Electronic structure and charge transfer at heterogeneous functional interfaces in energy conversion devices

Area of Science:

• Materials Science
• Physical Chemistry
• Renewable Energy

Background:

• Interfaces between photoactive materials and electrodes are critical for photovoltaic and photoelectrochemical cell performance.
• These interfaces govern band alignment, charge separation, and recombination, influencing device efficiency and stability.

Purpose of the Study:

• To provide an atomistic perspective on functional interfaces in dye-sensitized solar cells (DSSCs), dye-sensitized photoelectrochemical cells (DSPECs), and perovskite solar cells (PSCs).
• To emphasize the role of interfacial electronic structure in charge-transfer processes and device performance.
• To outline rational design strategies for optimizing heterogeneous functional interfaces in solar energy conversion.

Main Methods:

• Synergistic use of photoelectron spectroscopy and first-principles simulations (DFT, hybrid functionals, beyond-DFT).
• Quantification of band offsets, interface dipoles, defect states, and electronic coupling.
• Modeling of charge-transfer dynamics using projection operator diabatization and non-adiabatic methods.

Main Results:

• Detailed atomistic insights into interfacial electronic structure.
• Quantification of key interfacial parameters influencing charge transfer.
• Demonstration of the synergy between experimental spectroscopy and theoretical simulations.

Conclusions:

• Interfacial electronic structure is paramount for optimizing solar cell performance.
• A combined experimental and computational approach enables rational design of advanced solar energy materials.
• This review provides a framework for developing next-generation photovoltaic and photoelectrochemical technologies.