In this talk, I will discuss our group's efforts toward the development of solid-state organic laser candidate emitting compounds. We employ automated systems to synthesize and characterize them, as well as make devices out of them. This is part of a large international collaboration that can be thought of as a delocalized laboratory.

Small molecules containing refractory elements such as metals and phosphorus hold important clues to understanding astrochemistry and the connection between gas-phase matter and solid-state constituents of the interstellar medium. They also are extremely relevant for the origin of life and the delivery of the biogenic elements to planet surfaces. Studies of these types of molecules in interstellar space have clearly been driven by laboratory spectroscopy. For almost three decades, the Ziurys lab has been conducting measurements of rotational spectra of highly reactive metal and phosphorus-bearing species, and subsequently searching for these molecules in the interstellar medium with radio telescopes. These studies have led to the interstellar detection of exotic metal-bearing radicals such as FeCN and VO, as well as new phosphorus compounds such as CCP and SiP. Critical to this endeavor has been the development of unusual synthetic methods to create these unstable molecules, and the challenge of unraveling spectra of states with high spin and orbital angular momenta. Molecules of recent interest include metal dicarbide species, for example, TiC₂. An overview of the laboratory spectroscopy work will be presented, and their implications in unraveling the chemistry between the stars.

For roughly a century, spectroscopy has been our window into the molecular domain. It has served as a benchmark for the development of new theoretical methods in quantum chemistry, which in turn have aided the assignment and characterization of molecular spectra. The advent of quantum computing is no exception. Quantum computers have the potential to greatly increase the scale and accuracy of simulated molecular systems. However, current "digital" quantum computers will remain limited in size and number of operations in the near future due to environmental noise. Conversely, analog quantum computers may be used to simulate realistic molecular systems with current technology. They consist of controllable quantum devices with a system-specific mapping onto a quantum system of interest, such as a molecule. I will present our recent work on the development of an analog quantum toolkit for the simulation of vibronic coupling Hamiltonians, including the prediction of vibronic spectra. I will show the theoretical capabilities and limits of our approach, and show proof-of-principle experimental results from collaborators. Finally, I will discuss what is next in the exciting world of analog quantum simulation.

This talk will describe the application of sum frequency generation (SFG) vibrational spectroscopy to understand the relationship between interfacial charge transfer, solvation structure, and surface reactivity at electrode/electrolyte interfaces. Observing interfacial solvation structure under conditions relevant for electrocatalysis represents a major challenge for bridging surface science and electrochemistry. Employing plasmon-enhanced SFG, it is possible to detect the very low steady state surface coverage of CO produced on gold during electrochemical reduction of CO₂ and to use this as a Stark reporter of interfacial solvation structure. Because CO₂ reduction is extremely sensitive to catalyst surface structure, it is necessary to differentiate between CO adsorbed to inactive (i.e., spectator) sites compared to CO produced directly at active surface sites. Separating signals from these species, we show that electrolyte cations retain their entire solvation shell upon adsorption to inactive sites, while active sites retain only a single water layer between the gold surface and the adsorbed cation. We also measure the total interfacial electric field as a function of electrolyte cation and show that this field can be separated into two independent contributions from the electrochemical double layer (Stern field) and from the polar solvation environment (Onsager field). Although both contributions to the electric field depend strongly on the identity of the alkali cation, correlating SFG spectra with reaction kinetics reveals that it is actually the solvation-mediated Onsager field that governs the cation-specific chemical reactivity at the electrode/electrolyte interface. These findings highlight the importance of understanding and controlling interfacial solvation in electrochemical systems, a challenge that will require ongoing collaboration between experiment and theory.