% IMPORTANT: The following is UTF-8 encoded. This means that in the presence % of non-ASCII characters, it will not work with BibTeX 0.99 or older. % Instead, you should use an up-to-date BibTeX implementation like “bibtex8” or % “biber”. @ARTICLE{Dai:425975, author = {Dai, Shaobo and Funk, Lisa-Marie and von Pappenheim, Fabian Rabe and Sautner, Viktor and Paulikat, Mirko and Schröder, Benjamin and Uranga, Jon and Mata, Ricardo A. and Tittmann, Kai}, title = {{L}ow-barrier hydrogen bonds in enzyme cooperativity}, journal = {Nature / Physical science}, volume = {573}, number = {7775}, issn = {1476-4687}, address = {London}, publisher = {Macmillan28177}, reportid = {PUBDB-2019-03518}, pages = {609 - 613}, year = {2019}, note = {© Springer Nature Limited; Post referee fulltext in progress; Embargo 12 months from publication}, abstract = {The underlying molecular mechanisms of cooperativity and allosteric regulation are well understood for many proteins, with haemoglobin and aspartate transcarbamoylase serving as prototypical examples1,2. The binding of effectors typically causes a structural transition of the protein that is propagated through signalling pathways to remote sites and involves marked changes on the tertiary and sometimes even the quaternary level1,2,3,4,5. However, the origin of these signals and the molecular mechanism of long-range signalling at an atomic level remain unclear5,6,7,8. The different spatial scales and timescales in signalling pathways render experimental observation challenging; in particular, the positions and movement of mobile protons cannot be visualized by current methods of structural analysis. Here we report the experimental observation of fluctuating low-barrier hydrogen bonds as switching elements in cooperativity pathways of multimeric enzymes. We have observed these low-barrier hydrogen bonds in ultra-high-resolution X-ray crystallographic structures of two multimeric enzymes, and have validated their assignment using computational calculations. Catalytic events at the active sites switch between low-barrier hydrogen bonds and ordinary hydrogen bonds in a circuit that consists of acidic side chains and water molecules, transmitting a signal through the collective repositioning of protons by behaving as an atomistic Newton’s cradle. The resulting communication synchronizes catalysis in the oligomer. Our studies provide several lines of evidence and a working model for not only the existence of low-barrier hydrogen bonds in proteins, but also a connection to enzyme cooperativity. This finding suggests new principles of drug and enzyme design, in which sequences of residues can be purposefully included to enable long-range communication and thus the regulation of engineered biomolecules.}, cin = {EMBL-User}, ddc = {530}, cid = {I:(DE-H253)EMBL-User-20120814}, pnm = {6G3 - PETRA III (POF3-622)}, pid = {G:(DE-HGF)POF3-6G3}, experiment = {EXP:(DE-H253)P-P13-20150101 / EXP:(DE-H253)P-P14-20150101}, typ = {PUB:(DE-HGF)16}, pubmed = {pmid:31534226}, UT = {WOS:000488247600064}, doi = {10.1038/s41586-019-1581-9}, url = {https://bib-pubdb1.desy.de/record/425975}, }