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Tetramethyleneethane Diradical, and Arsenic and Selenium Oxides Rashel Makane Mokambe Sumpter

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Tetramethyleneethane Diradical, and Arsenic and Selenium Oxides Rashel Makane Mokambe Sumpter University of North Dakota UND Scholarly Commons Theses and Dissertations Theses, Dissertations, and Senior Projects January 2012 Theoretical Studies Of The Ground And Low- Lying Excited States Of [3,3']bidiazirinylidene(c2n4), Tetramethyleneethane Diradical, And Arsenic And Selenium Oxides Rashel Makane Mokambe Sumpter Follow this and additional works at: https://commons.und.edu/theses Recommended Citation Mokambe Sumpter, Rashel Makane, "Theoretical Studies Of The Ground And Low-Lying Excited States Of [3,3']bidiazirinylidene(c2n4), Tetramethyleneethane Diradical, And Arsenic And Selenium Oxides" (2012). Theses and Dissertations. 1301. https://commons.und.edu/theses/1301 This Dissertation is brought to you for free and open access by the Theses, Dissertations, and Senior Projects at UND Scholarly Commons. It has been accepted for inclusion in Theses and Dissertations by an authorized administrator of UND Scholarly Commons. For more information, please contact [email protected]. THEORETICAL STUDIES OF THE GROUND AND LOW-LYING EXCITED STATES OF [3,3’]BIDIAZIRINYLIDENE(C2N4), TETRAMETHYLENEETHANE DIRADICAL, AND ARSENIC AND SELENIUM OXIDES by Rashel Makane Mokambe Sumpter Bachelor of Science, University of Lagos, 1988 Master of Science, University of Lagos, 1989 A Dissertation Submitted to the Graduate Faculty of the University of North Dakota In partial fulfillment of the requirements for the degree of Doctor of Philosophy Grand Forks, North Dakota August 2012 This dissertation, submitted by Rashel Makane Mokambe Sumpter in partial fulfillment of the requirements for the Degree of Doctor of Philosophy from the University of North Dakota, has been read by the Faculty Advisory Committee under whom the work has been done and is hereby approved. Dr. Mark R Hoffmann (Chairperson) Dr. Harmon Abrahamson Dr. Lothar Stahl Dr. Kathryn A Thomasson Dr. Ju Kim This dissertation meets the standards for appearance, conforms to the style and format requirements of the Graduate School of the University of North Dakota, and is hereby approved. Dr. Wayne Swisher Dean of the Graduate School Date ii PERMISSION Title: Theoretical Studies of The Ground And Low-Lying Excited States of [3,3’]Bidiazirinylidene(C2N4), Tetramethyleneethane Diradical, And Arsenic And Selenium Oxides Department: Chemistry Degree: Doctor of Philosophy In presenting this dissertation in partial fulfillment of the requirements for a graduate degree from the University of North Dakota, I agree that the library of this University shall make it freely available for inspection. I further agree that the permission for extensive copying for scholarly purpose may be granted by the professor who supervised my dissertation work or, in his absence, by the chairperson of the department or the dean of the Graduate School. It is understood that any copying or publication or other use of this dissertation or part thereof for financial gain shall not be allowed without my written permission. It is also understood that due recognition shall be given to me and to the University of North Dakota in any scholarly use which may be made of any material in my dissertation. Signature Rashel Makane Mokambe Sumpter Date 06-21-12 iii TABLE OF CONTENTS Page LIST OF FIGURES ......................................................................................................... viii LIST OF TABLES .............................................................................................................. x ABBREVIATIONS ......................................................................................................... xiii ACKNOWLEDGEMENTS ............................................................................................. xvi ABSTRACT ................................................................................................................... xviii CHAPTER I. INTRODUCTION .............................................................................................. 1 [3,3′]Bidiazirinylidene (C2N4) ........................................................................ 3 Tetramethyleneethane diradical (C6H8) .......................................................... 5 Arsenic oxides ................................................................................................. 8 Selenium oxides ............................................................................................ 10 Organization and Structure ........................................................................... 13 II. METHODS OF MOLECULAR ELECTRONIC STRUCTURE THEORY .... 15 The Hartree-Fock Approximation ................................................................. 16 Møller-Plesset Perturbation (MP2) Theory .................................................. 22 Coupled Cluster Theory (CC) ....................................................................... 26 Multiconfigurational Self-Consistent Field (MCSCF) Theory ..................... 30 Macroconfiguration Approach ...................................................................... 33 iv Second-Order Generalized Van Vleck Perturbation Theory (GVVPT2) ..... 36 Density Functional Theory (DFT) ................................................................ 40 III. GROUND AND LOW-LYING EXCITED ELECTRONIC STATES OF [3,3’] BIDIAZIRINYLIDENE (C2N4) in D2h symmetry ............................................ 46 Introduction ................................................................................................... 46 Computational details ................................................................................... 49 Electronic and molecular structures .............................................................. 54 Summary ....................................................................................................... 68 GROUND AND LOW-LYING EXCITED ELECTRONIC STATES OF [3,3’] BIDIAZIRINYLIDENE (C2N4) in C2v symmetry ............................................ 71 Introduction ................................................................................................... 71 Computational details ................................................................................... 73 Electronic and molecular structures .............................................................. 78 Summary ....................................................................................................... 93 IV. MULTIREFERENCE PERTURBATION THEORY STUDIES OF THE LOWEST SINGLET AND TRIPLET ELECTRONIC STATES OF TETRAMETHYLENEETHANE DIRADICAL .............................................. 95 Introduction ................................................................................................... 95 Computational details ................................................................................... 97 Summary ..................................................................................................... 108 V. THEORETICAL STUDY OF ARSENIC OXIDES ....................................... 110 Introduction ................................................................................................. 110 Computational details ................................................................................. 112 Results and discussion ................................................................................ 113 v Monomeric Arsenic oxides ..................................................................... 113 Arsenic monoxide (AsO) .................................................................... 113 Arsenic dioxide (AsO2) ....................................................................... 115 Arsenic trioxide (AsO3) ...................................................................... 118 Reaction enthalpies of the oxidation of monomeric aoxides .............. 119 Dimeric Arsenic Oxides .......................................................................... 120 Diarsenic trioxides (As2O3) ................................................................ 121 Diarsenic pentaoxide (As2O5) ............................................................. 125 Reaction energies of dimeric arsenic oxides ....................................... 127 Summary ..................................................................................................... 135 VI. THEORETICAL STUDY OF SELENIUM OXIDES .................................... 137 Introduction ................................................................................................. 137 Computational details ................................................................................. 139 Results and discussion ................................................................................ 140 Monomeric selenium oxides ................................................................... 140 Selenium monoxide (SeO) .................................................................. 140 Selenium dioxide (SeO2) .................................................................... 141 Selenium trioxide (SeO3) .................................................................... 143 Reaction enthalpies for the oxidation of monoxides and dioxides of selenium .............................................................................................. 145 Dimeric Selenium Oxide......................................................................... 146 Diselenium trioxide (Se2O3) ............................................................... 147 Diselenium pentaoxide (Se2O5) .........................................................
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