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Establishing Design Principles for Complex Intermetallics: Chemical Pressures, Interface Nuclei, and Cluster Substitutions
Establishing Design Principles for Complex Intermetallics: Chemical Pressures, Interface Nuclei, and Cluster Substitutions
상세정보
- 자료유형
- 학위논문 서양
- 최종처리일시
- 20260202105651
- ISBN
- 9798270249489
- DDC
- 546
- 서명/저자
- Establishing Design Principles for Complex Intermetallics: Chemical Pressures, Interface Nuclei, and Cluster Substitutions
- 발행사항
- [Sl] : The University of Wisconsin - Madison, 2025
- 발행사항
- Ann Arbor : ProQuest Dissertations & Theses, 2025
- 형태사항
- 362 p
- 주기사항
- Source: Dissertations Abstracts International, Volume: 87-06, Section: B.
- 주기사항
- Advisor: Fredrickson, Daniel C.
- 학위논문주기
- Thesis (Ph.D.)--The University of Wisconsin - Madison, 2025.
- 초록/해제
- 요약Intermetallic compounds-solid-state materials formed from two or more metallic elements-exhibit remarkable structural diversity, often featuring complex assemblies that make predicting and interpreting their formations challenging. The work in this dissertation establishes and applies new strategies for understanding and designing such structures by focusing on the role of packing tensions, or chemical pressures, and their relief through shared geometric motifs.Chapter 2 begins with density functional theory (DFT) Chemical Pressure (CP) analysis of Mo₄Zr₉P; revealing how problematic polyhedral units, icosahedra and tricapped trigonal prisms, combine buffered by a framework of face-sharing octahedra. We then use data-mining techniques to find related intergrowth structures with octahedral networks, creating a family of structures that build upon the idea of buffering frameworks.Chapter 3 establishes the basis of the interface nucleus approach followed by Chapter 4 which builds upon the approach to create the interface nucleus complementarity (INC) metric - a chemical pressure-based metric to evaluate the likelihood of two parent structures intergrowing at a shared geometric interface, which we term the interface nucleus. Data-mining techniques are used to identify candidates with complementary CPs at their interface nuclei, these pairings serve as predictions for the formation of a complex intermetallic structure containing both parents structure motifs bridged by the interface nucleus. Chapter 4 demonstrates the predictive capability of this method through the synthesis of PrMg4Zn10, an intergrowth structure of the EuMg5 and MgZn2 types, as predicted.Exploration of the Pr-Mg-Zn system led to the discovery of another compound: PrMg1.6Zn5.4, presented in Chapter 5, which is found to be a massive cubic intermetallic structure containing over 2,000 atoms in the unit cell. Structural analysis describes PrMg1.6Zn5.4 as being a Laves phase and Heusler/BCC intergrowth. CP analysis highlights that over-compressed Pr environments in the Heusler phase and the preference for expanded coordination environments drive the incorporation of Laves phase units, validating a chemical pressure-based intergrowth model.Finally, Chapter 6 presents Mo4FeGa17.25-xGex (x ~ 2.1), a structural variant of the Ti2Ni type which has substituted select tetrahedra for singular atoms. Additionally, we find that the network of face-sharing octahedra can accommodate one additional Ga/Ge atoms per unit cell, creating a dumbbell instead of a single atom vertex on one of the octahedra. Chemical bonding analysis, electron counting, and chemical pressure analysis provide insight into why and how the structure manages to accommodate an additional atom.Overall, this dissertation establishes how intermetallic structures, despite their complexity, can be understood in terms of simple modular pieces and uses this approach along with DFT-Chemical Pressure methods to construct design principles, such as the interface nucleus concept and cluster substitution, for the formation of new intermetallics.
- 일반주제명
- Inorganic chemistry
- 일반주제명
- Chemistry
- 일반주제명
- Engineering
- 일반주제명
- Materials science
- 키워드
- Crystallography
- 키워드
- Intermetallics
- 키워드
- Metal alloys
- 기타저자
- The University of Wisconsin - Madison Chemistry
- 기본자료저록
- Dissertations Abstracts International. 87-06B.
- 전자적 위치 및 접속
- 로그인 후 원문을 볼 수 있습니다.
MARC
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■00520260202105651
■006m o d
■007cr#unu||||||||
■020 ▼a9798270249489
■035 ▼a(MiAaPQ)AAI32402610
■040 ▼aMiAaPQ▼cMiAaPQ
■0820 ▼a546
■1001 ▼aGressel, Danica G.
■24510▼aEstablishing Design Principles for Complex Intermetallics: Chemical Pressures, Interface Nuclei, and Cluster Substitutions
■260 ▼a[Sl]▼bThe University of Wisconsin - Madison▼c2025
■260 1▼aAnn Arbor▼bProQuest Dissertations & Theses▼c2025
■300 ▼a362 p
■500 ▼aSource: Dissertations Abstracts International, Volume: 87-06, Section: B.
■500 ▼aAdvisor: Fredrickson, Daniel C.
■5021 ▼aThesis (Ph.D.)--The University of Wisconsin - Madison, 2025.
■520 ▼aIntermetallic compounds-solid-state materials formed from two or more metallic elements-exhibit remarkable structural diversity, often featuring complex assemblies that make predicting and interpreting their formations challenging. The work in this dissertation establishes and applies new strategies for understanding and designing such structures by focusing on the role of packing tensions, or chemical pressures, and their relief through shared geometric motifs.Chapter 2 begins with density functional theory (DFT) Chemical Pressure (CP) analysis of Mo₄Zr₉P; revealing how problematic polyhedral units, icosahedra and tricapped trigonal prisms, combine buffered by a framework of face-sharing octahedra. We then use data-mining techniques to find related intergrowth structures with octahedral networks, creating a family of structures that build upon the idea of buffering frameworks.Chapter 3 establishes the basis of the interface nucleus approach followed by Chapter 4 which builds upon the approach to create the interface nucleus complementarity (INC) metric - a chemical pressure-based metric to evaluate the likelihood of two parent structures intergrowing at a shared geometric interface, which we term the interface nucleus. Data-mining techniques are used to identify candidates with complementary CPs at their interface nuclei, these pairings serve as predictions for the formation of a complex intermetallic structure containing both parents structure motifs bridged by the interface nucleus. Chapter 4 demonstrates the predictive capability of this method through the synthesis of PrMg4Zn10, an intergrowth structure of the EuMg5 and MgZn2 types, as predicted.Exploration of the Pr-Mg-Zn system led to the discovery of another compound: PrMg1.6Zn5.4, presented in Chapter 5, which is found to be a massive cubic intermetallic structure containing over 2,000 atoms in the unit cell. Structural analysis describes PrMg1.6Zn5.4 as being a Laves phase and Heusler/BCC intergrowth. CP analysis highlights that over-compressed Pr environments in the Heusler phase and the preference for expanded coordination environments drive the incorporation of Laves phase units, validating a chemical pressure-based intergrowth model.Finally, Chapter 6 presents Mo4FeGa17.25-xGex (x ~ 2.1), a structural variant of the Ti2Ni type which has substituted select tetrahedra for singular atoms. Additionally, we find that the network of face-sharing octahedra can accommodate one additional Ga/Ge atoms per unit cell, creating a dumbbell instead of a single atom vertex on one of the octahedra. Chemical bonding analysis, electron counting, and chemical pressure analysis provide insight into why and how the structure manages to accommodate an additional atom.Overall, this dissertation establishes how intermetallic structures, despite their complexity, can be understood in terms of simple modular pieces and uses this approach along with DFT-Chemical Pressure methods to construct design principles, such as the interface nucleus concept and cluster substitution, for the formation of new intermetallics.
■590 ▼aSchool code: 0262.
■650 4▼aInorganic chemistry
■650 4▼aChemistry
■650 4▼aEngineering
■650 4▼aMaterials science
■653 ▼aCrystallography
■653 ▼aIntermetallics
■653 ▼aMetal alloys
■653 ▼aSolid-state chemistry
■653 ▼aChemical Pressure
■690 ▼a0488
■690 ▼a0794
■690 ▼a0537
■690 ▼a0485
■71020▼aThe University of Wisconsin - Madison▼bChemistry.
■7730 ▼tDissertations Abstracts International▼g87-06B.
■790 ▼a0262
■791 ▼aPh.D.
■792 ▼a2025
■793 ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17361008▼nKERIS▼z이 자료의 원문은 한국교육학술정보원에서 제공합니다.
