Our group investigates the fundamental photophysical and electrochemical processes that govern the performance of functional semiconductors. By combining thin-film synthesis, photoelectrochemistry, and advanced spectroscopy, we aim to uncover how charge carriers interact with the lattice and interfaces, and how these interactions determine the efficiency of light-driven reactions.
Transition metal nitrides (TMNs) offer stronger bonding covalency than oxides, leading to improved charge transport. Yet, semiconducting TMNs remain largely unexplored due to the difficulty of material synthesis. Using reactive sputter deposition, our group creates a growth environment rich in highly reactive nitrogen species, enabling the formation of metastable nitride thin films that are otherwise challenging to obtain. For example, we have synthesized Ta3N5 films derived from metastable Ta2N3 precursors. These films naturally incorporate sub-nitride impurities near the substrate interface, which facilitate electron transport and allow a 100 nm Ta3N5 photoanode to outperform much thicker oxide-derived counterparts. This approach enhances photoelectrochemical performance while reducing tantalum usage, opening a scalable route toward efficient nitride-based solar energy conversion.
Originally developed for water splitting and solar fuel production, photoelectrochemical methods are now emerging as powerful tools for organic synthesis. Photoelectrodes can not only replace traditional organometallic catalysts but also offer distinct reaction selectivity under light-driven conditions. Our group investigates the electron transfer kinetics and surface reaction mechanism that govern these processes, aiming to reveal how photoexcited carriers mediate selective chemical transformations and to expand the scope of light-driven synthetic chemistry.
Ternary oxides are promising materials for photoelectrochemical energy conversion because of their chemical robustness, low fabrication cost, and tunable optoelectronic properties. However, understanding their intrinsic charge transport—particularly polaronic conduction—is often hindered by the grain boundaries present in conventional polycrystalline thin films. Our group has developed a chemical solution epitaxy approach that enables the growth of highly oriented, epitaxial thin films of complex metal oxides using a cost-effective, scalable process. This method minimizes grain boundary density and provides well-defined crystallographic control, allowing us to probe anisotropic charge transport and carrier dynamics with unprecedented clarity.
In transition metal oxides, the ionic nature of chemical bonding allows electrons to localize on metal cations, distorting the surrounding lattice and forming small polarons. These self-trapped charge carriers play a crucial role in determining charge transport. We employ transient absorption spectroscopy to monitor the ultrafast formation and relaxation of polaronic states, and resonant inelastic X-ray scattering (RIXS) to directly observe phonon energy shifts associated with electron-phonon coupling. Together, these techniques provide deep insight into how lattice interactions dictate carrier mobility.
Halide perovskites (ABX3) combine strong light absorption with solution-processable synthesis, making them ideal for optoelectronic applications. Our research explores how intentionally introduced defects influence their electronic properties and phase stability. Upon optical excitation, excitons can locally distort the lattice, forming self-trapped exciton (STE) states. By studying the interplay between electronic excitations and lattice dynamics, we aim to uncover the mechanisms that govern performance and stability, guiding the design of next-generation perovskite-based devices.