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

Title: Evidence for a quantum dipole liquid state in an organic quasi–two-dimensional material

Abstract

Mott insulators are commonly pictured with electrons localized on lattice sites, with their low-energy degrees of freedom involving spins only. Here, we observe emergent charge degrees of freedom in a molecule-based Mott insulator kappa-(BEDT-TTF)(2)Hg(SCN)(2)Br, resulting in a quantum dipole liquid state. Electrons localized on molecular dimer lattice sites form electric dipoles that do not order at low temperatures and fluctuate with frequency detected experimentally in our Raman spectroscopy experiments. The heat capacity and Raman scattering response are consistent with a scenario in which the composite spin and electric dipole degrees of freedom remain fluctuating down to the lowest measured temperatures.

Authors:
ORCiD logo; ORCiD logo; ; ORCiD logo; ; ; ; ORCiD logo
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science - Office of Basic Energy Sciences - Materials Sciences and Engineering Division - Midwest Integrated Center for Computational Materials (MICCoM); National High Magnetic Field Laboratory (NHMFL); USDOE Office of Science (SC)
OSTI Identifier:
1483416
DOE Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article
Journal Name:
Science
Additional Journal Information:
Journal Volume: 360; Journal Issue: 6393; Journal ID: ISSN 0036-8075
Publisher:
AAAS
Country of Publication:
United States
Language:
English

Citation Formats

Hassan, Nora, Cunningham, Streit, Mourigal, Martin, Zhilyaeva, Elena I., Torunova, Svetlana A., Lyubovskaya, Rimma N., Schlueter, John A., and Drichko, Natalia. Evidence for a quantum dipole liquid state in an organic quasi–two-dimensional material. United States: N. p., 2018. Web. doi:10.1126/science.aan6286.
Hassan, Nora, Cunningham, Streit, Mourigal, Martin, Zhilyaeva, Elena I., Torunova, Svetlana A., Lyubovskaya, Rimma N., Schlueter, John A., & Drichko, Natalia. Evidence for a quantum dipole liquid state in an organic quasi–two-dimensional material. United States. doi:10.1126/science.aan6286.
Hassan, Nora, Cunningham, Streit, Mourigal, Martin, Zhilyaeva, Elena I., Torunova, Svetlana A., Lyubovskaya, Rimma N., Schlueter, John A., and Drichko, Natalia. Thu . "Evidence for a quantum dipole liquid state in an organic quasi–two-dimensional material". United States. doi:10.1126/science.aan6286.
@article{osti_1483416,
title = {Evidence for a quantum dipole liquid state in an organic quasi–two-dimensional material},
author = {Hassan, Nora and Cunningham, Streit and Mourigal, Martin and Zhilyaeva, Elena I. and Torunova, Svetlana A. and Lyubovskaya, Rimma N. and Schlueter, John A. and Drichko, Natalia},
abstractNote = {Mott insulators are commonly pictured with electrons localized on lattice sites, with their low-energy degrees of freedom involving spins only. Here, we observe emergent charge degrees of freedom in a molecule-based Mott insulator kappa-(BEDT-TTF)(2)Hg(SCN)(2)Br, resulting in a quantum dipole liquid state. Electrons localized on molecular dimer lattice sites form electric dipoles that do not order at low temperatures and fluctuate with frequency detected experimentally in our Raman spectroscopy experiments. The heat capacity and Raman scattering response are consistent with a scenario in which the composite spin and electric dipole degrees of freedom remain fluctuating down to the lowest measured temperatures.},
doi = {10.1126/science.aan6286},
journal = {Science},
issn = {0036-8075},
number = 6393,
volume = 360,
place = {United States},
year = {2018},
month = {6}
}

Works referenced in this record:

Raman scattering in a Heisenberg S = 1 2 antiferromagnet on the triangular lattice
journal, May 2008


Quantum melting of magnetic order in an organic dimer Mott-insulating system
journal, May 2016


Spin liquids in frustrated magnets
journal, March 2010


Physical Properties of Some ET-Based Organic Metals and Superconductors with Mercury Containing Anions
journal, December 1996

  • Lyubovskii, R. B.; Lyubovskaya, R. N.; Dyachenko, O. A.
  • Journal de Physique I, Vol. 6, Issue 12
  • DOI: 10.1051/jp1:1996178

Dynamical Reduction of the Dimensionality of Exchange Interactions and the “Spin-Liquid” Phase of κ - ( BEDT TTF ) 2 X
journal, August 2017


Thermodynamic properties of a spin-1/2 spin-liquid state in a κ-type organic salt
journal, April 2008

  • Yamashita, Satoshi; Nakazawa, Yasuhiro; Oguni, Masaharu
  • Nature Physics, Vol. 4, Issue 6
  • DOI: 10.1038/nphys942

A new series of ET-based organic metals: Synthesis, crystal structure and properties
journal, March 1993


Optical Properties of Two-Dimensional Organic Conductors: Signatures of Charge Ordering and Correlation Effects
journal, November 2004

  • Dressel, Martin; Drichko, Natalia
  • Chemical Reviews, Vol. 104, Issue 11
  • DOI: 10.1021/cr030642f

Dynamical properties of a strongly correlated model for quarter-filled layered organic molecular crystals
journal, December 2003


Charge-Fluctuation Contribution to the Raman Response in Superconducting Cuprates
journal, September 2005


Antiferromagnetic fluctuations in a quasi-two-dimensional organic superconductor detected by Raman spectroscopy
journal, October 2015


Temperature dependence of Raman-active optical phonons in Bi 2 Se 3 and Sb 2 Te 3
journal, February 2012

  • Kim, Y.; Chen, X.; Wang, Z.
  • Applied Physics Letters, Vol. 100, Issue 7
  • DOI: 10.1063/1.3685465

Drude weight in quasi-two-dimensional organic conductors close to the Mott transition: Optical studies of the bandwidth, filling and temperature dependence
journal, September 2007

  • Drichko, Natalia; Dumm, Michael; Faltermeier, Daniel
  • Physica C: Superconductivity and its Applications, Vol. 460-462
  • DOI: 10.1016/j.physc.2007.03.375

Quantum spin liquid states
journal, April 2017


Thermodynamic Properties of κ-(BEDT-TTF)2X Salts: Electron Correlations and Superconductivity
journal, June 2012


Metallic state and charge-order metal-insulator transition in the quasi-two-dimensional conductor κ -(BEDT-TTF) 2 Hg(SCN) 2 Cl
journal, February 2014


The C=C Stretching Vibrations of κ-(BEDT–TTF) 2 Cu[N(CN) 2 ]Br and Its Isotope Analogues
journal, December 2001

  • Maksimuk, Mikhail; Yakushi, Kyuya; Taniguchi, Hiromi
  • Journal of the Physical Society of Japan, Vol. 70, Issue 12
  • DOI: 10.1143/JPSJ.70.3728

Examination of the Charge-Sensitive Vibrational Modes in Bis(ethylenedithio)tetrathiafulvalene
journal, August 2005

  • Yamamoto, Takashi; Uruichi, Mikio; Yamamoto, Kaoru
  • The Journal of Physical Chemistry B, Vol. 109, Issue 32
  • DOI: 10.1021/jp050247o

Spin-Orbital Singlet and Quantum Critical Point on the Diamond Lattice: FeSc 2 S 4
journal, March 2009


A quantum dipolar spin liquid
journal, February 2018


Metal-insulator transition in the dimerized organic conductor κ ( BEDT-TTF ) 2 Hg ( SCN ) 2 Br
journal, August 2017


Raman Spectroscopy Study of Charge Fluctuation in the Spin-Liquid Candidate κ-(BEDT-TTF) 2 Cu 2 (CN) 3
journal, August 2015

  • Yakushi, Kyuya; Yamamoto, Kaoru; Yamamoto, Takashi
  • Journal of the Physical Society of Japan, Vol. 84, Issue 8
  • DOI: 10.7566/JPSJ.84.084711

Raman scattering for triangular lattices spin-1/2 Heisenberg antiferromagnets
journal, March 2007


Ferroelectric quantum criticality
journal, March 2014

  • Rowley, S. E.; Spalek, L. J.; Smith, R. P.
  • Nature Physics, Vol. 10, Issue 5
  • DOI: 10.1038/nphys2924

Pressure dependence of the metal-insulator transition in κ -(BEDT-TTF) 2 Hg(SCN) 2 Cl: optical and transport studies
journal, December 2016


The nature of boson peak in Raman scattering in glasses
journal, March 1986


Magnetic Raman Scattering Study of Spin Frustrated Systems, κ-(BEDT-TTF) 2 X
journal, July 2014

  • Nakamura, Yuto; Yoneyama, Naoki; Sasaki, Takahiko
  • Journal of the Physical Society of Japan, Vol. 83, Issue 7
  • DOI: 10.7566/JPSJ.83.074708

Quantum electric-dipole liquid on a triangular lattice
journal, February 2016

  • Shen, Shi-Peng; Wu, Jia-Chuan; Song, Jun-Da
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms10569

Inelastic light scattering from correlated electrons
journal, January 2007


Resonating valence-bond theory of phase transitions and superconductivity in La 2 CuO 4 -based compounds
journal, June 1987


Charge-order fluctuations and superconductivity in two-dimensional organic metals
journal, May 2014


Quantum electric dipoles in spin-liquid dimer Mott insulator κ -ET 2 Cu 2 ( CN ) 3
journal, December 2010


Absence of charge order in the dimerized κ -phase BEDT-TTF salts
journal, December 2012


Spin Liquid State in an Organic Mott Insulator with a Triangular Lattice
journal, September 2003


Magnetoelectric effect in organic molecular solids
journal, February 2016

  • Naka, Makoto; Ishihara, Sumio
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep20781

Paired electron crystal: Order from frustration in the quarter-filled band
journal, June 2011


Revision of Model Parameters for κ -Type Charge Transfer Salts: An Ab Initio Study
journal, August 2009


Optical Properties of a Quantum Spin Liquid Candidate Material, κ-(BEDT-TTF) 2 Ag 2 (CN) 3
journal, January 2017

  • Nakamura, Yuto; Hiramatsu, Takaaki; Yoshida, Yukihiro
  • Journal of the Physical Society of Japan, Vol. 86, Issue 1
  • DOI: 10.7566/JPSJ.86.014710