Nanotubes from the Misfit Layered Compound (SmS)1.19TaS2: Atomic Structure, Charge Transfer, and Electrical Properties

Sreedhara, M. B.; Bukvišová, Kristýna; Khadiev, Azat; Citterberg, Daniel; Cohen, Hagai; Balema, Viktor; K. Pathak, Arjun; Novikov, Dmitri; Leitus, Gregory; Kaplan-Ashiri, Ifat; Kolíbal, Miroslav; Enyashin, Andrey N.; Houben, Lothar; Tenne, Reshef

doi:10.1021/acs.chemmater.1c04106

Title: Nanotubes from the Misfit Layered Compound (SmS)_1.19TaS₂: Atomic Structure, Charge Transfer, and Electrical Properties

Journal Article · 09 February 2022 · Chemistry of Materials

DOI: https://doi.org/10.1021/acs.chemmater.1c04106 · OSTI ID:2469481

^[1]; Bukvišová, Kristýna ^[2]; Khadiev, Azat ^[3]; Citterberg, Daniel ^[2];

^[1]; Balema, Viktor ^[4]; K. Pathak, Arjun ^[5]; Novikov, Dmitri ^[3]; Leitus, Gregory ^[1]; Kaplan-Ashiri, Ifat ^[1];

^[2];

^[6];

^[1];

^[1]

Weizmann Institute of Science, Rehovot (Israel)
Brno University of Technology (Czech Republic)
Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
Ames Laboratory (AMES), Ames, IA (United States); ProChem Inc., Rockford, IL (United States)
State Univ. of New York (SUNY), Buffalo, NY (United States)
Russian Academy of Sciences (RAS), Ekaterinburg (Russian Federation). Institute of Solid State Chemistry (ISSC UB RAS); Ural Federal Univ., Ekaterinburg (Russian Federation)

Misfit layered compounds (MLCs) MX-TX₂, where M, T = metal atoms and X = S, Se, or Te, and their nanotubes are of significant interest due to their rich chemistry and unique quasi-1D structure. In particular, LnX-TX₂ (Ln = rare-earth atom) constitute a relatively large family of MLCs, from which nanotubes have been synthesized. The properties of MLCs can be tuned by the chemical and structural interplay between LnX and TX₂ sublayers and alloying of each of the Ln, T, and X elements. In order to engineer them to gain desirable performance, a detailed understanding of their complex structure is indispensable. MLC nanotubes are a relative newcomer and offer new opportunities. In particular, like WS₂ nanotubes before, the confinement of the free carriers in these quasi-1D nanostructures and their chiral nature offer intriguing physical behavior. High-resolution transmission electron microscopy in conjunction with a focused ion beam are engaged to study SmS-TaS₂ nanotubes and their cross-sections at the atomic scale. The atomic resolution images distinctly reveal that Ta is in trigonal prismatic coordination with S atoms in a hexagonal structure. Furthermore, the position of the sulfur atoms in both the SmS and the TaS₂ sublattices is revealed. X-ray photoelectron spectroscopy, electron energy loss spectroscopy, and X-ray absorption spectroscopy are carried out. These analyses conclude that charge transfer from the Sm to the Ta atoms leads to filling of the Ta 5d_z² level, which is confirmed by density functional theory (DFT) calculations. Transport measurements show that the nanotubes are semimetallic with resistivities in the range of 10^–4 Ω·cm at room temperature, and magnetic susceptibility measurements show a superconducting transition at 4 K.

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Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: AC02-07CH11358

OSTI ID:: 2469481

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 4 Vol. 34; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Nanotubes from the Misfit Layered Compound (SmS)1.19TaS2: Atomic Structure, Charge Transfer, and Electrical Properties

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Title: Nanotubes from the Misfit Layered Compound (SmS)_1.19TaS₂: Atomic Structure, Charge Transfer, and Electrical Properties