[{"project":[{"grant_number":"P29902","_id":"26031614-B435-11E9-9278-68D0E5697425","call_identifier":"FWF","name":"Quantum rotations in the presence of a many-body environment"},{"_id":"25681D80-B435-11E9-9278-68D0E5697425","grant_number":"291734","call_identifier":"FP7","name":"International IST Postdoc Fellowship Programme"}],"title":"Variational approaches to quantum impurities: from the Fröhlich polaron to the angulon","file":[{"access_level":"open_access","creator":"dernst","file_size":1309966,"file_id":"5896","content_type":"application/pdf","file_name":"2019_MolecularPhysics_Li.pdf","date_created":"2019-01-29T08:32:57Z","checksum":"178964744b636a6f036372f4f090a657","relation":"main_file","date_updated":"2020-07-14T12:47:13Z"}],"department":[{"_id":"MiLe"}],"publication_status":"published","doi":"10.1080/00268976.2019.1567852","type":"journal_article","publisher":"Taylor & Francis","license":"https://creativecommons.org/licenses/by/4.0/","_id":"5886","related_material":{"record":[{"id":"8958","relation":"dissertation_contains","status":"public"}]},"date_created":"2019-01-27T22:59:10Z","article_processing_charge":"No","date_published":"2019-01-18T00:00:00Z","tmp":{"name":"Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)","image":"/images/cc_by.png","legal_code_url":"https://creativecommons.org/licenses/by/4.0/legalcode","short":"CC BY (4.0)"},"external_id":{"isi":["000474641400008"]},"quality_controlled":"1","author":[{"id":"4B7E523C-F248-11E8-B48F-1D18A9856A87","first_name":"Xiang","last_name":"Li","full_name":"Li, Xiang"},{"last_name":"Bighin","first_name":"Giacomo","orcid":"0000-0001-8823-9777","id":"4CA96FD4-F248-11E8-B48F-1D18A9856A87","full_name":"Bighin, Giacomo"},{"id":"38CB71F6-F248-11E8-B48F-1D18A9856A87","orcid":"0000-0001-5973-0874","first_name":"Enderalp","last_name":"Yakaboylu","full_name":"Yakaboylu, Enderalp"},{"full_name":"Lemeshko, Mikhail","first_name":"Mikhail","orcid":"0000-0002-6990-7802","id":"37CB05FA-F248-11E8-B48F-1D18A9856A87","last_name":"Lemeshko"}],"citation":{"ista":"Li X, Bighin G, Yakaboylu E, Lemeshko M. 2019. Variational approaches to quantum impurities: from the Fröhlich polaron to the angulon. Molecular Physics.","apa":"Li, X., Bighin, G., Yakaboylu, E., &#38; Lemeshko, M. (2019). Variational approaches to quantum impurities: from the Fröhlich polaron to the angulon. <i>Molecular Physics</i>. Taylor &#38; Francis. <a href=\"https://doi.org/10.1080/00268976.2019.1567852\">https://doi.org/10.1080/00268976.2019.1567852</a>","ieee":"X. Li, G. Bighin, E. Yakaboylu, and M. Lemeshko, “Variational approaches to quantum impurities: from the Fröhlich polaron to the angulon,” <i>Molecular Physics</i>. Taylor &#38; Francis, 2019.","short":"X. Li, G. Bighin, E. Yakaboylu, M. Lemeshko, Molecular Physics (2019).","ama":"Li X, Bighin G, Yakaboylu E, Lemeshko M. Variational approaches to quantum impurities: from the Fröhlich polaron to the angulon. <i>Molecular Physics</i>. 2019. doi:<a href=\"https://doi.org/10.1080/00268976.2019.1567852\">10.1080/00268976.2019.1567852</a>","mla":"Li, Xiang, et al. “Variational Approaches to Quantum Impurities: From the Fröhlich Polaron to the Angulon.” <i>Molecular Physics</i>, Taylor &#38; Francis, 2019, doi:<a href=\"https://doi.org/10.1080/00268976.2019.1567852\">10.1080/00268976.2019.1567852</a>.","chicago":"Li, Xiang, Giacomo Bighin, Enderalp Yakaboylu, and Mikhail Lemeshko. “Variational Approaches to Quantum Impurities: From the Fröhlich Polaron to the Angulon.” <i>Molecular Physics</i>. Taylor &#38; Francis, 2019. <a href=\"https://doi.org/10.1080/00268976.2019.1567852\">https://doi.org/10.1080/00268976.2019.1567852</a>."},"ec_funded":1,"ddc":["530"],"scopus_import":"1","publication_identifier":{"issn":["0026-8976"]},"status":"public","has_accepted_license":"1","oa_version":"Published Version","oa":1,"month":"01","file_date_updated":"2020-07-14T12:47:13Z","day":"18","user_id":"2DF688A6-F248-11E8-B48F-1D18A9856A87","language":[{"iso":"eng"}],"publication":"Molecular Physics","date_updated":"2026-07-07T05:31:10Z","das_tickbox":"1","year":"2019","isi":1,"abstract":[{"text":"Problems involving quantum impurities, in which one or a few particles are interacting with a macroscopic environment, represent a pervasive paradigm, spanning across atomic, molecular, and condensed-matter physics. In this paper we introduce new variational approaches to quantum impurities and apply them to the Fröhlich polaron–a quasiparticle formed out of an electron (or other point-like impurity) in a polar medium, and to the angulon–a quasiparticle formed out of a rotating molecule in a bosonic bath. We benchmark these approaches against established theories, evaluating their accuracy as a function of the impurity-bath coupling.","lang":"eng"}]},{"title":"Reaction rate theory for supramolecular kinetics: application to protein aggregation","issue":"21-22","publication_status":"published","publisher":"Taylor & Francis","type":"journal_article","doi":"10.1080/00268976.2018.1474280","acknowledgement":"We thank Claudia Flandoli for the help with illustrations.","_id":"10358","article_processing_charge":"No","date_created":"2021-11-26T12:08:02Z","keyword":["physical chemistry"],"page":"3055-3065","quality_controlled":"1","external_id":{"arxiv":["1803.04851"]},"date_published":"2018-05-24T00:00:00Z","author":[{"last_name":"Michaels","first_name":"Thomas C. T.","full_name":"Michaels, Thomas C. T."},{"full_name":"Liu, Lucie X.","first_name":"Lucie X.","last_name":"Liu"},{"full_name":"Curk, Samo","last_name":"Curk","first_name":"Samo"},{"last_name":"Bolhuis","first_name":"Peter G.","full_name":"Bolhuis, Peter G."},{"last_name":"Šarić","orcid":"0000-0002-7854-2139","id":"bf63d406-f056-11eb-b41d-f263a6566d8b","first_name":"Anđela","full_name":"Šarić, Anđela"},{"last_name":"Knowles","first_name":"Tuomas P. J.","full_name":"Knowles, Tuomas P. J."}],"intvolume":"       116","volume":116,"citation":{"ista":"Michaels TCT, Liu LX, Curk S, Bolhuis PG, Šarić A, Knowles TPJ. 2018. Reaction rate theory for supramolecular kinetics: application to protein aggregation. Molecular Physics. 116(21–22), 3055–3065.","short":"T.C.T. Michaels, L.X. Liu, S. Curk, P.G. Bolhuis, A. Šarić, T.P.J. Knowles, Molecular Physics 116 (2018) 3055–3065.","ieee":"T. C. T. Michaels, L. X. Liu, S. Curk, P. G. Bolhuis, A. Šarić, and T. P. J. Knowles, “Reaction rate theory for supramolecular kinetics: application to protein aggregation,” <i>Molecular Physics</i>, vol. 116, no. 21–22. Taylor &#38; Francis, pp. 3055–3065, 2018.","apa":"Michaels, T. C. T., Liu, L. X., Curk, S., Bolhuis, P. G., Šarić, A., &#38; Knowles, T. P. J. (2018). Reaction rate theory for supramolecular kinetics: application to protein aggregation. <i>Molecular Physics</i>. Taylor &#38; Francis. <a href=\"https://doi.org/10.1080/00268976.2018.1474280\">https://doi.org/10.1080/00268976.2018.1474280</a>","mla":"Michaels, Thomas C. T., et al. “Reaction Rate Theory for Supramolecular Kinetics: Application to Protein Aggregation.” <i>Molecular Physics</i>, vol. 116, no. 21–22, Taylor &#38; Francis, 2018, pp. 3055–65, doi:<a href=\"https://doi.org/10.1080/00268976.2018.1474280\">10.1080/00268976.2018.1474280</a>.","ama":"Michaels TCT, Liu LX, Curk S, Bolhuis PG, Šarić A, Knowles TPJ. Reaction rate theory for supramolecular kinetics: application to protein aggregation. <i>Molecular Physics</i>. 2018;116(21-22):3055-3065. doi:<a href=\"https://doi.org/10.1080/00268976.2018.1474280\">10.1080/00268976.2018.1474280</a>","chicago":"Michaels, Thomas C. T., Lucie X. Liu, Samo Curk, Peter G. Bolhuis, Anđela Šarić, and Tuomas P. J. Knowles. “Reaction Rate Theory for Supramolecular Kinetics: Application to Protein Aggregation.” <i>Molecular Physics</i>. Taylor &#38; Francis, 2018. <a href=\"https://doi.org/10.1080/00268976.2018.1474280\">https://doi.org/10.1080/00268976.2018.1474280</a>."},"status":"public","publication_identifier":{"eissn":["1362-3028"],"issn":["0026-8976"]},"scopus_import":"1","arxiv":1,"main_file_link":[{"url":"https://arxiv.org/abs/1803.04851","open_access":"1"}],"oa_version":"Preprint","oa":1,"month":"05","extern":"1","language":[{"iso":"eng"}],"article_type":"original","user_id":"8b945eb4-e2f2-11eb-945a-df72226e66a9","day":"24","date_updated":"2021-11-26T12:39:58Z","publication":"Molecular Physics","abstract":[{"text":"Probing reaction mechanisms of supramolecular processes in soft and biological matter, such as protein aggregation, is inherently challenging. This is because these processes involve multiple molecular mechanisms that are associated with the rearrangement of large numbers of weak bonds, resulting in complex free energy landscapes with many kinetic barriers. Reaction rate measurements at different temperatures can offer unprecedented insights into the underlying molecular mechanisms. However, to be able to interpret such measurements, a key challenge is to establish which properties of the complex free energy landscapes are probed by the reaction rate. Here, we present a reaction rate theory for supramolecular kinetics based on Kramers theory of diffusive reactions over multiple kinetic barriers. We find that reaction rates for protein aggregation are of the Arrhenius–Eyring type and that the associated activation energies probe only one relevant barrier along the respective free energy landscapes. We apply this advancement to interpret, in experiments and in coarse-grained computer simulations, reaction rates of amyloid aggregation in terms of molecular mechanisms and associated thermodynamic signatures. These results suggest a practical extension of the concept of rate-determining steps for complex supramolecular processes and establish a general platform for probing the underlying energy landscape using kinetic measurements.","lang":"eng"}],"year":"2018"}]