New Spin on Metal-Insulator Transitions

A special issue of Crystals (ISSN 2073-4352). This special issue belongs to the section "Inorganic Crystalline Materials".

Deadline for manuscript submissions: closed (20 April 2022) | Viewed by 60234

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Guest Editor
Institute of Solid State Physics, TU Wien, Wiedner Hauptstr. 8-10, 1040 Vienna, Austria
Interests: condensed matter physics; correlated electron systems; frustrated magnetism; quantum spin liquids; unconventional superconductivity; bad & strange metals; Mott metal-insulator transition; organic conductors; optical spectroscopy; nuclear magnetic resonance (NMR); uniaxial strain

Special Issue Information

Dear Colleagues,

Metal-insulator transitions (MITs) constitute a core subject of fundamental condensed-matter research. The localization of conduction electrons has been observed in a large variety of materials and gives rise to intriguing quantum phenomena such as unconventional superconductivity and exotic magnetism. Nearby a MIT, minuscule changes of interaction strength via chemical substitution, doping, physical pressure or even disorder can trigger spectacular resistivity changes from zero in a superconductor to infinity in an insulator near T = 0. While approaching an insulating state from the conducting side, deviations from Fermi-liquid transport in bad and strange metals are the rule rather than the exception, discussed in terms of spatial inhomogeneity and quantum criticality. Moreover, charge localization upon MITs has crucial impact on the magnetic degrees of freedom that are intensely studied towards the possible realization of a quantum spin liquid.

Solving the puzzles of correlated electron systems and the emergent phenomena around MITs has triggered enormous effort. As the drosophila of electron-electron interactions, the Mott MIT receives particular attention from theory as it can be studied using the Hubbard model. On the experimental side, the topic has been recently boosted by the advent of twisted Moiré bilayer systems, but true bulk materials, such as organic charge-transfer salts, fullerides and transition-metal oxides, remain indispensable for elucidating macroscopic quantum phases such as unconventional superconductivity and frustrated magnetism. Various novel methods have become available lately to tune and map the complex evolution of the metallic and insulating phases at cryogenic temperatures, including uniaxial strain and imaging techniques such as near-field microscopy. Also controlled variation of disorder has been utilized to study Griffiths phases and Anderson-type MITs.

This Special Issue shall provide a glimpse into the latest progress in answering the open questions around MITs, and is also open to reports on advancements towards possible applications.

Dr. Andrej Pustogow
Guest Editor

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Keywords

  • correlated electron systems
  • Mott metal-insulator transition
  • Anderson localization
  • bad & strange metals
  • non-Fermi liquid transport
  • unconventional superconductivity
  • quantum criticality
  • critical endpoint
  • charge order
  • frustrated magnetism
  • quantum spin liquids
  • antiferromagnetic order
  • magneto-elastic coupling
  • first order transitions
  • second order transitions
  • structural phase transitions
  • electronic phase separation
  • percolation
  • structural properties
  • dielectric properties
  • transport properties
  • magnetic properties
  • optical properties
  • thermodynamic properties
  • NMR and ESR
  • scanning near-field optical microscopy (SNOM)
  • materials synthesis
  • band structure calculations
  • dynamical mean-field theory (DMFT)
  • Hubbard model
  • organic conductors
  • molecular charge-transfer salts
  • alkali fullerides A3C60
  • vanadium oxides
  • transition-metal compounds

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Published Papers (20 papers)

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Editorial

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2 pages, 176 KiB  
Editorial
New Spin on Metal-Insulator Transitions
by Andrej Pustogow
Crystals 2023, 13(1), 64; https://doi.org/10.3390/cryst13010064 - 30 Dec 2022
Viewed by 1380
Abstract
Metal-insulator transitions (MITs) constitute a core subject of fundamental condensed-matter research [...] Full article
(This article belongs to the Special Issue New Spin on Metal-Insulator Transitions)

Research

Jump to: Editorial, Review, Other

20 pages, 9783 KiB  
Article
A New Charge-Ordered Molecular Conductor: κ-(BEDT-TTF)2K+(18-crown-6)[CoII(NCS)4]∙(H2O)
by Andrei A. Bardin, Tatiana G. Prokhorova and Lev I. Buravov
Crystals 2023, 13(10), 1504; https://doi.org/10.3390/cryst13101504 - 16 Oct 2023
Viewed by 1313
Abstract
A new molecular conductor, i.e., κ-(BEDT-TTF)2K+(18-crown-6)[CoII(NCS)4]∙(H2O), is semiconductive with substantial charge gap values (ΔE) of 0.57 eV (measured) and 0.37 eV (calculated). There is a full band separation despite formal [...] Read more.
A new molecular conductor, i.e., κ-(BEDT-TTF)2K+(18-crown-6)[CoII(NCS)4]∙(H2O), is semiconductive with substantial charge gap values (ΔE) of 0.57 eV (measured) and 0.37 eV (calculated). There is a full band separation despite formal average charge on BEDT-TTF of +0.5 and κ(kappa)-type packing of BEDT-TTF dimers that favors high conductivity. X-ray crystal structure analysis reveals complete charge ordering with full Coulomb charge on unique BEDT-TTF radical cations A (QA = +1), while unique molecules B are uncharged (QB = 0). Geometries of A (flat) and B (bent) differ considerably and are in accordance with the ascribing charges. Charge segregation is enhanced by forming tight face-to-face BEDT-TTF dimers AA (QAA = +2) and BB (QBB = 0). Strongly interacting double-charged dimers AA form “superstripes” running along a that are interleaved along b with chains of neutral dimers BB. Peculiar extremely thick (13.7 Å) four-decker insulating anion layers cast strong Coulomb potential onto the conductive layers predetermining charge localization in the latter. Full article
(This article belongs to the Special Issue New Spin on Metal-Insulator Transitions)
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13 pages, 2400 KiB  
Article
Neural Network Solver for Small Quantum Clusters
by Nicholas Walker, Samuel Kellar, Yi Zhang, Ka-Ming Tam and Juana Moreno
Crystals 2022, 12(9), 1269; https://doi.org/10.3390/cryst12091269 - 6 Sep 2022
Cited by 3 | Viewed by 2503
Abstract
Machine learning approaches have recently been applied to the study of various problems in physics. Most of these studies are focused on interpreting the data generated by conventional numerical methods or the data on an existing experimental database. An interesting question is whether [...] Read more.
Machine learning approaches have recently been applied to the study of various problems in physics. Most of these studies are focused on interpreting the data generated by conventional numerical methods or the data on an existing experimental database. An interesting question is whether it is possible to use a machine learning approach, in particular a neural network, for solving the many-body problem. In this paper, we present a neural network solver for the single impurity Anderson model, the paradigm of an interacting quantum problem in small clusters. We demonstrate that the neural-network-based solver provides quantitative accurate results for the spectral function as compared to the exact diagonalization method. This opens the possibility of utilizing the neural network approach as an impurity solver for other many-body numerical approaches, such as the dynamical mean field theory. Full article
(This article belongs to the Special Issue New Spin on Metal-Insulator Transitions)
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24 pages, 5774 KiB  
Article
How to Recognize the Universal Aspects of Mott Criticality?
by Yuting Tan, Vladimir Dobrosavljević and Louk Rademaker
Crystals 2022, 12(7), 932; https://doi.org/10.3390/cryst12070932 - 30 Jun 2022
Cited by 5 | Viewed by 2558
Abstract
In this paper we critically discuss several examples of two-dimensional electronic systems displaying interaction-driven metal-insulator transitions of the Mott (or Wigner–Mott) type, including dilute two-dimension electron gases (2DEG) in semiconductors, Mott organic materials, as well as the recently discovered transition-metal dichalcogenide (TMD) moiré [...] Read more.
In this paper we critically discuss several examples of two-dimensional electronic systems displaying interaction-driven metal-insulator transitions of the Mott (or Wigner–Mott) type, including dilute two-dimension electron gases (2DEG) in semiconductors, Mott organic materials, as well as the recently discovered transition-metal dichalcogenide (TMD) moiré bilayers. Remarkably similar behavior is found in all these systems, which is starting to paint a robust picture of Mott criticality. Most notable, on the metallic side a resistivity maximum is observed whose temperature scale vanishes at the transition. We compare the available experimental data on these systems to three existing theoretical scenarios: spinon theory, Dynamical Mean Field Theory (DMFT) and percolation theory. We show that the DMFT and percolation pictures for Mott criticality can be distinguished by studying the origins of the resistivity maxima using an analysis of the dielectric response. Full article
(This article belongs to the Special Issue New Spin on Metal-Insulator Transitions)
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11 pages, 3547 KiB  
Article
A Database for Crystalline Organic Conductors and Superconductors
by Owen Ganter, Kevin Feeny, Morgan Brooke-deBock, Stephen M. Winter and Charles C. Agosta
Crystals 2022, 12(7), 919; https://doi.org/10.3390/cryst12070919 - 28 Jun 2022
Cited by 2 | Viewed by 2838
Abstract
We present a prototype database for quasi two-dimensional crystalline organic conductors and superconductors based on molecules related to bis(ethylenedithio)tetrathiafulvalene (BEDT-TTF, ET). The database includes crystal structures, calculated electronic structures, and experimentally measured properties such as the superconducting transition temperature and critical magnetic fields. [...] Read more.
We present a prototype database for quasi two-dimensional crystalline organic conductors and superconductors based on molecules related to bis(ethylenedithio)tetrathiafulvalene (BEDT-TTF, ET). The database includes crystal structures, calculated electronic structures, and experimentally measured properties such as the superconducting transition temperature and critical magnetic fields. We obtained crystal structures from the Cambridge Structural Database and created a crystal structure analysis algorithm to identify cation molecules and execute tight binding electronic structure calculations. We used manual data entry to encode experimentally measured properties reported in publications. Crystalline organic conductors and superconductors exhibit a wide variety of electronic ground states, particularly those with correlations. We hope that this database will ultimately lead to a better understanding of the fundamental mechanisms of such states. Full article
(This article belongs to the Special Issue New Spin on Metal-Insulator Transitions)
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10 pages, 2327 KiB  
Article
Optical Conductivity Spectra of Charge-Crystal and Charge-Glass States in a Series of θ-Type BEDT-TTF Compounds
by Kenichiro Hashimoto, Ryota Kobayashi, Satoshi Ohkura, Satoru Sasaki, Naoki Yoneyama, Masayuki Suda, Hiroshi M. Yamamoto and Takahiko Sasaki
Crystals 2022, 12(6), 831; https://doi.org/10.3390/cryst12060831 - 12 Jun 2022
Cited by 2 | Viewed by 2833
Abstract
In the 3/4-filled band system θ-(BEDT-TTF)2X with a two-dimensional triangular lattice, charge ordering (CO) often occurs due to strong inter-site Coulomb repulsion. However, the strong geometrical frustration of the triangular lattice can prohibit long-range CO, resulting in a charge-glass state [...] Read more.
In the 3/4-filled band system θ-(BEDT-TTF)2X with a two-dimensional triangular lattice, charge ordering (CO) often occurs due to strong inter-site Coulomb repulsion. However, the strong geometrical frustration of the triangular lattice can prohibit long-range CO, resulting in a charge-glass state in which the charge configurations are randomly distributed. Here, we investigate the charge-glass states of orthorhombic and monoclinic θ-type BEDT-TTF salts by measuring the electrical resistivity and optical conductivity spectra. We find a substantial difference between the charge-glass states of the orthorhombic and monoclinic systems. The charge-glass state in the orthorhombic system with an isotropic triangular lattice exhibits larger low-energy excitations than that in the monoclinic one with an anisotropic triangular lattice and becomes more metallic as the isotropy of the triangular lattice increases. These results can be understood by the different charge-glass formation mechanisms in the two systems: in the orthorhombic system, the charge-glass state originates from geometric frustration due to the equilateral triangular lattice, leading to metallic 3-fold COs, whereas in the monoclinic system, the charge-glass formation originates from geometric frustration of the isosceles triangular lattice, in which the charge-glass state is described by the superposition of insulating 2-fold stripe COs. Full article
(This article belongs to the Special Issue New Spin on Metal-Insulator Transitions)
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22 pages, 7726 KiB  
Article
Grain-Size-Induced Collapse of Variable Range Hopping and Promotion of Ferromagnetism in Manganite La0.5Ca0.5MnO3
by Nikolina Novosel, David Rivas Góngora, Zvonko Jagličić, Emil Tafra, Mario Basletić, Amir Hamzić, Teodoro Klaser, Željko Skoko, Krešimir Salamon, Ivna Kavre Piltaver, Mladen Petravić, Bojana Korin-Hamzić, Silvia Tomić, Boris P. Gorshunov, Tao Zhang, Tomislav Ivek and Matija Čulo
Crystals 2022, 12(5), 724; https://doi.org/10.3390/cryst12050724 - 19 May 2022
Cited by 6 | Viewed by 2878
Abstract
Among transition metal oxides, manganites have attracted significant attention because of colossal magnetoresistance (CMR)—a magnetic field-induced metal–insulator transition close to the Curie temperature. CMR is closely related to the ferromagnetic (FM) metallic phase which strongly competes with the antiferromagnetic (AFM) charge ordered (CO) [...] Read more.
Among transition metal oxides, manganites have attracted significant attention because of colossal magnetoresistance (CMR)—a magnetic field-induced metal–insulator transition close to the Curie temperature. CMR is closely related to the ferromagnetic (FM) metallic phase which strongly competes with the antiferromagnetic (AFM) charge ordered (CO) phase, where conducting electrons localize and create a long range order giving rise to insulator-like behavior. One of the major open questions in manganites is the exact origin of this insulating behavior. Here we report a dc resistivity and magnetization study on manganite La1xCaxMnO3 ceramic samples with different grain size, at the very boundary between CO/AFM insulating and FM metallic phases x=0.5. Clear signatures of variable range hopping (VRH) are discerned in resistivity, implying the disorder-induced (Anderson) localization of conducting electrons. A significant increase of disorder associated with the reduction in grain size, however, pushes the system in the opposite direction from the Anderson localization scenario, resulting in a drastic decrease of resistivity, collapse of the VRH, suppression of the CO/AFM phase and growth of an FM contribution. These contradictory results are interpreted within the standard core-shell model and recent theories of Anderson localization of interacting particles. Full article
(This article belongs to the Special Issue New Spin on Metal-Insulator Transitions)
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13 pages, 10543 KiB  
Article
Fingerprints of Topotactic Hydrogen in Nickelate Superconductors
by Liang Si, Paul Worm and Karsten Held
Crystals 2022, 12(5), 656; https://doi.org/10.3390/cryst12050656 - 4 May 2022
Cited by 15 | Viewed by 4879
Abstract
Superconductivity has entered the nickel age marked by enormous experimental and theoretical efforts. Notwithstanding, synthesizing nickelate superconductors remains extremely challenging, not least due to incomplete oxygen reduction and topotactic hydrogen. Here, we present density-functional theory calculations for nickelate superconductors with additional topotactic hydrogen [...] Read more.
Superconductivity has entered the nickel age marked by enormous experimental and theoretical efforts. Notwithstanding, synthesizing nickelate superconductors remains extremely challenging, not least due to incomplete oxygen reduction and topotactic hydrogen. Here, we present density-functional theory calculations for nickelate superconductors with additional topotactic hydrogen or oxygen, namely La1xSrxNiO2Hδ and LaNiO2+δ. We identify a phonon mode as a possible indication for topotactic hydrogen and discuss the charge redistribution patterns around oxygen and hydrogen impurities. Full article
(This article belongs to the Special Issue New Spin on Metal-Insulator Transitions)
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8 pages, 2018 KiB  
Article
A Discrepancy in Thermal Conductivity Measurement Data of Quantum Spin Liquid β′-EtMe3Sb[Pd(dmit)2]2 (dmit = 1,3-Dithiol-2-thione-4,5-dithiolate)
by Reizo Kato, Masashi Uebe, Shigeki Fujiyama and Hengbo Cui
Crystals 2022, 12(1), 102; https://doi.org/10.3390/cryst12010102 - 13 Jan 2022
Cited by 12 | Viewed by 3319
Abstract
A molecular Mott insulator β′-EtMe3Sb[Pd(dmit)2]2 is a quantum spin liquid candidate. In 2010, it was reported that thermal conductivity of β′-EtMe3Sb[Pd(dmit)2]2 is characterized by its large value and gapless behavior (a finite temperature-linear [...] Read more.
A molecular Mott insulator β′-EtMe3Sb[Pd(dmit)2]2 is a quantum spin liquid candidate. In 2010, it was reported that thermal conductivity of β′-EtMe3Sb[Pd(dmit)2]2 is characterized by its large value and gapless behavior (a finite temperature-linear term). In 2019, however, two other research groups reported opposite data (much smaller value and a vanishingly small temperature-linear term) and the discrepancy in the thermal conductivity measurement data emerges as a serious problem concerning the ground state of the quantum spin liquid. Recently, the cooling rate was proposed to be an origin of the discrepancy. We examined effects of the cooling rate on electrical resistivity, low-temperature crystal structure, and 13C-NMR measurements and could not find any significant cooling rate dependence. Full article
(This article belongs to the Special Issue New Spin on Metal-Insulator Transitions)
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8 pages, 3185 KiB  
Article
Metallic Conduction and Carrier Localization in Two-Dimensional BEDO-TTF Charge-Transfer Solid Crystals
by Hiroshi Ito, Motoki Matsuno, Seiu Katagiri, Shinji K. Yoshina, Taishi Takenobu, Manabu Ishikawa, Akihiro Otsuka, Hideki Yamochi, Yukihiro Yoshida, Gunzi Saito, Yongbing Shen and Masahiro Yamashita
Crystals 2022, 12(1), 23; https://doi.org/10.3390/cryst12010023 - 24 Dec 2021
Cited by 2 | Viewed by 3248
Abstract
Charge-transfer salts based on bis(ethylenedioxy)tetrathiafulvalene (BEDO-TTF or BO for short) provide a stable two-dimensional (2D) metallic state, while the electrical resistance often shows an upturn at low temperatures below ~10 K. Such 2D weak carrier localization was first recognized for BO salts in [...] Read more.
Charge-transfer salts based on bis(ethylenedioxy)tetrathiafulvalene (BEDO-TTF or BO for short) provide a stable two-dimensional (2D) metallic state, while the electrical resistance often shows an upturn at low temperatures below ~10 K. Such 2D weak carrier localization was first recognized for BO salts in the Langmuir–Blodgett films fabricated with fatty acids; however, it has not been characterized in charge-transfer solid crystals. In this paper, we discuss the carrier localization of two crystalline BO charge-transfer salts with or without magnetic ions at low temperatures through the analysis of the weak negative magnetoresistance. The phase coherence lengths deduced with temperature dependence are largely dominated by the electron–electron scattering mechanism. These results indicate that the resistivity upturn at low temperatures is caused by the 2D weak localization. Disorders causing elastic scattering within the metallic domains, such as those of terminal ethylene groups, should be suppressed to prevent the localization. Full article
(This article belongs to the Special Issue New Spin on Metal-Insulator Transitions)
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12 pages, 2019 KiB  
Article
Electronic Heat Capacity and Lattice Softening of Partially Deuterated Compounds of κ-(BEDT-TTF)2Cu[N(CN)2]Br
by Yuki Matsumura, Shusaku Imajo, Satoshi Yamashita, Hiroki Akutsu and Yasuhiro Nakazawa
Crystals 2022, 12(1), 2; https://doi.org/10.3390/cryst12010002 - 21 Dec 2021
Cited by 4 | Viewed by 2917
Abstract
Thermodynamic investigation by calorimetric measurements of the layered organic superconductors, κ-(BEDT-TTF)2Cu[N(CN)2]Br and its partially deuterated compounds of κ-(d[2,2]-BEDT-TTF)2Cu[N(CN)2]Br and κ-(d[3,3]-BEDT-TTF)2Cu[N(CN)2]Br, performed in a wide temperature range is reported. The latter two [...] Read more.
Thermodynamic investigation by calorimetric measurements of the layered organic superconductors, κ-(BEDT-TTF)2Cu[N(CN)2]Br and its partially deuterated compounds of κ-(d[2,2]-BEDT-TTF)2Cu[N(CN)2]Br and κ-(d[3,3]-BEDT-TTF)2Cu[N(CN)2]Br, performed in a wide temperature range is reported. The latter two compounds were located near the metal–insulator boundary in the dimer-Mott phase diagram. From the comparison of the temperature dependences of their heat capacities, we indicated that lattice heat capacities of the partially deuterated compounds were larger than that of the pristine compound below about 40 K. This feature probably related to the lattice softening was discussed also by the sound velocity measurement, in which the dip-like structures of the Δv/v were observed. We also discussed the variation of the electronic heat capacity under magnetic fields. From the heat capacity data at magnetic fields up to 6 T, we evaluated that the normal-state γ value of the partially deuterated compound, κ-(d[3,3]-BEDT-TTF)2Cu[N(CN)2]Br, was about 3.1 mJ K−2 mol−1. Under the magnetic fields higher than 3.0 T, we observed that the magnetic-field insulating state was induced due to the instability of the mid-gap electronic state peculiar for the two-dimensional dimer-Mott system. Even though the volume fraction was much reduced, the heat capacity of κ-(d[3,3]-BEDT-TTF)2Cu[N(CN)2]Br showed a small hump structure probably related to the strong coupling feature of the superconductivity near the boundary. Full article
(This article belongs to the Special Issue New Spin on Metal-Insulator Transitions)
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10 pages, 739 KiB  
Article
Tuning Charge Order in (TMTTF)2X by Partial Anion Substitution
by Andrej Pustogow, Daniel Dizdarevic, Sebastian Erfort, Olga Iakutkina, Valentino Merkl, Gabriele Untereiner and Martin Dressel
Crystals 2021, 11(12), 1545; https://doi.org/10.3390/cryst11121545 - 10 Dec 2021
Cited by 2 | Viewed by 2725
Abstract
In the quasi-one-dimensional (TMTTF)2X compounds with effectively quarter-filled bands, electronic charge order is stabilized from the delicate interplay of Coulomb repulsion and electronic bandwidth. The correlation strength is commonly tuned by physical pressure or chemical substitution with stoichiometric ratios of anions [...] Read more.
In the quasi-one-dimensional (TMTTF)2X compounds with effectively quarter-filled bands, electronic charge order is stabilized from the delicate interplay of Coulomb repulsion and electronic bandwidth. The correlation strength is commonly tuned by physical pressure or chemical substitution with stoichiometric ratios of anions and cations. Here, we investigate the charge-ordered state through partial substitution of the anions in (TMTTF)2[AsF6]1x[SbF6]x with x0.3, determined from the intensity of infrared vibrations, which is sufficient to suppress the spin-Peierls state. Our dc transport experiments reveal a transition temperature TCO = 120 K and charge gap ΔCO=430 K between the values of the two parent compounds (TMTTF)2AsF6 and (TMTTF)2SbF6. Upon plotting the two parameters for different (TMTTF)2X, we find a universal relationship between TCO and ΔCO yielding that the energy gap vanishes for transition temperatures TCO60 K. While these quantities indicate that the macroscopic correlation strength is continuously tuned, our vibrational spectroscopy results probing the local charge disproportionation suggest that 2δ is modulated on a microscopic level. Full article
(This article belongs to the Special Issue New Spin on Metal-Insulator Transitions)
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10 pages, 3836 KiB  
Article
Fermi Surface Structure and Isotropic Stability of Fulde-Ferrell-Larkin-Ovchinnikov Phase in Layered Organic Superconductor β″-(BEDT-TTF)2SF5CH2CF2SO3
by Shiori Sugiura, Hiroki Akutsu, Yasuhiro Nakazawa, Taichi Terashima, Syuma Yasuzuka, John A. Schlueter and Shinya Uji
Crystals 2021, 11(12), 1525; https://doi.org/10.3390/cryst11121525 - 7 Dec 2021
Cited by 1 | Viewed by 3083
Abstract
The Fermi surface structure of a layered organic superconductor β-(BEDT-TTF)2SF5CH2CF2SO3 was determined by angular-dependent magnetoresistance oscillations measurements and band-structure calculations. This salt was found to have two small pockets with the same [...] Read more.
The Fermi surface structure of a layered organic superconductor β-(BEDT-TTF)2SF5CH2CF2SO3 was determined by angular-dependent magnetoresistance oscillations measurements and band-structure calculations. This salt was found to have two small pockets with the same area: a deformed square hole pocket and an elliptic electron pocket. Characteristic corrugations in the field dependence of the interlayer resistance in the superconducting phase were observed at any in-plane field directions. The features were ascribed to the commensurability (CM) effect between the Josephson vortex lattice and the periodic nodal structure of the superconducting gap in the Fulde–Ferrell–Larkin–Ovchinnikov (FFLO) phase. The CM effect was observed in a similar field region for various in-plane field directions, in spite of the anisotropic nature of the Fermi surface. The results clearly showed that the FFLO phase stability is insensitive to the in-plane field directions. Full article
(This article belongs to the Special Issue New Spin on Metal-Insulator Transitions)
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11 pages, 3223 KiB  
Article
The FFLO State in the Dimer Mott Organic Superconductor κ-(BEDT-TTF)2Cu[N(CN)2]Br
by Shusaku Imajo and Koichi Kindo
Crystals 2021, 11(11), 1358; https://doi.org/10.3390/cryst11111358 - 8 Nov 2021
Cited by 4 | Viewed by 2607
Abstract
The superconducting phase diagram for a quasi-two-dimensional organic superconductor, κ-(BEDT-TTF)2Cu[N(CN)2]Br, was studied using pulsed magnetic field penetration depth measurements under rotating magnetic fields. At low temperatures, Hc2 was abruptly suppressed even by small tilts of the applied fields [...] Read more.
The superconducting phase diagram for a quasi-two-dimensional organic superconductor, κ-(BEDT-TTF)2Cu[N(CN)2]Br, was studied using pulsed magnetic field penetration depth measurements under rotating magnetic fields. At low temperatures, Hc2 was abruptly suppressed even by small tilts of the applied fields owing to the orbital pair-breaking effect. In magnetic fields parallel to the conducting plane, the temperature dependence of the upper critical field Hc2 exhibited an upturn and exceeded the Pauli limit field HP in the lower temperature region. Further analyses with the second derivative of the penetration depth showed an anomaly at 31–32 T, which roughly corresponded to HP. The origin of the anomaly should not be related to the orbital effect, but the paramagnetic effect, which is almost isotropic in organic salts, because it barely depends on the field angle. Based on these results, the observed anomaly is most likely due to the transition between the Bardeen-Cooper-Schrieffer (BCS) and the Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) states. Additionally, we discuss the phase diagram and physical parameters of the transition by comparing them with other FFLO candidates. Full article
(This article belongs to the Special Issue New Spin on Metal-Insulator Transitions)
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16 pages, 744 KiB  
Article
Real Space Quantum Cluster Formulation for the Typical Medium Theory of Anderson Localization
by Ka-Ming Tam, Hanna Terletska, Tom Berlijn, Liviu Chioncel and Juana Moreno
Crystals 2021, 11(11), 1282; https://doi.org/10.3390/cryst11111282 - 22 Oct 2021
Cited by 1 | Viewed by 2206
Abstract
We develop a real space cluster extension of the typical medium theory (cluster-TMT) to study Anderson localization. By construction, the cluster-TMT approach is formally equivalent to the real space cluster extension of the dynamical mean field theory. Applying the developed method to the [...] Read more.
We develop a real space cluster extension of the typical medium theory (cluster-TMT) to study Anderson localization. By construction, the cluster-TMT approach is formally equivalent to the real space cluster extension of the dynamical mean field theory. Applying the developed method to the 3D Anderson model with a box disorder distribution, we demonstrate that cluster-TMT successfully captures the localization phenomena in all disorder regimes. As a function of the cluster size, our method obtains the correct critical disorder strength for the Anderson localization in 3D, and systematically recovers the re-entrance behavior of the mobility edge. From a general perspective, our developed methodology offers the potential to study Anderson localization at surfaces within quantum embedding theory. This opens the door to studying the interplay between topology and Anderson localization from first principles. Full article
(This article belongs to the Special Issue New Spin on Metal-Insulator Transitions)
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14 pages, 1507 KiB  
Article
Dielectric Anomaly and Charge Fluctuations in the Non-Magnetic Dimer Mott Insulator λ-(BEDT-STF)2GaCl4
by Olga Iakutkina, Roland Rosslhuber, Atsushi Kawamoto and Martin Dressel
Crystals 2021, 11(9), 1031; https://doi.org/10.3390/cryst11091031 - 27 Aug 2021
Cited by 2 | Viewed by 2183
Abstract
The dimer Mott insulator λ-(BEDT-STF)2GaCl4 undergoes no magnetic order down to the lowest temperatures, suggesting the formation of a novel quantum disordered state. Our frequency and temperature-dependent investigations of the dielectric response reveal a relaxor-like behavior below [...] Read more.
The dimer Mott insulator λ-(BEDT-STF)2GaCl4 undergoes no magnetic order down to the lowest temperatures, suggesting the formation of a novel quantum disordered state. Our frequency and temperature-dependent investigations of the dielectric response reveal a relaxor-like behavior below T100 K for all three axes, similar to other spin liquid candidates. Optical measurement of the charge-sensitive vibrational mode ν27(b1u) identifies a charge disproportionation Δρ0.04e on the dimer that exists up to room temperature and originates from inequivalent molecules in the weakly coupled dimers. The linewidth of the charge sensitive mode is broader than that of typical organic conductors, supporting the existence of a disordered electronic state. Full article
(This article belongs to the Special Issue New Spin on Metal-Insulator Transitions)
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Review

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28 pages, 12776 KiB  
Review
Ingredients for Generalized Models of κ-Phase Organic Charge-Transfer Salts: A Review
by Kira Riedl, Elena Gati and Roser Valentí
Crystals 2022, 12(12), 1689; https://doi.org/10.3390/cryst12121689 - 22 Nov 2022
Cited by 6 | Viewed by 2764
Abstract
The families of organic charge-transfer salts κ-(BEDT-TTF)2X and κ-(BETS)2X, where BEDT-TTF and BETS stand for the organic donor molecules C10H8S8 and C10H8S4Se4, respectively, [...] Read more.
The families of organic charge-transfer salts κ-(BEDT-TTF)2X and κ-(BETS)2X, where BEDT-TTF and BETS stand for the organic donor molecules C10H8S8 and C10H8S4Se4, respectively, and X for an inorganic electron acceptor, have been proven to serve as a powerful playground for the investigation of the physics of frustrated Mott insulators. These materials have been ascribed a model character, since the dimerization of the organic molecules allows to map these materials onto a single band Hubbard model, in which the dimers reside on an anisotropic triangular lattice. By changing the inorganic unit X or applying physical pressure, the correlation strength and anisotropy of the triangular lattice can be varied. This has led to the discovery of a variety of exotic phenomena, including quantum-spin liquid states, a plethora of long-range magnetic orders in proximity to a Mott metal-insulator transition, and unconventional superconductivity. While many of these phenomena can be described within this effective one-band Hubbard model on a triangular lattice, it has become evident in recent years that this simplified description is insufficient to capture all observed magnetic and electronic properties. The ingredients for generalized models that are relevant include, but are not limited to, spin-orbit coupling, intra-dimer charge and spin degrees of freedom, electron-lattice coupling, as well as disorder effects. Here, we review selected theoretical and experimental discoveries that clearly demonstrate the relevance thereof. At the same time, we outline that these aspects are not only relevant to this class of organic charge-transfer salts, but are also receiving increasing attention in other classes of inorganic strongly correlated electron systems. This reinforces the model character that the κ-phase organic charge-transfer salts have for understanding and discovering novel phenomena in strongly correlated electron systems from a theoretical and experimental point of view. Full article
(This article belongs to the Special Issue New Spin on Metal-Insulator Transitions)
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15 pages, 4461 KiB  
Review
Superconductivity and Charge Ordering in BEDT-TTF Based Organic Conductors with β″-Type Molecular Arrangement
by Yoshihiko Ihara and Shusaku Imajo
Crystals 2022, 12(5), 711; https://doi.org/10.3390/cryst12050711 - 17 May 2022
Cited by 7 | Viewed by 2383
Abstract
Exotic superconductivity that appears near the charge ordering instability has attracted significant interest since the beginning of superconducting study. The discovery of possible coexistence of charge ordering and superconductivity in cuprates and kagome metals has further fascinated researchers in recent years. In this [...] Read more.
Exotic superconductivity that appears near the charge ordering instability has attracted significant interest since the beginning of superconducting study. The discovery of possible coexistence of charge ordering and superconductivity in cuprates and kagome metals has further fascinated researchers in recent years. In this review, we focus on the BEDT-TTF-based organic superconductor with β″-type molecular packing sequence, which shows the charge ordering transition in the very vicinity of superconducting transition, and summarize the experimental results reported up to the present. At the charge ordering temperature, ultrasonic measurement detects the softening of the crystal lattice, and 13C-NMR measurement shows an increase in nuclear spin-lattice relaxation rate divided by temperature 1/T1T. These results suggest that low-energy dynamics are activated near the charge ordering transition, leading us to invoke the charge-fluctuation mediated superconducting pairing mechanism. Full article
(This article belongs to the Special Issue New Spin on Metal-Insulator Transitions)
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15 pages, 5569 KiB  
Review
Simultaneous Control of Bandfilling and Bandwidth in Electric Double-Layer Transistor Based on Organic Mott Insulator κ-(BEDT-TTF)2Cu[N(CN)2]Cl
by Yoshitaka Kawasugi and Hiroshi M. Yamamoto
Crystals 2022, 12(1), 42; https://doi.org/10.3390/cryst12010042 - 28 Dec 2021
Cited by 6 | Viewed by 2752
Abstract
The physics of quantum many-body systems have been studied using bulk correlated materials, and recently, moiré superlattices formed by atomic bilayers have appeared as a novel platform in which the carrier concentration and the band structures are highly tunable. In this brief review, [...] Read more.
The physics of quantum many-body systems have been studied using bulk correlated materials, and recently, moiré superlattices formed by atomic bilayers have appeared as a novel platform in which the carrier concentration and the band structures are highly tunable. In this brief review, we introduce an intermediate platform between those systems, namely, a band-filling- and bandwidth-tunable electric double-layer transistor based on a real organic Mott insulator κ-(BEDT-TTF)2Cu[N(CN)2]Cl. In the proximity of the bandwidth-control Mott transition at half filling, both electron and hole doping induced superconductivity (with almost identical transition temperatures) in the same sample. The normal state under electric double-layer doping exhibited non-Fermi liquid behaviors as in many correlated materials. The doping levels for the superconductivity and the non-Fermi liquid behaviors were highly doping-asymmetric. Model calculations based on the anisotropic triangular lattice explained many phenomena and the doping asymmetry, implying the importance of the noninteracting band structure (particularly the flat part of the band). Full article
(This article belongs to the Special Issue New Spin on Metal-Insulator Transitions)
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Other

18 pages, 4808 KiB  
Perspective
Are Heavy Fermion Strange Metals Planckian?
by Mathieu Taupin and Silke Paschen
Crystals 2022, 12(2), 251; https://doi.org/10.3390/cryst12020251 - 12 Feb 2022
Cited by 16 | Viewed by 5332
Abstract
Strange metal behavior refers to a linear temperature dependence of the electrical resistivity that is not due to electron–phonon scattering. It is seen in numerous strongly correlated electron systems, from the heavy fermion compounds, via transition metal oxides and iron pnictides, to magic [...] Read more.
Strange metal behavior refers to a linear temperature dependence of the electrical resistivity that is not due to electron–phonon scattering. It is seen in numerous strongly correlated electron systems, from the heavy fermion compounds, via transition metal oxides and iron pnictides, to magic angle twisted bi-layer graphene, frequently in connection with unconventional or “high temperature” superconductivity. To achieve a unified understanding of these phenomena across the different materials classes is a central open problem in condensed matter physics. Tests whether the linear-in-temperature law might be dictated by Planckian dissipation—scattering with the rate kBT/—are receiving considerable attention. Here we assess the situation for strange metal heavy fermion compounds. They allow to probe the regime of extreme correlation strength, with effective mass or Fermi velocity renormalizations in excess of three orders of magnitude. Adopting the same procedure as done in previous studies, i.e., assuming a simple Drude conductivity with the above scattering rate, we find that for these strongly renormalized quasiparticles, scattering is much weaker than Planckian, implying that the linear temperature dependence should be due to other effects. We discuss implications of this finding and point to directions for further work. Full article
(This article belongs to the Special Issue New Spin on Metal-Insulator Transitions)
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