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Atomic Layer Deposition of Vanadium Dioxide and a Temperature-dependent Optical Model

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Published on: May 23, 2018

Revisiting the Robin-Day Classification through Switchable Electronic States in Multimetallic Vanadium Oxides.

Nghia Le¹, Pere Miró¹

¹Department of Chemistry, University of Iowa, Iowa City, Iowa 52242, United States.

Journal of the American Chemical Society

|April 14, 2026

Summary

Redox topology modulation in polyoxovanadate clusters controls electronic states. Ligand tuning and light can switch between localized and delocalized redox states, enabling molecular switch design.

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Area of Science:

Inorganic Chemistry
Materials Science
Computational Chemistry

Background:

Polyoxovanadate-alkoxide clusters are redox-active and electronically tunable.
The oxygen-deficient [(V6O5)(μ6-O)(μ2-OCH3)12] cluster serves as a model for studying redox state localization and delocalization.

Purpose of the Study:

To introduce and investigate redox topology modulation as a mechanism controlling electromer stability in polyoxovanadate clusters.
To explore the impact of ligand coordination and electronic structure on redox behavior and molecular switching capabilities.

Main Methods:

Computational studies, including density functional theory (DFT) and time-dependent DFT (TD-DFT), were employed.
Analysis of redox topology, ligand-field tuning, and photoinduced intervalence charge transfer was performed.

Main Results:

The noncoordinated cluster exhibits a localized, hybrid Robin-Day class I/II ground state with a V(III) center.
Ligand coordination of strong donors destabilizes the localized topology, favoring an all-V(IV) electromer ground state.
Photoexcitation of V(IV) species induces charge transfer, leading to a valence-trapped class II excited state.

Conclusions:

Redox topology modulation is a viable design principle for creating molecular switches tunable by chemical stimuli or light.
The Robin-Day classification may require revision for multicenter systems, with valence behavior being excitation-specific.