First-Principles Nanocapacitor Simulations of the Optical Dielectric Constant in Water Ice
Year: 2025
Type: article
Abstract: We introduce a combined density functional theory and nonequilibrium Green's function framework to compute the capacitance of nanocapacitors and directly extract the dielectric response of a subnanometer dielectric under bias. We identify that at the nanoscale conventional capacitance evaluations based on stored charge per unit voltage suffer from an ill-posed partitioning of electrode and dielectric charge. This partitioning directly impacts the geometric definition of capacitance through the capacitor width, which in turn makes the evaluation of dielectric response uncertain. This ambiguous separation further induces spurious interfacial polarizability when analyzed via maximally localized Wannier functions. Focusing on crystalline ice, we develop a robust charge-separation protocol that yields unique capacitance-derived polarizability and dielectric constants, unequivocally demonstrating that confinement alters neither ice's intrinsic electronic response nor its insensitivity to proton order. Our results lay the groundwork for rigorous interpretation of capacitor measurements in low-dimensional dielectric materials.
Source: Physical Review Letters
DOI: 10.1103/8sjg-ybfw
Authors: Anthony Mannino, Graciele M. Arvelos, Kedarsh Kaushik, Emilio Artacho, Pablo Ordejon, Alexandre R. Rocha, Luana S. Pedroza, Marivi Fernández-Serra
Language: English
Subfield: Atomic and Molecular Physics, and Optics
Field: Physics and Astronomy
Domain: Physical Sciences
Open Access status: green
Funders: National Science Foundation, Empire State Development's Division of Science, Technology and Innovation, Institut Català de Nanociència i Nanotecnologia, European Commission, Fundação de Amparo à Pesquisa do Estado de São Paulo, Coordenação de Aperfeiçoamento de Pessoal de Nível Superior, Conselho Nacional de Desenvolvimento Científico e Tecnológico, Ministerio de Ciencia e Innovación, Centro Nacional de Processamento de Alto Desempenho em São Paulo, Stony Brook University, Engineering and Physical Sciences Research Council, Agencia Estatal de Investigación, Division of Materials Research, H2020 European Research Council
Awards: Collaborative Research: Optimally designed exchange-correlation functionals for solids using machine learning, Theoretical Condensed Matter Cambridge - Critical Mass Grant, G2344088346, G2711492644, G2854585307, G5027037093, MRI: Acquisition of SeaWulf - A Reconfigurable Computer System for Research and Education, G513388344, G5251241609, G548787232, G5683704876, G6605876378, G6866058724, G6901580522, MRI: Acquisition of a computer system for Research and Education – Seawulf, Atomistic simulations of electrochemistry
OpenAlex ID: W4417220146