<p>Li-ion batteries (LIBs) are currently pervasive across portable electronics and electric vehicles and are on the ascent for large-scale applications such as grid storage. However, commercial LIBs based on intercalation chemistries are inching toward their theoretical energy density limits. Consequently, the rapidly growing demands of energy storage have necessitated a recent renaissance in exploring battery systems beyond Li-ion chemistry. Next-generation batteries that utilize Li metal as the anode can improve the energy density and power density of LIBs. Despite the theoretical promise, the commercialization of metal-based batteries requires overcoming several hurdles, stemming from the unstable nature of Li in liquid electrolytes. Upon repeated charging, the metal anode undergoes unrestricted growth of dendrites, devolving to a thermal runaway in extreme circumstances. By replacing the organic liquid electrolyte with a non-flammable solid electrolyte, solid-state batteries (SSBs) can potentially provide enhanced safety attributes over liquid electrolyte cells. Upon pairing of solid electrolytes with a Li metal anode, such systems present the unique possibility of engineering batteries with high energy density and fast charging rates. However, there are a number of technical challenges and fundamental scientific advances necessary for SSBs to achieve reliable electrochemical performance. The formation of dendritic morphologies during charging and the loss of active area at the anode-electrolyte interface during discharging are two critical limitations that need to be addressed.</p> <p>In this thesis, the morphological stability of the Li metal anode is examined based on the mechanistic interaction of electrochemical reaction, ionic transport and surface self-diffusion, that is further dependent on aspects including the thermal field and electrolyte composition. The origin of electrochemical-mechanical instability and metal penetration due to heterogeneities in solid-state electrolytes such as grain boundaries will be analyzed. The phenomenon of contact loss at solid-solid interfaces due to the competing interaction between electrochemical dissolution and Li mechanics will be studied. Lastly, the mechanistic attributes governing the thermal stability of solid-solid interfaces in solid-state batteries will be examined. Overall, the dissertation will focus on understanding the fundamental mechanisms underlying the evolution of solid-liquid and solid-solid interfaces in energy storage and derive potential design guidelines toward achieving stable morphologies in metal-based batteries.</p>

Superconducting qubits are a promising technology for building a scalable quantum computer. An important architecture employed in the field is called Circuit Quantum Electrodynamics (circuit QED), where such qubits are combined with high quality microwave cavities to study the interaction between artificial atoms and single microwave photons. The ultra-strong coupling achieved in these systems allows for control and readout of the quantum state of qubits to perform quantum information processing. The work on circuit QED performed in this thesis consisted of realizing an experimental setup for qubit experiments in a new laboratory, investigating the coherence and decay of higher energy levels of superconducting transmon qubits and finally demonstrating a novel coaxial form of circuit QED. Designing and building a 3D circuit QED setup involved the following main accomplishments: producing high quality 3D cavities; designing and installing the cryogenic microwave setup as well as the room temperature amplification and data acquisition circuitry; successfully developing a recipe for the fabrication of Josephson junctions; controlling and measuring superconducting 3D transmon qubits at 10mK. Several qubits were fully characterised and have shown coherence times of several microseconds and relaxation times up to 25&mu;s. Superconducting qubits in fact possess higher energy levels that can provide significant computational advantages in quantum information applications. In experiments performed at MIT, preparation and control of the five lowest states of a transmon qubit was demonstrated, followed by an investigation of the phase coherence and decay dynamics of these higher energy levels. The decay was found to proceed mainly sequentially with relaxation times in excess of 20&mu;s for all transitions. A direct measurement of the charge dispersion of these levels was performed to explore their characteristics of dephasing. This experiment was also reproduced on a 3D transmon fabricated and measured in Oxford, where due to a higher effective qubit temperature a multi-level decay model including thermal excitations was developed to explain the observed relaxation dynamics. Finally, a coaxial transmon, which we name the coaxmon, is presented and measured with a coaxial LC readout resonator and input/output coupling ports placed inline along the third dimension. This novel coaxial circuit QED architecture holds great promise for developing a scalable planar grid of qubits to build a quantum computer.