Local Response Theory of Electrified Interfaces from Screened Effective Charges
Abstract
First-principles, electronic-structure simulations provide direct access to ground-state, global system properties. In the context of computational electrochemistry these are, e.g., bias-dependent energies, free energies, work functions, and capacitances. However, a comparably systematic local description of how these quantities respond to biasing via interfacial charging is still missing. Here, we introduce the screened electrochemical Born effective charge (SEBEC), a mixed total-energy derivative that measures the force response of an atomic degree of freedom to interfacial charging under electrochemical boundary conditions. SEBECs play the role for electrochemistry that Born effective charges play in the modern theory of polarization: they provide an unambiguous decomposition of global response and generate the same formal structures for structural relaxation, capacitance, and electrochemical Stark tuning that are familiar from solid-state response theory. The broader implication is a local response framework that brings electrochemical interfaces closer to the conceptual rigor long established for insulating solids.
Related
- Thermal Aging Behavior of PFA-Insulated Cables for Future Electrified Aircraft: From Material Evolution to Cable-Level Mechanical Response
- Ag/Ti Electrodes for Electrochemical Nitrate Reduction: Revealing Highly Effective Interfaces by In‐Situ Electrochemical Mass Spectrometry
- Phase-Controlled Efficient Nitrate-to-Dinitrogen Electroreduction on an α-Co/NC@CNT Electrified Membrane Platform
- Effective Elasticity of Anatase-Derived TiO2 Nanoclusters: Volume Normalization, Directional Response, and Structure–Property Correlations
- Adaptive Expansions of the Optimized Effective Potential in Physically Motivated Response Spaces
BibTeX
@misc{hormann2026local,
title = {{Local Response Theory of Electrified Interfaces from Screened Effective Charges}},
author = {Nicolas G. Hörmann and Nicolas Bergmann and Karsten Reuter},
howpublished = {arXiv},
year = {2026},
month = sep,
doi = {10.48550/arxiv.2609.13542},
eprint = {2609.13542},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2609.13542},
}
RIS
TY - UNPB
TI - Local Response Theory of Electrified Interfaces from Screened Effective Charges
AU - Nicolas G. Hörmann
AU - Nicolas Bergmann
AU - Karsten Reuter
PY - 2026
DA - 2026/09/11
PB - arXiv
DO - 10.48550/arxiv.2609.13542
UR - https://arxiv.org/abs/2609.13542
AB - First-principles, electronic-structure simulations provide direct access to ground-state, global system properties. In the context of computational electrochemistry these are, e.g., bias-dependent energies, free energies, work functions, and capacitances. However, a comparably systematic local description of how these quantities respond to biasing via interfacial charging is still missing. Here, we introduce the screened electrochemical Born effective charge (SEBEC), a mixed total-energy derivative that measures the force response of an atomic degree of freedom to interfacial charging under electrochemical boundary conditions. SEBECs play the role for electrochemistry that Born effective charges play in the modern theory of polarization: they provide an unambiguous decomposition of global response and generate the same formal structures for structural relaxation, capacitance, and electrochemical Stark tuning that are familiar from solid-state response theory. The broader implication is a local response framework that brings electrochemical interfaces closer to the conceptual rigor long established for insulating solids.
ER -