Interfaces of Materials

Interfaces are critical to how materials perform — not only in application, where they are often the limiting factor in device performance, but also in processing and manufacturing. Our computational studies evaluate the stability and compatibility of materials interfaces, revealing how and why they degrade and guiding solutions, such as protective coatings, to stabilize them. Joule 2, 2016-2046 (2018)

• Electrochemical stability, including the degradation reactions and decomposition products that form under operating voltage. ACS Appl. Mater. Interfaces 7, 23685-23693 (2015); J. Mater. Chem. A 4, 3253-3266 (2016); Adv. Sci. 1600517 (2017)
• Interface stability and compatibility, essential for materials to work in a device — revealing the chemical reactions and degradation products that form when two materials are placed in contact. ACS Appl. Mater. Interfaces 7, 23685-23693 (2015); J. Mater. Chem. A 4, 3253-3266 (2016)
• Interface coatings, to further stabilize interfaces so materials can work in a device. Adv. Sci. 1600517 (2017); ACS Energy Lett. 4, 2444-2451 (2019); Energy Storage Mater. 41, 571-580 (2021)

These approaches are highly extendable to other interface problems across many applications.

Beyond thermodynamic stability, interfaces can also fail dynamically during device operation. We study the atomistic behavior of these buried interfaces with an atomic and time resolution that is very hard to access experimentally. This provides a unique approach for studying the complex dynamics of buried solid interfaces across a wide range of problems and applications.

• Dynamic mechanisms of electrochemical stripping and plating at Li/solid-electrolyte interfaces, and related phenomena such as diffusion, interfacial defects, failure mechanisms, and crystallization. Adv. Mater. 33, 2008081 (2021); Angew. Chem. Int. Ed. 60, 21494 (2021); Nat. Commun. 14, 2986 (2023)

Computation Prediction Confirmed

• Discovered a nanometer-thin amorphous Li layer at the Li/solid-electrolyte interface, and predicted that Li(110)/solid-electrolyte interfaces resist nanopore formation and enable higher cycling rates Angew. Chem. Int. Ed. 60, 21494 (2021) → confirmed experimentally Nat. Synth. 4, 552-561 (2025)
• Predicted the amorphous-to-BCC Li deposition pathway at solid-electrolyte interfaces Nat. Commun. 14, 2986 (2023) → confirmed experimentally Nat. Mater. 24, 581-588 (2025)
• Revealed the trends in cation moisture stability from systematic first-principles thermodynamic screening of hydrolysis reactions, guiding cation selection for air-stable Li/Na solid electrolytes Angew. Chem. Int. Ed. 59, 17472 (2020) → confirmed industrially: a chloride solid electrolyte using the predicted best-moisture-stability cation combination (In/Zn/Cd) was patented for improved air stability Chinese Patent CN121748511A

Related Talks

• Design Principles for Solid Electrolyte–Electrode Interfaces in All-Solid-State Li-Ion Batteries: Insight from First-Principles Computation
• Electrochemical Stabilities of Solid Electrolytes
• Computational Study on Interface Stability of All-Solid-State Li-ion Batteries
• Computational Design of Stable Coating for Solid-State Li-ion Batteries