---
_id: '10358'
abstract:
- lang: eng
  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.
acknowledgement: We thank Claudia Flandoli for the help with illustrations.
article_processing_charge: No
article_type: original
arxiv: 1
author:
- first_name: Thomas C. T.
  full_name: Michaels, Thomas C. T.
  last_name: Michaels
- first_name: Lucie X.
  full_name: Liu, Lucie X.
  last_name: Liu
- first_name: Samo
  full_name: Curk, Samo
  last_name: Curk
- first_name: Peter G.
  full_name: Bolhuis, Peter G.
  last_name: Bolhuis
- first_name: Anđela
  full_name: Šarić, Anđela
  id: bf63d406-f056-11eb-b41d-f263a6566d8b
  last_name: Šarić
  orcid: 0000-0002-7854-2139
- first_name: Tuomas P. J.
  full_name: Knowles, Tuomas P. J.
  last_name: Knowles
citation:
  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>'
  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>'
  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>.'
  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.'
  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.'
  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>.'
  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.
date_created: 2021-11-26T12:08:02Z
date_published: 2018-05-24T00:00:00Z
date_updated: 2021-11-26T12:39:58Z
day: '24'
doi: 10.1080/00268976.2018.1474280
extern: '1'
external_id:
  arxiv:
  - '1803.04851'
intvolume: '       116'
issue: 21-22
keyword:
- physical chemistry
language:
- iso: eng
main_file_link:
- open_access: '1'
  url: https://arxiv.org/abs/1803.04851
month: '05'
oa: 1
oa_version: Preprint
page: 3055-3065
publication: Molecular Physics
publication_identifier:
  eissn:
  - 1362-3028
  issn:
  - 0026-8976
publication_status: published
publisher: Taylor & Francis
quality_controlled: '1'
scopus_import: '1'
status: public
title: 'Reaction rate theory for supramolecular kinetics: application to protein aggregation'
type: journal_article
user_id: 8b945eb4-e2f2-11eb-945a-df72226e66a9
volume: 116
year: '2018'
...