2D inorganic bimolecular crystals, consisting of two different inorganic molecules, are expected to possess novel physical and chemical properties due to the synergistic effect of the individual components. However, 2D inorganic bimolecular crystals remain unexploited because of the difficulties in preparation arising from non‐typical layered structures and intricate intermolecular interactions. Here, the synthesis of 2D inorganic bimolecular crystal SbI₃·3S₈ nanobelts via a facile vertical microspacing sublimation strategy is reported. The as‐synthesized SbI₃·3S₈ nanobelts exhibit strong in‐plane anisotropy of phonon vibrations and intramolecular vibrations as well as show anisotropic light absorption with a high dichroism ratio of 3.9. Furthermore, it is revealed that the second harmonic generation intensity of SbI₃·3S₈ nanobelts is highly dependent on the excitation wavelength and crystallographic orientation. This work can inspire the growth of more 2D inorganic bimolecular crystals and excite potential applications for bimolecular optoelectronic devices.

中文翻译：

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具有强平面内各向异性的2D无机双分子晶体用于二阶非线性光学。

由两个不同的无机分子组成的2D无机双分子晶体由于各个组分的协同作用，有望具有新颖的物理和化学性质。然而，由于非典型的层状结构和复杂的分子间相互作用导致制备困难，二维无机双分子晶体仍未开发。在此，通过简便的垂直微间距升华策略合成了2D无机双分子晶体SbI ₃ ·3S ₈纳米带。合成后的SbI ₃ ·3S ₈纳米带表现出很强的声子振动和分子内振动的面内各向异性，并且具有各向异性的光吸收，并且具有高达3.9的二色性。此外，揭示了SbI ₃ ·3S ₈纳米带的二次谐波产生强度高度依赖于激发波长和晶体学取向。这项工作可以激发更多的2D无机双分子晶体的生长，并激发双分子光电器件的潜在应用。