Variational design principles for nonequilibrium colloidal assembly
Abstract
Using large deviation theory and principles of stochastic optimal control, we show that rare molecular dynamics trajectories conditioned on assembling a specific target structure encode a set of interactions and external forces that lead to enhanced stability of that structure. Such a relationship can be formulated into a variational principle, for which we have developed an associated optimization algorithm and have used it to determine optimal forces for targeted self-assembly within nonequilibrium steady-states. We illustrate this perspective on inverse design in a model of colloidal cluster assembly within linear shear flow. We find that colloidal clusters can be assembled with high yield using specific short-range interactions of tunable complexity. Shear decreases the yields of rigid clusters, while small values of shear increase the yields of nonrigid clusters. The enhancement or suppression of the yield due to shear is rationalized with a generalized linear response theory. Furthermore, by studying 21 unique clusters made of six, seven, or eight particles, we uncover basic design principles for targeted assembly out of equilibrium.
- Authors:
-
- Univ. of California, Berkeley, CA (United States)
- Univ. of California, Berkeley, CA (United States); Kavli Energy NanoScience Inst., Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1832544
- Alternate Identifier(s):
- OSTI ID: 1755961
- Grant/Contract Number:
- AC02-05CH11231; SC0019375
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 154; Journal Issue: 1; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Molecular dynamics; Calculus of variations; Optimization algorithms; Stochastic processes; Probability theory; Linear response; Control theory; Machine learning; Self assembly; Colloids
Citation Formats
Das, Avishek, and Limmer, David T. Variational design principles for nonequilibrium colloidal assembly. United States: N. p., 2021.
Web. doi:10.1063/5.0038652.
Das, Avishek, & Limmer, David T. Variational design principles for nonequilibrium colloidal assembly. United States. https://doi.org/10.1063/5.0038652
Das, Avishek, and Limmer, David T. Wed .
"Variational design principles for nonequilibrium colloidal assembly". United States. https://doi.org/10.1063/5.0038652. https://www.osti.gov/servlets/purl/1832544.
@article{osti_1832544,
title = {Variational design principles for nonequilibrium colloidal assembly},
author = {Das, Avishek and Limmer, David T.},
abstractNote = {Using large deviation theory and principles of stochastic optimal control, we show that rare molecular dynamics trajectories conditioned on assembling a specific target structure encode a set of interactions and external forces that lead to enhanced stability of that structure. Such a relationship can be formulated into a variational principle, for which we have developed an associated optimization algorithm and have used it to determine optimal forces for targeted self-assembly within nonequilibrium steady-states. We illustrate this perspective on inverse design in a model of colloidal cluster assembly within linear shear flow. We find that colloidal clusters can be assembled with high yield using specific short-range interactions of tunable complexity. Shear decreases the yields of rigid clusters, while small values of shear increase the yields of nonrigid clusters. The enhancement or suppression of the yield due to shear is rationalized with a generalized linear response theory. Furthermore, by studying 21 unique clusters made of six, seven, or eight particles, we uncover basic design principles for targeted assembly out of equilibrium.},
doi = {10.1063/5.0038652},
journal = {Journal of Chemical Physics},
number = 1,
volume = 154,
place = {United States},
year = {Wed Jan 06 00:00:00 EST 2021},
month = {Wed Jan 06 00:00:00 EST 2021}
}
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