Precision shooting: Sampling long transition pathways

Autor(en)

Michael Grünwald, Christoph Dellago, Phillip L. Geissler

Abstrakt

The kinetics of collective rearrangements in solution, such as protein folding and nanocrystal phase transitions, often involve free energy barriers that are both long and rough. Applying methods of transition path sampling to harvest simulated trajectories that exemplify such processes is typically made difficult by a very low acceptance rate for newly generated trajectories. We address this problem by introducing a new generation algorithm based on the linear short time behavior of small disturbances in phase space. Using this "precision shooting" technique, arbitrarily small disturbances can be propagated in time, and any desired acceptance ratio of shooting moves can be obtained. We demonstrate the method for a simple but computationally problematic isomerization process in a dense liquid of soft spheres. We also discuss its applicability to barrier-crossing events involving metastable intermediate states.

Organisation(en)

Computergestützte Physik und Physik der Weichen Materie

Externe Organisation(en)

University of California, Berkeley

Journal

Journal of Chemical Physics

Band

129

Anzahl der Seiten

8

ISSN

0021-9606

DOI

https://doi.org/10.1063/1.2978000

Publikationsdatum

2008

Peer-reviewed

Ja

ÖFOS 2012

103036 Theoretische Physik, 103009 Festkörperphysik, 104022 Theoretische Chemie, 103029 Statistische Physik

Link zum Portal

https://ucrisportal.univie.ac.at/de/publications/17223fc9-0563-4c4c-8684-63c73bdb9e8c