The effects of a magnetic field on the Mott transition, a longstanding issue in condensed matter physics, are studied using magnetoresistance measurements for organic Mott insulators, lambda-(BETS)2GaBrxCl4-x, up to 55 T. We demonstrate that an insulator-to-metal transition with a first-order nature and a successive superconductor-toinsulator-to-metal transition are induced by magnetic fields. We discuss the difference in magnetic susceptibility between the insulating and metallic phases, which is a key factor in inducing these transitions. Field induced transitions in experimentally feasible fields under ambient pressure conditions lead to further experimental verification of Mott transitions.
The molecular pathogenesis of nonalcoholic steatohepatitis (NASH) includes a complex interaction of metabolic stress and inflammatory stimuli. Considering the therapeutic goals of NASH, it is important to determine whether the treatment can prevent the progression from NASH to hepatocellular carcinoma. Taxifolin, also known as dihydroquercetin, is a natural bioactive flavonoid with antioxidant and anti-inflammatory properties commonly found in various foods and health supplement products. In this study, we demonstrated that Taxifolin treatment markedly prevented the development of hepatic steatosis, chronic inflammation, and liver fibrosis in a murine model of NASH. Its mechanisms include a direct action on hepatocytes to inhibit lipid accumulation. Taxifolin also increased brown adipose tissue activity and suppressed body weight gain through at least two distinct pathways: direct action on brown adipocytes and indirect action via fibroblast growth factor 21 production in the liver. Notably, the Taxifolin treatment after NASH development could effectively prevent the development of liver tumors. Collectively, this study provides evidence that Taxifolin shows pleiotropic effects for the treatment of the NASH continuum. Our data also provide insight into the novel mechanisms of action of Taxifolin, which has been widely used as a health supplement with high safety.
Type 2 diabetes mellitus is associated with an increased risk of dementia, potentially through multifactorial pathologies, including neuroinflammation. Therefore, there is a need to identify novel agents that can suppress neuroinflammation and prevent cognitive impairment in diabetes. In the present study, we demonstrated that a high-glucose (HG) environment elevates the intracellular reactive oxygen species (ROS) levels and triggers inflammatory responses in the mouse microglial cell line BV-2. We further found that thioredoxin-interacting protein (TXNIP), a ROS-responsive positive regulator of the nucleotide-binding oligomerization domain (NOD)-like receptor family pyrin domain-containing 3 (NLRP3) inflammasome, was also upregulated, followed by NLRP3 inflammasome activation and subsequent interleukin-1beta (IL-1β) production in these cells. Conversely, caspase-1 was not significantly activated, suggesting the involvement of noncanonical pathways in these inflammatory responses. Moreover, our results demonstrated that taxifolin, a natural flavonoid with antioxidant and radical scavenging activities, suppressed IL-1β production by reducing the intracellular ROS levels and inhibiting the activation of the TXNIP–NLRP3 axis. These findings suggest the novel anti-inflammatory effects of taxifolin on microglia in an HG environment, which could help develop novel strategies for suppressing neuroinflammation in diabetes.
The band structure and magnetic properties of organic charge-transfer salt lambda-(BEDSe-TTF)(2)GaCl4 [BEDSe-TTF: bis(ethylenediseleno)tetrathiafulvalene; abbreviated as lambda-BEDSe] are investigated. The re-ported crystal structure is confirmed using x-ray diffraction measurements, and the transfer integrals are calculated. The degree of electron correlation U/W (U: on-site Coulomb repulsion, W: bandwidth) of lambda-BEDSe is larger than one and comparable to that of the isostructural Mott insulator lambda-(ET)(2)GaCl4 (ET: bis(ethylenedithio)tetrathiafulvalene, abbreviated as lambda-ET), whereas the U/W of the superconducting salt lambda-(BETS)(2)GaCl4 [BETS: bis(ethylenedithio)tetraselenafulvalene] is smaller than one. C-13-NMR and mu SR measurements revealed that lambda-BEDSe undergoes an antiferromagnetic (AF) ordering below T-N = 22 K. In the AF state, discrete C-13-NMR spectra with a remaining central peak are observed, indicating the commensurate AF spin structure also observed in lambda-ET. The similarity of the structural and magnetic properties between lambda-BEDSe and lambda-ET suggests that both salts are in the same electronic phase, i.e., the physical properties of lambda-BEDSe can be understood by the universal phase diagram of bandwidth-controlled lambda-type organic conductors obtained by donor molecule substitution.
In kappa-(BEDT-TTF)(2)Cu[N(CN)(2)]X (X = Cl, Br) salts, where BEDT-TTF denotes bis(ethylenedithio)tetrathiafulvalene, the electronic properties can be characterized using a universal pressure-temperature phase diagram. Previous research [T. Kobayashi et al., Phys. Rev. B 100, 195115 (2019)] revealed a low-temperature insulating phase without antiferromagnetic ordering in the isostructural X = I (hereafter, kappa-I) salt, which cannot be understood using the universal phase diagram. In addition, the kappa-I salt naturally contains electronic inhomogeneity because of the development of a superlattice structure and/or disorder of the ethylene end groups. This could lead to physical properties that are different from those described by the universal phase diagram of kappa-type salts. To investigate the relationship between the electronic inhomogeneity and universal phase diagram, C-13 NMR measurements were performed under pressure on this material. With increasing pressure, an increase in the bandwidth was revealed from a decrease in the Knight shift. The accompanying suppression of the inhomogeneity at low temperatures was evident from the linewidth. Once the inhomogeneity was suppressed, superconductivity was observed. The temperature dependence of the Knight shift and spin-lattice relaxation rate in the superconducting state is similar to that previously observed for kappa-type salts, indicating that the symmetry of the superconducting gap is a d wave. When pressure was applied and the electronic inhomogeneity was suppressed, the physical properties of the kappa-I salt were found to be qualitatively identical to those of the high-pressure side on the universal phase diagram. These results indicate that the ratio of electronic inhomogeneity to bandwidth is an essential parameter for this system.
We have performed 13C NMR measurements on ??-(BEDT-STF)2FexGa1???xCl4 and evaluated Fe content dependence of the magnetic properties. We found that the angle dependence of the Knight shift of ??-(BEDT-STF)2FexGa1???xCl4 changes depending on the Fe content, which is explained by the exchange fields through the ??-d interaction and dipole fields. An antiferromagnetic ordering was observed in all Fe content samples except for ??-(BEDT-STF)2GaCl4 (x = 0). This indicates that the antiferromagnetic ground state is stabilized by the interaction between ?? and 3d spins. From the linewidths of the NMR spectra measured at the lowest temperature, we confirmed that the size of the ordered ?? spin moment is independent of the Fe content. Based on the results, we discuss the role of ??-d interaction for the stabilization of the antiferromagnetic ordering and the mechanism of the unconventional magnetism of 3d spins observed in ??-d systems.
We present the results of $^{69,71}$Ga-NMR measurements on an organic antiferromagnet $λ$-(BEDSe-TTF)$_2$GaCl$_4$ [BEDSe-TTF=bis(ethylenediseleno)tetrathiafulvalene], with comparison to reports on $λ$-(BETS)$_2$GaCl$_4$ [BETS=bis(ethylenedithio)tetraselenafulvalene] [T. Kobayashi et al., Phys. Rev. B 102, 235131 (2020)]. We found that the dynamics of two crystallographically independent ethylene groups induce two types of quadrupolar relaxation in the high-temperature region. As the ethylene motion freezes, hyperfine (HF) interactions develop between $π$ spin and Ga nuclear spin below 100 K, and thereby magnetic fluctuations of the $π$-spin system are detected even from the Ga site. The HF interaction in $λ$-(BETS)$_2$GaCl$_4$ was more than twice as large as in $λ$-(BEDSe-TTF)$_2$GaCl$_4$, implying that the short contacts between Cl atoms and the chalcogens of fulvalene part are essential for the transferred HF interaction. We propose that NMR using nuclei in anion layers is useful for studying interlayer interactions in organic conductors, which have not been studied experimentally. In addition, because the mechanism of the transferred HF interaction is considered to be the same as $π$-$d$ interaction in isostructural Fe-containing $λ$-type salts, our findings aid in the understanding of their physical properties.
We performed $^{13}\mathrm{C}$ NMR measurements on an organic superconductor $\ensuremath{\lambda}\text{\ensuremath{-}}{(\mathrm{B}\mathrm{E}\mathrm{T}\mathrm{S})}_{2}\mathrm{Ga}{\mathrm{Cl}}_{4}$ [BETS: bis(ethylenedithio)tetraselenafulvalene] to investigate the pressure effect on the spin density wave (SDW) fluctuations at low temperatures, which were observed at ambient pressure. We found that the spin-lattice relaxation rate divided by temperature $(1/{T}_{1}T)$ is significantly enhanced at low temperatures at 3 kbar, implying enhancement of the SDW fluctuation. When further pressure is applied, increase in $1/{T}_{1}T$ at low temperatures is suppressed and $1/{T}_{1}T$ becomes temperature independent, indicating the Fermi liquid state. Moreover, we revealed that the Korringa factor under pressure becomes double compared to its value at ambient pressure, suggesting a significant change in electron correlation. We discuss the effect of the SDW fluctuation and the electron correlation on the unconventional superconductivity.
Coulomb repulsion among conduction electrons in solids hinders their motion and leads to a rise in resistivity. A regime of electronic phase separation is expected at the first-order phase transition between a correlated metal and a paramagnetic Mott insulator, but remains unexplored experimentally as well as theoretically nearby T = 0. We approach this issue by assessing the complex permittivity via dielectric spectroscopy, which provides vivid mapping of the Mott transition and deep insight into its microscopic nature. Our experiments utilizing both physical pressure and chemical substitution consistently reveal a strong enhancement of the quasi-static dielectric constant ε 1 when correlations are tuned through the critical value. All experimental trends are captured by dynamical mean-field theory of the single-band Hubbard model supplemented by percolation theory. Our findings suggest a similar ’dielectric catastrophe’ in many other correlated materials and explain previous observations that were assigned to multiferroicity or ferroelectricity.
The band structure and magnetic properties of organic charge-transfer salt $\lambda$-(BEDSe-TTF)$_2$GaCl$_4$ (BEDSe-TTF: bis(ethylenediseleno)tetrathiafulvalene, abbreviated as $\lambda$-BEDSe) were investigated. The reported crystal structure was confirmed by the X-ray diffraction measurement, and the transfer integrals were calculated. The degree of electron correlation $U/W$ ($U$: on-site Coulomb repulsion, $W$: bandwidth) of $\lambda$-BEDSe is larger than one and comparable to that of isostructural Mott insulator $\lambda$-(ET)$_2$GaCl$_4$ (ET: bis(ethylenedithio)tetrathiafulvalene, abbreviated as $\lambda$-ET), whereas $U/W$ of superconducting salt $\lambda$-(BETS)$_2$GaCl$_4$ (BETS: bis(ethylenedithio)tetraselenafulvalene) is smaller than one. $^{13}$C-NMR and $\mu$SR measurements revealed that $\lambda$-BEDSe undergoes an antiferromagnetic (AF) ordering below $22$ K. In the AF state, discrete $^{13}$C-NMR spectra with a remaining central peak were observed, indicating the commensurate AF spin structure also observed in $\lambda$-ET. The similarity between structural and magnetic properties of $\lambda$-BEDSe and $\lambda$-ET indicates that both salts are in the same electronic phase, namely, physical properties of $\lambda$-BEDSe can be understood by the universal phase diagram of bandwidth-controlled $\lambda$-type organic conductors by donor molecule substitution. Furthermore, polymorphism was not obtained in the synthesis of this material, unlike for many other $\lambda$-type salts. The absence of polymorphism will allow us to construct electronic phases next to the superconducting phase, where a strange paramagnetic insulating phase is sandwiched between superconducting and AF phases.
A. Ito, T. Kobayashi, ∗ D. P. Sari, 3 I. Watanabe, Y. Saito, A. Kawamoto, H. Tsunakawa, K. Satoh, † and H. Taniguchi Graduate School of Science and Engineering, Saitama University, Saitama, 338-8570, Japan Innovative Global Program, College of Engineering, Shibaura Institute of Technology, Saitama 337-8570, Japan Advanced Meson Science Laboratory, RIKEN, Saitama 351-0198, Japan Institute of Physics, Goethe-University Frankfurt, 60438 Frankfurt (M), Germany Department of Condensed Matter Physics, Graduate School of Science, Hokkaido University, Sapporo 060-0810, Japan (Dated: December 14, 2021)
In this work, the thermodynamic properties of the organic superconductor lambda-(BETS)(2)GaCl4 are investigated to study a high-field superconducting state known as the putative Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) phase. We observed a small thermodynamic anomaly in the field H-FFLO similar to 10 T, which corresponds to the Pauli limiting field H-P. This anomaly probably originates from a transition from a uniform superconducting state to the FFLO state. H-FFLO does not show a strong-field angular dependence due to a quasi-isotropic paramagnetic effect in lambda-(BETS)(2)GaCl4. The thermodynamic anomaly at H-FFLO is smeared out. and the low-temperature upper critical field H-c2 changes significantly if fields are not parallel to the conducting plane, even for a deviation of similar to 0.5 degrees. This behavior indicates that the high-field state is very unstable, as it is influenced by the strongly anisotropic orbital effect. Our results are consistent with the theoretical predictions on the FFLO state and show that the high-field superconductivity is probably an FFLO state in lambda-(BETS)(2)GaCl4 from a thermodynamic point of view.
Background & Aim CLBS12 (autologous, mobilized peripheral blood derived selected CD34 cells) has previously been studied for the treatment of No-Option Critical Limb Ischemia (NOCLI) in Phase 1 and 2 studies in Japan and the United States. These studies demonstrated statistically significant improvement in key outcome measures including reduced Rutherford category, improved walking distance, reduction in pain, improvement in blood flow and tissue oxygenation, reduction in size and number of ulcers, and improved amputation-free survival. In one of the Japan studies, more than 80% of subjects treated with a single administration of CD34 cells became CLI-free and maintained this status through 4 years of observation. The promising results of these studies led to discussions with the PMDA regarding the design of a confirmatory study that, with a favorable outcome, could support registration of CLBS12 in Japan for NOCLI under the new regenerative medicine regulations. Methods, Results & Conclusion The study is a prospective, randomized clinical trial in subjects with arteriosclerosis obliterans (ASO; n=30) or Buerger's Disease (BD; n=5). All patients receive standard-of-care treatment (SOC). The study calls for randomization of 30 subjects with ASO to receive either CLBS12 or to continue with SOC alone. Additionally, 5 subjects with BD were to be allocated to a sub-study and receive CLBS12 while continuing SOC treatment. The primary endpoint for the study is ability to achieve a continuous CLI-free state. Other key measures include progression-free, amputation-free, and overall survival; Rutherford category; tissue oxygenation; blood flow; ulcer size, depth, and infection; pain; and quality-of-life. For preparation of CLBS12, subjects are mobilized with GCSF 5 µg/day for 5 days, then undergo apheresis to collect a mononuclear cell fraction. CD34 cells are separated using a magnetic separation method. CLBS12 is formulated as a cell suspension in proprietary media in a 10 mL volume for administration as a series of 20 intramuscular injections in one affected limb. The study was initiated in December 2017 and is expected to be completed in 2020. The BD sub-study has enrolled 6 subjects and half have achieved a continuous CLI-free state. Interim data from the trial will be presented. CLBS12 (autologous, mobilized peripheral blood derived selected CD34 cells) has previously been studied for the treatment of No-Option Critical Limb Ischemia (NOCLI) in Phase 1 and 2 studies in Japan and the United States. These studies demonstrated statistically significant improvement in key outcome measures including reduced Rutherford category, improved walking distance, reduction in pain, improvement in blood flow and tissue oxygenation, reduction in size and number of ulcers, and improved amputation-free survival. In one of the Japan studies, more than 80% of subjects treated with a single administration of CD34 cells became CLI-free and maintained this status through 4 years of observation. The promising results of these studies led to discussions with the PMDA regarding the design of a confirmatory study that, with a favorable outcome, could support registration of CLBS12 in Japan for NOCLI under the new regenerative medicine regulations. The study is a prospective, randomized clinical trial in subjects with arteriosclerosis obliterans (ASO; n=30) or Buerger's Disease (BD; n=5). All patients receive standard-of-care treatment (SOC). The study calls for randomization of 30 subjects with ASO to receive either CLBS12 or to continue with SOC alone. Additionally, 5 subjects with BD were to be allocated to a sub-study and receive CLBS12 while continuing SOC treatment. The primary endpoint for the study is ability to achieve a continuous CLI-free state. Other key measures include progression-free, amputation-free, and overall survival; Rutherford category; tissue oxygenation; blood flow; ulcer size, depth, and infection; pain; and quality-of-life. For preparation of CLBS12, subjects are mobilized with GCSF 5 µg/day for 5 days, then undergo apheresis to collect a mononuclear cell fraction. CD34 cells are separated using a magnetic separation method. CLBS12 is formulated as a cell suspension in proprietary media in a 10 mL volume for administration as a series of 20 intramuscular injections in one affected limb. The study was initiated in December 2017 and is expected to be completed in 2020. The BD sub-study has enrolled 6 subjects and half have achieved a continuous CLI-free state. Interim data from the trial will be presented.
For the unconventional organic superconductor λ -(BETS) 2 GaCl 4 [
We performed $^{13}\mathrm{C}$-NMR measurements on an organic superconductor $\ensuremath{\lambda}\text{\ensuremath{-}}{(\mathrm{BETS})}_{2}{\mathrm{GaCl}}_{4}$ to investigate the superconducting (SC) gap symmetry, where BETS stands for bis(ethylenedithio)tetraselenafulvalene. As the temperature approaches 0 K, the Knight shift in the SC state decreases; the nuclear spin-lattice relaxation rate $1/{T}_{1}$ shows cubic temperature dependence below the SC transition temperature ${T}_{c}$ without a coherence peak. These results can be understood in terms of $d$-wave superconductivity. Moreover, an increase in $1/{T}_{1}T$ at lower temperatures was observed just above ${T}_{c}$; this behavior can be interpreted as an effect of spin-density-wave (SDW) fluctuation. We suggest that the $d$-wave superconductivity of $\ensuremath{\lambda}\text{\ensuremath{-}}{(\mathrm{BETS})}_{2}{\mathrm{GaCl}}_{4}$ originates from SDW fluctuation.
We have performed C-13 NMR measurements on lambda-(BEDT-STF)(2)FeCl4 to reveal the mechanism of unconventional paramagneticlike behavior observed in A-type molecular pi-d systems. C-13 NMR spectra and nuclear spin-lattice relaxation rate 1/T-1 revealed that the pi and 3d electron systems undergo an antiferromagnetic transition simultaneously at 16 K with the assistance of the pi-d interaction. We found that the sublattice magnetizations of the pi and 3d spins show different temperature dependence below T-N, which is derived from the magnetic coupling between the two sublattice systems with different magnetic natures. We discuss the relationship between the two different magnetization processes and the unconventional magnetic behavior in lambda-type molecular pi-d system.
This paper identifies the electronic state just close to the superconducting phase in a system of organic conductors lambda-(BETS)2GaBrxCl4-x as a spin-density-wave state, using nuclear magnetic resonance and resistivity measurements. This finding explains the unexplainable enhancement of spin fluctuation at low temperatures in lambda-(BETS)2GaCl4 and suggests that the superconductivity of lambda-type salts is mediated by spin-density-wave fluctuations.
The spin-liquid candidate $\kappa$-(ET)$_2$Cu$_2$(CN)$_3$ [ET: bis(ethylenedithio)tetrathiafulvalene] does not exhibit magnetic ordering down to a very low temperature, but shows a mysterious anomaly at 6 K. The origin of the so-called 6 K anomaly is still under debate. We carried out nuclear quadrupole resonance (NQR) measurements on the copper sites of the insulating layers, which are sensitive to the charge dynamics unlike the conventional spin-1/2 nuclear magnetic resonance (NMR). The main finding of this study is that the observation of a sharp peak behavior in the nuclear spin-lattice relaxation rate $T_1^{-1}$ of $^{63}$Cu NQR at 6 K while $T_1^{-1}$ of both $^{13}$C and $^{1}$H NMR show no clear anomaly. This behavior can be understood as a second-order phase transition related to charge disproportionation in the ET layers.
An electron paramagnetic resonance study for an organic superconductor beta"-(BEDT-TTF)(4)[(H3O)Ga(C2O4)(3)]center dot C6H5NO2 reveals that superconductivity coexists uniformly with the charge ordered state in one material. In the charge ordered state, the interplane spin exchange is gapped, while the in-plane conductivity is not significantly modified. This anisotropic behavior is explained by an exotic charge ordered state, in which molecular-site-selective carrier localization coexists with conducting carriers on other molecules. The relationship between superconductivity and this conductive charge ordered state is investigated.