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Directed ultrafast ...
Directed ultrafast conformational changes accompany electron transfer in a photolyase as resolved by serial crystallography.
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- Cellini, Andrea, 1991 (author)
- Gothenburg University,Göteborgs universitet,Institutionen för kemi och molekylärbiologi,Department of Chemistry and Molecular Biology,Univ Gothenburg, Dept Chem & Mol Biol, Gothenburg, Sweden.
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- Shankar, Madan Kumar (author)
- Uppsala universitet,Biokemi,Univ Gothenburg, Dept Chem & Mol Biol, Gothenburg, Sweden
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- Nimmrich, Amke (author)
- Univ Gothenburg, Dept Chem & Mol Biol, Gothenburg, Sweden
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- Hunt, Leigh Anna (author)
- Uppsala universitet,Fysikalisk kemi
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- Monrroy, Leonardo (author)
- Uppsala universitet,Biokemi
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- Mutisya, Jennifer (author)
- Uppsala universitet,Biokemi,Univ Gothenburg, Dept Chem & Mol Biol, Gothenburg, Sweden,Paul Scherrer Inst, Villigen, Switzerland.
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- Furrer, Antonia (author)
- Paul Scherrer Inst, Villigen, Switzerland.
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- Beale, Emma V (author)
- Paul Scherrer Inst, Villigen, Switzerland.
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- Carrillo, Melissa (author)
- Paul Scherrer Inst, Villigen, Switzerland.
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- Malla, Tek Narsingh (author)
- Univ Wisconsin Milwaukee, Phys Dept, Milwaukee, WI 53211 USA.
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- Maj, Piotr (author)
- Uppsala universitet,Institutionen för kemi - BMC,Univ Gothenburg, Dept Chem & Mol Biol, Gothenburg, Sweden
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- Vrhovac, Lidija, 1994- (author)
- Uppsala universitet,Biokemi,Univ Gothenburg, Dept Chem & Mol Biol, Gothenburg, Sweden
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- Dworkowski, Florian (author)
- Paul Scherrer Inst, Villigen, Switzerland.
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- Cirelli, Claudio (author)
- Paul Scherrer Inst, Villigen, Switzerland.
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- Maj, Michał (author)
- Uppsala universitet,Fysikalisk kemi
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- Ozerov, Dmitry (author)
- Paul Scherrer Inst, Villigen, Switzerland.
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- Stojković, Emina A (author)
- NE Illinois Univ, Dept Biol, Chicago, IL USA.
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- Hammarström, Leif, 1964- (author)
- Uppsala universitet,Fysikalisk kemi
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- Bacellar, Camila (author)
- Paul Scherrer Inst, Villigen, Switzerland.
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- Standfuss, Jörg (author)
- Paul Scherrer Inst, Villigen, Switzerland.
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Maj, Michał (author)
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- Schmidt, Marius (author)
- Univ Wisconsin Milwaukee, Phys Dept, Milwaukee, WI 53211 USA.
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- Weinert, Tobias (author)
- Paul Scherrer Inst, Villigen, Switzerland.
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- Ihalainen, Janne A (author)
- Univ Jyvaskyla, Nanosci Ctr, Dept Biol & Environm Sci, Jyvaskyla, Finland.
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- Wahlgren, Weixiao Yuan, 1970 (author)
- Gothenburg University,Göteborgs universitet,Institutionen för kemi och molekylärbiologi,Department of Chemistry and Molecular Biology,Univ Gothenburg, Dept Chem & Mol Biol, Gothenburg, Sweden.;Univ Gothenburg, Swedish NMR Ctr, Gothenburg, Sweden.;Univ Gothenburg, Swedish NMR Ctr, Gothenburg, Sweden.
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- Westenhoff, Sebastian, 1978 (author)
- Uppsala universitet,Gothenburg University,Göteborgs universitet,Institutionen för kemi och molekylärbiologi,Department of Chemistry and Molecular Biology,Biokemi,Univ Gothenburg, Dept Chem & Mol Biol, Gothenburg, Sweden
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(creator_code:org_t)
- Springer Nature, 2024
- 2024
- English.
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In: Nature chemistry. - : Springer Nature. - 1755-4349 .- 1755-4330.
- Related links:
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https://doi.org/10.1...
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https://uu.diva-port... (primary) (Raw object)
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https://gup.ub.gu.se...
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https://doi.org/10.1...
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Abstract
Subject headings
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- Charge-transfer reactions in proteins are important for life, such as in photolyases which repair DNA, but the role of structural dynamics remains unclear. Here, using femtosecond X-ray crystallography, we report the structural changes that take place while electrons transfer along a chain of four conserved tryptophans in the Drosophila melanogaster (6-4) photolyase. At femto- and picosecond delays, photoreduction of the flavin by the first tryptophan causes directed structural responses at a key asparagine, at a conserved salt bridge, and by rearrangements of nearby water molecules. We detect charge-induced structural changes close to the second tryptophan from 1 ps to 20 ps, identifying a nearby methionine as an active participant in the redox chain, and from 20 ps around the fourth tryptophan. The photolyase undergoes highly directed and carefully timed adaptations of its structure. This questions the validity of the linear solvent response approximation in Marcus theory and indicates that evolution has optimized fast protein fluctuations for optimal charge transfer.
Subject headings
- NATURVETENSKAP -- Biologi -- Biokemi och molekylärbiologi (hsv//swe)
- NATURAL SCIENCES -- Biological Sciences -- Biochemistry and Molecular Biology (hsv//eng)
- NATURVETENSKAP -- Biologi -- Strukturbiologi (hsv//swe)
- NATURAL SCIENCES -- Biological Sciences -- Structural Biology (hsv//eng)
- NATURVETENSKAP -- Kemi -- Teoretisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Theoretical Chemistry (hsv//eng)
Publication and Content Type
- ref (subject category)
- art (subject category)
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- By the author/editor
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Cellini, Andrea, ...
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Shankar, Madan K ...
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Nimmrich, Amke
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Hunt, Leigh Anna
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Monrroy, Leonard ...
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Mutisya, Jennife ...
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show more...
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Furrer, Antonia
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Beale, Emma V
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Carrillo, Meliss ...
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Malla, Tek Narsi ...
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Maj, Piotr
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Vrhovac, Lidija, ...
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Dworkowski, Flor ...
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Cirelli, Claudio
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Maj, Michał
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Ozerov, Dmitry
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Stojković, Emina ...
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Hammarström, Lei ...
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Bacellar, Camila
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Standfuss, Jörg
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Schmidt, Marius
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Weinert, Tobias
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Ihalainen, Janne ...
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Wahlgren, Weixia ...
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Westenhoff, Seba ...
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- About the subject
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- NATURAL SCIENCES
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NATURAL SCIENCES
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and Biological Scien ...
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and Biochemistry and ...
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- NATURAL SCIENCES
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NATURAL SCIENCES
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and Biological Scien ...
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and Structural Biolo ...
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- NATURAL SCIENCES
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NATURAL SCIENCES
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and Chemical Science ...
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and Theoretical Chem ...
- Articles in the publication
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Nature chemistry
- By the university
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University of Gothenburg
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Uppsala University