Direct spectroscopic evidence for mixed-valence Tl in the low carrier-density superconductor Pb1-xTlxTe

Walmsley, P.; Liu, C.; Palczewski, A. D.; Giraldo-Gallo, P.; Olson, C. G.; Fisher, I. R.; Kaminski, A.

doi:10.1103/physrevb.98.184506

Direct spectroscopic evidence for mixed-valence Tl in the low carrier-density superconductor ${Pb}_{1 - x} {Tl}_{x} Te$

Journal Article · Thu Nov 15 00:00:00 EST 2018 · Physical Review. B

DOI:https://doi.org/10.1103/physrevb.98.184506· OSTI ID:1487218

Walmsley, P. ^[1]; Liu, C. ^[2]; Palczewski, A. D. ^[3]; Giraldo-Gallo, P. ^[4]; Olson, C. G. ^[5]; Fisher, I. R. ^[1]; Kaminski, A. ^[5]

Stanford Univ., CA (United States). Geballe Lab. for Advanced Materials and Dept. of Applied Physics
Ames Lab. and Iowa State Univ., Ames, IA (United States). Dept. of Physics and Astronomy; Southern Univ. of Science and Technology (SUSTech), Shenzhen, Guangdong (China)
Ames Lab. and Iowa State Univ., Ames, IA (United States). Dept. of Physics and Astronomy; Thomas Jefferson National Accelerator Facility (TJNAF), Newport News, VA (United States)
Stanford Univ., CA (United States). Geballe Lab. for Advanced Materials and Dept. of Applied Physics; Univ. de Los Andes, Bogotá (Colombia). Dept. of Physics
Ames Lab. and Iowa State Univ., Ames, IA (United States). Dept. of Physics and Astronomy

Upon doping with Tl the narrow band-gap semiconductor PbTe exhibits anomalously high-temperature superconductivity despite a very low carrier-density as well as signatures of the Kondo effect despite an absence of magnetic moments. These phenomena have been explained by invoking 2e fluctuations of the valence of the Tl dopants, but a direct measurement of the mixed valency implied by such a mechanism has not been reported to date. Here in this work we present the unambiguous observation of multiple valences of Tl in Tl-doped PbTe via photoemission spectroscopy measurements. It is shown via a quantitative analysis that the suppression of the carrier density in compositions exhibiting superconductivity and Kondo-like behavior can be accounted for by mixed valency, thus arguing against a self-compensation scenario proposed elsewhere for this material and strengthening the case for valence fluctuation models. In addition to the identification of Tl⁺ and Tl³⁺ a possible third intermediate local charge-density is suggested by full fits to the data, the origins of which are also discussed but remain unclear.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-07CH11358

OSTI ID:: 1487218

Alternate ID(s):: OSTI ID: 1482285

Report Number(s):: IS-J--9823

Journal Information:: Physical Review. B, Journal Name: Physical Review. B Journal Issue: 18 Vol. 98; ISSN 2469-9950; ISSN PRBMDO

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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