Designing and harnessing quantum properties are at the core of quantum information sciences, and open new frontiers in contemporary chemistry and physics. Examples include controlling vibronic coherence and molecular exciton in chemistry, or engineering metal-insulator transition and superconductivity in condensed matter physics. We aim to develop “quantum knobs” that tune charge, spin, and orbital degrees of freedom by controlling interfacial interactions amongst molecular-to-nanoscale material entities and map the resultant emergent quantum effects using spectro-microscopies under cryogenic and magnetic conditions. Particularly, we focus on designing and probing correlated electron systems, strongly-interacting exciton systems, and 2D magnetic systems. These systems can undergo quantum phase transitions and form ordered ground states due to changes in fundamental parameters at a Hamiltonian level rather than the temperature in the more familiar thermal phase transitions. The research in the Bai Lab is highly interdisciplinary, bridging the frontiers of quantum research in condensed matter physics and materials design in contemporary chemistry: this laboratory will pioneer new concepts, phenomena, and functions that are defined by quantum emergence.