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Electron Dynamics in Molecular Qubit...

Mirzoyan, Ruben,

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Electron Dynamics in Molecular Qubits and Catalytic Films /

Record Type:	Electronic resources : Monograph/item
Title/Author:	Electron Dynamics in Molecular Qubits and Catalytic Films // Ruben Mirzoyan.
Author:	Mirzoyan, Ruben,
Description:	1 electronic resource (315 pages)
Notes:	Source: Dissertations Abstracts International, Volume: 86-06, Section: B.
Contained By:	Dissertations Abstracts International86-06B.
Subject:	Electrons. -
Online resource:	https://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=31771493
ISBN:	9798346792871

Electron Dynamics in Molecular Qubits and Catalytic Films /
Mirzoyan, Ruben,

Electron Dynamics in Molecular Qubits and Catalytic Films /Ruben Mirzoyan. - 1 electronic resource (315 pages)

Source: Dissertations Abstracts International, Volume: 86-06, Section: B.

This thesis investigates two major themes within the realm of molecular and materials chemistry: spin-phonon coupling in molecular qubits and electrocatalysis in cobalt oxyhydroxide thin films. Across four chapters and one appendix, this work explores the intricacies of electron spin relaxation mechanisms within transition metal complexes and the catalytic properties of cobalt oxyhydroxide films through an array of spectroscopies and magnetic field effects.Chapter 1 reviews recent advancements in molecular quantum information science, emphasizing the decoherence mechanisms in transition metal complex-based qubits. This chapter categorizes the different regimes of decoherence-spin-spin, motional, and spin-phonon-and discusses the contributions of intramolecular vibrations to the spin-phonon decoherence regime using a dynamic ligand field model. This provides a framework for designing molecular qubits tailored to various operational environments.Chapter 2, Part 1 introduces a general ligand field theory model to quantify the spin-phonon coupling in S = ½ transition metal complexes. The model evaluates the influence of spin-orbit coupling, ligand field energy gradients, and covalency dynamics on spin-phonon interactions. Through DFT and TDDFT calculations, the chapter correlates theoretical models with experimental quantum coherence properties in Cu(II) and V(IV)-based molecular qubits, offering a benchmark for future qubit design. Chapter 2, Part 2 enhances the model from Part 1 by adding temperature dependence and utilizing group theory selection rules. The model accurately forecasts relative experimental T1 trends and identifies vibrational modes responsible for decoherence, enhancing understanding of room temperature coherence in these systems.Chapter 3 employs steady-state and time-resolved spectroelectrochemical techniques to study the photoexcited states of amorphous cobalt-phosphate (CoPi) and cobalt-borate (CoBi) oxyhydroxide films used in oxygen evolution catalysis. The analysis reveals key insights into the dynamic defect states and electron transport mechanisms, differentiating the electronic properties and behaviors of CoPi and CoBi despite their structural similarities.Chapter 4 oversees the development of a unique magneto-electrochemical setup and demonstrates a 30-40% increase in electrocatalytic current for water splitting under a 1.5 T magnetic field, independently of the cobalt-phosphate oxyhydroxide catalyst. This enhancement, attributed to the facilitated removal of O2 gas bubbles, underscores the potential synergistic effects of magnetic fields in electrocatalysis and highlights the need for further investigation into such interactions.Appendix A addresses the ongoing debate on the vibrational modes contributing most to electron spin relaxation in S = ½ transition metal complexes. It uses Raman spectroscopy to experimentally identify vibrational energies and symmetries, providing critical experimental data for refining spinvibrational coupling models.

English

ISBN: 9798346792871Subjects--Topical Terms:

516581
Electrons.

Electron Dynamics in Molecular Qubits and Catalytic Films /
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520 $a This thesis investigates two major themes within the realm of molecular and materials chemistry: spin-phonon coupling in molecular qubits and electrocatalysis in cobalt oxyhydroxide thin films. Across four chapters and one appendix, this work explores the intricacies of electron spin relaxation mechanisms within transition metal complexes and the catalytic properties of cobalt oxyhydroxide films through an array of spectroscopies and magnetic field effects.Chapter 1 reviews recent advancements in molecular quantum information science, emphasizing the decoherence mechanisms in transition metal complex-based qubits. This chapter categorizes the different regimes of decoherence-spin-spin, motional, and spin-phonon-and discusses the contributions of intramolecular vibrations to the spin-phonon decoherence regime using a dynamic ligand field model. This provides a framework for designing molecular qubits tailored to various operational environments.Chapter 2, Part 1 introduces a general ligand field theory model to quantify the spin-phonon coupling in S = ½ transition metal complexes. The model evaluates the influence of spin-orbit coupling, ligand field energy gradients, and covalency dynamics on spin-phonon interactions. Through DFT and TDDFT calculations, the chapter correlates theoretical models with experimental quantum coherence properties in Cu(II) and V(IV)-based molecular qubits, offering a benchmark for future qubit design. Chapter 2, Part 2 enhances the model from Part 1 by adding temperature dependence and utilizing group theory selection rules. The model accurately forecasts relative experimental T1 trends and identifies vibrational modes responsible for decoherence, enhancing understanding of room temperature coherence in these systems.Chapter 3 employs steady-state and time-resolved spectroelectrochemical techniques to study the photoexcited states of amorphous cobalt-phosphate (CoPi) and cobalt-borate (CoBi) oxyhydroxide films used in oxygen evolution catalysis. The analysis reveals key insights into the dynamic defect states and electron transport mechanisms, differentiating the electronic properties and behaviors of CoPi and CoBi despite their structural similarities.Chapter 4 oversees the development of a unique magneto-electrochemical setup and demonstrates a 30-40% increase in electrocatalytic current for water splitting under a 1.5 T magnetic field, independently of the cobalt-phosphate oxyhydroxide catalyst. This enhancement, attributed to the facilitated removal of O2 gas bubbles, underscores the potential synergistic effects of magnetic fields in electrocatalysis and highlights the need for further investigation into such interactions.Appendix A addresses the ongoing debate on the vibrational modes contributing most to electron spin relaxation in S = ½ transition metal complexes. It uses Raman spectroscopy to experimentally identify vibrational energies and symmetries, providing critical experimental data for refining spinvibrational coupling models.
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