Advanced precursor design for atomic layer deposition and chemical vapour deposition of gold metal

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Creator: 

Griffiths, Matthew Bertram Edward

Date: 

2020

Abstract: 

This thesis first outlines the current state-of-the-art of gold CVD and ALD precursors based on their precursor figures of merit (σ). Then, this thesis demonstrates the ability to control the structure of deposited nanoparticles by CVD, using a combination of thermogravimetric analysis (TGA), scanning electron microscopy (SEM), and X-ray photoelectron spectroscopy (XPS) to elucidate the mechanism of growth. With the help of expert collaborators, this thesis then summarizes multiple ALD studies on the first gold ALD precursor, (PMe3)AuMe3 including an assessment on its mechanism of ALD growth. In order to improve on the existing state-of-the-art of gold precursors, this thesis then describes a systematic assessment of gold(I) precursor design. Using a combination of TGA, differential scanning calorimetry (DSC), x-ray crystallography, and density functional theory (DFT) computational techniques, we attempt to delineate why certain ligands work well for gold(I) and we develop the precursor figure of merit (σ). With a knowledge of the design factors that make a good precursor from the standpoint of thermolysis, this thesis then describes a study where the rate of CVD of various gold(I) precursors is compared by in situ monitoring using a combination of quartz crystal microbalance (QCM) and quadrupole mass spectrometry (QMS). This study culminates in a new idea in the field of ALD: the rational design of a kinetically-limited ALD process. We then show that the kinetic implications of steric bulk that are ubiquitous in solution-phase synthetic chemistry can also be exploited in the fields of CVD and ALD. Finally, this thesis describes a study where a self-limiting gold(I) precursor is rationally designed. A family of these types of precursors is presented, and the self-limiting capability of these precursors is demonstrated using our in-situ monitoring methodology. We then show that highly conductive and high-purity gold thin films can be deposited with one precursor, and the films rival or best the current body of literature of gold films that are deposited by ALD.

Subject: 

Inorganic Chemistry
Physical Chemistry

Language: 

English

Publisher: 

Carleton University

Contributor: 

Co-author: 
Glenn Yap
Co-author: 
McLeod Jennifer
Co-author: 
Giorgi Javier
Co-author: 
Koponen Sara
Co-author: 
Eduardo Solano
Co-author: 
Christophe Detavernier
Co-author: 
Goran Bacic
Co-author: 
David Mandia
Co-author: 
Jason Masuda
Co-author: 
Tao Zeng
Co-author: 
Zachary Dubrawski

Thesis Degree Name: 

Doctor of Philosophy: 
Ph.D.

Thesis Degree Level: 

Doctoral

Thesis Degree Discipline: 

Chemistry

Parent Collection: 

Theses and Dissertations

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