Journal
CHEMISTRY OF MATERIALS
Volume 25, Issue 5, Pages 808-814Publisher
AMER CHEMICAL SOC
DOI: 10.1021/cm400147p
Keywords
valence tautomers; intramolecular electron-transfer; optical spectroscopy; solvatochromism; Mossbauer spectroscopy
Funding
- DGI [CTQ2010-19501]
- Networking Research Center on Bioengineering, Biomaterials, and Nanomedicine (CIBER-BBN)
- Generalitat de Catalunya [2009SGR00516]
- Consejo Superior de Investigaciones Cientificas (CSIC)
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Bistability of valence tautomeric donor-acceptor dyads formed by covalently linking a ferrocene-based electron-donor and the perchlorotriphenylmethyl radical, as the electron-acceptor, is tuned via a chemical modification of the ferrocene group. Specifically, the methylation of the ferrocene unit increases the strength of the donor group stabilizing the zwitterionic state in polar solvents and leading to an intriguing coexistence of neutral and zwitterionic species in solvents of intermediate polarity. Bistability in the crystalline phase is demonstrated by temperature dependent Mossbauer spectra. This complex and interesting behavior is quantitatively rationalized in the framework of a bottom-up modeling strategy. Optical spectra in solution are first analyzed to extract and parametrize an effective two-state molecular model, which is then adopted to rationalize the observed bistability in the solid state as due to cooperative electrostatic interchromophore interactions.
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