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Ultrafast Nanoscale Structural Dynamics in Complex Oxide Thin Films and Heterostructures: Implications on Electrical and Magnetic Phenomena
Ultrafast Nanoscale Structural Dynamics in Complex Oxide Thin Films and Heterostructures: ...
Ultrafast Nanoscale Structural Dynamics in Complex Oxide Thin Films and Heterostructures: Implications on Electrical and Magnetic Phenomena

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자료유형  
 학위논문 서양
최종처리일시  
20250211153024
ISBN  
9798896077855
DDC  
620.11
저자명  
Sri Gyan, Deepankar.
서명/저자  
Ultrafast Nanoscale Structural Dynamics in Complex Oxide Thin Films and Heterostructures: Implications on Electrical and Magnetic Phenomena
발행사항  
[Sl] : The University of Wisconsin - Madison, 2024
발행사항  
Ann Arbor : ProQuest Dissertations & Theses, 2024
형태사항  
181 p
주기사항  
Source: Dissertations Abstracts International, Volume: 86-04, Section: B.
주기사항  
Advisor: Evans, Paul G.
학위논문주기  
Thesis (Ph.D.)--The University of Wisconsin - Madison, 2024.
초록/해제  
요약In complex oxide electronic and magnetic materials, the interplay between microscopic degrees of freedom-such as electrons, spins, orbitals, and the lattice-plays a crucial role in determining their equilibrium physical properties. Femtosecond optical excitation provides a powerful means to perturb one or more of these degrees of freedom, driving the system into non-equilibrium states and enabling the dynamic control of electronic and magnetic behaviors on femto- to pico-second timescales. A comprehensive understanding of these dynamics is essential for advancing next-generation technologies, such as spintronics and optoelectronics. My dissertation research leverages recent advancements in ultrafast x-ray sources, including free-electron lasers, to probe the structural dynamics of materials, shedding light on the underlying mechanisms that govern these phenomena. Specifically, this work investigates photoinduced structural responses in complex oxide heterostructures using time-resolved x-ray diffraction techniques.The first part of this dissertation focuses on ultrafast magnetization dynamics in the ferrimagnetic thin film heterostructure Pt/Gd3Fe5O12/Gd3Ga5O12 (Pt/GdIG/GGG), which has potential applications in spin-Seebeck devices. Time-resolved optical pump x-ray probe technique, combined with resonant magnetic diffraction, was employed to simultaneously investigate phonon and magnon dynamics. To establish a foundation for understanding the dynamical responses, the equilibrium magnetization configuration in the heterostructure was first characterized. Resonant diffraction experiments at the Gd L2 resonance edge, paired with theoretical calculations, provided insights into the magnetic anisotropy and equilibrium magnetization of GdIG thin film. In the optical pump-x-ray probe experiment, the optical absorption induced transient heating of the Pt layer leads to the excitation of phonons and magnons in the GdIG layer. A detailed investigation of phonon propagation within the Pt layer, along with the thermal transport from Pt to GdIG, was critical. Acoustic phonon propagation in the Pt layer was further explored by measuring the time-dependent diffraction pattern from the Pt layer, revealing parameters such as acoustic impedance, mean free path, and the Gruneisen anharmonicity parameter. Thermal modeling with the measured time-dependent diffracted intensity from Pt quantified the interfacial thermal conductance of the Pt/GdIG interface. Finally, the time-resolved resonant diffraction experiment captured magnetization dynamics in response to the photoexcited strain pulses, with the evidence suggesting the excitation of a non-dispersive Gd precessional mode as well. The wavevector-resolved experiments also probed the magnon-phonon coupling regime in the GdIG.The second part of this dissertation examines the structural dynamics of ferroelectric/dielectric superlattices following optical excitation near the nominal bandgap of the constituent layers. Wavevector- and time-resolved diffraction experiments on a PbTiO3/SrTiO3 (PTO/STO) superlattice, featuring a 180° stripe domain pattern, uncovered a novel, non-dispersive ~1 THz mode that was not predicted by elastic modeling. The experimental results, combined with dynamical phase field modeling by our collaborators, revealed that this mode is associated with a dynamical transition in the polar texture at the domain boundary. These findings demonstrate the existence of picosecond-scale transitions in ferroelectric thin films with polar textures upon optical excitation. Additional experiments on a monodomain BaTiO3/CaTiO3 (BTO/CTO) superlattice thin film revealed opposing photoinduced effects in the component layers: polarization enhancement in the ferroelectric BTO layers and polarization suppression in the CTO layers, resulting in the dynamical compression of the CTO layers. The research described in this thesis underscores the potential of ultrafast x-ray diffraction techniques to uncover complex dynamic phenomena in oxide heterostructures. It lays the groundwork for future studies aimed at discovering novel non-equilibrium modes and interactions. These methodologies enable experiments that can probe the excitation of specific phonon or magnon modes and their wavevector dependence, offering deeper insights into how these modes propagate and influence material behavior. Such insights will be instrumental in designing future experiments to explore complex phonon-phonon or magnon-phonon hybridizations.
일반주제명  
Materials science
일반주제명  
Engineering
키워드  
Free electron laser diffraction
키워드  
Magnons
키워드  
Phonons
키워드  
Resonant magnetic diffraction
키워드  
Ultrafast structural dynamics
기타저자  
The University of Wisconsin - Madison Materials Science and Engineering
기본자료저록  
Dissertations Abstracts International. 86-04B.
전자적 위치 및 접속  
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MARC

 008250123s2024        us                              c    eng  d
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■040    ▼aMiAaPQ▼cMiAaPQ
■0820  ▼a620.11
■1001  ▼aSri  Gyan,  Deepankar.
■24510▼aUltrafast  Nanoscale  Structural  Dynamics  in  Complex  Oxide  Thin  Films  and  Heterostructures:  Implications  on  Electrical  and  Magnetic  Phenomena
■260    ▼a[Sl]▼bThe  University  of  Wisconsin  -  Madison▼c2024
■260  1▼aAnn  Arbor▼bProQuest  Dissertations  &  Theses▼c2024
■300    ▼a181  p
■500    ▼aSource:  Dissertations  Abstracts  International,  Volume:  86-04,  Section:  B.
■500    ▼aAdvisor:  Evans,  Paul  G.
■5021  ▼aThesis  (Ph.D.)--The  University  of  Wisconsin  -  Madison,  2024.
■520    ▼aIn  complex  oxide  electronic  and  magnetic  materials,  the  interplay  between  microscopic  degrees  of  freedom-such  as  electrons,  spins,  orbitals,  and  the  lattice-plays  a  crucial  role  in  determining  their  equilibrium  physical  properties.  Femtosecond  optical  excitation  provides  a  powerful  means  to  perturb  one  or  more  of  these  degrees  of  freedom,  driving  the  system  into  non-equilibrium  states  and  enabling  the  dynamic  control  of  electronic  and  magnetic  behaviors  on  femto-  to  pico-second  timescales.  A  comprehensive  understanding  of  these  dynamics  is  essential  for  advancing  next-generation  technologies,  such  as  spintronics  and  optoelectronics.  My  dissertation  research  leverages  recent  advancements  in  ultrafast  x-ray  sources,  including  free-electron  lasers,  to  probe  the  structural  dynamics  of  materials,  shedding  light  on  the  underlying  mechanisms  that  govern  these  phenomena.  Specifically,  this  work  investigates  photoinduced  structural  responses  in  complex  oxide  heterostructures  using  time-resolved  x-ray  diffraction  techniques.The  first  part  of  this  dissertation  focuses  on  ultrafast  magnetization  dynamics  in  the  ferrimagnetic  thin  film  heterostructure  Pt/Gd3Fe5O12/Gd3Ga5O12  (Pt/GdIG/GGG),  which  has  potential  applications  in  spin-Seebeck  devices.  Time-resolved  optical  pump  x-ray  probe  technique,  combined  with  resonant  magnetic  diffraction,  was  employed  to  simultaneously  investigate  phonon  and  magnon  dynamics.  To  establish  a  foundation  for  understanding  the  dynamical  responses,  the  equilibrium  magnetization  configuration  in  the  heterostructure  was  first  characterized.  Resonant  diffraction  experiments  at  the  Gd  L2  resonance  edge,  paired  with  theoretical  calculations,  provided  insights  into  the  magnetic  anisotropy  and  equilibrium  magnetization  of  GdIG  thin  film.  In  the  optical  pump-x-ray  probe  experiment,  the  optical  absorption  induced  transient  heating  of  the  Pt  layer  leads  to  the  excitation  of  phonons  and  magnons  in  the  GdIG  layer.  A  detailed  investigation  of  phonon  propagation  within  the  Pt  layer,  along  with  the  thermal  transport  from  Pt  to  GdIG,  was  critical.  Acoustic  phonon  propagation  in  the  Pt  layer  was  further  explored  by  measuring  the  time-dependent  diffraction  pattern  from  the  Pt  layer,  revealing  parameters  such  as  acoustic  impedance,  mean  free  path,  and  the  Gruneisen  anharmonicity  parameter.  Thermal  modeling  with  the  measured  time-dependent  diffracted  intensity  from  Pt  quantified  the  interfacial  thermal  conductance  of  the  Pt/GdIG  interface.  Finally,  the  time-resolved  resonant  diffraction  experiment  captured  magnetization  dynamics  in  response  to  the  photoexcited  strain  pulses,  with  the  evidence  suggesting  the  excitation  of  a  non-dispersive  Gd  precessional  mode  as  well.  The  wavevector-resolved  experiments  also  probed  the  magnon-phonon  coupling  regime  in  the  GdIG.The  second  part  of  this  dissertation  examines  the  structural  dynamics  of  ferroelectric/dielectric  superlattices  following  optical  excitation  near  the  nominal  bandgap  of  the  constituent  layers.  Wavevector-  and  time-resolved  diffraction  experiments  on  a  PbTiO3/SrTiO3  (PTO/STO)  superlattice,  featuring  a  180°  stripe  domain  pattern,  uncovered  a  novel,  non-dispersive  ~1  THz  mode  that  was  not  predicted  by  elastic  modeling.  The  experimental  results,  combined  with  dynamical  phase  field  modeling  by  our  collaborators,  revealed  that  this  mode  is  associated  with  a  dynamical  transition  in  the  polar  texture  at  the  domain  boundary.  These  findings  demonstrate  the  existence  of  picosecond-scale  transitions  in  ferroelectric  thin  films  with  polar  textures  upon  optical  excitation.  Additional  experiments  on  a  monodomain  BaTiO3/CaTiO3  (BTO/CTO)  superlattice  thin  film  revealed  opposing  photoinduced  effects  in  the  component  layers:  polarization  enhancement  in  the  ferroelectric  BTO  layers  and  polarization  suppression  in  the  CTO  layers,  resulting  in  the  dynamical  compression  of  the  CTO  layers.  The  research  described  in  this  thesis  underscores  the  potential  of  ultrafast  x-ray  diffraction  techniques  to  uncover  complex  dynamic  phenomena  in  oxide  heterostructures.  It  lays  the  groundwork  for  future  studies  aimed  at  discovering  novel  non-equilibrium  modes  and  interactions.  These  methodologies  enable  experiments  that  can  probe  the  excitation  of  specific  phonon  or  magnon  modes  and  their  wavevector  dependence,  offering  deeper  insights  into  how  these  modes  propagate  and  influence  material  behavior.  Such  insights  will  be  instrumental  in  designing  future  experiments  to  explore  complex  phonon-phonon  or  magnon-phonon  hybridizations.
■590    ▼aSchool  code:  0262.
■650  4▼aMaterials  science
■650  4▼aEngineering
■653    ▼aFree  electron  laser  diffraction
■653    ▼aMagnons
■653    ▼aPhonons
■653    ▼aResonant  magnetic  diffraction
■653    ▼aUltrafast  structural  dynamics
■690    ▼a0794
■690    ▼a0537
■71020▼aThe  University  of  Wisconsin  -  Madison▼bMaterials  Science  and  Engineering.
■7730  ▼tDissertations  Abstracts  International▼g86-04B.
■790    ▼a0262
■791    ▼aPh.D.
■792    ▼a2024
■793    ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17164624▼nKERIS▼z이  자료의  원문은  한국교육학술정보원에서  제공합니다.

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