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Summary The ingenious construction of electron donor-acceptor (D-A) systems has been proven to be the major trend for advanced performance optoelectronic materials. However, the related development is undiversified and has become stereotyped in recent years, and the explorations of innovative architecture with both prominent optoelectronic properties and innovatively coined optoelectronic mechanisms are appealing, yet significantly challenging tasks. Here, we exploit a series of unique Janus luminogens, namely TAOs, with unique charge separation in a simple five-membered mesoionic ring. TAOs, having low molecular weight (∼329 g mol−1), present efficient aggregation-induced red/near-infrared emission (550–850 nm) with up to 21.5% of fluorescence quantum yield. An original mechanism, termed bended intramolecular charge transfer (BICT), is proposed to understand the fluorescence behavior. It is experimentally demonstrated that TAOs exhibit great potential for use as molecular transistors and can be efficiently utilized in living cells, bacteria, and brain imaging in a straightforward manner by using intravenous postinjection with outstanding photostability and biocompatibility.

Molecular electronics is one of the promising technologies for future electronic applications that is currently gaining a lot of interest. This is because if single molecule could be used as active electronic components this would provide an ultimate device miniaturization. Previously studied molecules provide almost exclusively two terminal devices. In this paper, three-leg molecular devices are examined employing a first-principles study based on density functional theory coupled to the non-equilibrium Green’s function formalism. We illustrate the feasibility of building a prototype molecular transistor using three-leg molecules directly contacted to gold electrodes. We discuss the different factors that control the transport through this molecular transistor. Moreover, we show that a functional standalone NAND logic gate can be implemented using a single three-leg molecular device.