Electronic, Optical, Mechanical and Li-Ion Storage Properties of Novel Benzotrithiophene-Based Graphdiyne Monolayers Explored by First Principles and Machine Learning

Recently, benzotrithiophene graphdiyne (BTT-GDY), a novel two-dimensional (2D) carbon-based material, was grown via bottom-up synthesis strategy. Using the BTT-GDY lattice and by replacing S atoms with N, NH O, we designed three GDY lattices, which named BTHP-, BTP- BTF-GDY, respectively. Next, explored structural, electronic, mechanical, optical, photocatalytic Li-ion storage properties, as well carrier mobilities, of monolayers. Phonon dispersion relations, mechanical failure behavior were using machine learning interatomic potentials (MLIPs). The obtained HSE06 results reveal that BTX-GDYs (X = P, F, T) are direct gap semiconductors band gaps in range 2.49–2.65 eV, whereas BTHP-GDY shows narrow indirect 0.06 eV. With appropriate offsets, good mobilities strong capability for absorption visible ultraviolet light, BTF- BTT-GDYs predicted to be promising candidates overall water splitting. nanosheet, noticeably, found yield an ultrahigh capacity over 2400 mAh/g. findings provide comprehensive vision critical physical properties BTT-based nanosheets highlight their potential applications nanoelectronics energy conversion systems.