Abstract
We show that polyoxometalates (POMs) are an excellent redoxactive acceptor on which to base high performance 2nd order non-linear optical (NLO) chromophores. This is demonstrated through three new organoimido-Lindqvist derivatives with HRS beta(0)-values exceeding those of any dipolar organic system with comparable donor, pi-system and absorption profile. Thus, organoimido POMs may provide a new generation of high performance, high transparency, and potentially redox-switchable NLO materials.