The density-of-States and equilibrium charge dynamics of redox-active switches

The density-of-states of redox-active molecular scale switches is the origin of a measurable pseudo-capacitance that possesses an intrinsic quantum capacitive nature with applications that spans nanoscale electronics, molecular sensing, field-effect devices and so on. In the present work, we demonst...

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Detalhes bibliográficos
Autores: Bueno, Paulo Roberto [UNESP], Cruzeiro, Vinícius Wilian D., Roitberg, Adrian E., Feliciano, Gustavo T. [UNESP]
Formato: artículo
Estado:Versión publicada
Fecha de publicación:2021
País:Brasil
Recursos:Universidade Estadual Paulista (UNESP)
Repositorio:Repositório Institucional da UNESP
Idioma:inglés
OAI Identifier:oai:repositorio.unesp.br:11449/233136
Acesso em linha:http://dx.doi.org/10.1016/j.electacta.2021.138410
http://hdl.handle.net/11449/233136
Access Level:acceso abierto
Palavra-chave:Constant redox potential
Electrochemical capacitance
Electrochemical density-of-states
Electron transfer
Modified electrodes
Molecular dynamics
Redox-active interfaces
Descrição
Resumo:The density-of-states of redox-active molecular scale switches is the origin of a measurable pseudo-capacitance that possesses an intrinsic quantum capacitive nature with applications that spans nanoscale electronics, molecular sensing, field-effect devices and so on. In the present work, we demonstrate that the equilibrium occupancy and shape of this density-of-states, which is associated with the energy state of the interface, can be accurately simulated using statistical mechanics, particularly by applying computational methods based on a constant (electro)chemical potential. This permits the simulation of experimental current-voltage responses and, consequently, the prediction and design of the properties of derived nanoscale devices.