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

• Autor(a) principal: Bueno, Paulo Roberto [UNESP]
• Data de Publicação: 2021
• Outros Autores: Cruzeiro, Vinícius Wilian D., Roitberg, Adrian E., Feliciano, Gustavo T. [UNESP]
• Tipo de documento: Artigo
• Idioma: eng
• Título da fonte: Repositório Institucional da UNESP
• Texto Completo: http://dx.doi.org/10.1016/j.electacta.2021.138410; http://hdl.handle.net/11449/233136
• topic: Constant redox potential; Electrochemical capacitance; Electrochemical density-of-states; Electron transfer; Modified electrodes; Molecular dynamics; Redox-active interfaces

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.