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Recent theoretical investigations of quantum spin liquids have described phenomenology amenable to experimental observation using scanning tunneling microscopy. This includes characteristic resonances found at the edge of the upper Hubbard band of the host Mott insulator, that under certain conditions shift into the Mott gap under external magnetic field [W.-Y. He and P. A. Lee, arXiv:2212.08767]. In light of this we report scanning tunneling microscopy observations, in samples of the quantum spin liquid candidate 1T-TaS2, of a conductance peak at the upper Hubbard band edge and its magnetic field dependent behavior. These observations potentially represent evidence for the existence of a quantum spin liquid in 1T TaS2. We also observe samples in which such field dependence is absent, but with no observed correlate for the presence or absence of field dependence. This suggests one or more material properties controlling electronic behavior that are yet to be understood, and should help to motivate renewed investigation of the microscopic degrees of freedom in play in 1T-TaS2, as well as the possible realization of a quantum spin liquid phase., Comment: 5 pages, 2 figures

Electron-phonon-driven charge density waves can in some circumstances allow electronic correlations to become predominant, driving a system into a Mott insulating state. New insights into both the Mott state and preceding charge density wave may result from observations of the coupled dynamics of their underlying degrees of freedom. Here, tunneling injection of single electrons into the upper Hubbard band of the Mott charge-density-wave material 1T-TaS2 reveals extraordinarily narrow electronic excitations which couple to amplitude mode phonons associated with the charge density wave's periodic lattice distortion. This gives a vivid microscopic view of the interplay between excitations of the Mott state and the lattice dynamics of its charge density wave precursor., Comment: 8 pages, 5 figures, with Supplementary Information (6 pages, 8 figures). Accepted for publication in Physical Review X

A quantum spin liquid (QSL) is an exotic state of matter characterized by quantum entanglement and the absence of any broken symmetry. A long-standing open problem, which is a key for fundamental understanding the mysterious QSL states, is how the quantum fluctuations respond to randomness due to quenched disorder. Transition metal dichalcogenide 1T-TaS$_2$ is a candidate material that hosts a QSL ground state with spin-1/2 on the two-dimensional perfect triangular lattice. Here, we performed systematic studies of low-temperature heat capacity and thermal conductivity on pure, Se-substituted and electron irradiated crystals of 1T-TaS$_2$. In pure 1T-TaS$_2$, the linear temperature term of the heat capacity $\gamma T$ and the finite residual linear term of the thermal conductivity in the zero-temperature limit $\kappa_{0}/T\equiv\kappa/T(T\rightarrow0)$ are clearly resolved, consistent with the presence of gapless spinons with a Fermi surface. Moreover, while the strong magnetic field slightly enhances $\kappa_0/T$, it strongly suppresses $\gamma$. These unusual contrasting responses to magnetic field imply the coexistence of two types of gapless excitations with itinerant and localized characters. Introduction of additional weak random exchange disorder in 1T-Ta(S$_{1-x}$Se$_x$)$_2$ leads to vanishing of $\kappa_0/T$, indicating that the itinerant gapless excitations are sensitive to the disorder. On the other hand, in both pure and Se-substituted systems, the magnetic contribution of the heat capacity obeys a universal scaling relation, which is consistent with a theory that assumes the presence of localized orphan spins forming random singlets. Electron irradiation in pure 1T-TaS$_2$ largely enhances $\gamma$ and changes the scaling function dramatically, suggesting a possible new state of spin liquid., Comment: 10 pages, 9 figures. arXiv admin note: text overlap with arXiv:1803.06100

The chiral crystal is characterized by a lack of mirror symmetry and an inversion center, resulting in the inequivalent right- and left-handed structures. In the noncentrosymmetric crystal structure, the spin and momentum of electrons are locked in the reciprocal space with the help of the spin-orbit interaction. To reveal the spin textures of chiral crystals, here we investigate the spin and electronic structure in p-type semiconductor elemental tellurium with a chiral crystal structure by using spin- and angle-resolved photoemission spectroscopy. Our data demonstrate that the highest valence band crossing the Fermi level has a spin component parallel to the electron momentum around the BZ corners. Significantly, we have also confirmed that the spin polarization is reversed in the crystal with the opposite chirality. The results indicate that the spin textures of the right- and left-handed chiral crystals are hedgehog-like, leading to unconventional magnetoelectric effects and nonreciprocal phenomena., Comment: 15 pages, 4 figures

If a material with an odd number of electrons per unit cell turns out to be insulating, Mott localisation may be invoked as an explanation. This is widely accepted for the layered compound 1T-TaS2, which has a low-temperature insulating phase comprising charge order clusters with 13 unpaired orbitals each. But if the stacking of layers doubles up the unit cell to include an even number of orbitals, the nature of the insulating state is ambiguous. Here, scanning tunnelling microscopy (STM) reveals two distinct terminations of the charge order in 1T-TaS2, the sign of such a double-layer stacking pattern. However, spectroscopy at both terminations allows us to disentangle unit-cell doubling effects and determine that Mott localisation alone is enough to drive gap formation. We also observe the collapse of Mottness at an extrinsically restacked termination, demonstrating that the microscopic mechanism of insulator-metal transitions lies in degrees of freedom of interlayer stacking., Comment: 9 pages, 6 figures, including Supplementary Information

To reveal the nature of elementary excitations in a quantum spin liquid (QSL), we measured low temperature thermal conductivity and specific heat of 1T-TaS$_2$, a QSL candidate material with frustrated triangular lattice of spin-1/2. The nonzero temperature linear specific heat coefficient $\gamma$ and the finite residual linear term of the thermal conductivity in the zero temperature limit $\kappa_0/T=\kappa/T(T\rightarrow 0)$ are clearly resolved. This demonstrates the presence of highly mobile gapless excitations, which is consistent with fractionalized spinon excitations that form a Fermi surface. Remarkably, an external magnetic field strongly suppresses $\gamma$, whereas it enhances $\kappa_0/T$. This unusual contrasting behavior in the field dependence of specific heat and thermal conductivity can be accounted for by the presence of two types of gapless excitations with itinerant and localized characters, as recently predicted theoretically (I. Kimchi et al., arXiv:1803.00013 (2018)). This unique feature of 1T-TaS$_2$ provides new insights into the influence of quenched disorder on the QSL., Comment: 6 pages, 4 figures

A valley degree of freedom (DOF) in transition metal dichalcogenides with broken inversion symmetry can be controlled through spin and orbital DOFs owing to their valley-contrasting characters. Another important aspect of the spin and orbital DOFs is that they affect quasiparticle scattering processes that govern the valley lifetime. Here we combine quasiparticle-interference (QPI) imaging experiments and theoretical simulations to study the roles of the spin and orbital DOFs in 3R-NbS2. We find that the QPI signal arising from an inter-valley scattering is noticeably weaker than that caused by an intra-valley scattering. We show that this behavior is predominantly associated with the orbital DOF, signifying the different spin and orbital structures of spin-split bands at each valley. These findings provide important insights into understanding the valley-related transport properties., Comment: 12 pages, 6 figures, accepted for publication in PRB

We report the lattice dynamics of transition metal thin films by using the ultrafast electron diffraction. We observe a suppression of the diffraction intensity in a few picosecond after the photoexcitation, which is directly interpreted as the lattice heating via the electron-phonon interaction. The electron-phonon coupling constants for Au, Cu and Mo are quantitatively evaluated by employing the two-temperature model, which are consistent with those obtained by optical pump-probe methods. The variation in the lattice dynamics of the transition metals are systematically explained by the strength of the electron-phonon coupling, arising from the elemental dependence of the electronic structure and atomic mass., Comment: 5 pages, 4 figures, 1 table

We present a comparative study of high carrier density transport in mono-, bi-, and trilayer graphene using electric-double-layer transistors to continuously tune the carrier density up to values exceeding 10^{14} cm^{-2}. Whereas in monolayer the conductivity saturates, in bi- and trilayer flling of the higher energy bands is observed to cause a non-monotonic behavior of the conductivity, and a large increase in the quantum capacitance. These systematic trends not only show how the intrinsic high-density transport properties of graphene can be accessed by field-effect, but also demonstrate the robustness of ion-gated graphene, which is crucial for possible future applications., Comment: 4 figures, 4 pages

In this study, it is shown that in a layered nitride superconductor, i.e., LixZrNCl (0.07<=x<=0.21), the superconducting order parameter is highly anisotropic in a sample with x=0.12, as inferred from both the temperature and the magnetic field dependences of the muon depolarization rate (sigma_s, proportional to the superfluid density). Moreover, the tendency of strong anisotropy with an increase in x is indicated by the T dependence of sigma_s. These observations are in good agreement with the recent theory that predicts the development of anisotropy in a d+id' gap upon carrier filling to the bands with disconnected Fermi surfaces on a honeycomb lattice., Comment: 5 pages, 5 figures

Using single-crystal transistors, we have performed a systematic experimental study of electronic transport through oxidized copper/rubrene interfaces as a function of temperature and bias. We find that the measurements can be reproduced quantitatively in terms of the thermionic emission theory for Schottky diodes, if the effect of the bias-induced barrier lowering is included. Our analysis emphasizes the role of the coupling between metal and molecules, which in our devices is weak due to the presence of an oxide layer at the surface of the copper electrodes., Comment: 4 pages, 3 figures

$^7$Li and $^1$H NMR and magnetization measurements in \lpc (Pc$\equiv$C$_{32}$H$_{16}$N$_8$), recently proposed as a strongly correlated metal, are presented. Two different low-frequency dynamics are evidenced. The first one, probed by $^1$H nuclei gives rise to a slowly relaxing magnetization at low temperature and is associated with the freezing of MnPc $S=3/2$ spins. This dynamic is similar to the one observed in pristine $\beta$-MnPc and originates from Li depleted chain segments. The second one, evidenced by $^7$Li spin-lattice relaxation rate, is associated with the hopping of the electrons along Li-rich chains. The characteristic correlation times for the two dynamics are derived and the role of disorder is briefly discussed., Comment: 7 two-columns pages, 11 figures

The relationship between magnetic order and ferroelectric properties has been investigated for MnWO$_4$ with long-wavelength magnetic structure. Spontaneous electric polarization is observed in an elliptical spiral spin phase. The magnetic-field dependence of electric polarization indicates that the noncollinear spin configuration plays a key role for the appearance of ferroelectric phase. An electric polarization flop from the b direction to the a direction has been observed when a magnetic field above 10T is applied along the b axis. This result demonstrates that an electric polarization flop can be induced by a magnetic field in a simple system without rare-earth f-moments., Comment: 9 pages, 4 figures

Hall effect is detected in organic field-effect transistors, using appropriately shaped rubrene (C42H28) single crystals. It turned out that inverse Hall coefficient, having a positive sign, is close to the amount of electric-field induced charge upon the hole accumulation. The presence of the normal Hall effect means that the electromagnetic character of the surface charge is not of hopping carriers but resembles that of a two-dimensional hole-gas system.

High pressure Raman experiments were performed on bundled double wall carbon nanotubes (DWCNTs). We observe peculiar regularity in the strength of the inner-outer tube (intratube) interaction, which is attributed to the interplay between the tube size and the intratube spacing. Moreover, a pressure-induced red shift of the band gap energies of the probed inner tubes is deduced from the Raman spectra. These experimental findings reveal that the interaction between primary and secondary shells, although generally assumed to be weak, determines the dynamics in the interior of the DWCNTs., Comment: PDF with 13 pages, 2 figures, submitted to Physical Review Letters

The pressure response of double-wall carbon nanotubes has been investigated by means of Raman spectroscopy up to 10 GPa. The intensity of the radial breathing modes of the outer tubes decreases rapidly but remain observable up to 9 GPa, exhibiting a behavior similar (but less pronounced) to that of single-wall carbon nanotubes, which undergo a shape distortion at higher pressures. In addition, the tangential band of the external tubes broadens and decreases in amplitude. The corresponding Raman features of the internal tubes appear to be considerably less sensitive to pressure. All findings lead to the conclusion that the outer tubes act as a protection shield for the inner tubes whereas the latter increase the structural stability of the outer tubes upon pressure application., Comment: PDF with 15 pages, 3 figures, 1 table; submitted to Physical Review B

The surface conductivity is measured by a four-probe technique for pentacene and rubrene single-crystals laminated on polarized and nearly unpolarized molecular monolayers with application of perpendicular electric fields. The polarization of the self-assembled monolayers (SAMs) shifts the threshold gate voltage, while maintaining a very low subthreshold swing of the single-crystal devices (0.11 V/decade). The results, excluding influences of parasitic contacts and grain boundaries, demonstrate SAM-induced nanoscale charge injection up to ~10^12 cm^-2 at the surface of the organic single crystals., Comment: submitted to Appl. Phys. Lett

We report a $^{11}$B NMR line shape and spin-lattice relaxation rate ($1/(T_1T)$) study of pure and lightly carbon doped MgB$_{2-x}$C$_{x}$ for $x=0$, 0.02, and 0.04, in the vortex state and in magnetic field of 23.5 kOe. We show that while pure MgB$_2$ exhibits the magnetic field distribution from superposition of the normal and the Abrikosov state, slight replacement of boron with carbon unveils the magnetic field distribution of the pure Abrikosov state. This indicates a considerable increase of $H_{c2}^c$ with carbon doping with respect to pure MgB$_2$. The spin-lattice relaxation rate $1/(T_1T)$ demonstrates clearly the presence of a coherence peak right below $T_c$ in pure MgB$_2$, followed by a typical BCS decrease on cooling. However, at temperatures lower than $\approx 10$K strong deviation from the BCS behavior is observed, probably from residual contribution of the vortex dynamics. In the carbon doped systems both the coherence peak and the BCS temperature dependence of $1/(T_1T)$ weaken, an effect attributed to the gradual shrinking of the $\sigma $ hole cylinders of the Fermi surface with electron doping., Comment: 8 pages, 6 figures, submitted to Phys. Rev. B

We report an insulator-metal-insulator transition in films of five metal phthalocyanines (MPc) doped with alkali atoms. Electrical conduction measurements demonstrate that increasing the alkali concentration results in the formation of a metallic state for all systems. Upon further doping, the films reenter the insulating state. Structural and Raman spectroscopy studies reveal the formation of new crystalline phases upon doping and are consistent with the phenomena originating from charge transfer between the intercalated alkali atoms and MPc, in a similar fashion to what has been so far observed only in C60. Due to the presence of a molecular spin, large exchange energy, and a two-fold orbital degeneracy in MPc, our findings are of interest in the study of controllable magnetism in molecular materials and in the investigation of new, recently predicted electronic phases., Comment: Replaced with published version

The polarized optical reflectance spectra of the quasi two dimensional organic correlated electron system $\kappa$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]$Y$, $Y =$ Br and Cl are measured in the infrared region. The former shows the superconductivity at $T_{\rm c} \simeq$ 11.6 K and the latter does the antiferromagnetic insulator transition at $T_{\rm N} \simeq$ 28 K. Both the specific molecular vibration mode $\nu_{3}(a_{g})$ of the BEDT-TTF molecule and the optical conductivity hump in the mid-infrared region change correlatively at $T^{*} \simeq$ 38 K of $\kappa$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Br, although no indication of $T^{*}$ but the insulating behaviour below $T_{\rm ins} \simeq$ 50-60 K are found in $\kappa$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Cl. The results suggest that the electron-molecular vibration coupling on the $\nu_{3}(a_{g})$ mode becomes weak due to the enhancement of the itinerant nature of the carriers on the dimer of the BEDT-TTF molecules below $T^{*}$, while it does strong below $T_{\rm ins}$ because of the localized carriers on the dimer. These changes are in agreement with the reduction and the enhancement of the mid-infrared conductivity hump below $T^{*}$ and $T_{\rm ins}$, respectively, which originates from the transitions between the upper and lower Mott-Hubbard bands. The present observations demonstrate that two different metallic states of $\kappa$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Br are regarded as {\it a correlated good metal} below $T^{*}$ including the superconducting state and {\it a half filling bad metal} above $T^{*}$. In contrast the insulating state of $\kappa$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Cl below $T_{\rm ins}$ is the Mott insulator., Comment: 8 pages, 7 figures

The evolution of the superconducting properties of the carbon-doped MgB2 superconductors, MgB(2-x)Cx (x= 0.02, 0.04, 0.06) have been investigated by the transverse-field muon spin rotation (TF-muSR) technique. The low-temperature depolarisation rate, sigma(0) at 0.6 T which is proportional to the second moment of the field distribution of the vortex lattice decreases monotonically with increasing electron doping and decreasing Tc. In addition, the temperature dependence of sigma(T) has been analysed in terms of a two-gap model. The size of the two superconducting gaps decreases linearly as the carbon content increases, while the doping effect is more pronounced for the smaller gap related to the 3D pi-sheets of the Fermi surface., Comment: 7 pages, 2 Figures, 1 Table, Europhys. Lett. in press

Microwave study using cavity perturbation technique revealed that the conductivity of antiferromagnet (NH$_3$)K$_{3-x}$Rb$_x$C$_{60}$ at 200K is already 3-4 orders of magnitude smaller than those of superconductors, K$_3$C$_{60}$ and (NH$_3$)$_x$NaRb$_2$C$_{60}$, and that the antiferromagnetic compounds are {\it insulators} below 250K without metal-insulator transitions. The striking difference in the magnitude of the conductivity between these materials strongly suggests that the Mott-Hubbard transition in the ammoniated alkali fullerides is driven by a reduction of lattice symmetry from face-centered-cubic to face-centered-orthorhombic, rather than by the magnetic ordering., Comment: accepted for publication in PRL

This paper has been withdrawn by the authors, because of serious experimental problems., Comment: This paper has been withdrawn by the authors, because a serious experimental problems

We report that the ternary MgB2-xCx compounds adopt an isostructural AlB2-type hexagonal structure in a relatively small range of nominal carbon concentration, x<0.1. The lattice parameter a decreases almost linearly with increasing carbon content x, while the c parameter remains unchanged, indicating that carbon is exclusively substituted in the boron honeycomb layer without affecting the interlayer interactions. The superconducting transition temperature Tc, determined by magnetometry experiments, also decreases quasilinearly as a function of the carbon concentration. The structural and electronic behavior of MgB2-xCx displays a remarkable similarity with the isoelectronic Mg1-xAlxB2 despite the different substitution sites., Comment: 9 pages, 4 figures

High-pressure resistivity experiments were performed on the recently discovered superconductor, MgB2. Tc decreases quasi-linearly with applied pressure to 1.4 GPa at a rate of -2.0(1) K/GPa, which is somewhat larger than that derived from recently-reported ac susceptibility measurements. The reduction of Tc is consistent with the BCS picture, in a similar way to the C60-based superconductors. Taking into account the pressure dependence of the unit cell volume, V, the volume coefficient of Tc, d(lnTc)/dV is significantly large., Comment: 6 pages, 2 figures

Considerable excitement has been caused recently by the discovery that the binary boride system with stoichiometry MgB2 is superconducting at the remarkably high temperature of 39 K (1). This potentially opens the way to even higher Tc values in a new family of superconductors with unexpectedly simple composition and structure. The simplicity in the electronic and crystal structures could allow the understanding of the physics of high-Tc superconductivity without the presence of the multitude of complicated features, associated with the cuprates. Synchrotron X-ray diffraction was used to measure the isothermal compressibility of MgB2, revealing a stiff tightly-packed incompressible solid with only moderate bonding anisotropy between intra- and inter-layer directions. These results, combined with the pressure evolution of the superconducting transition temperature, Tc establish its relation to the B and Mg bonding distances over a broad range of values., Comment: 6 pages, 3 figures

Raman shift dependence of charge transfer is studied in the two fulleride families of AxBa3C60 (x=0,3; A=K,Rb) and KxSm2.75C60 (x=0,3.25). It is found that the Raman spectra are essentially identical to each other for all ternary fullerides, The results show a crossover point at the boundary of t1u and t1g bands for the Raman shift dependence of charge transfer. For the t1u fullerides, the Ag(2) pinch mode follows the characteristic shift of ~6.3cm-1 per elementary charge widely observed in KxC60. The two Ag modes in t1g fullerides show a complicated behavior. An anomalous Raman shift is observed in the t1g fullerides. This anomalous Raman shift of the two Ag modes could not be explained only by charge transfer., Comment: 12 pages, 4 figures, submitted to Phys. Rev. B (Feburary 3, 1999)

Raman spectra are reported for Ba doped fullerides, BaxC60(x=3,4,and 6). The lowest frequency Hg modes split into five components for Ba4C60 and Ba6C60 even at room temperature, allowing us a quantitative analysis based on the electron-phonon couping theory. For the superconducting Ba4C60, the density of states at the Fermi energy was derived as 7 eV-1, while the total value of electron-phonon coupling \lambda was found to be 1.0, which is comparable to that of K3C60. The tangential Ag(2) mode, which is known as a sensitive probe for the degree of charge transfer on C60 molecule, shows a remarkable shift depending on the Ba concentration, being roughly consistent with the full charge transfer from Ba to C60. An effect of hybridization between Ba and C60 \pi orbitals is also discussed., Comment: 15 pages, 6 figures submitted to Phys. Rev. B (December 1,1998)

A novel fulleride Sm6C60 has been synthesized using high temperature solid state reaction. The Rietveld refinement on high resolution synchrotron X-ray powder diffraction data shows that Sm6C60 is isostructural with body-centered cubic A6C60 (A=K, Ba). Raman spectrum of Sm6C60 is similar to that of Ba6C60, and the frequencies of two Ag modes in Sm6C60 are nearly the same as that of Ba6C60, suggesting that Sm is divalent and hybridization between C60 molecules and the Sm atom could exist in Sm6C60. Resistivity measurement shows a weak T-linear behavior above 180 K, the transport at low temperature is mainly dominated by granular-metal theory., Comment: 9 pages, 3 figures, submitted to Phys. Rev. B (March 12, 1999)