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Title: The role of pressure in inverse design for assembly

Abstract

Isotropic pairwise interactions that promote the self-assembly of complex particle morphologies have been discovered by inverse design strategies derived from the molecular coarse-graining literature. While such approaches provide an avenue to reproduce structural correlations, thermodynamic quantities such as the pressure have typically not been considered in self-assembly applications. In this work, we demonstrate that relative entropy optimization can be used to discover potentials that self-assemble into targeted cluster morphologies with a prescribed pressure when the iterative simulations are performed in the isothermal-isobaric ensemble. The benefits of this approach are twofold. First, the structure and the thermodynamics associated with the optimized interaction can be controlled simultaneously. Second, by varying the pressure in the optimization, a family of interparticle potentials that all self-assemble the same structure can be systematically discovered, allowing for a deeper understanding of self-assembly of a given target structure and providing multiple assembly routes for its realization. Selecting an appropriate simulation ensemble to control the thermodynamic properties of interest is a general design strategy that could also be used to discover interaction potentials that self-assemble structures having, for example, a specified chemical potential.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3]; ORCiD logo [4]
  1. Univ. of Texas, Austin, TX (United States). Dept. of Chemical Engineering; Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Theoretical Division
  2. Univ. of Texas, Austin, TX (United States). Dept. of Chemical Engineering; Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Theoretical Division, and Center for Nonlinear Studies
  3. Univ. of Texas, Austin, TX (United States). Dept. of Chemical Engineering
  4. Univ. of Texas, Austin, TX (United States). Dept. of Chemical Engineering, and Dept. of Physics
Publication Date:
Research Org.:
Los Alamos National Laboratory (LANL), Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1566116
Report Number(s):
LA-UR-19-25001
Journal ID: ISSN 0021-9606; TRN: US2000974
Grant/Contract Number:  
89233218CNA000001
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 151; Journal Issue: 10; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS

Citation Formats

Lindquist, Beth A., Jadrich, Ryan B., Howard, Michael P., and Truskett, Thomas M. The role of pressure in inverse design for assembly. United States: N. p., 2019. Web. doi:10.1063/1.5112766.
Lindquist, Beth A., Jadrich, Ryan B., Howard, Michael P., & Truskett, Thomas M. The role of pressure in inverse design for assembly. United States. doi:10.1063/1.5112766.
Lindquist, Beth A., Jadrich, Ryan B., Howard, Michael P., and Truskett, Thomas M. Sat . "The role of pressure in inverse design for assembly". United States. doi:10.1063/1.5112766. https://www.osti.gov/servlets/purl/1566116.
@article{osti_1566116,
title = {The role of pressure in inverse design for assembly},
author = {Lindquist, Beth A. and Jadrich, Ryan B. and Howard, Michael P. and Truskett, Thomas M.},
abstractNote = {Isotropic pairwise interactions that promote the self-assembly of complex particle morphologies have been discovered by inverse design strategies derived from the molecular coarse-graining literature. While such approaches provide an avenue to reproduce structural correlations, thermodynamic quantities such as the pressure have typically not been considered in self-assembly applications. In this work, we demonstrate that relative entropy optimization can be used to discover potentials that self-assemble into targeted cluster morphologies with a prescribed pressure when the iterative simulations are performed in the isothermal-isobaric ensemble. The benefits of this approach are twofold. First, the structure and the thermodynamics associated with the optimized interaction can be controlled simultaneously. Second, by varying the pressure in the optimization, a family of interparticle potentials that all self-assemble the same structure can be systematically discovered, allowing for a deeper understanding of self-assembly of a given target structure and providing multiple assembly routes for its realization. Selecting an appropriate simulation ensemble to control the thermodynamic properties of interest is a general design strategy that could also be used to discover interaction potentials that self-assemble structures having, for example, a specified chemical potential.},
doi = {10.1063/1.5112766},
journal = {Journal of Chemical Physics},
number = 10,
volume = 151,
place = {United States},
year = {2019},
month = {9}
}

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Cited by: 3 works
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Figures / Tables:

FIG. 1 FIG. 1: (a) The dimensionless isotropic pairwise interaction, $βu(r)$, discovered via inverse design using IBI in Ref. 7. This interaction drives self assembly of particles into various microphase-separated states as a function of number density ($ρ$) in the canonical ensemble. (b,c) The corresponding radial distribution function and cluster size distribution,more » respectively, at $ρσ$3 = 0.144. (d) A snapshot of clusters that assemble onto a lattice using the interaction shown in panel a at $ρσ$3 = 0.144. See Ref. 7 for further simulation details.« less

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Works referenced in this record:

Inverse Design of Self-Assembling Frank-Kasper Phases and Insights Into Emergent Quasicrystals
journal, January 2018

  • Lindquist, Beth A.; Jadrich, Ryan B.; Piñeros, William D.
  • The Journal of Physical Chemistry B, Vol. 122, Issue 21
  • DOI: 10.1021/acs.jpcb.7b11841

Bottom-up coarse-grained models that accurately describe the structure, pressure, and compressibility of molecular liquids
journal, December 2015

  • Dunn, Nicholas J. H.; Noid, W. G.
  • The Journal of Chemical Physics, Vol. 143, Issue 24
  • DOI: 10.1063/1.4937383

Recent Advances in the Theory and Simulation of Model Colloidal Microphase Formers
journal, August 2016

  • Zhuang, Yuan; Charbonneau, Patrick
  • The Journal of Physical Chemistry B, Vol. 120, Issue 32
  • DOI: 10.1021/acs.jpcb.6b05471

Optimizing Topographical Templates for Directed Self-Assembly of Block Copolymers via Inverse Design Simulations
journal, December 2013

  • Hannon, Adam F.; Ding, Yi; Bai, Wubin
  • Nano Letters, Vol. 14, Issue 1
  • DOI: 10.1021/nl404067s

Perspective: Evolutionary design of granular media and block copolymer patterns
journal, April 2016

  • Jaeger, Heinrich M.; de Pablo, Juan J.
  • APL Materials, Vol. 4, Issue 5
  • DOI: 10.1063/1.4948270

Exotic fluids and crystals of soft polymeric colloids
journal, August 2002

  • Likos, Christos N.; Hoffmann, Norman; L$ouml$wen, Hartmut
  • Journal of Physics: Condensed Matter, Vol. 14, Issue 33
  • DOI: 10.1088/0953-8984/14/33/309

Systematic study of temperature and density variations in effective potentials for coarse-grained models of molecular liquids
journal, January 2019

  • Lebold, Kathryn M.; Noid, W. G.
  • The Journal of Chemical Physics, Vol. 150, Issue 1
  • DOI: 10.1063/1.5050509

Exploiting classical nucleation theory for reverse self-assembly
journal, December 2010

  • Miller, William L.; Cacciuto, Angelo
  • The Journal of Chemical Physics, Vol. 133, Issue 23
  • DOI: 10.1063/1.3524307

Generalized phase behavior of cluster formation in colloidal dispersions with competing interactions
journal, January 2014

  • Godfrin, P. Douglas; Valadez-Pérez, Néstor E.; Castañeda-Priego, Ramon
  • Soft Matter, Vol. 10, Issue 28
  • DOI: 10.1039/c3sm53220h

Inverse optimization techniques for targeted self-assembly
journal, January 2009


Assembly of particle strings via isotropic potentials
journal, March 2019

  • Banerjee, D.; Lindquist, B. A.; Jadrich, R. B.
  • The Journal of Chemical Physics, Vol. 150, Issue 12
  • DOI: 10.1063/1.5088604

Inverse methods for material design
journal, May 2014

  • Jain, Avni; Bollinger, Jonathan A.; Truskett, Thomas M.
  • AIChE Journal, Vol. 60, Issue 8
  • DOI: 10.1002/aic.14491

Repulsive potentials, clumps and the metastable glass phase
journal, April 1994

  • Klein, W.; Gould, Harvey; Ramos, Raphael A.
  • Physica A: Statistical Mechanics and its Applications, Vol. 205, Issue 4
  • DOI: 10.1016/0378-4371(94)90233-x

GROMACS: Fast, flexible, and free
journal, January 2005

  • Van Der Spoel, David; Lindahl, Erik; Hess, Berk
  • Journal of Computational Chemistry, Vol. 26, Issue 16
  • DOI: 10.1002/jcc.20291

Observation of Small Cluster Formation in Concentrated Monoclonal Antibody Solutions and Its Implications to Solution Viscosity
journal, April 2014

  • Yearley, Eric J.; Godfrin, Paul D.; Perevozchikova, Tatiana
  • Biophysical Journal, Vol. 106, Issue 8
  • DOI: 10.1016/j.bpj.2014.02.036

Optimized monotonic convex pair potentials stabilize low-coordinated crystals
journal, January 2011

  • Marcotte, É.; Stillinger, F. H.; Torquato, S.
  • Soft Matter, Vol. 7, Issue 6
  • DOI: 10.1039/c0sm01205j

Fast Parallel Algorithms for Short-Range Molecular Dynamics
journal, March 1995


Nonlinear Machine Learning of Patchy Colloid Self-Assembly Pathways and Mechanisms
journal, April 2014

  • Long, Andrew W.; Ferguson, Andrew L.
  • The Journal of Physical Chemistry B, Vol. 118, Issue 15
  • DOI: 10.1021/jp500350b

Inverse Design of Bulk Morphologies in Multiblock Polymers Using Particle Swarm Optimization
journal, August 2017


Rational design of patchy colloids via landscape engineering
journal, January 2018

  • Long, Andrew W.; Ferguson, Andrew L.
  • Molecular Systems Design & Engineering, Vol. 3, Issue 1
  • DOI: 10.1039/c7me00077d

Equilibrium Cluster Phases and Low-Density Arrested Disordered States: The Role of Short-Range Attraction and Long-Range Repulsion
journal, July 2004


Why do ultrasoft repulsive particles cluster and crystallize? Analytical results from density-functional theory
journal, June 2007

  • Likos, Christos N.; Mladek, Bianca M.; Gottwald, Dieter
  • The Journal of Chemical Physics, Vol. 126, Issue 22
  • DOI: 10.1063/1.2738064

Reentrant and Isostructural Transitions in a Cluster-Crystal Former
journal, December 2010


Coarse-graining errors and numerical optimization using a relative entropy framework
journal, March 2011

  • Chaimovich, Aviel; Shell, M. Scott
  • The Journal of Chemical Physics, Vol. 134, Issue 9
  • DOI: 10.1063/1.3557038

Ground-State Clusters for Short-Range Attractive and Long-Range Repulsive Potentials
journal, November 2004

  • Mossa, S.; Sciortino, F.; Tartaglia, P.
  • Langmuir, Vol. 20, Issue 24
  • DOI: 10.1021/la048554t

Origin and detection of microstructural clustering in fluids with spatial-range competitive interactions
journal, April 2015

  • Jadrich, Ryan B.; Bollinger, Jonathan A.; Johnston, Keith P.
  • Physical Review E, Vol. 91, Issue 4
  • DOI: 10.1103/physreve.91.042312

Inverse Design of Colloidal Crystals via Optimized Patchy Interactions
journal, August 2018

  • Chen, D.; Zhang, G.; Torquato, S.
  • The Journal of Physical Chemistry B, Vol. 122, Issue 35
  • DOI: 10.1021/acs.jpcb.8b05627

Microphase separation versus the vapor-liquid transition in systems of spherical particles
journal, March 1999

  • Sear, Richard P.; Gelbart, William M.
  • The Journal of Chemical Physics, Vol. 110, Issue 9
  • DOI: 10.1063/1.478338

A Comparison of Barostats for the Mechanical Characterization of Metal–Organic Frameworks
journal, November 2015

  • Rogge, S. M. J.; Vanduyfhuys, L.; Ghysels, A.
  • Journal of Chemical Theory and Computation, Vol. 11, Issue 12
  • DOI: 10.1021/acs.jctc.5b00748

Macrocrystal Phases in Charged Colloidal Suspensions
journal, July 1988


Enhanced density fluctuations in fluid systems with competing interactions
journal, September 2000


Cluster formation in fluids with competing short-range and long-range interactions
journal, March 2014

  • Sweatman, Martin B.; Fartaria, Rui; Lue, Leo
  • The Journal of Chemical Physics, Vol. 140, Issue 12
  • DOI: 10.1063/1.4869109

Cluster formation, waterlike anomalies, and re-entrant melting for a family of bounded repulsive interaction potentials
journal, March 2010


Colloidal systems with competing interactions: from an arrested repulsive cluster phase to a gel
journal, January 2009

  • Toledano, Juan Carlos Fernandez; Sciortino, Francesco; Zaccarelli, Emanuela
  • Soft Matter, Vol. 5, Issue 12
  • DOI: 10.1039/b818169a

Equilibrium cluster formation in concentrated protein solutions and colloids
journal, November 2004

  • Stradner, Anna; Sedgwick, Helen; Cardinaux, Frédéric
  • Nature, Vol. 432, Issue 7016
  • DOI: 10.1038/nature03109

Canonical sampling through velocity rescaling
journal, January 2007

  • Bussi, Giovanni; Donadio, Davide; Parrinello, Michele
  • The Journal of Chemical Physics, Vol. 126, Issue 1
  • DOI: 10.1063/1.2408420

The multiscale coarse-graining method. V. Isothermal-isobaric ensemble
journal, April 2010

  • Das, Avisek; Andersen, Hans C.
  • The Journal of Chemical Physics, Vol. 132, Issue 16
  • DOI: 10.1063/1.3394862

Colloidal cluster phases, gelation and nuclear matter
journal, October 2004


Theory for the phase behaviour of a colloidal fluid with competing interactions
journal, September 2008


Inverse design of simple pair potentials for the self-assembly of complex structures
journal, November 2018

  • Adorf, Carl S.; Antonaglia, James; Dshemuchadse, Julia
  • The Journal of Chemical Physics, Vol. 149, Issue 20
  • DOI: 10.1063/1.5063802

Inverting the design path for self-assembled block copolymers
journal, January 2017

  • Gadelrab, Karim R.; Hannon, Adam F.; Ross, Caroline A.
  • Molecular Systems Design & Engineering, Vol. 2, Issue 5
  • DOI: 10.1039/c7me00062f

Optimizing the formation of colloidal compounds with components of different shapes
journal, December 2017

  • Escobedo, Fernando A.
  • The Journal of Chemical Physics, Vol. 147, Issue 21
  • DOI: 10.1063/1.5006047

Dynamical Arrest in Attractive Colloids: The Effect of Long-Range Repulsion
journal, May 2005

  • Campbell, Andrew I.; Anderson, Valerie J.; van Duijneveldt, Jeroen S.
  • Physical Review Letters, Vol. 94, Issue 20
  • DOI: 10.1103/physrevlett.94.208301

Robust structural identification via polyhedral template matching
journal, May 2016

  • Larsen, Peter Mahler; Schmidt, Søren; Schiøtz, Jakob
  • Modelling and Simulation in Materials Science and Engineering, Vol. 24, Issue 5
  • DOI: 10.1088/0965-0393/24/5/055007

Inverse design of multicomponent assemblies
journal, March 2018

  • Piñeros, William D.; Lindquist, Beth A.; Jadrich, Ryan B.
  • The Journal of Chemical Physics, Vol. 148, Issue 10
  • DOI: 10.1063/1.5021648

A test of systematic coarse-graining of molecular dynamics simulations: Thermodynamic properties
journal, October 2012

  • Fu, Chia-Chun; Kulkarni, Pandurang M.; Scott Shell, M.
  • The Journal of Chemical Physics, Vol. 137, Issue 16
  • DOI: 10.1063/1.4759463

Screening and designing patchy particles for optimized self-assembly propensity through assembly pathway engineering
journal, January 2012

  • Jankowski, Eric; Glotzer, Sharon C.
  • Soft Matter, Vol. 8, Issue 10
  • DOI: 10.1039/c2sm07101k

Probabilistic inverse design for self-assembling materials
journal, May 2017

  • Jadrich, R. B.; Lindquist, B. A.; Truskett, T. M.
  • The Journal of Chemical Physics, Vol. 146, Issue 18
  • DOI: 10.1063/1.4981796

Communication: Thermodynamic signatures of cluster formation in fluids with competing interactions
journal, July 2012

  • Bomont, Jean-Marc; Bretonnet, Jean-Louis; Costa, Dino
  • The Journal of Chemical Physics, Vol. 137, Issue 1
  • DOI: 10.1063/1.4733390

Optimising minimal building blocks for addressable self-assembly
journal, January 2017


Communication: Inverse design for self-assembly via on-the-fly optimization
journal, September 2016

  • Lindquist, Beth A.; Jadrich, Ryan B.; Truskett, Thomas M.
  • The Journal of Chemical Physics, Vol. 145, Issue 11
  • DOI: 10.1063/1.4962754

Visualization and analysis of atomistic simulation data with OVITO–the Open Visualization Tool
journal, December 2009


Coarse-graining entropy, forces, and structures
journal, December 2011

  • Rudzinski, Joseph F.; Noid, W. G.
  • The Journal of Chemical Physics, Vol. 135, Issue 21
  • DOI: 10.1063/1.3663709

Perspective: Coarse-grained models for biomolecular systems
journal, September 2013

  • Noid, W. G.
  • The Journal of Chemical Physics, Vol. 139, Issue 9
  • DOI: 10.1063/1.4818908

Machine learning and data science in soft materials engineering
journal, December 2017


The relative entropy is fundamental to multiscale and inverse thermodynamic problems
journal, October 2008

  • Shell, M. Scott
  • The Journal of Chemical Physics, Vol. 129, Issue 14
  • DOI: 10.1063/1.2992060

Mesophases of soft-sphere aggregates
journal, January 2009

  • Shin, Homin; Grason, Gregory M.; Santangelo, Christian D.
  • Soft Matter, Vol. 5, Issue 19
  • DOI: 10.1039/b904103f

Assembly of nothing: equilibrium fluids with designed structured porosity
journal, January 2016

  • Lindquist, Beth A.; Jadrich, Ryan B.; Truskett, Thomas M.
  • Soft Matter, Vol. 12, Issue 10
  • DOI: 10.1039/c5sm03068d

Biopolymer-directed synthesis of high-surface-area magnetite colloidal nanocrystal clusters for dual drug delivery in prostate cancer
journal, January 2012

  • Xu, Shuai; Sun, Chuanyu; Guo, Jia
  • Journal of Materials Chemistry, Vol. 22, Issue 36
  • DOI: 10.1039/c2jm34877b

Equilibrium Phase Behavior of the Square-Well Linear Microphase-Forming Model
journal, April 2016

  • Zhuang, Yuan; Charbonneau, Patrick
  • The Journal of Physical Chemistry B, Vol. 120, Issue 26
  • DOI: 10.1021/acs.jpcb.6b02167

Inverse design of simple pairwise interactions with low-coordinated 3D lattice ground states
journal, January 2013

  • Jain, Avni; Errington, Jeffrey R.; Truskett, Thomas M.
  • Soft Matter, Vol. 9, Issue 14
  • DOI: 10.1039/c3sm27785b

Deriving effective mesoscale potentials from atomistic simulations: Mesoscale Potentials from Atomistic Simulations
journal, August 2003

  • Reith, Dirk; Pütz, Mathias; Müller-Plathe, Florian
  • Journal of Computational Chemistry, Vol. 24, Issue 13
  • DOI: 10.1002/jcc.10307

Continuous Freezing in Three Dimensions
journal, May 2003


Comparative atomistic and coarse-grained study of water: What do we lose by coarse-graining?
journal, January 2009


Turning statistical physics models into materials design engines
journal, December 2015

  • Miskin, Marc Z.; Khaira, Gurdaman; de Pablo, Juan J.
  • Proceedings of the National Academy of Sciences, Vol. 113, Issue 1
  • DOI: 10.1073/pnas.1509316112

    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.