“…Several important applications including sensors 3 , memory devices 4 , photovoltaics 5 , atomically-thin holograms 6 , electrically and optically modulated high harmonic generation 7 – 9 based on vdW layered materials have been demonstrated to substantiate their prospects till date. Noticeably, these applications are primarily realized on traditional mono- and binary-element vdW layered materials such as graphene, black phosphorous, GeAs, ReS 2 and transition metal dichalcogenides, therefore the material-associated inherent limitations such as elementary crystal structures, simple chemical compositions, material-dependent electronic and optical responses make the applications relatively monotonous and further confine their adaptability 10 – 13 . To address these limitations of mono- and binary-element materials, multi-element vdW layered materials 14 , 15 facilitate an alternative and versatile testbed for realizing innovative electronic, photonic and optoelectronic applications 10 – 12 , according to their complex crystal structures, stoichiometric variations, and exceptional physical and chemical properties such as high charge carrier mobility 10 , 16 , favorable band structure 17 , unique phonon vibrations 11 , 17 , linear dichroism transition 18 , 19 , and robust air stability.…”