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As an emerging class of hybrid complexes, donor–acceptor (D–A) hybrid heterostructures, which combine the advantages of both organic and inorganic photoactive components, provide excellent platforms for the fabrication of photochromic materials with enhanced photo-responsive performances. Herein, four novel hybrid heterostructures, namely H3TPT·(PW12O40)·2NMP (1), (H1.5TPT)2·(PW12O40) (2), (H3TPT)2·(SiW12O40)·2Cl·2MeCN (3), and H3TPT·(HPMo12O40)·Cl·3NMP (4) (TPT is tri(4-pyridyl)-s-triazine, NMP is N-methylpyrrolidone), have been synthesized and characterized. Benefitting from the strong interactions (anion–π interactions) and matching electron energy levels between the donors and acceptors, some of them exhibited ultrafast photochromic behaviour even up to 1 second. Furthermore, based on experimental and theoretical calculations, the plausible PIET process and structure–activity relationship have been discussed in detail. [ABSTRACT FROM AUTHOR]

Comprehensive Summary: The development of novel building blocks with sp3‐hybridized‐carbon‐free conjugated skeletons is important to further advance and enrich nonfullerene acceptors (NFAs), but this remains a challenge due to the lack of strategies to effectively modulate the aggregation behavior of resulting NFAs. Herein, two novel nitrogen‐bridged octacyclic ladder‐type heteroarenes end‐capped with thiophene rings (BTPS) or selenophene rings (BTPSe) are designed and synthesized as the donor cores for constructing NFAs (MQX‐2 and MQX‐4). It is found that replacing the sulfur atoms (MQX‐2) at the outer positions of the heteroarene core with selenium atoms (MQX‐4) can effectively modulate the molecular packing mode of the NFAs. The incorporation of selenium atoms induces stronger O···Se noncovalent interaction than O···S, thus promoting the formation of mixed H/J‐type aggregates in MQX‐4. Benefiting from more electron hopping channels, MQX‐4 exhibits higher electron transport (more than 1‐fold enhancement) and photovoltaic properties compared to MQX‐2, which forms only H‐type aggregates. [ABSTRACT FROM AUTHOR]

Inelastic electron transfer, regarded as one of the potential mechanisms to explain odorant recognition in atomic-scale processes, is still a matter of intense debate. Here, we study multiphonon processes of electron transfer using the Markvart model and calculate their lifetimes with the values of key parameters widely adopted in olfactory systems. We find that these multiphonon processes are as quick as the single phonon process, which suggests that contributions from different phonon modes of an odorant molecule should be included for electron transfer in olfaction. Meanwhile, the temperature dependence of electron transfer could be analyzed effectively based on the reorganization energy which is expanded into the linewidth of multiphonon processes. Our theoretical results not only enrich the knowledge of the mechanism of olfaction recognition, but also provide insights into quantum processes in biological systems. [ABSTRACT FROM AUTHOR]