2022
DOI: 10.1002/anie.202215537
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Electrochemically‐Switched 2nd Order Non‐Linear Optical Response in an Arylimido‐Polyoxometalate with High Contrast and Cyclability

Abstract: Electrochemically switched 2 nd order non-linear optical responses have been demonstrated for the first time in polyoxometalates (POMs), with an arylimido-derivative showing a leading combination of high on/off contrast (94%), high visible transparency, and cyclability. Spectro-electrochemical and TD-DFT studies indicate that the switch-off results from weakened charge transfer (CT) character of the electronic transitions in the reduced state. This represents the first study of an imido-POM reduced state, and … Show more

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Cited by 4 publications
(2 citation statements)
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“…S3, ESI†) show [Mo 6 O 18 NR] 2−/3− reductions for all three compounds that are highly reversible on the CV timescale, however, with no steric bulk around the imido group the reduced states are not stable enough for investigation of switched properties. 9,14 The reduction potentials E 1/2 trend more negative, in line with the trend in calculated NPA charges (Fig. S5, ESI†), as the strength of communication between –NPh 2 donor and POM acceptor increases across the bridge from diphenylacetylene 2 , to stilbene 3 and phenyl 1 .…”
supporting
confidence: 72%
See 1 more Smart Citation
“…S3, ESI†) show [Mo 6 O 18 NR] 2−/3− reductions for all three compounds that are highly reversible on the CV timescale, however, with no steric bulk around the imido group the reduced states are not stable enough for investigation of switched properties. 9,14 The reduction potentials E 1/2 trend more negative, in line with the trend in calculated NPA charges (Fig. S5, ESI†), as the strength of communication between –NPh 2 donor and POM acceptor increases across the bridge from diphenylacetylene 2 , to stilbene 3 and phenyl 1 .…”
supporting
confidence: 72%
“…They can also have significant 3rd order properties, 8 and recently demonstrated reversible, redox switched NLO responses. 9 Thus, such POMophores have the potential to yield high-activity, switchable NLO materials while avoiding problems for efficiency and stability that result from reabsorption of second harmonic (SH) light.…”
mentioning
confidence: 99%