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Hui‐Min Zhou Lin Xiong Ling Chen Li‐Ming Wu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(29):10084-10088
The essence of rational design syntheses of functional inorganic materials lies in understanding and control of crystal structures that determine the physical properties. AgGaS2 has the highest figure of merit for IR nonlinear optical interactions to date, but suffers low laser‐induced damage threshold (LIDT). The partial Li substitution of Ag atoms is now shown to push up the bottom of the conduction band and flatten the top of the valence band, leading to an ultrawide band gap of 3.40 eV (record high for AgGaS2, indicating a transparency edging nearly 180 nm shorter than that of AgGaS2), which gives Li0.60Ag0.40GaS2 a LIDT 8.6 times stronger when AgGaS2 is compared. Li0.60Ag0.40GaS2 exhibits 1.1 times stronger nonlinear susceptibility, which is because the energy‐favorable Li substitution gradually decreases the sulfur dislocation in the lattice, which allows a better geometric superposition of nonlinear optical tensors. 相似文献
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Cheng‐Hao Liu Muhammad Rizwan Niazi Dmitrii F. Perepichka 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(48):17473-17482
π‐Conjugated organic materials possess a wide range of tunable optoelectronic properties which are dictated by their molecular structure and supramolecular arrangement. While many efforts have been put into tuning the molecular structure to achieve the desired properties, rational supramolecular control remains a challenge. Here, we report a novel series of supramolecular materials formed by the co‐assembly of weak π‐electron donor (indolo[2,3‐a]carbazole) and acceptor (aromatic o‐quinones) molecules via complementary hydrogen bonding. The resulting polarization creates a drastic perturbation of the molecular energy levels, causing strong charge transfer in the weak donor–acceptor pairs. This leads to a significant lowering (up to 1.5 eV) of the band gaps, intense absorption in the near‐IR region, very short π‐stacking distances (≥3.15 Å), and strong ESR signals in the co‐crystals. By varying the strength of the acceptor, the characteristics of the complexes can be tuned between intrinsic, gate‐, or light‐induced semiconductivity with a p‐type or ambipolar transport mechanism. 相似文献
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