Direct spectroscopic evidence for mixed-valence Tl in the low carrier-density superconductor
Abstract
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.
- Authors:
-
- 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
- Publication Date:
- Research Org.:
- Ames Laboratory (AMES), Ames, IA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1487218
- Alternate Identifier(s):
- OSTI ID: 1482285
- Report Number(s):
- IS-J-9823
Journal ID: ISSN 2469-9950; PRBMDO
- Grant/Contract Number:
- AC02-07CH11358; FA9550-09-1-0583; DMR 9212658
- Resource Type:
- Journal Article: Accepted Manuscript
- Journal Name:
- Physical Review. B
- Additional Journal Information:
- Journal Volume: 98; Journal Issue: 18; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY
Citation Formats
Walmsley, P., Liu, C., Palczewski, A. D., Giraldo-Gallo, P., Olson, C. G., Fisher, I. R., and Kaminski, A. Direct spectroscopic evidence for mixed-valence Tl in the low carrier-density superconductor Pb1-xTlxTe. United States: N. p., 2018.
Web. doi:10.1103/physrevb.98.184506.
Walmsley, P., Liu, C., Palczewski, A. D., Giraldo-Gallo, P., Olson, C. G., Fisher, I. R., & Kaminski, A. Direct spectroscopic evidence for mixed-valence Tl in the low carrier-density superconductor Pb1-xTlxTe. United States. https://doi.org/10.1103/physrevb.98.184506
Walmsley, P., Liu, C., Palczewski, A. D., Giraldo-Gallo, P., Olson, C. G., Fisher, I. R., and Kaminski, A. 2018.
"Direct spectroscopic evidence for mixed-valence Tl in the low carrier-density superconductor Pb1-xTlxTe". United States. https://doi.org/10.1103/physrevb.98.184506. https://www.osti.gov/servlets/purl/1487218.
@article{osti_1487218,
title = {Direct spectroscopic evidence for mixed-valence Tl in the low carrier-density superconductor Pb1-xTlxTe},
author = {Walmsley, P. and Liu, C. and Palczewski, A. D. and Giraldo-Gallo, P. and Olson, C. G. and Fisher, I. R. and Kaminski, A.},
abstractNote = {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.},
doi = {10.1103/physrevb.98.184506},
url = {https://www.osti.gov/biblio/1487218},
journal = {Physical Review. B},
issn = {2469-9950},
number = 18,
volume = 98,
place = {United States},
year = {Thu Nov 15 00:00:00 EST 2018},
month = {Thu Nov 15 00:00:00 EST 2018}
}
Web of Science
Works referenced in this record:
Superconductivity in Charge Kondo Systems
journal, April 2005
- Dzero, Maxim; Schmalian, Jörg
- Physical Review Letters, Vol. 94, Issue 15
Evidence for Charge Kondo Effect in Superconducting Tl-Doped PbTe
journal, April 2005
- Matsushita, Y.; Bluhm, H.; Geballe, T. H.
- Physical Review Letters, Vol. 94, Issue 15
Heavy-fermion behavior in a negative- U Anderson model
journal, May 1991
- Taraphder, A.; Coleman, P.
- Physical Review Letters, Vol. 66, Issue 21
Thermopower of thermoelectric materials with resonant levels: PbTe:Tl versus PbTe:Na and
journal, May 2018
- Wiendlocha, Bartlomiej
- Physical Review B, Vol. 97, Issue 20
Type II superconducting parameters of Tl-doped PbTe determined from heat capacity and electronic transport measurements
journal, October 2006
- Matsushita, Y.; Wianecki, P. A.; Sommer, A. T.
- Physical Review B, Vol. 74, Issue 13
Complex role for thallium in PbTe:Tl from local probe studies
journal, April 2013
- Keiber, T.; Bridges, F.; Sales, B. C.
- Physical Review B, Vol. 87, Issue 14
The charge state of Tl impurities in PbTe
journal, May 1988
- Waddington, S. D.; Weightman, P.; Grassie, A. D. C.
- Journal of Physics C: Solid State Physics, Vol. 21, Issue 14
Double-valence-fluctuating molecules and superconductivity
journal, November 1985
- Hirsch, J. E.; Scalapino, D. J.
- Physical Review B, Vol. 32, Issue 9
Formation and Optical Absorption Spectra of Mixed Valence State of Tl in Tl 2 Nb 2 O 6+ x with Pyrochlore Structure
journal, January 1996
- Mizoguchi, Hiroshi; Kawazoe, Hiroshi; Ueda, Takahiro
- Bulletin of the Chemical Society of Japan, Vol. 69, Issue 1
Indirect nuclear exchange coupling and electronic structure of the layered semiconductor TlS: NMR study and band structure calculation
journal, April 2004
- Panich, A. M.; Kashida, S.
- Journal of Physics: Condensed Matter, Vol. 16, Issue 18
Doping Induced Evolution of Fermi Surface in Low Carrier Superconductor Tl-Doped PbTe
journal, June 2008
- Nakayama, K.; Sato, T.; Takahashi, T.
- Physical Review Letters, Vol. 100, Issue 22
Mixed-valence impurities in lead telluride-based solid solutions
journal, August 2002
- Volkov, Boris A.; Ryabova, Ludmila I.; Khokhlov, Dmitrii R.
- Physics-Uspekhi, Vol. 45, Issue 8
Superconductivity in metals containing negative-U centers. Exciton and phonon models
journal, January 1991
- Mal'shukov, A. G.
- Solid State Communications, Vol. 77, Issue 1
Superconductivity in doped semiconductors
journal, July 2015
- Bustarret, E.
- Physica C: Superconductivity and its Applications, Vol. 514
Anomalous 125 Te Nuclear Spin Relaxation Coincident with Charge Kondo Behavior in Superconducting Pb 1− x Tl x Te
journal, February 2018
- Mukuda, Hidekazu; Matsumura, Takashi; Maki, Shota
- Journal of the Physical Society of Japan, Vol. 87, Issue 2
Resonant levels in bulk thermoelectric semiconductors
journal, January 2012
- Heremans, Joseph P.; Wiendlocha, Bartlomiej; Chamoire, Audrey M.
- Energy Environ. Sci., Vol. 5, Issue 2
Thallium dopant in lead chalcogenides: investigation methods and peculiarities
journal, August 1998
- Nemov, S. A.; Ravich, Yu I.
- Physics-Uspekhi, Vol. 41, Issue 8
Deep and resonance states in A IV B VI semiconductors
journal, January 1985
- Kaĭdanov, V. I.; Ravich, Yu I.
- Soviet Physics Uspekhi, Vol. 28, Issue 1
Fermi surface evolution of Na-doped PbTe studied through density functional theory calculations and Shubnikov–de Haas measurements
journal, November 2016
- Giraldo-Gallo, P.; Sangiorgio, B.; Walmsley, P.
- Physical Review B, Vol. 94, Issue 19
Missing valence states, diamagnetic insulators, and superconductors
journal, December 1988
- Varma, C. M.
- Physical Review Letters, Vol. 61, Issue 23
Doping of PbTe with Group-III elements: An ionic lattice approach
journal, March 1981
- Weiser, K.
- Physical Review B, Vol. 23, Issue 6
Superconducting enhancement due to negative- U impurities: Monte Carlo study of a local exciton model
journal, April 1989
- Schüttler, H. - B.; Jarrell, M.; Scalapino, D. J.
- Physical Review B, Vol. 39, Issue 10
Behaviour of group IIIA impurities in PbTe: implications to improve thermoelectric efficiency
journal, September 2010
- Xiong, K.; Lee, G.; Gupta, R. P.
- Journal of Physics D: Applied Physics, Vol. 43, Issue 40
Superconductivity and transport properties of narrow-gap semiconductor Pb(Tl)Te film by HWE growth
journal, September 1996
- Murakami, Hironaru; Hattori, Wataru; Aoki, Ryozo
- Physica C: Superconductivity, Vol. 269, Issue 1-2
Mixed-valence compounds
journal, April 1976
- Varma, C. M.
- Reviews of Modern Physics, Vol. 48, Issue 2
Rational design of p-type thermoelectric PbTe: temperature dependent sodium solubility
journal, January 2013
- Yamini, Sima Aminorroaya; Ikeda, Teruyuki; Lalonde, Aaron
- Journal of Materials Chemistry A, Vol. 1, Issue 31
Deep and resonance states in A<sup>IV</sup> B<sup>VI</sup> semiconductors [Глубокие и резонансные состояния в полупроводниках типа AIVBVI]
journal, January 1985
- Kaidanov, V. I.; Ravich, Yu. I.
- Uspekhi Fizicheskih Nauk, Vol. 145, Issue 1
Thallium dopant in lead chalcogenides: investigation methods and peculiarities [Primes' talliya v khal'kogenidakh svintsa: metody issledovaniya i osobennosti]
journal, January 1998
- Nemov, S. A.; Ravich, Yu. I.
- Uspekhi Fizicheskih Nauk, Vol. 168, Issue 8
Mixed-valence impurities in lead telluride-based solid solutions [Primesi s peremennoi valentnost'yu v tverdykh rastvorakh na osnove tellurida svintsa]
journal, January 2002
- Volkov, Boris A.; Ryabova, Ludmila I.; Khokhlov, Dmitrii R.
- Uspekhi Fizicheskih Nauk, Vol. 172, Issue 8
Evidence for charge Kondo effect in superconducting Tl-doped PbTe
conference, August 2005
- Fisher, I. R.; Matsushita, Y.; Bluhm, H.
- Optics & Photonics 2005, SPIE Proceedings
Anomalous ^{125}Te Nuclear Spin Relaxation Coincident with Charge Kondo Behavior in Superconducting Pb_{1-x}Tl_{x}Te
text, January 2017
- Mukuda, H.; Matsumura, T.; Maki, S.
- arXiv
Evidence for charge Kondo effect in superconducting Tl-doped PbTe
text, January 2004
- Matsushita, Y.; Bluhm, H.; Geballe, T. H.
- arXiv
The ageing brain, neuroleptic drugs and the enigma of schizophrenia
journal, May 1988
- Waddington, John L.
- Irish Journal of Medical Science, Vol. 157, Issue 5
Works referencing / citing this record:
Physics of Superconducting Transition Temperatures
journal, November 2019
- Kivelson, Steven A.
- Journal of Superconductivity and Novel Magnetism, Vol. 33, Issue 1