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Transmorphic Nucleation of Solids in Liquid Thin Films
Transmorphic Nucleation of Solids in Liquid Thin Films
Transmorphic Nucleation of Solids in Liquid Thin Films

상세정보

자료유형  
 학위논문 서양
최종처리일시  
20250211153147
ISBN  
9798384486305
DDC  
620.11
저자명  
Shen, Bonan.
서명/저자  
Transmorphic Nucleation of Solids in Liquid Thin Films
발행사항  
[Sl] : Columbia University, 2024
발행사항  
Ann Arbor : ProQuest Dissertations & Theses, 2024
형태사항  
131 p
주기사항  
Source: Dissertations Abstracts International, Volume: 86-04, Section: B.
주기사항  
Advisor: Im, James S.
학위논문주기  
Thesis (Ph.D.)--Columbia University, 2024.
초록/해제  
요약This dissertation focuses on identifying and analyzing the mechanism of solid nucleation in liquid thin films. In doing so, we identify and describe a previously unrecognized mechanism of nucleation in condensed systems referred to as transmorphic nucleation. This cluster-shape-change-based mechanism is revealed as a general heterogeneous nucleation mechanism applicable to discontinuous phase transformations occurring in continuous or pre-patterned thin films, as well as in numerous materials systems that possess morphologically and chemically non-trivial heterogeneous-nucleation-catalyzing interfaces (e.g., polycrystalline materials, embedded nano-crystals, and materials with structured interfaces).Identifying, deciphering, and modeling the nature and details associated with how a new phase can nucleate in thin-film materials can be both scientifically meaningful for understanding discontinuous phase transformations in general, and technologically important for engineering various thin-film-based and nano-material-based applications and devices in particular. Classical nucleation theory (CNT) has long been established and regarded as the most practicable treatment that captures the thermodynamic and kinetic essence of the nucleation phenomenon in condensed systems in the simplest and most effective manner. Through a close examination of the theory, we identify and propose morphological equilibrium hypothesis (MEH) as an essential element of CNT. Our shape-transition-based model for transmorphic nucleation in thin films presented in this thesis illustrates that this hypothesis can be violated. As such, the CNT formulation is lacking in capturing the occurrence of the MEH-deviating shape evolution of the clusters, as for instance encountered during the process of transmorphic nucleation.In this dissertation, we conceptually, theoretically, and numerically examine and analyze the kinetic pathway through which nucleation of solids takes place in encapsulated liquid thin films. This example was selected for investigation because it is a particularly simple system, which in turn permits one to make clear, definitive, and general conclusions. A new nucleation mechanism of transmorphic nucleation is discovered in the process. This mechanism is defined generally as the nucleation mechanism through which supercritical clusters are generated from subcritical clusters during an irreversible and morphological-equilibrium-deviating shape evolution initiated when the fluctuating embryos encounter a local growth-inducing element in the catalyzing interface. Both thermodynamic and kinetic analyses in accordance with our transmorphic nucleation mechanism are carried out using a novel adaptation of established theoretical formulations and numerical modeling methods. The kinetic pathway of transmorphic nucleation is described, and transmorphic nucleation temperature window is thermodynamically identified. The kinetic aspect of transmorphic nucleation in thin films is uniquely captured by keeping track of two coupled population distribution profiles of equilibrium-morphology-adhering cluster shapes.Overall, the thesis starts with critical and deconstructive examination of CNT. It builds on our theory of phase initiation and evolution in condensed systems, i.e., Gibbs-Thomson variation (GTV) and Gibbs-Thomson function (GTF), and our interpretation of CNT to investigate steady-state and transient transmorphic nucleation in thin films. The thesis also examines and analyzes all other modes of shape-transition-affected nucleation in thin films outside the transmorphic nucleation domain to provide the comprehensive description of the entire map of nucleation mechanisms in thin-film systems. As far as the implications of the current work on the classical theory of nucleation is concerned, we illustrate how the phenomenon of transmorphic nucleation which violates MEH that forms the basis of CNT, reveals this previously unrecognized limitation of the current formulation of the classical theory of nucleation. The results presented in this dissertation further show that the GTV-based approach, which we identify as the foundation upon which CNT is formulated, can address the MEH-violating shape evolution of subcritical to supercritical clusters.
일반주제명  
Materials science
일반주제명  
Nuclear engineering
일반주제명  
Nanoscience
일반주제명  
Morphology
키워드  
Nucleation
키워드  
Phase transformations
키워드  
Thin films
키워드  
Solid nucleation
키워드  
Classical nucleation theory
기타저자  
Columbia University Materials Science and Engineering
기본자료저록  
Dissertations Abstracts International. 86-04B.
전자적 위치 및 접속  
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MARC

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■1001  ▼aShen,  Bonan.
■24510▼aTransmorphic  Nucleation  of  Solids  in  Liquid  Thin  Films
■260    ▼a[Sl]▼bColumbia  University▼c2024
■260  1▼aAnn  Arbor▼bProQuest  Dissertations  &  Theses▼c2024
■300    ▼a131  p
■500    ▼aSource:  Dissertations  Abstracts  International,  Volume:  86-04,  Section:  B.
■500    ▼aAdvisor:  Im,  James  S.
■5021  ▼aThesis  (Ph.D.)--Columbia  University,  2024.
■520    ▼aThis  dissertation  focuses  on  identifying  and  analyzing  the  mechanism  of  solid  nucleation  in  liquid  thin  films.  In  doing  so,  we  identify  and  describe  a  previously  unrecognized  mechanism  of  nucleation  in  condensed  systems  referred  to  as  transmorphic  nucleation.  This  cluster-shape-change-based  mechanism  is  revealed  as  a  general  heterogeneous  nucleation  mechanism  applicable  to  discontinuous  phase  transformations  occurring  in  continuous  or  pre-patterned  thin  films,  as  well  as  in  numerous  materials  systems  that  possess  morphologically  and  chemically  non-trivial  heterogeneous-nucleation-catalyzing  interfaces  (e.g.,  polycrystalline  materials,  embedded  nano-crystals,  and  materials  with  structured  interfaces).Identifying,  deciphering,  and  modeling  the  nature  and  details  associated  with  how  a  new  phase  can  nucleate  in  thin-film  materials  can  be  both  scientifically  meaningful  for  understanding  discontinuous  phase  transformations  in  general,  and  technologically  important  for  engineering  various  thin-film-based  and  nano-material-based  applications  and  devices  in  particular.  Classical  nucleation  theory  (CNT)  has  long  been  established  and  regarded  as  the  most  practicable  treatment  that  captures  the  thermodynamic  and  kinetic  essence  of  the  nucleation  phenomenon  in  condensed  systems  in  the  simplest  and  most  effective  manner.  Through  a  close  examination  of  the  theory,  we  identify  and  propose  morphological  equilibrium  hypothesis  (MEH)  as  an  essential  element  of  CNT.  Our  shape-transition-based  model  for  transmorphic  nucleation  in  thin  films  presented  in  this  thesis  illustrates  that  this  hypothesis  can  be  violated.  As  such,  the  CNT  formulation  is  lacking  in  capturing  the  occurrence  of  the  MEH-deviating  shape  evolution  of  the  clusters,  as  for  instance  encountered  during  the  process  of  transmorphic  nucleation.In  this  dissertation,  we  conceptually,  theoretically,  and  numerically  examine  and  analyze  the  kinetic  pathway  through  which  nucleation  of  solids  takes  place  in  encapsulated  liquid  thin  films.  This  example  was  selected  for  investigation  because  it  is  a  particularly  simple  system,  which  in  turn  permits  one  to  make  clear,  definitive,  and  general  conclusions.  A  new  nucleation  mechanism  of  transmorphic  nucleation  is  discovered  in  the  process.  This  mechanism  is  defined  generally  as  the  nucleation  mechanism  through  which  supercritical  clusters  are  generated  from  subcritical  clusters  during  an  irreversible  and  morphological-equilibrium-deviating  shape  evolution  initiated  when  the  fluctuating  embryos  encounter  a  local  growth-inducing  element  in  the  catalyzing  interface.  Both  thermodynamic  and  kinetic  analyses  in  accordance  with  our  transmorphic  nucleation  mechanism  are  carried  out  using  a  novel  adaptation  of  established  theoretical  formulations  and  numerical  modeling  methods.  The  kinetic  pathway  of  transmorphic  nucleation  is  described,  and  transmorphic  nucleation  temperature  window  is  thermodynamically  identified.  The  kinetic  aspect  of  transmorphic  nucleation  in  thin  films  is  uniquely  captured  by  keeping  track  of  two  coupled  population  distribution  profiles  of  equilibrium-morphology-adhering  cluster  shapes.Overall,  the  thesis  starts  with  critical  and  deconstructive  examination  of  CNT.  It  builds  on  our  theory  of  phase  initiation  and  evolution  in  condensed  systems,  i.e.,  Gibbs-Thomson  variation  (GTV)  and  Gibbs-Thomson  function  (GTF),  and  our  interpretation  of  CNT  to  investigate  steady-state  and  transient  transmorphic  nucleation  in  thin  films.  The  thesis  also  examines  and  analyzes  all  other  modes  of  shape-transition-affected  nucleation  in  thin  films  outside  the  transmorphic  nucleation  domain  to  provide  the  comprehensive  description  of  the  entire  map  of  nucleation  mechanisms  in  thin-film  systems.  As  far  as  the  implications  of  the  current  work  on  the  classical  theory  of  nucleation  is  concerned,  we  illustrate  how  the  phenomenon  of  transmorphic  nucleation  which  violates  MEH  that  forms  the  basis  of  CNT,  reveals  this  previously  unrecognized  limitation  of  the  current  formulation  of  the  classical  theory  of  nucleation.  The  results  presented  in  this  dissertation  further  show  that  the  GTV-based  approach,  which  we  identify  as  the  foundation  upon  which  CNT  is  formulated,  can  address  the  MEH-violating  shape  evolution  of  subcritical  to  supercritical  clusters.  
■590    ▼aSchool  code:  0054.
■650  4▼aMaterials  science
■650  4▼aNuclear  engineering
■650  4▼aNanoscience
■650  4▼aMorphology
■653    ▼aNucleation
■653    ▼aPhase  transformations
■653    ▼aThin  films
■653    ▼aSolid  nucleation
■653    ▼aClassical  nucleation  theory
■690    ▼a0794
■690    ▼a0565
■690    ▼a0552
■690    ▼a0287
■71020▼aColumbia  University▼bMaterials  Science  and  Engineering.
■7730  ▼tDissertations  Abstracts  International▼g86-04B.
■790    ▼a0054
■791    ▼aPh.D.
■792    ▼a2024
■793    ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17165194▼nKERIS▼z이  자료의  원문은  한국교육학술정보원에서  제공합니다.

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