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Metastable Phase Formation and Materials Discovery in Complex Oxide Thin Films via Laser Spike Annealing- [electronic resource]
Metastable Phase Formation and Materials Discovery in Complex Oxide Thin Films via Laser S...
Metastable Phase Formation and Materials Discovery in Complex Oxide Thin Films via Laser Spike Annealing- [electronic resource]

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자료유형  
 학위논문파일 국외
최종처리일시  
20240214101637
ISBN  
9798380316903
DDC  
620.11
저자명  
Connolly, Aine.
서명/저자  
Metastable Phase Formation and Materials Discovery in Complex Oxide Thin Films via Laser Spike Annealing - [electronic resource]
발행사항  
[S.l.]: : Cornell University., 2023
발행사항  
Ann Arbor : : ProQuest Dissertations & Theses,, 2023
형태사항  
1 online resource(152 p.)
주기사항  
Source: Dissertations Abstracts International, Volume: 85-03, Section: B.
주기사항  
Advisor: Thompson, Michael O.
학위논문주기  
Thesis (Ph.D.)--Cornell University, 2023.
사용제한주기  
This item must not be sold to any third party vendors.
초록/해제  
요약Rapid thermal processing of materials, particularly processing techniques with high quench rates, have been demonstrated to form and stabilize ambient quenched non-equilibrium metastable phases. These phases often have distinct structures and properties, dramatically expanding the materials space available for applications. One such technique is Laser Spike Annealing (LSA), where a scanned laser over a thin-film material enables heating and quench rates of up to 107 K/s. The development of a high-throughput variant, lateral gradient LSA, has recently been exploited to create time, temperature and composition maps of phase formation in a broad range of systems. Successful integration of this technique with active learning algorithms has further allowed autonomous searching, driving a new era of combinatorial high throughput materials discovery.While the autonomous searches can identify the ultimate structures formed, the evolution of the structure during LSA is difficult to study directly. Post-processing analysis of terminal structures can only infer transient changes that may be essential to understanding the kinetic behavior. In this work, we present a novel technique through which sub-millisecond materials transformations can be followed in situ during LSA, using the unique geometry of LSA to transform the time axis to a spatial dimension. Optical microscopy and X-ray diffraction are used to follow the sequences of metastable phase formation in situ for eleven oxide films as a function of both time and temperature, with time resolution down to 100 µs.Bi2O3, with a high oxygen ion conductivity in the δ-phase, is a polymorphic system of particular interest. Using in situ methods, we show that at high temperatures the δ-phase forms prior to melt and that at low temperatures the sputter-deposited amorphous precursor continually transforms to a two-phase region of δ + β due to the structural similarities between these phases and the low free energy cost of formation. In the Ga2o3 system, a widely studied ultra-wide bandgap semiconductor, we find that the defective-spinel γ-phase is the always first nucleating structure from as-deposited amorphous films, with a continuous solid-solid transformation to β occurring with increased temperatures. These results provide critical insight into the mechanisms determining the initial nucleating phase at high quench rates in oxide thin films.The ability to track and study the evolution of materials in situ provides a dramatic increase in the kinetic information accessible to researchers, which can be coupled with combinatorial and autonomous searches to more rapidly explore and understand metastable structures and their resultant properties.
일반주제명  
Materials science.
일반주제명  
Thermodynamics.
키워드  
Laser annealing
키워드  
Materials discovery
키워드  
Metastable materials
키워드  
Oxides
키워드  
Thin films
기타저자  
Cornell University Materials Science and Engineering
기본자료저록  
Dissertations Abstracts International. 85-03B.
기본자료저록  
Dissertation Abstract International
전자적 위치 및 접속  
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MARC

 008240612s2023      us  |||||||||||||||c||eng  d
■001000016934640
■00520240214101637
■006m          o    d                
■007cr#unu||||||||
■020    ▼a9798380316903
■035    ▼a(MiAaPQ)AAI30631889
■040    ▼aMiAaPQ▼cMiAaPQ
■0820  ▼a620.11
■1001  ▼aConnolly,  Aine.▼0(orcid)0000-0002-2721-5621
■24510▼aMetastable  Phase  Formation  and  Materials  Discovery  in  Complex  Oxide  Thin  Films  via  Laser  Spike  Annealing▼h[electronic  resource]
■260    ▼a[S.l.]:▼bCornell  University.  ▼c2023
■260  1▼aAnn  Arbor  :▼bProQuest  Dissertations  &  Theses,  ▼c2023
■300    ▼a1  online  resource(152  p.)
■500    ▼aSource:  Dissertations  Abstracts  International,  Volume:  85-03,  Section:  B.
■500    ▼aAdvisor:  Thompson,  Michael  O.
■5021  ▼aThesis  (Ph.D.)--Cornell  University,  2023.
■506    ▼aThis  item  must  not  be  sold  to  any  third  party  vendors.
■520    ▼aRapid  thermal  processing  of  materials,  particularly  processing  techniques  with  high  quench  rates,  have  been  demonstrated  to  form  and  stabilize  ambient  quenched  non-equilibrium  metastable  phases.  These  phases  often  have  distinct  structures  and  properties,  dramatically  expanding  the  materials  space  available  for  applications.  One  such  technique  is  Laser  Spike  Annealing  (LSA),  where  a  scanned  laser  over  a  thin-film  material  enables  heating  and  quench  rates  of  up  to  107  K/s.  The  development  of  a  high-throughput  variant,  lateral  gradient  LSA,  has  recently  been  exploited  to  create  time,  temperature  and  composition  maps  of  phase  formation  in  a  broad  range  of  systems.  Successful  integration  of  this  technique  with  active  learning  algorithms  has  further  allowed  autonomous  searching,  driving  a  new  era  of  combinatorial  high  throughput  materials  discovery.While  the  autonomous  searches  can  identify  the  ultimate  structures  formed,  the  evolution  of  the  structure  during  LSA  is  difficult  to  study  directly.  Post-processing  analysis  of  terminal  structures  can  only  infer  transient  changes  that  may  be  essential  to  understanding  the  kinetic  behavior.  In  this  work,  we  present  a  novel  technique  through  which  sub-millisecond  materials  transformations  can  be  followed  in  situ  during  LSA,  using  the  unique  geometry  of  LSA  to  transform  the  time  axis  to  a  spatial  dimension.  Optical  microscopy  and  X-ray  diffraction  are  used  to  follow  the  sequences  of  metastable  phase  formation  in  situ  for  eleven  oxide  films  as  a  function  of  both  time  and  temperature,  with  time  resolution  down  to  100  µs.Bi2O3,  with  a  high  oxygen  ion  conductivity  in  the  δ-phase,  is  a  polymorphic  system  of  particular  interest.  Using  in  situ  methods,  we  show  that  at  high  temperatures  the  δ-phase  forms  prior  to  melt  and  that  at  low  temperatures  the  sputter-deposited  amorphous  precursor  continually  transforms  to  a  two-phase  region  of  δ  +  β  due  to  the  structural  similarities  between  these  phases  and  the  low  free  energy  cost  of  formation.  In  the  Ga2o3  system,  a  widely  studied  ultra-wide  bandgap  semiconductor,  we  find  that  the  defective-spinel  γ-phase  is  the  always  first  nucleating  structure  from  as-deposited  amorphous  films,  with  a  continuous  solid-solid  transformation  to  β  occurring  with  increased  temperatures.  These  results  provide  critical  insight  into  the  mechanisms  determining  the  initial  nucleating  phase  at  high  quench  rates  in  oxide  thin  films.The  ability  to  track  and  study  the  evolution  of  materials  in  situ  provides  a  dramatic  increase  in  the  kinetic  information  accessible  to  researchers,  which  can  be  coupled  with  combinatorial  and  autonomous  searches  to  more  rapidly  explore  and  understand  metastable  structures  and  their  resultant  properties.
■590    ▼aSchool  code:  0058.
■650  4▼aMaterials  science.
■650  4▼aThermodynamics.
■653    ▼aLaser  annealing
■653    ▼aMaterials  discovery
■653    ▼aMetastable  materials
■653    ▼aOxides
■653    ▼aThin  films
■690    ▼a0794
■690    ▼a0348
■71020▼aCornell  University▼bMaterials  Science  and  Engineering.
■7730  ▼tDissertations  Abstracts  International▼g85-03B.
■773    ▼tDissertation  Abstract  International
■790    ▼a0058
■791    ▼aPh.D.
■792    ▼a2023
■793    ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T16934640▼nKERIS▼z이  자료의  원문은  한국교육학술정보원에서  제공합니다.
■980    ▼a202402▼f2024

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