Nanotubes from ternary WS2(1- x)Se2 xalloys: Stoichiometry modulated tunable optical properties

Nanotubes of transition metal dichalcogenides such as WS2 and MoS2 offer unique quasi-1D properties and numerous potential applications. Replacing sulfur by selenium would yield ternary WS2(1–x)Se2x (0 ≤ x ≤ 1; WSSe) nanotubes, which are expected to reveal strong modulation in their absorption edge as a function of selenium content, xSe. Solid WO2.72 oxide nanowhiskers were employed as a sacrificial template to gain a high yield of the nanotubes with a rather uniform size distribution. Though sulfur and selenium belong to the same period, their chemical reactivity with oxide nanowhiskers differed appreciably. Here, the closed ampoule technique was utilized to achieve the completion of the solid–vapor reaction in short time scales instead of the conventional flow reactor method. The structure and chemical composition of the nanotubes were analyzed in detail. X-ray and electron diffractions indicated a systematic modulation of the WSSe lattice upon increasing the selenium content. Detailed chemical mapping showed that the sulfur and selenium atoms are distributed in random positions on the anion lattice site of the nanotubes. The optical excitonic features and absorption edges of the WSSe nanotubes do not vary linearly with the composition xSe, which was further confirmed by density functional theory calculations. The WSSe nanotubes were shown to exhibit strong light–matter interactions forming exciton–polariton quasiparticles, which was corroborated by finite-difference time-domain simulations. Transient absorption analysis permitted following the excited state dynamics and elucidating the mechanism of the strong coupling. Thus, nanotubes of the ternary WSSe alloys offer strong band gap tunability, which would be useful for multispectral vision devices and other optoelectronic applications.The support of the Israel Science Foundation (grant no. 7130970101), Irving and Cherna Moskowitz Center for Nano and Bio-Nano Imaging, the Perlman Family Foundation, and the Kimmel Center for Nanoscale Science (grant no. 43535000350000) is greatly acknowledged. K.Z. acknowledges China Scholarship Council (grant no. 2020008500162) for the research fellowship. I.P. is the encumbent of the Sharon Zuckerman research fellow chair. S.H. and R.A. acknowledge funding from the European Union’s Horizon 2020 research and innovation program under the Marie Sklodowska-Curie grant agreement no. 889546, from the Spanish MICINN (project grant PID2019-104739GB-100/AEI/10.13039/501100011033), and from the Government of Aragon (project DGA E13-20R). R.A. acknowledges funding from the European Union H2020 program “ESTEEM3” (823717).Peer reviewe