h i s s t r u c t u r e a l l o w e d an a c c u r a t e d e t e r m i n a t i o n of t h e geometry of a l l t h r e e chromophores. A l l chromophores a r e d e f i n e d i n t h e i r e n t i r e t y a n d e x h i b i t v e r y s i m i l a r g e o m e t r y i n t h e i r t e t r a p y r r o l e p a r t . The s t r u c t u r e o f a p h y c o c y a n o b i l i n chromophore r e s e m b l e s a c l e a v e d p o r p h y r i n w h i c h has been u n f o l d e d by a t w i s t o f r o u g h l y 180° a r o u n d t h e C5-C6 and C14-C15 bonds. A c c o r d i n g l y , t h e c o n f i g u r a t i o n / c o n f o r m a t i o n of *) p r e s e n t a d d r e s s : L a b o r a t o r y of M o l e c u l a r B i o l o g y , M.R.C., Cambridge CB2 2QH, U.K. Photosynthetic Light-Harvesting Systems © 1988 Walter de Gruyter & Co., Berlin · New York 196 F i g , Ι; a) S t e r e o s c o p i c v i e w o f chromophore ß84, t h e s i d e - c h a i n a s p a r t a t e ß87 and the COC-backbone ( p a r t of h e l i x E) . b) Same model, r o t a t e d by a p p r o x i m a t e l y 90 d e g r e e around v e r t i c a l d i r e c t i o n . 197 F i g . 2; a) S t e r e o s c o p i c v i e w of chromophore ßl55, t h e s i d e - c h a i n o f a s p a r t a t e ß3 9 and t h e COC-backbone (G-H loop and p a r t o f h e l i x A) . t h e chromophores i s Z - a n t i , Z-syn, Z - a n t i ( w i t h t h e e x c e p t i o n of t h e " c o n f i g u r a t i o n " of C14-C15 of chromophore ßl55, which i s almost midway between Ζ and E ) . A l l t h r e e chromophores show a common p r i n c i p l e o f i n t e r a c t i o n w i t h t h e p r o t e i n . They a r c h around a s p a r t a t e r e s i d u e s (0t87, β87, β39), the n i t r o g e n atoms of p y r r o l e s Β and C b e i n g w i t h i n hydrogen-bonding d i s t a n c e t o one o f t h e c a r b o x y l a t e oxygens ( F i g s . 1 and 2) . Most o f t h e p r o p i o n i c s i d e - c h a i n s o f t h e chromophores form s a l t - b r i d g e s w i t h a r g i n i n e and l y s i n e r e s i d u e s . I n v i e w of t h e l o c a l symmetry between t h e a - and ß-subunit ( 1 ) , the s i m i l a r i t y of t h e s t r u c t u r e s o f Ot84 and ß84 i s not s u r p r i s i n g , a l t h o u g h i t has t o be c o n s i d e r e d t h a t t h e y occupy q u i t e d i f f e r e n t p o s i t i o n s i n the t r i m e r i c a g g r e g a t e . cc84 i s s h i e l d e d by the n e i g h b o u r i n g monomer, whereas ß84 i s l o c a t e d a t t h e i n n e r s i d e of t h e c e n t r a l c h a n n e l . I t i s s t r i k i n g , 198 however, t h a t a l s o ßl55 e x h i b i t s a v e r y s i m i l a r geometry, d e s p i t e i t s d i s t i n c t p o s i t i o n i n t h e s u b u n i t a t t h e G-H loop. Moreover, t h e same c h r o m o p h o r e - a s p a r t a t e i n t e r a c t i o n i s observed, t h e i n t e r a c t i n g a s p a r t a t e ß39 b e i n g p r o v i d e d by h e l i x Β ( F i g . 2 ) . The t h r e e chromophores of C-PC d i f f e r i n t h e i r s p e c t r a l p r o p e r t i e s ( s e e e.g. r e f . 5 ) . To a s s i g n t h e d i f f e r e n t s p e c t r a to t h e i n d i v i d u a l chromophores, p o l a r i z e d o p t i c a l s p e c t r o s c o p y on s i n g l e c r y s t a l s t o g e t h e r w i t h t h e knowledge o f t h e chromophore p o s i t i o n s and o r i e n t a t i o n s p r o v i d e s a p o w e r f u l method. P o l a r i z e d a b s o r p t i o n and f l u o r e s c e n c e s p e c t r a o f s i n g l e C-PC c r y s t a l s from Mastigocladus laminosus have been r e c o r d e d ( 6 ) . The c r y s t a l s show d i c h r o i s m . The p o s i t i o n o f t h e a b s o r p t i o n maximum s h i f t s from 612 nm (E p a r a l l e l t o t h e o p t i c a l a x i s c) t o 62 6 nm (E p e r p e n d i c u l a r t o c) . The p o l a r i z e d a b s o r p t i o n s p e c t r a can be s i m u l a t e d w e l l o n l y - u s i n g t h e d e c o n v o l u t e d s o l u t i o n s p e c t r a o f t h e i n d i v i d u a l chromophores (5) and t h e o r i e n t a t i o n s o f t h e chromophores (4) - i f t h e s h o r t and long w a v e l e n g t h component s p e c t r a o f t h e ß-subunit (ß s and ß f , r e s p e c t i v e l y ) a r e a s s i g n e d t o chromophores ßl55 and ß84, r e s p e c t i v e l y . The p o l a r i z a t i o n component of t h e f l u o r e s c e n c e from s i n g l e c r y s t a l s i s about 2.9 t i m e s more i n t e n s e p e r p e n d i c u l a r t o the t h r e e - f o l d t r i m e r a x i s t h a n p a r a l l e l t o i t . From t h e known i n c l i n a t i o n o f t h e chromophores t o w a r d s t h e t r i m e r a x i s i n t e n s i t y r a t i o s o f 11.0, 1.6 and 0.25 would be e x p e c t e d , i f one of t h e chromophores <X84, ß84 and ßl55, r e s p e c t i v e l y , would f l u o r e s c e s o l e l y . F l u o r e s c e n s e o r i g i n a t i n g f r o m b o t h chromophores 0C84 and ß84, however, would y i e l d an i n t e n s i t y r a t i o o f 3.0, comparing f a v o u r a b l e w i t h t h e o b s e r v e d r a t i o . I t can be e x c l u d e d t h a t ßl55 c o n t r i b u t e s a s u b s t a n t i a l p a r t t o the o b s e r v e d f l u o r e s c e n s e . T h i s g i v e s f u r t h e r d i r e c t e v i d e n c e t h a t ßl55 i s the ß s~chromophore. I t can be deduced, t h e r e f o r e , t h a t t h e n e t energy flow i n t h e t r i m e r s (and hexamers) i s d i r e c t e d 199 from t h e p e r i p h e r a l ßl55 chromophores t o t h e 0C84 - ß84 p a i r . R e f e r e n c e s 1. S c h i r m e r , T., W. Bode, R. Huber, W. S i d l e r , H. Zuber. 1985. J . M o l . B i o l . ISA, 257. 2. S c h i r m e r , T., R. Huber, M. S c h n e i d e r , W. Bode, M. M i l l e r , M.L. H a c k e r t . 1986. J . M o l . B i o l . 188 r 651. 3. Rümbeli, R., Τ. Schirmer, W. Bode, W. S i d l e r , H. Zuber. 1985. J . M o l . B i o l . 1 M , 197. 4. S c h i r m e r , Τ., W. Bode, R. Huber. 1987. J . M o l . B i o l . 677. 5. Mimuro Μ., P. F u g l i s t a l l e r , R. Rümbeli, Η. Zuber. 1985. Biochim. Biophys. A c t a . 848. 155. 6. S c h i r m e r . T., M.G. V i n c e n t . 1987. Biochim. B i o p h y s . A c t a . 893. 379. 

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High-resolution crystal structure of C-Phycocyanin and polarized optical spectra of single crystals

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