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Investigations Into Structure and Properties of Atomically-Precise Transition Metal-Chalcogenide Clusters of Crte and Ligated Cr6te8(Pet3)6

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Investigations Into Structure and Properties of Atomically-Precise Transition Metal-Chalcogenide Clusters of Crte and Ligated Cr6te8(Pet3)6 Virginia Commonwealth University VCU Scholars Compass Theses and Dissertations Graduate School 2017 Investigations into structure and properties of atomically-precise transition metal-chalcogenide clusters of CrTe and ligated Cr6Te8(PEt3)6 Anthony F. Pedicini Virginia Commonwealth University Follow this and additional works at: https://scholarscompass.vcu.edu/etd Part of the Atomic, Molecular and Optical Physics Commons, Materials Chemistry Commons, and the Physical Chemistry Commons © The Author Downloaded from https://scholarscompass.vcu.edu/etd/4963 This Dissertation is brought to you for free and open access by the Graduate School at VCU Scholars Compass. It has been accepted for inclusion in Theses and Dissertations by an authorized administrator of VCU Scholars Compass. For more information, please contact [email protected]. © Copyright by Anthony F. Pedicini, 2017 All Rights Reserved Investigations into structure and properties of atomically- precise transition metal-chalcogenide clusters of CrTe and ligated Cr6Te8(PEt3)6 A Dissertation Submitted in Partial Fulfillment of the Requirements for the Degree of Doctor of Philosophy in Nanoscience & Nanotechnology at Virginia Commonwealth University by Anthony Filippo Pedicini B.S., Physics & B.S. Applied Mathematics Virginia Commonwealth University, 2011 M.S. Physics Virginia Commonwealth University, 2013 Director: Shiv N. Khanna, Ph.D. Chairman and Commonwealth Professor, Department of Physics Virginia Commonwealth University Richmond, Virginia July, 2017 Contents List of Figures ................................................................................................................................ iv Abstract ........................................................................................................................................ viii 1 Introduction ............................................................................................................................ 1 Novel Materials and Magic Clusters ................................................................................ 1 Transition Metal—Chalcogenides: Filled Electronic Valence in Periodic Systems ........ 7 Periodic Solids with Ligated Transition Metal—Chalcogenides ................................... 10 Motivation ........................................................................................................... 10 Superatomic Clusters and Their Solids ............................................................... 10 Alterations Upon Electronic Properties of Superatomic Clusters ....................... 14 Transition Metal-Chalcogenides at The Extremum: Chromium and Tellurium, Purpose of the Present Study ............................................................................................................. 15 Organization of This Thesis ........................................................................................... 18 2 Computational Approach ..................................................................................................... 20 Overview ........................................................................................................................ 20 Background .................................................................................................................... 20 The Electronic Problem & The Born—Oppenheimer Approximation ............... 20 Pauli ..................................................................................................................... 24 The Hartree—Fock Approximation .................................................................... 25 Density Functional Theory ............................................................................................. 27 Overview ............................................................................................................. 27 The Hohenberg—Kohn Theorems ...................................................................... 28 The Kohn—Sham Formulation ........................................................................... 31 Exchange—Correlation Functionals ................................................................... 34 Mulliken Population and Hirschfeld Charge Analyses ....................................... 35 Computational Methods ................................................................................................. 37 3 Atomically-Precise Binary CrxTey Clusters ......................................................................... 40 Overview & Two-Dimensional CrTe ............................................................................. 40 Pure Systems of Chromium, and Tellurium ................................................................... 42 Overview ............................................................................................................. 42 Tellurium Clusters ............................................................................................... 42 A Brief History of Small Chromium Clusters ..................................................... 43 ii Small Clusters of Pure Chromium ...................................................................... 47 Summary ............................................................................................................. 49 The CrxTey Clusters ........................................................................................................ 51 Overview ............................................................................................................. 51 Geometries & Structure ....................................................................................... 52 Summary ............................................................................................................. 64 CrxTey Series Properties ................................................................................................. 66 Hirshfeld Charge Density, Average Bond Distances, and “Malleability” of Chromium ......................................................................................................................... 68 Removal Energies & Fragmentation Pathways ................................................... 70 Summary ............................................................................................................. 74 CrxTey Electronic Properties .......................................................................................... 76 Overview ............................................................................................................. 76 Cr1Tey (y= 1 – 4) ................................................................................................. 77 Cr2Tey (y = 1 – 4) ................................................................................................ 81 Cr3Tey (y = 1 – 5) ................................................................................................ 85 Cr4Tey (y = 1 – 6) ................................................................................................ 87 Cr5Tey (y = 1 – 7) ................................................................................................ 96 Cr6Tey (y = 1 – 6) ................................................................................................ 99 Cr6Tey (y = 7, 8) ................................................................................................ 102 Discussion & Conclusions ........................................................................................... 108 7 4 Electronic Properties of Cr6Te8(PEt3)6 and Alteration Through Ligand Exchange ......... 110 Overview ...................................................................................................................... 110 Change of Basis Set...................................................................................................... 110 7 The Cr6Te8 Metal Core: QZ4P vs. TZ2P (Frozen Core) ............................................. 112 7 The Cr6Te8(PEt3)6 Cluster ........................................................................................... 116 7 Robustness of Cr6Te8(PEt3)6 ............................................................................ 121 Ligand Exchange .......................................................................................................... 123 Discussion & Conclusions ........................................................................................... 131 5 Summary & Future Directions ........................................................................................... 132 Crx Bond Lengths .............................................................................................. 135 CrxTey Bond Distances ...................................................................................... 137 References ................................................................................................................................... 147 iii List of Figures - - Figure 1-1. Etching reaction of aluminum anions (Al5 – Al24 ) with oxygen. ............................... 5 - Figure 1-2. Superatomic Orbitals and Al13 . ................................................................................... 5 Figure 1-3. Ligated Transition Metal-Chalcogenide Clusters and Their Assemblies. ................. 11 Figure 1-4. Magnetic behavior of the [Ni9Te6(PEt3)8][C60] cluster assembly. ............................. 12 Figure 1-5. Inverse magnetic susceptibility versus temperature measurements. .......................... 16 Figure
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