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Valency-Controlled Multiphotochromism: Gated Switching and Photoswitchable Lewis Superacidity at Silicon.

Lennart Stoess¹, Valentin D Hannibal¹, Lutz Greb¹

¹Anorganisch-Chemisches Institut, Ruprechts-Karls Universität Heidelberg, Heidelberg, Germany.

Angewandte Chemie (International Ed. in English)

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Summary

Researchers developed a novel method using silicon valency to control multiphotochromism for molecular information storage. This breakthrough enables precise control over switching states and photoreactivity in advanced materials.

Keywords:

chemistry diarylethene frustrated lewis pair lewis acids and bases metathesis photochemistry salt metathesis reaction silicon valency

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Area of Science:

Materials Science
Organic Chemistry
Supramolecular Chemistry

Background:

Multiphotochromic systems offer potential for multistate molecular information storage.
Controlling switching-state distributions and interchromophore communication in these systems remains a challenge.

Purpose of the Study:

To demonstrate silicon valency as a molecular control element for gating multiphotochromism.
To explore the modulation of electronic coupling and photoreactivity through silicon coordination states.

Main Methods:

Synthesized two silicon-based diarylethene Lewis acids.
Investigated stepwise cyclization and interconversion between tetra- and pentacoordinate silicon states.
Utilized donor coordination to modulate photoreactivity and switching behavior.

Main Results:

Demonstrated stepwise twofold cyclization controlled by silicon valency.
Showcased how donor coordination enables selective monocyclization, wavelength-gated activation, or suppression of photoreactivity.
Achieved photoswitchable Lewis superacidity and access to distributions beyond statistical photochemical limits via dynamic bond metathesis.

Conclusions:

Silicon valency serves as a versatile molecular control element for multiphotochromic systems.
Established a new design principle for creating advanced molecular information storage and photoswitchable materials.
Opened avenues for developing materials with tunable Lewis acidity and controlled photoreactivity.