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Crystal Chemistry and Seismic Wavespeeds of Dense Oxyhydroxides: Hydrogen Transport in Earth's Lower Mantle
Crystal Chemistry and Seismic Wavespeeds of Dense Oxyhydroxides: Hydrogen Transport in Ear...
Crystal Chemistry and Seismic Wavespeeds of Dense Oxyhydroxides: Hydrogen Transport in Earth's Lower Mantle

Detailed Information

자료유형  
 학위논문 서양
최종처리일시  
20260202104750
ISBN  
9798290653846
DDC  
540
저자명  
Strozewski, Benjamin Thomas.
서명/저자  
Crystal Chemistry and Seismic Wavespeeds of Dense Oxyhydroxides: Hydrogen Transport in Earths Lower Mantle
발행사항  
[Sl] : California Institute of Technology, 2025
발행사항  
Ann Arbor : ProQuest Dissertations & Theses, 2025
형태사항  
175 p
주기사항  
Source: Dissertations Abstracts International, Volume: 87-03, Section: B.
주기사항  
Advisor: Jackson, Jennifer.
학위논문주기  
Thesis (Ph.D.)--California Institute of Technology, 2025.
초록/해제  
요약In this thesis, I perform a thorough investigation of the electronic and elastic properties of the dense oxyhydroxide (Al,Fe)-phase H (Al 0.84Fe3+0.07Mg 0.02Si 0.06OOH). This phase represents a realistic composition in a solid solution which has been hypothesized to carry 'water', in the form of hydrogen, to the lowermost depths of Earth's mantle. Its propensity for water storage and elastic properties are affected by hydrogen bond symmetrization and a high-low spin crossover of Fe3+ atoms, respectively. In order to determine changes in hydrogen bonding environment, I use synchrotron infrared spectroscopy and Raman spectroscopy, which identify O-H vibrational modes in the crystal structure and changes in their frequencies with pressure. These vibrational modes indicate that (Al,Fe)-phase H likely stores additional hydrogen as defects and that hydrogen bonds are disordered at ambient pressure due to the substitution of cations of different valence states. I find that hydrogen atoms become dynamically disordered across sites at 10 GPa and conclude that hydrogen bond symmetrization in (Al,Fe)-phase H takes place at 35 GPa. I use powder X-ray diffraction to constrain the equation of state of this phase, providing fundamental constraints on its incompressibility and density at high pressures. I complement this equation of state with study of the electronic environment around the Fe atoms via nuclear resonant forward scattering in order to constrain the spin crossover of Fe3+ atoms between 48 and 63 GPa. I use nuclear resonant inelastic X-ray scattering measurements to determine the seismic wavespeeds of (Al,Fe)-phase H to 120 GPa, the base of the lowermost mantle. The measured seismic wavespeeds are incorporated into whole-rock models which suggest that (Al,Fe)-phase H contributes to seismic heterogeneity in the mid-mantle and that hydrous metabasalt containing (Al,Fe)-phase H could contribute to seismic anomalies associated with the edges of large, low, shear velocity provinces in the lowermost mantle as it heats during descent in the lowermost mantle. The combined results of this thesis elucidate a complete compression pathway during transport of a dense oxyhydroxide into the lower mantle in the context of changes in its electronic and elastic properties. I offer several observables which may be used to detect the presence of this phase in subducted metabasalt and comment on the implications for hydrogen storage in the deep Earth.
일반주제명  
Crystal structure
일반주제명  
Stainless steel
일반주제명  
Software packages
일반주제명  
Solid solutions
일반주제명  
Hydrogen bonds
일반주제명  
Single crystals
일반주제명  
Geological engineering
일반주제명  
Environmental science
키워드  
Elastic properties
키워드  
Raman spectroscopy
기타저자  
California Institute of Technology Geological and Planetary Sciences
기본자료저록  
Dissertations Abstracts International. 87-03B.
전자적 위치 및 접속  
로그인 후 원문을 볼 수 있습니다.

MARC

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■1001  ▼aStrozewski,  Benjamin  Thomas.
■24510▼aCrystal  Chemistry  and  Seismic  Wavespeeds  of  Dense  Oxyhydroxides:  Hydrogen  Transport  in  Earth's  Lower  Mantle
■260    ▼a[Sl]▼bCalifornia  Institute  of  Technology▼c2025
■260  1▼aAnn  Arbor▼bProQuest  Dissertations  &  Theses▼c2025
■300    ▼a175  p
■500    ▼aSource:  Dissertations  Abstracts  International,  Volume:  87-03,  Section:  B.
■500    ▼aAdvisor:  Jackson,  Jennifer.
■5021  ▼aThesis  (Ph.D.)--California  Institute  of  Technology,  2025.
■520    ▼aIn  this  thesis,  I  perform  a  thorough  investigation  of  the  electronic  and  elastic  properties  of  the  dense  oxyhydroxide  (Al,Fe)-phase  H  (Al  0.84Fe3+0.07Mg  0.02Si  0.06OOH).  This  phase  represents  a  realistic  composition  in  a  solid  solution  which  has  been  hypothesized  to  carry  'water',  in  the  form  of  hydrogen,  to  the  lowermost  depths  of  Earth's  mantle.  Its  propensity  for  water  storage  and  elastic  properties  are  affected  by  hydrogen  bond  symmetrization  and  a  high-low  spin  crossover  of  Fe3+  atoms,  respectively.  In  order  to  determine  changes  in  hydrogen  bonding  environment,  I  use  synchrotron  infrared  spectroscopy  and  Raman  spectroscopy,  which  identify  O-H  vibrational  modes  in  the  crystal  structure  and  changes  in  their  frequencies  with  pressure.  These  vibrational  modes  indicate  that  (Al,Fe)-phase  H  likely  stores  additional  hydrogen  as  defects  and  that  hydrogen  bonds  are  disordered  at  ambient  pressure  due  to  the  substitution  of  cations  of  different  valence  states.  I  find  that  hydrogen  atoms  become  dynamically  disordered  across  sites  at  10  GPa  and  conclude  that  hydrogen  bond  symmetrization  in  (Al,Fe)-phase  H  takes  place  at  35  GPa.  I  use  powder  X-ray  diffraction  to  constrain  the  equation  of  state  of  this  phase,  providing  fundamental  constraints  on  its  incompressibility  and  density  at  high  pressures.  I  complement  this  equation  of  state  with  study  of  the  electronic  environment  around  the  Fe  atoms  via  nuclear  resonant  forward  scattering  in  order  to  constrain  the  spin  crossover  of  Fe3+  atoms  between  48  and  63  GPa.  I  use  nuclear  resonant  inelastic  X-ray  scattering  measurements  to  determine  the  seismic  wavespeeds  of  (Al,Fe)-phase  H  to  120  GPa,  the  base  of  the  lowermost  mantle.  The  measured  seismic  wavespeeds  are  incorporated  into  whole-rock  models  which  suggest  that  (Al,Fe)-phase  H  contributes  to  seismic  heterogeneity  in  the  mid-mantle  and  that  hydrous  metabasalt  containing  (Al,Fe)-phase  H  could  contribute  to  seismic  anomalies  associated  with  the  edges  of  large,  low,  shear  velocity  provinces  in  the  lowermost  mantle  as  it  heats  during  descent  in  the  lowermost  mantle.  The  combined  results  of  this  thesis  elucidate  a  complete  compression  pathway  during  transport  of  a  dense  oxyhydroxide  into  the  lower  mantle  in  the  context  of  changes  in  its  electronic  and  elastic  properties.  I  offer  several  observables  which  may  be  used  to  detect  the  presence  of  this  phase  in  subducted  metabasalt  and  comment  on  the  implications  for  hydrogen  storage  in  the  deep  Earth.
■590    ▼aSchool  code:  0037.
■650  4▼aCrystal  structure
■650  4▼aStainless  steel
■650  4▼aSoftware  packages
■650  4▼aSolid  solutions
■650  4▼aHydrogen  bonds
■650  4▼aSingle  crystals
■650  4▼aGeological  engineering
■650  4▼aEnvironmental  science
■653    ▼aElastic  properties
■653    ▼aRaman  spectroscopy
■690    ▼a0466
■690    ▼a0768
■71020▼aCalifornia  Institute  of  Technology▼bGeological  and  Planetary  Sciences.
■7730  ▼tDissertations  Abstracts  International▼g87-03B.
■790    ▼a0037
■791    ▼aPh.D.
■792    ▼a2025
■793    ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17358777▼nKERIS▼z이  자료의  원문은  한국교육학술정보원에서  제공합니다.

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