skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Evolution of nontrivial Fermi surface features in the band structures of the homologous members Pb 5 Bi 6 Se 14 and Pb 5 Bi 12 Se 23

Abstract

High-quality single crystals of (PbSe)5(Bi2Se3)3m were grown and analyzed by nuclear magnetic resonance (NMR) spectroscopy. We report on 77Se and 207Pb NMR shifts and nuclear spin-lattice relaxation measurements in the naturally formed heterostructure homology (PbSe)5(Bi2Se3)3m with m = 1 (Pb5Bi6Se14) and m = 2 (Pb5Bi12Se23). A distinct site-specific contribution has been detected for both nuclei as a function of temperature, which reveals an electronic changeover from a semiconducting (Pb5Bi6Se14) to a semimetalliclike (Pb5Bi12Se23) system with nontrivial band structure features near the Fermi level. The temperature dependences of the relaxation rates are dominated by significant changes in the topology of energy dispersions accompanied with band edges and crossings in the region of the Fermi surface. These results, which interrogate nuclear spin interactions from selected atomic sites, clearly expose the effects of the added Bi2Se3 layer on the crystal and electronic structure of (Pb5Bi12Se23). These findings provide direct microscopic insight into the unconventional and dual nature of the electronic structure of these homologous thermoelectric and topologically nontrivial compounds.

Authors:
 [1];  [2];  [3];  [4];  [1]
  1. Univ. of California, Los Angeles, CA (United States)
  2. Northwestern Univ., Evanston, IL (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
  4. Northwestern Univ., Evanston, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
U.S. Department of Defense (DOD) - Defense Advanced Research Projects Agency (DARPA); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1616697
Alternate Identifier(s):
OSTI ID: 1607616
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 101; Journal Issue: 11; 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; crystal structure; homologous compounds; electronic band gap; Fermi surface; heterostructure; NMR

Citation Formats

Koumoulis, D., Fang, L., Chung, D. Y., Kanatzidis, M. G., and Bouchard, L. -S. Evolution of nontrivial Fermi surface features in the band structures of the homologous members Pb5Bi6Se14 and Pb5Bi12Se23. United States: N. p., 2020. Web. doi:10.1103/PhysRevB.101.115309.
Koumoulis, D., Fang, L., Chung, D. Y., Kanatzidis, M. G., & Bouchard, L. -S. Evolution of nontrivial Fermi surface features in the band structures of the homologous members Pb5Bi6Se14 and Pb5Bi12Se23. United States. doi:https://doi.org/10.1103/PhysRevB.101.115309
Koumoulis, D., Fang, L., Chung, D. Y., Kanatzidis, M. G., and Bouchard, L. -S. Mon . "Evolution of nontrivial Fermi surface features in the band structures of the homologous members Pb5Bi6Se14 and Pb5Bi12Se23". United States. doi:https://doi.org/10.1103/PhysRevB.101.115309. https://www.osti.gov/servlets/purl/1616697.
@article{osti_1616697,
title = {Evolution of nontrivial Fermi surface features in the band structures of the homologous members Pb5Bi6Se14 and Pb5Bi12Se23},
author = {Koumoulis, D. and Fang, L. and Chung, D. Y. and Kanatzidis, M. G. and Bouchard, L. -S.},
abstractNote = {High-quality single crystals of (PbSe)5(Bi2Se3)3m were grown and analyzed by nuclear magnetic resonance (NMR) spectroscopy. We report on 77Se and 207Pb NMR shifts and nuclear spin-lattice relaxation measurements in the naturally formed heterostructure homology (PbSe)5(Bi2Se3)3m with m = 1 (Pb5Bi6Se14) and m = 2 (Pb5Bi12Se23). A distinct site-specific contribution has been detected for both nuclei as a function of temperature, which reveals an electronic changeover from a semiconducting (Pb5Bi6Se14) to a semimetalliclike (Pb5Bi12Se23) system with nontrivial band structure features near the Fermi level. The temperature dependences of the relaxation rates are dominated by significant changes in the topology of energy dispersions accompanied with band edges and crossings in the region of the Fermi surface. These results, which interrogate nuclear spin interactions from selected atomic sites, clearly expose the effects of the added Bi2Se3 layer on the crystal and electronic structure of (Pb5Bi12Se23). These findings provide direct microscopic insight into the unconventional and dual nature of the electronic structure of these homologous thermoelectric and topologically nontrivial compounds.},
doi = {10.1103/PhysRevB.101.115309},
journal = {Physical Review B},
number = 11,
volume = 101,
place = {United States},
year = {2020},
month = {3}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 1 work
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Direct Chemical Fine-Tuning of Electronic Properties in Sc 2 Ir 6− x Pd x B
journal, August 2016

  • Koumoulis, Dimitrios; Scheifers, Jan P.; St. Touzani, Rachid
  • ChemPhysChem, Vol. 17, Issue 19
  • DOI: 10.1002/cphc.201600512

Effects of Cd vacancies and unconventional spin dynamics in the Dirac semimetal Cd 3 As 2
journal, August 2017

  • Koumoulis, Dimitrios; Taylor, Robert E.; McCormick, Jeffrey
  • The Journal of Chemical Physics, Vol. 147, Issue 8
  • DOI: 10.1063/1.4999467

NMR study of native defects in PbSe
journal, September 2014


77Se Low-Temperature NMR in the Bi2Se3 Single Crystalline Topological Insulator
journal, February 2018

  • Antonenko, A. O.; Nefedov, D. Yu.; Charnaya, E. V.
  • Applied Magnetic Resonance, Vol. 49, Issue 6
  • DOI: 10.1007/s00723-018-0986-1

Unusual 209Bi NMR quadrupole effects in topological insulator Bi2Se3
journal, May 2019

  • Guehne, Robin; Chlan, Vojtěch; Williams, Grant V. M.
  • Journal of Magnetic Resonance, Vol. 302
  • DOI: 10.1016/j.jmr.2019.03.008

A Combined NMR and DFT Study of Narrow Gap Semiconductors: The Case of PbTe
journal, April 2013

  • Taylor, Robert E.; Alkan, Fahri; Koumoulis, Dimitrios
  • The Journal of Physical Chemistry C, Vol. 117, Issue 17
  • DOI: 10.1021/jp3101877

Hyperfine coupling and spin polarization in the bulk of the topological insulator Bi 2 Se 3
journal, February 2015


Dirac fermions and superconductivity in the homologous structures ( Ag x Pb 1 x Se ) 5 ( Bi 2 Se 3 ) 3 m ( m = 1 , 2 )
journal, July 2014


77 Se and 63 Cu NMR studies of the electronic correlations in Cu x TiSe 2 ( x = 0.05, 0.07)
journal, June 2010


Pseudogap opening in single-crystal YMn 4 Al 8 investigated through Mn 55 and Al 27 NMR measurements
journal, December 2018


β -detected NMR of Li 8 + in Bi, Sb, and the topological insulator Bi 0.9 Sb 0.1
journal, December 2014


Se 77 nuclear magnetic resonance of topological insulator Bi 2 Se 3
journal, May 2016


Structural Evolution and Phase Homologies for “Design” and Prediction of Solid-State Compounds
journal, April 2005

  • Kanatzidis, Mercouri G.
  • Accounts of Chemical Research, Vol. 38, Issue 4
  • DOI: 10.1021/ar040176w

Electronic inhomogeneity in n - and p -type PbTe detected by 125 Te NMR
journal, September 2013


Selenium Becomes Metallic in Ru−Se Fuel Cell Catalysts:  An EC-NMR and XPS Investigation
journal, December 2007

  • Babu, Panakkattu K.; Lewera, Adam; Chung, Jong Ho
  • Journal of the American Chemical Society, Vol. 129, Issue 49
  • DOI: 10.1021/ja077498q

Pseudogap in Fe 2 VGa : NMR evidence
journal, January 2001


Spin–Lattice Relaxation in Bismuth Chalcogenides
journal, August 2012

  • Taylor, Robert E.; Leung, Belinda; Lake, Michael P.
  • The Journal of Physical Chemistry C, Vol. 116, Issue 32
  • DOI: 10.1021/jp307051z

Nanoscale β-nuclear magnetic resonance depth imaging of topological insulators
journal, June 2015

  • Koumoulis, Dimitrios; Morris, Gerald D.; He, Liang
  • Proceedings of the National Academy of Sciences, Vol. 112, Issue 28
  • DOI: 10.1073/pnas.1502330112

Nuclear spin-lattice relaxation by optically bistable defects in CdF 2 : In
journal, April 2002


Observation of the Meyer–Neldel rule in nanocrystalline PbSe thin films
journal, October 2014


Nuclear magnetic relaxation and resonnance line shift in metals
journal, July 1950


NMR evidence for the partially gapped state in CeOs 2 Al 10
journal, November 2010


Spin-rotation symmetry breaking in the superconducting state of CuxBi2Se3
journal, May 2016

  • Matano, K.; Kriener, M.; Segawa, K.
  • Nature Physics, Vol. 12, Issue 9
  • DOI: 10.1038/nphys3781

NMR probe of bulk electronic structures in H + beam irradiated Bi2Te3 topological insulator
journal, March 2019


The role of point defects in PbS, PbSe and PbTe: a first principles study
journal, August 2015


NMR as a Probe of Band Inversion in Topologically Nontrivial Half-Heusler Compounds
journal, July 2014

  • Nowak, Bogdan; Kaczorowski, Dariusz
  • The Journal of Physical Chemistry C, Vol. 118, Issue 31
  • DOI: 10.1021/jp505320w

NMR Evidence for the Topologically Nontrivial Nature in a Family of Half-Heusler Compounds
journal, March 2016

  • Zhang, Xiaoming; Hou, Zhipeng; Wang, Yue
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep23172

Site-Specific Contributions to the Band Inversion in a Topological Crystalline Insulator
journal, June 2015

  • Koumoulis, Dimitrios; Chasapis, Thomas Christos; Leung, Belinda
  • Advanced Electronic Materials, Vol. 1, Issue 8
  • DOI: 10.1002/aelm.201500117

127 I and 207 Pb Solid-State NMR Spectroscopy and Nuclear Spin Relaxation in PbI 2 : A Preliminary Study
journal, April 2014

  • Taylor, R. E.; Beckmann, Peter A.; Bai, Shi
  • The Journal of Physical Chemistry C, Vol. 118, Issue 17
  • DOI: 10.1021/jp5023423

Pb5Bi24Se41: A new member of the homologous series forming topological insulator heterostructures
journal, January 2015


NMR Probe of Metallic States in Nanoscale Topological Insulators
journal, January 2013


Understanding Bulk Defects in Topological Insulators from Nuclear-Spin Interactions
journal, December 2013

  • Koumoulis, Dimitrios; Leung, Belinda; Chasapis, Thomas C.
  • Advanced Functional Materials, Vol. 24, Issue 11
  • DOI: 10.1002/adfm.201302673

Probing the bulk electronic states of Bi 2 Se 3 using nuclear magnetic resonance
journal, August 2012


27Al NMR Study of the Metal Cluster Compound Al50C120H180
journal, March 2007


S 119 n spin-lattice relaxation in α -SnF 2
journal, June 2009


Optoelectronic devices, plasmonics, and photonics with topological insulators
journal, March 2017

  • Politano, Antonio; Viti, Leonardo; Vitiello, Miriam S.
  • APL Materials, Vol. 5, Issue 3
  • DOI: 10.1063/1.4977782

Crystal Structure and Transport Properties of the Homologous Compounds (PbSe) 5 (Bi 2 Se 3 ) 3 m ( m = 2, 3)
journal, December 2017


NMR Study of Si:As and Si:P near the metal-insulator transition
journal, February 1986


Manipulation of Topological States and the Bulk Band Gap Using Natural Heterostructures of a Topological Insulator
journal, December 2012


Stretched exponential relaxation arising from a continuous sum of exponential decays
journal, November 2006


Nuclear magnetic resonance Knight shifts in the presence of strong spin–orbit and crystal-field potentials
journal, July 2016


Band Structure and Laser Action in Pb x Sn 1 x Te
journal, June 1966

  • Dimmock, J. O.; Melngailis, I.; Strauss, A. J.
  • Physical Review Letters, Vol. 16, Issue 26, p. 1193-1196
  • DOI: 10.1103/PhysRevLett.16.1193

NMR Signature of Evolution of Ductile-to-Brittle Transition in Bulk Metallic Glasses
journal, November 2011


Topological interface states in the natural heterostructure (PbSe) 5 ( Bi 2 Se 3 ) 6 with Bi Pb defects
journal, January 2018


Nuclear magnetic resonance as a probe of electronic states of Bi 2 Se 3
journal, May 2013


Two-band model interpretation of the p - to n -transition in ternary tetradymite topological insulators
journal, August 2015

  • Chasapis, T. C.; Koumoulis, D.; Leung, B.
  • APL Materials, Vol. 3, Issue 8
  • DOI: 10.1063/1.4922857

125 Te NMR and Seebeck Effect in Bi 2 Te 3 Synthesized from Stoichiometric and Te-Rich Melts
journal, October 2016

  • Levin, E. M.; Riedemann, T. M.; Howard, A.
  • The Journal of Physical Chemistry C, Vol. 120, Issue 44
  • DOI: 10.1021/acs.jpcc.6b06973

Band inversion mechanism in topological insulators: A guideline for materials design
journal, June 2012


NMR evidence for the coexistence of double structure in CaAlSi
journal, July 2006


Thermoelectric Properties of Polycrystalline n-Type Pb5Bi6Se14
journal, October 2016

  • Sassi, S.; Candolfi, C.; Ohorodniichuk, V.
  • Journal of Electronic Materials, Vol. 46, Issue 5
  • DOI: 10.1007/s11664-016-4976-5

Tight-binding theory of NMR shifts in topological insulators Bi 2 Se 3 and Bi 2 Te 3
journal, September 2016