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Title: Emergence of coherence in the charge-density wave state of 2H-NbSe2

Abstract

A charge density wave (CDW) state has a broken symmetry described by a complex order parameter with an amplitude and a phase. The conventional view, based on clean, weak-coupling systems, is that a finite amplitude and long-range phase coherence set in simultaneously at the CDW transition temperature Tcdw. Here we investigate, using photoemission, X-ray scattering and scanning tunneling microscopy, the canonical CDW compound 2H-NbSe2 intercalated with Mn and Co and show that the conventional view is untenable. We find that, either at high temperature or at large intercalation, CDW order becomes short- range with a well-defined amplitude that impacts the electronic dispersion, giving rise to an energy gap. The phase transition at Tcdw marks the onset of long-range order with global phase coherence leading to sharp electronic excitations. Our observations emphasize the importance of phase fluctuations in strongly coupled CDW systems and provide insights into the significance of phase incoherence in ‘pseudogap’ states.

Authors:
 [1];  [2];  [3];  [3];  [4];  [5];  [6];  [6];  [7];  [8];  [4]; ORCiD logo [9];  [10]; ORCiD logo [7];  [11];  [11];  [7]; ORCiD logo [7]
  1. Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Virginia, Charlottesville, VA (United States)
  2. Univ. of Virginia, Charlottesville, VA (United States); Univ. of Illinois, Chicago, IL (United States)
  3. Temple Univ., Philadelphia, PA (United States)
  4. Argonne National Lab. (ANL), Argonne, IL (United States); Karlsruhe Inst. of Technology (Germany)
  5. Drexel Univ., Philadelphia, PA (United States)
  6. Argonne National Lab. (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)
  7. Argonne National Lab. (ANL), Argonne, IL (United States)
  8. Argonne National Lab. (ANL), Argonne, IL (United States); Cornell Univ., Ithaca, NY (United States)
  9. Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Amsterdam (Netherlands)
  10. Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Illinois, Chicago, IL (United Sates)
  11. The Ohio State Univ., Columbus, OH (United States)
Publication Date:
Research Org.:
Temple Univ., Philadelphia, PA (United States); The Ohio State Univ., Columbus, OH (United States); Argonne National Laboratory (ANL), Argonne, IL (United States); Energy Frontier Research Centers (EFRC) (United States). Center for the Computational Design of Functional Layered Materials (CCDM); Energy Frontier Research Centers (EFRC) (United States). Center for Complex Materials from First Principles (CCM); Univ. of Texas, Austin, TX (United States); Argonne National Laboratory (ANL), Argonne, IL (United States
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Netherlands Organization for Scientific Research (NWO) (Netherlands)
OSTI Identifier:
1219582
Alternate Identifier(s):
OSTI ID: 1210744; OSTI ID: 1356631
Grant/Contract Number:  
SC0012575; SC0005035; FG02-07ER46423; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 6; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 36 MATERIALS SCIENCE; catalysis (heterogeneous); solar (photovoltaic); energy storage (including batteries and capacitors); hydrogen and fuel cells; defects; mechanical behavior; materials and chemistry by design; synthesis (novel materials)

Citation Formats

Chatterjee, U., Zhao, J., Iavarone, M., Di Capua, R., Castellan, J. P., Karapetrov, G., Malliakas, C. D., Kanatzidis, M. G., Claus, H., Ruff, J. P. C., Weber, F., van Wezel, J., Campuzano, J. C., Osborn, R., Randeria, M., Trivedi, N., Norman, M. R., and Rosenkranz, S. Emergence of coherence in the charge-density wave state of 2H-NbSe2. United States: N. p., 2015. Web. doi:10.1038/ncomms7313.
Chatterjee, U., Zhao, J., Iavarone, M., Di Capua, R., Castellan, J. P., Karapetrov, G., Malliakas, C. D., Kanatzidis, M. G., Claus, H., Ruff, J. P. C., Weber, F., van Wezel, J., Campuzano, J. C., Osborn, R., Randeria, M., Trivedi, N., Norman, M. R., & Rosenkranz, S. Emergence of coherence in the charge-density wave state of 2H-NbSe2. United States. https://doi.org/10.1038/ncomms7313
Chatterjee, U., Zhao, J., Iavarone, M., Di Capua, R., Castellan, J. P., Karapetrov, G., Malliakas, C. D., Kanatzidis, M. G., Claus, H., Ruff, J. P. C., Weber, F., van Wezel, J., Campuzano, J. C., Osborn, R., Randeria, M., Trivedi, N., Norman, M. R., and Rosenkranz, S. Tue . "Emergence of coherence in the charge-density wave state of 2H-NbSe2". United States. https://doi.org/10.1038/ncomms7313. https://www.osti.gov/servlets/purl/1219582.
@article{osti_1219582,
title = {Emergence of coherence in the charge-density wave state of 2H-NbSe2},
author = {Chatterjee, U. and Zhao, J. and Iavarone, M. and Di Capua, R. and Castellan, J. P. and Karapetrov, G. and Malliakas, C. D. and Kanatzidis, M. G. and Claus, H. and Ruff, J. P. C. and Weber, F. and van Wezel, J. and Campuzano, J. C. and Osborn, R. and Randeria, M. and Trivedi, N. and Norman, M. R. and Rosenkranz, S.},
abstractNote = {A charge density wave (CDW) state has a broken symmetry described by a complex order parameter with an amplitude and a phase. The conventional view, based on clean, weak-coupling systems, is that a finite amplitude and long-range phase coherence set in simultaneously at the CDW transition temperature Tcdw. Here we investigate, using photoemission, X-ray scattering and scanning tunneling microscopy, the canonical CDW compound 2H-NbSe2 intercalated with Mn and Co and show that the conventional view is untenable. We find that, either at high temperature or at large intercalation, CDW order becomes short- range with a well-defined amplitude that impacts the electronic dispersion, giving rise to an energy gap. The phase transition at Tcdw marks the onset of long-range order with global phase coherence leading to sharp electronic excitations. Our observations emphasize the importance of phase fluctuations in strongly coupled CDW systems and provide insights into the significance of phase incoherence in ‘pseudogap’ states.},
doi = {10.1038/ncomms7313},
journal = {Nature Communications},
number = ,
volume = 6,
place = {United States},
year = {Tue Feb 17 00:00:00 EST 2015},
month = {Tue Feb 17 00:00:00 EST 2015}
}

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Works referenced in this record:

Importance of phase fluctuations in superconductors with small superfluid density
journal, March 1995

  • Emery, V. J.; Kivelson, S. A.
  • Nature, Vol. 374, Issue 6521
  • DOI: 10.1038/374434a0

Microscopic model of charge-density waves in 2 H Ta Se 2
journal, July 1977


Strong-Coupling Theory of Charge-Density-Wave Transitions
journal, July 1983


On the origin of charge-density waves in select layered transition-metal dichalcogenides
journal, May 2011


Preformed Excitonic Liquid Route to a Charge Density Wave in 2 H TaSe 2
journal, June 2011


Electronic structure of two-dimensional hexagonal diselenides: Charge density waves and pseudogap behavior
journal, April 2012

  • Kuchinskii, E. Z.; Nekrasov, I. A.; Sadovskii, M. V.
  • Journal of Experimental and Theoretical Physics, Vol. 114, Issue 4
  • DOI: 10.1134/S1063776112020252

Single- and two-particle energy gaps across the disorder-driven superconductor–insulator transition
journal, July 2011

  • Bouadim, Karim; Loh, Yen Lee; Randeria, Mohit
  • Nature Physics, Vol. 7, Issue 11
  • DOI: 10.1038/nphys2037

Spectroscopic evidence for a pseudogap in the normal state of underdoped high-Tc superconductors
journal, July 1996

  • Ding, H.; Yokoya, T.; Campuzano, J. C.
  • Nature, Vol. 382, Issue 6586
  • DOI: 10.1038/382051a0

Excitation Gap in the Normal State of Underdoped Bi2Sr2CaCu2O8+delta
journal, July 1996


Vortex-like excitations and the onset of superconducting phase fluctuation in underdoped La2-xSrxCuO4
journal, August 2000

  • Xu, Z. A.; Ong, N. P.; Wang, Y.
  • Nature, Vol. 406, Issue 6795
  • DOI: 10.1038/35020016

Localization of preformed Cooper pairs in disordered superconductors
journal, January 2011

  • Sacépé, Benjamin; Dubouchet, Thomas; Chapelier, Claude
  • Nature Physics, Vol. 7, Issue 3
  • DOI: 10.1038/nphys1892

Observation of a pairing pseudogap in a two-dimensional Fermi gas
journal, November 2011

  • Feld, Michael; Fröhlich, Bernd; Vogt, Enrico
  • Nature, Vol. 480, Issue 7375
  • DOI: 10.1038/nature10627

Quasiparticle Spectra, Charge-Density Waves, Superconductivity, and Electron-Phonon Coupling in 2 H N b S e 2
journal, February 2004


Extended Phonon Collapse and the Origin of the Charge-Density Wave in 2 H NbSe 2
journal, September 2011


Study of Superlattice Formation in 2 H -Nb Se 2 and 2 H -Ta Se 2 by Neutron Scattering
journal, March 1975


Nb–Nb Interactions Define the Charge Density Wave Structure of 2H-NbSe 2
journal, January 2013

  • Malliakas, Christos D.; Kanatzidis, Mercouri G.
  • Journal of the American Chemical Society, Vol. 135, Issue 5
  • DOI: 10.1021/ja3120554

Charge-density waves and localization in electron-irradiated 1 T T a S 2
journal, May 1981


Effect of Te doping on superconductivity and charge-density wave in dichalcogenides 2H-NbSe 2- x Te x ( x = 0, 0.1, 0.2)
journal, August 2007


Two Energy Gaps and Fermi-Surface “Arcs” in NbSe 2
journal, April 2009


Gaps and kinks in the electronic structure of the superconductor 2 H -NbSe 2 from angle-resolved photoemission at 1 K
journal, June 2012


Quantum phase transition from triangular to stripe charge order in NbSe2
journal, January 2013

  • Soumyanarayanan, A.; Yee, M. M.; He, Y.
  • Proceedings of the National Academy of Sciences, Vol. 110, Issue 5
  • DOI: 10.1073/pnas.1211387110

Charge-density-wave mechanism in the 2 H NbSe 2 family: Angle-resolved photoemission studies
journal, May 2001


Charge-Density-Wave Mechanism in 2 H NbSe 2 : Photoemission Results
journal, May 1999


Primary Role of the Barely Occupied States in the Charge Density Wave Formation of NbSe 2
journal, November 2008


BCS-Like Bogoliubov Quasiparticles in High- T c Superconductors Observed by Angle-Resolved Photoemission Spectroscopy
journal, May 2003


Direct observation of particle-hole mixing in the superconducting state by angle-resolved photoemission
journal, June 1996


Particle–hole symmetry breaking in the pseudogap state of Bi2201
journal, April 2010

  • Hashimoto, Makoto; He, Rui-Hua; Tanaka, Kiyohisa
  • Nature Physics, Vol. 6, Issue 6
  • DOI: 10.1038/nphys1632

Evidence for Pairing above the Transition Temperature of Cuprate Superconductors from the Electronic Dispersion in the Pseudogap Phase
journal, September 2008


Charge-density waves observed at 4.2 K by scanning-tunneling microscopy
journal, February 1988


Spatial and energy variation of the local density of states in the charge density wave phase of 2H–NbSe2
journal, March 1996

  • Mallet, P.
  • Journal of Vacuum Science & Technology B: Microelectronics and Nanometer Structures, Vol. 14, Issue 2
  • DOI: 10.1116/1.588402

Visualizing the charge density wave transition in 2 H - NbSe 2 in real space
journal, June 2014


Electronic state of NbSe2 investigated by STM/STS
journal, May 2003


Electronic phase diagram of high-temperature copper oxide superconductors
journal, May 2011

  • Chatterjee, U.; Ai, D.; Zhao, J.
  • Proceedings of the National Academy of Sciences, Vol. 108, Issue 23
  • DOI: 10.1073/pnas.1101008108

Localized Superconductivity in the Quantum-Critical Region of the Disorder-Driven Superconductor-Insulator Transition in TiN Thin Films
journal, December 2007


Growth of faceted niobium diselenide
journal, March 1994


Extended X-ray Absorption Fine Structure spectroscopy in Co 0.013 NbSe 2
journal, January 2010


Effect of magnetic impurities on the vortex lattice properties in NbSe 2 single crystals
journal, November 2008


Photoemission in the High-T c Superconductors
book, January 2008


Particle-Hole Symmetry Breaking in the Pseudogap State of Bi2201
text, January 2009


Observation of a pairing pseudogap in a two-dimensional Fermi gas
text, January 2011


Electronic phase diagram of high temperature copper oxide superconductors
text, January 2013


Nb–Nb Interactions Define the Charge Density Wave Structure of 2H-NbSe 2
journal, January 2013

  • Malliakas, Christos D.; Kanatzidis, Mercouri G.
  • Journal of the American Chemical Society, Vol. 135, Issue 5
  • DOI: 10.1021/ja3120554

Vortex-like excitations and the onset of superconducting phase fluctuation in underdoped La2-xSrxCuO4
journal, August 2000

  • Xu, Z. A.; Ong, N. P.; Wang, Y.
  • Nature, Vol. 406, Issue 6795
  • DOI: 10.1038/35020016

Localization of preformed Cooper pairs in disordered superconductors
journal, January 2011

  • Sacépé, Benjamin; Dubouchet, Thomas; Chapelier, Claude
  • Nature Physics, Vol. 7, Issue 3
  • DOI: 10.1038/nphys1892

Electronic phase diagram of high-temperature copper oxide superconductors
journal, May 2011

  • Chatterjee, U.; Ai, D.; Zhao, J.
  • Proceedings of the National Academy of Sciences, Vol. 108, Issue 23
  • DOI: 10.1073/pnas.1101008108

On the origin of charge-density waves in select layered transition-metal dichalcogenides
journal, May 2011


Weak pinning and hexatic order in a doped two-dimensional charge-density-wave system
journal, June 1991


Excitation Gap in the Normal State of Underdoped Bi2Sr2CaCu2O8+delta
journal, July 1996


Observation of a pairing pseudogap in a two-dimensional Fermi gas
text, January 2011


A quantum phase transition from triangular to stripe charge order in NbSe$_{2}$
text, January 2012


Works referencing / citing this record:

2D Group IVB Transition Metal Dichalcogenides
journal, August 2018

  • Yan, Chaoyi; Gong, Chuanhui; Wangyang, Peihua
  • Advanced Functional Materials, Vol. 28, Issue 39
  • DOI: 10.1002/adfm.201803305

Edge-Epitaxial Growth of 2D NbS 2 -WS 2 Lateral Metal-Semiconductor Heterostructures
journal, August 2018


Charge order from orbital-dependent coupling evidenced by NbSe2
journal, May 2015

  • Flicker, Felix; van Wezel, Jasper
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms8034

Using controlled disorder to probe the interplay between charge order and superconductivity in NbSe2
journal, July 2018


Distinction between pristine and disorder-perturbed charge density waves in ZrTe3
journal, January 2020


Pressure-induced metallization and superconducting phase in ReS 2
journal, March 2017


Evidence for topological defects in a photoinduced phase transition
journal, October 2018


Intimate link between charge density wave, pseudogap and superconducting energy scales in cuprates
journal, April 2019


Enhancement of superconducting properties and flux pinning mechanism on Cr0.0005NbSe2 single crystal under Hydrostatic pressure
journal, January 2019


Spectroscopic signature of moment-dependent electron–phonon coupling in 2H-TaS 2
journal, January 2017

  • Wijayaratne, Kapila; Zhao, Junjing; Malliakas, Christos
  • Journal of Materials Chemistry C, Vol. 5, Issue 43
  • DOI: 10.1039/c7tc02641b

High-temperature charge density wave correlations in La 1.875 Ba 0.125 CuO 4 without spin–charge locking
journal, November 2017

  • Miao, H.; Lorenzana, J.; Seibold, G.
  • Proceedings of the National Academy of Sciences, Vol. 114, Issue 47
  • DOI: 10.1073/pnas.1708549114

Atomic-scale strain manipulation of a charge density wave
journal, June 2018

  • Gao, Shang; Flicker, Felix; Sankar, Raman
  • Proceedings of the National Academy of Sciences, Vol. 115, Issue 27
  • DOI: 10.1073/pnas.1718931115

Disorder raises the critical temperature of a cuprate superconductor
journal, May 2019

  • Leroux, Maxime; Mishra, Vivek; Ruff, Jacob P. C.
  • Proceedings of the National Academy of Sciences, Vol. 116, Issue 22
  • DOI: 10.1073/pnas.1817134116

Configurational electronic states in layered transition metal dichalcogenides
journal, August 2019

  • Vodeb, Jaka; Kabanov, Viktor V.; Gerasimenko, Yaroslav A.
  • New Journal of Physics, Vol. 21, Issue 8
  • DOI: 10.1088/1367-2630/ab3057

First-principles study of the thermodynamic and vibrational properties of ReS 2 under pressure
journal, December 2019


Unveiling hidden charge density waves in single-layer NbSe 2 by impurities
journal, November 2018


Pseudogaps and Emergence of Coherence in Two-Dimensional Electron Liquids in SrTiO 3
journal, July 2016


Local Real-Space View of the Achiral 1 T TiSe 2 2 × 2 × 2 Charge Density Wave
journal, March 2018


Dielectric Properties of NbxW1-xSe2 Alloys
journal, January 2019

  • Rigosi, Albert F.; Hill, Heather; Krylyuk, Sergiy
  • Journal of Research of the National Institute of Standards and Technology, Vol. 124
  • DOI: 10.6028/jres.124.035

Incommensurate Phonon Anomaly and the Nature of Charge Density Waves in Cuprates
text, January 2018


Charge Order from Orbital-dependent Coupling Evidenced by NbSe$_2$
text, January 2015


Disorder raises the critical temperature of a cuprate superconductor
text, January 2018


Distinction between pristine and disorder-perturbed charge density waves in ZrTe3
journal, January 2020