Quasiparticle effects and strong excitonic features in exfoliable 1D semiconducting materials

We report a first-principles study of the electronic and optical properties of recently identified one-dimensional semiconducting materials exfoliable from van der Waals-bonded bulk crystals. Specifically, we investigate four chalcogenide-based atomic chains, the covalently bonded S3 and Te3 chains, and polar-bonded As2S3 and Bi2Te3 chains, using a fully first-principles approach that combines density functional theory (DFT), density functional perturbation theory (DFPT), and many-body perturbation theory within the GW approximation and Bethe−Salpeter equation (BSE). Our vibrational analysis shows that the isolated, freestanding wires remain dynamically stable, with the zone-center optical phonon modes leading to infrared activity. The main finding of this study is the presence of very strong exciton binding energies (1−3 eV), which make these exfoliable 1D materials suitable platforms for room-temperature excitonic applications. Interestingly, the exciton character remains Wannier−Mott-like, as indicated by average electron−hole separations greater than the lattice constant. Notably, the optical gaps of these materials span a wide range - from infrared (0.8 eV, Bi2Te3), through the visible spectrum (yellow: 2.17 eV, Te3; blue: 2.71 eV, As2S3), up to ultraviolet (4.07 eV, S3) - highlighting their versatility for broadband optoelectronic applications. Our results offer a detailed, many-body perspective on the optoelectronic behavior of these low-dimensional materials and underscore their potential for applications in nanoscale optoelectronic devices.