Order from Disorder: Measuring Reversibility and Local Equilibration in Self-Assembly

Research output: ThesisDoctoral Thesis

Abstract

We illustrate self-assembly with several systems which aim to harness the process of assembly to create new functional structures. The concept of kinetic trapping preventing assembly and the importance of reversibility, breaking as well as making bonds, for avoiding such traps are introduced. We aim to identify
how reversible systems are, with the aim of aecting the prediction, control and
design of new systems.
In four systems a lattice gas model, and three models based upon patchy particle
schemes, a yield is dened and used to identify optimal assembly at a given
time. Three measurements relevant to reversibility are described, applied, and
compared with the results of similar studies. The rst simply counts the bonding
and un-bonding events, or kinks, over the whole assembly process and compares
the total number of events with the net bonding events. We measure values of
100 􀀀 1000kinks per bond in crystal systems, and 60 􀀀 200 for closed structures.
In analogy with a toy model the values can be related to a `forgivingness', a ratio
of bad bonding sites, to good ones.
We then turn to measurements at early times which allow for the prediction
of when assembly will occur. These include rate measurements of kinks which
provide an instant measure of reversibility and comparison of correlation and
response functions with the equilibrium
uctuation dissipation theory. These
methods examine the dynamics of the assembly process while our third approach
examines the structures during assembly. We examine how each of the measurements
provide information about the assembly process and how it relates to
the particles, their interactions and the nal structure. The possibility of using
the methods in combination is shown to be relevant to the prediction of assembly
and how they might be used to implement design and control schemes to improve
assembly.
LanguageEnglish
QualificationPh.D.
Awarding Institution
  • University of Bath
Supervisors/Advisors
  • Jack, Robert, Supervisor
Award date17 Oct 2012
StatusUnpublished - Aug 2012

Fingerprint

self assembly
assembly
disorders
predictions
harnesses
particle interactions
dissipation
trapping
traps
kinetics
gases
crystals

Cite this

@phdthesis{fd3dc3d6dd744118bf8e48595b535130,
title = "Order from Disorder: Measuring Reversibility and Local Equilibration in Self-Assembly",
abstract = "We illustrate self-assembly with several systems which aim to harness the process of assembly to create new functional structures. The concept of kinetic trapping preventing assembly and the importance of reversibility, breaking as well as making bonds, for avoiding such traps are introduced. We aim to identifyhow reversible systems are, with the aim of aecting the prediction, control anddesign of new systems.In four systems a lattice gas model, and three models based upon patchy particleschemes, a yield is dened and used to identify optimal assembly at a giventime. Three measurements relevant to reversibility are described, applied, andcompared with the results of similar studies. The rst simply counts the bondingand un-bonding events, or kinks, over the whole assembly process and comparesthe total number of events with the net bonding events. We measure values of100 􀀀 1000kinks per bond in crystal systems, and 60 􀀀 200 for closed structures.In analogy with a toy model the values can be related to a `forgivingness', a ratioof bad bonding sites, to good ones.We then turn to measurements at early times which allow for the predictionof when assembly will occur. These include rate measurements of kinks whichprovide an instant measure of reversibility and comparison of correlation andresponse functions with the equilibrium uctuation dissipation theory. Thesemethods examine the dynamics of the assembly process while our third approachexamines the structures during assembly. We examine how each of the measurementsprovide information about the assembly process and how it relates tothe particles, their interactions and the nal structure. The possibility of usingthe methods in combination is shown to be relevant to the prediction of assemblyand how they might be used to implement design and control schemes to improveassembly.",
author = "James Grant",
year = "2012",
month = "8",
language = "English",
school = "University of Bath",

}

TY - THES

T1 - Order from Disorder: Measuring Reversibility and Local Equilibration in Self-Assembly

AU - Grant,James

PY - 2012/8

Y1 - 2012/8

N2 - We illustrate self-assembly with several systems which aim to harness the process of assembly to create new functional structures. The concept of kinetic trapping preventing assembly and the importance of reversibility, breaking as well as making bonds, for avoiding such traps are introduced. We aim to identifyhow reversible systems are, with the aim of aecting the prediction, control anddesign of new systems.In four systems a lattice gas model, and three models based upon patchy particleschemes, a yield is dened and used to identify optimal assembly at a giventime. Three measurements relevant to reversibility are described, applied, andcompared with the results of similar studies. The rst simply counts the bondingand un-bonding events, or kinks, over the whole assembly process and comparesthe total number of events with the net bonding events. We measure values of100 􀀀 1000kinks per bond in crystal systems, and 60 􀀀 200 for closed structures.In analogy with a toy model the values can be related to a `forgivingness', a ratioof bad bonding sites, to good ones.We then turn to measurements at early times which allow for the predictionof when assembly will occur. These include rate measurements of kinks whichprovide an instant measure of reversibility and comparison of correlation andresponse functions with the equilibrium uctuation dissipation theory. Thesemethods examine the dynamics of the assembly process while our third approachexamines the structures during assembly. We examine how each of the measurementsprovide information about the assembly process and how it relates tothe particles, their interactions and the nal structure. The possibility of usingthe methods in combination is shown to be relevant to the prediction of assemblyand how they might be used to implement design and control schemes to improveassembly.

AB - We illustrate self-assembly with several systems which aim to harness the process of assembly to create new functional structures. The concept of kinetic trapping preventing assembly and the importance of reversibility, breaking as well as making bonds, for avoiding such traps are introduced. We aim to identifyhow reversible systems are, with the aim of aecting the prediction, control anddesign of new systems.In four systems a lattice gas model, and three models based upon patchy particleschemes, a yield is dened and used to identify optimal assembly at a giventime. Three measurements relevant to reversibility are described, applied, andcompared with the results of similar studies. The rst simply counts the bondingand un-bonding events, or kinks, over the whole assembly process and comparesthe total number of events with the net bonding events. We measure values of100 􀀀 1000kinks per bond in crystal systems, and 60 􀀀 200 for closed structures.In analogy with a toy model the values can be related to a `forgivingness', a ratioof bad bonding sites, to good ones.We then turn to measurements at early times which allow for the predictionof when assembly will occur. These include rate measurements of kinks whichprovide an instant measure of reversibility and comparison of correlation andresponse functions with the equilibrium uctuation dissipation theory. Thesemethods examine the dynamics of the assembly process while our third approachexamines the structures during assembly. We examine how each of the measurementsprovide information about the assembly process and how it relates tothe particles, their interactions and the nal structure. The possibility of usingthe methods in combination is shown to be relevant to the prediction of assemblyand how they might be used to implement design and control schemes to improveassembly.

M3 - Doctoral Thesis

ER -