The superconducting transition metal dichalcogenides 2H-NbSe$_2$ and 2H-NbS$_2$ are intensively studied on account of their unique electronic properties such as Ising superconductivity, found in multi- and monolayers, with upper critical fields beyond the Pauli limit. Even in bulk crystals, there are reports of multiband superconductivity and exotic states, such as the Fulde-Ferrell-Larkin-Ovchinnikov phase. In this work, we investigate the superconducting properties of 2H-NbS$_2$ through a detailed high-field mapping of the phase diagram by means of magnetotransport and magnetostriction experiments. We compare the phase diagram between bulk crystals and a 6~nm thick flake of 2H-NbS$_2$ and find a drastically enhanced Maki parameter in the flake, signifying a change of the relevant pair breaking mechanism from orbital to paramagnetic pair breaking, which we attribute to an effect of enhanced spin-orbit coupling.
We present here some newer characteristics pertaining to paramagnetic Meissner effect like response in a single crystal of the low Tc superconducting compound 2H-NbSe2 via a detailed study of effects of perturbation on the field-cooled magnetization response. In the temperature range, where an anomalous paramagnetic magnetization occurs, the field-cooled magnetization response is found to be highly metastable: it displays a curious tendency to switch randomly from a given paramagnetic value to a diamagnetic or to a different paramagnetic value, when the system is perturbed by an impulse of an …
Time reversal and spatial inversion are two key symmetries for conventional Bardeen-Cooper-Schrieffer (BCS) superconductivity. Breaking inversion symmetry can lead to mixed-parity Cooper pairing and unconventional superconducting properties. Two-dimensional (2D) NbSe$_2$ has emerged as a new non-centrosymmetric superconductor with the unique out-of-plane or Ising spin-orbit coupling (SOC). Here, we report the observation of an unusual continuous paramagnetic-limited superconductor-normal metal transition in 2D NbSe$_2$. Using tunneling spectroscopy under high in-plane magnetic fields, we obser…
Transition metal dichalcogenides (TMDCs) usually exhibit layered polytypic structures due to the weak interlayer coupling. 2H-NbSe2 is one of the most widely studied in the pristine TMDC family due to its high superconducting transition temperature (Tc = 7.3K) and the occurrence of a charge-density wave (CDW) order below 33 K. The coexistence of CDW with superconductivity poses an intriguing open question about the relationship between Fermi surface nesting and Cooper pairing. Past studies of this issue have mostly been focused on doping 2H-NbSe2 by 3d transition metals without significantly c…
The temperature and angular dependencies of the resistive upper critical magnetic field $B_{c2}$ reveal a dimensional crossover of the superconducting state in the highly anisotropic misfit-layer single crystal of (LaSe)$_{1.14}$(NbSe$_2$) with the critical temperature $T_c$ of 1.23 K. The temperature dependence of the upper critical field $B_{c2\parallel ab}(T)$ for a field orientation along the conducting $(ab)$-planes displays a characteristic upturn at 1.1 K and below this temperature the angular dependence of $B_{c2}$ has a cusp around the parallel field orientation. Both these typical fe…
The large size single crystals of (SnSe)$_{1.16}$(NbSe$_2$) misfit layered compound were grown and superconductivity with $T_c$ of 3.4 K was first discovered in this system. Powder X-ray diffraction (XRD) and high resolution transmission electron microscopy (HRTEM) clearly display the misfit feature between SnSe and NbSe$_2$ subsystems. The Sommerfeld coefficient $γ$ inferred from specific-heat measurements is 16.73 mJ mol$^{-1}$ K$^{-2}$, slightly larger than the usual misfit compounds. The normalized specific heat jump $Δ$$C_e$/$γ$$T_{\rm c}$ is about 0.98, and the electron-phonon coupling c…
We report a systematic study of thickness-dependent superconductivity and carrier transport properties in exfoliated layered 2H-NbS2. Hall-effect measurements reveal 2H-NbS2 in its normal state to be a p-type metal with hole mobility of 1-3 cm2/Vs. The superconducting transition temperature is found to decrease with thickness. We find that the suppression of superconductivity is due to disorder resulting from the incorporation of atmospheric oxygen and a reduced hole density. Cross-section transmission electron microscope (TEM) imaging reveals a chemical change of NbS2 in ambient conditions, r…
We report on high-pressure (p_max = 2.1 GPa) muon spin rotation experiments probing the temperature-dependent magnetic penetration depth in the layered superconductor 2H-NbSe_2. Upon increasing the pressure, we observe a substantial increase of the superfluid density n_s, which we find to scale linearly with T_c. This linear scaling is considered a hallmark feature of unconventional superconductivity, especially in high-temperature cuprate superconductors. Our current results, along with our earlier findings on 1T'-MoTe_2 (Z. Guguchia et. al., Nature Communications 8, 1082 (2017)), demonstrate…
Large Field-Free Superconducting Diode Effect with Nonmonotonic Polarity Reversals in NbSe$_2$/CrBr$_3$ Heterostructures
Southern University of Science and Technology（南方科技大学）；International Quantum Academy, and Shenzhen Branch, Hefei National Laboratory（国际量子科学院，合肥国家实验室深圳分院）；Eastern Institute for Advanced Study, Eastern Institute of Technology（宁波东方理工大学（暂名）先进研究院）；State Key Laboratory of Optoelectronic Materials and Technologies, Sun Yat‑sen University（中山大学光电信息材料与技术国家重点实验室）
We report superconductivity in Sn$_{x}$NbSe$_{2-δ}$, a topological nodal-line semimetal candidate with a noncentrosymmetric crystal structure. The superconducting transition temperature $T_{c}$ of this compound is extremely sensitive to Sn concentration $x$ and Se deficiency $δ$, 5.0 K for Sn$_{0.13}$NbSe$_{1.70}$ and 8.6 K for Sn$_{0.14}$NbSe$_{1.71}$ and Sn$_{0.15}$NbSe$_{1.69}$. In all samples, the temperature dependence of the upper critical field $H_{c2}(T)$ differs from the prediction of the Werthamer-Helfand-Hohenberg theory. While the zero-temperature value of the in-plane upper critic…
Bound states in superconductors are expected to exhibit a spatially resolved electron-hole asymmetry which is the hallmark of their quantum nature. This asymmetry manifests as oscillations at the Fermi wavelength, which is usually tiny and thus washed out by thermal broadening or by scattering at defects. Here we demonstrate theoretically and confirm experimentally that, when coupled to magnetic impurities, bound states in a vortex core exhibit an emergent axial electron-hole asymmetry on a much longer scale, set by the coherence length. We study vortices in 2H-NbSe$_2$ and in 2H-NbSe$_{1.8}$S…
We report detailed measurements of the interlayer magnetoresistance of the layered organic superconductor $κ-(BEDT-TTF)_2Cu(SCN)_2$ for temperatures down to 0.5 K and fields up to 30 tesla. The upper critical field is determined from the resistive transition for a wide range of temperatures and field directions. For magnetic fields parallel to the layers, the upper critical field increases approximately linearly with decreasing temperature. The upper critical field at low temperatures is compared to the Pauli paramagnetic limit, at which singlet superconductivity should be destroyed by the Zee…
Free energy of a layered superconductor with $ξ_{\perp} < d$ is calculated in a parallel magnetic field by means of the Gor'kov equations, where $ξ_{\perp}$ is a coherence length perpendicular to the layers and $d$ is an inter-layer distance. The free energy is shown to differ from that in the textbook Lawrence-Doniach model at high fields, where the Meissner currents are found to create an unexpected positive magnetic moment due to shrinking of the Cooper pairs "sizes" by a magnetic field. This paramagnetic intrinsic Meissner effect in a bulk is suggested to detect by measuring in-plane torqu…
We study angular-dependent magnetoresistance in a low $T_c$ layered cuprate Bi$_{2.15}$Sr$_{1.9}$CuO$_{6+δ}$. The low $T_c$ ~ 4 K allows complete suppression of superconductivity by modest magnetic fields and facilitate accurate analysis of the upper critical field $H_{c2}$. We observe an universal exponential decay of fluctuation conductivity in a broad range of temperatures above $T_c$ and propose a new method for extraction of $H_{c2}(T)$ from the scaling analysis of the fluctuation conductivity at $T>T_c$. Our main result is observation of a surprisingly low $H_{c2}$ anisotropy ~ 2, which …
The thermal conductivity of the layered s-wave superconductor NbSe_2 was measured down to T_c/100 throughout the vortex state. With increasing field, we identify two regimes: one with localized states at fields very near H_c1 and one with highly delocalized quasiparticle excitations at higher fields. The two associated length scales are most naturally explained as multi-band superconductivity, with distinct small and large superconducting gaps on different sheets of the Fermi surface.
The study of superconducting materials that also possess nontrivial correlations or interactions remains an active frontier of condensed matter physics. NbSe$_2$ belongs to this class of superconductors and recent research has focused on the two-dimensional properties of this layered material. Here an investigation of the superconducting-to-normal-state transition in NbSe$_2$ is detailed, and found to be driven by dynamically-created vortices. Under the application of RF radiation, these vortices allow for two novel Josephson effects to be observed. The first is a coupling between Josephson cu…
2H-NbSe2 is the prototype and most frequently studied of the well-known transition metal dichalcogenide (TMDC) superconductors. Widely acknowledged to be a conventional superconductor, its transition temperature to the superconducting state (Tc) is 7.3 K - a Tc that is substantially higher than those seen for the majority of TMDCs, where Tcs between 2 and 4 K are the norm. Here we report the intercalation of Cu into 2H-NbSe2 to make CuxNbSe2. As is typically found when chemically altering an optimal superconductor, Tc decreases with increasing x, but the way that Tc is suppressed in this case …
The thermal conductivity kappa of the layered s-wave superconductor NbSe_2 was measured down to T_c/100 throughout the vortex state. With increasing field, we identify two regimes: one with localized states at fields very near H_c1 and one with highly delocalized quasiparticle excitations at higher fields. The two associated length scales are naturally explained as multi-band superconductivity, with distinct small and large superconducting gaps on different sheets of the Fermi surface. This behavior is compared to that of the multi-band superconductor MgB_2 and the conventional superconductor …
Two-dimensional (2D) transition metal dichalcogenides (TMDs) have a range of unique physics properties and could be used in the development of electronics, photonics, spintronics and quantum computing devices. The mechanical exfoliation technique of micro-size TMD flakes has attracted particular interest due to its simplicity and cost effectiveness. However, for most applications, large area and high quality films are preferred. Furthermore, when the thickness of crystalline films is down to the 2D limit (monolayer), exotic properties can be expected due to the quantum confinement and symmetry…
Ultra low-loss microwave materials are crucial for enhancing quantum coherence and scalability of superconducting qubits. Van der Waals (vdW) heterostructure is an attractive platform for quantum devices due to the single-crystal structure of the constituent two-dimensional (2D) layered materials and the lack of dangling bonds at their atomically sharp interfaces. However, new fabrication and characterization techniques are required to determine whether these structures can achieve low loss in the microwave regime. Here we report the fabrication of superconducting microwave resonators using Nb…
Extreme in-plane upper critical magnetic fields $B_{c2//ab}$ strongly violating the Pauli paramagnetic limit have been observed in the misfit layer $(LaSe)_{1.14}(NbSe_2)$ and $(LaSe)_{1.14}(NbSe_2)_2$ single crystals with $T_c$ = 1.23 K and 5.7 K, respectively. The crystals show a two-dimensional to three-dimensional transition at temperatures slightly below $T_c$ with an upturn in the temperature dependence of $B_{c2//ab}$, a temperature dependent huge superconducting anisotropy and a cusplike behavior of the angular dependence of $B_{c2}$. Both misfits are characterized by a strong charge t…
A magnetic field is generally considered to be incompatible with superconductivity as it tends to spin-polarize electrons and breaks apart the opposite-spin singlet superconducting Cooper pairs. Here, an experimental phenomenon is observed that an intriguing reemergent superconductivity evolves from a conventional superconductivity undergoing a hump-like intermediate phase with a finite electric resistance in the van der Waals heterointerface of layered NbSe2 and CrCl3 flakes. This phenomenon merely occurred when the applied magnetic field is parallel to the sample plane and perpendicular to t…
2H-NbSe2 is known to be an archetype layered transitional metal dichalcogenide superconductor with a superconducting transition temperature of 7.3 K.In this article, we investigate the influence of Sn intercalation on superconducting properties of 2H-NbSe2. Sn being nonmagnetic and having no outer shell d-electrons unlike transition metals, one naively would presume that its effect on superconducting properties will be very marginal. However, our magnetic and transport studies reveal a significant reduction of both superconducting transition temperature and upper critical field [Tc and BC2 (0)…
Ising superconductivity in noncentrosymmetric bulk NbSe2
Pavol Jozef Šafárik University in Košice（科希策帕沃尔·约瑟夫·沙法里克大学）；Institute of Experimental Physics, Slovak Academy of Sciences（斯洛伐克科学院实验物理研究所）；Univ. Grenoble Alpes, CNRS, Grenoble INP*, Institut Néel（格勒诺布尔阿尔卑斯大学、法国国家科学研究中心、格勒诺布尔理工学院、内耳研究所）；Univ. Grenoble Alpes, CEA, Grenoble INP, IRIG, Pheliqs（格勒诺布尔阿尔卑斯大学、法国原子能和替代能源委员会、格勒诺布尔理工学院、IRIG、Pheliqs）；Institut des Matériaux Jean Rouxel, Université de Nantes and CNRS-UMR 6502（让·鲁克斯尔材料研究所、南特大学和法国国家科学研究中心联合研究单位6502）
In certain unconventional superconductors with sizable electronic correlations, the availability of closely competing pairing channels leads to characteristic soft collective fluctuations of the order parameters, which leave fingerprints in many observables and allow to scrutinize the phase competition. Superconducting layered materials, where electron-electron interactions are enhanced with decreasing thickness, are promising candidates to display these correlation effects. In this work, we report the existence of a soft collective mode in single-layer NbSe$_2$, observed as a characteristic r…
In quasi low dimensional superconductors under {\it parallel} magnetic fields applied along a conducting direction, vortex lattices with a modulation of Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) type {\it perpendicular} to the field may occur due to an enhanced paramagnetic depairing. As the strength of an in-plane field is varied in a Q2D material, the Josephson vortex lattices accompanied by nodal planes are formed in higher Landau level (LL) modes of the superconducting (SC) order parameter and show field-induced structural transitions. A change of orientation of nodal planes induced by these…
We explore the layered palladium oxides La$_2$PdO$_4$, LaPdO$_2$ and La$_4$Pd$_3$O$_8$ via ab initio calculations. La$_2$PdO$_4$, being low spin $d^8$, is quite different from its high spin nickel analog. Hypothetical LaPdO$_2$, despite its $d^9$ configuration, has a paramagnetic electronic structure very different from cuprates. On the other hand, the hypothetical trilayer compound La$_4$Pd$_3$O$_8$ ($d^{8.67}$) is more promising in that its paramagnetic electronic structure is very similar to that of overdoped cuprates. But even in the $d^9$ limit (achieved by partial substitution of La with…
Multigap superconductivity in Ising superconductors: The case of (LaSe)1.14(NbSe2)m misfit layer compounds
Sorbonne Université（索邦大学）；CNRS-UMR 7588（法国国家科学研究中心联合研究实验室7588）；Université Paris-Saclay（巴黎萨克雷大学）；Centre de Nanosciences et de Nanotechnologies（纳米科学与技术中心）；Institute of Experimental Physics, Slovak Academy of Sciences（斯洛伐克科学院实验物理研究所）；P. J. Safarik University（帕尔沙菲里克大学）；Universität Würzburg（维尔茨堡大学）；Université de Nantes（南特大学）；Institut des Matériaux Jean Rouxel（让·鲁克塞尔材料研究所）；CNR-SPIN（意大利国家研究委员会自旋物理研究所）；Università degli Studi dell’Aquila（阿奎拉大学）；University of Trento（特伦托大学）
The 1964 reports of Fulde, Ferrell, Larkin, and Ovchinnikov (FFLO or LOFF) on paramagnetic enhancement of superconductivity suggested that superconductivity can persist at applied magnetic fields above both its orbital and paramagnetic limits. By forming spatially alternating superconducting and paramagnetic regions, the increase in local magnetic field in the paramagnetic region allows a reduction in field inside the superconductor. We present an FFLO phase diagram model for layered organic superconductors and confirm it with high magnetic field data from four materials. Our work suggests tha…
Tunnel junctions, a well-established platform for high-resolution spectroscopy of superconductors, require defect-free insulating barriers with clean engagement to metals on both sides. Extending the range of materials accessible to tunnel junction fabrication, beyond the limited selection which allows high-quality oxide formation, requires the development of alternative fabrication techniques. Here we show that van-der-Waals (vdW) tunnel barriers, fabricated by stacking layered semiconductors on top of the transition metal dichalcogenide (TMD) superconductor NbSe$_2$, sustain a stable, low no…
The results of the ab initio FLAPW-GGA calculations of the band structure of the newly synthesized tetragonal (space group P4/nmm) layered iron phosphide-oxide: 17K superconductor Sr4Sc2Fe2P2O6 are presented. For Sr4Sc2Fe2P2O6 the optimized structural data, the energy bands, total and partial densities of states, Fermi surface topology, low-temperature electron specific heat and molar Pauli paramagnetic susceptibility have been determined and discussed in comparison with hypothetical isostructural iron arsenide-oxide phase Sr4Sc2Fe2As2O6 and related layered FeAs and FeP superconductors.
LaCo2B2 with a ThCr2Si2-type structure composed of alternately stacked La and CoB layers exhibits metallic electrical conductivity and Pauli paramagnetic behavior down to 2K. Bulk superconductivity with a Tc of ~4K emerges upon substitution with dopant elements; i.e., isovalent substitution to form (La1-xYx)Co2B2, or aliovalent substitution to form La(Co1-xFex)2B2. Highly covalent bonding between Co 3d and B 2p levels in the CoB layers, which is caused by the B 2p level being shallower than the Fermi level, removes magnetic ordering from Co 3d electrons even in the undoped samples.
Here in this short note, we report on the low dimensional 4d and 5d transition metals-chalcogenide based compounds i.e., Ta2PdxS6, showing semiconducting to superconducting transition around 4K with upper critical field outside Pauli paramagnetic limit. It seems couple of different superconducting phases do exist in these new set of compounds. Our short note in this regards is thought provoking, asking to explore various unearthed possible superconducting phases in (Nb/Ta)2Pdx(S/Se/Te)y systems.
Paramagnetic pair breaking is believed to be of increasing importance in many layered superconducting materials such as cuprates and organic compounds. Recently, strong evidence for a phase transition to the Fulde-Ferrell-Larkin-Ovchinnikov(FFLO) state has been obtained for the first time. We present a new theory of competing spin and orbital pair breaking in clean superconducting films or layers. As a general result, we find that the influence of orbital pair breaking on the paramagnetically limited phase boundary is rather strong, and its neglect seldom justified. This is particularly true f…
Transition metal dichalcogenides (TMDs) are quasi-two-dimensional layered compounds exhibiting strongly competing charge-density wave (CDW) and superconducting (SC) order parameters (OPs). The weak van der Waals interlayer bonding between hexagonal layers of octahedral or trigonal prismatic TMD building blocks allows for many polytypes. The non-superconducting $1T$ polytypes can have one or more CDWs. The $2H$ polytypes have two or more Fermi surfaces and saddle bands, allowing for dual orderings, which can be coexisting CDW and SC orderings, two SC gaps as in MgB$_2$, or two CDW gaps. The CDW…
In layered single band systems, the interlayer conductivity depends on the orientation of the in-plane magnetic field and takes maximum values when the magnetic field is perpendicular to flat regions of the Fermi surface. Extending this known results to multi-band systems, we propose an experiment to extract information about their Fermi surface topology. We discuss application of the formula to a FeAs-based superconductor, LaFeAsO$_{1-x}$F$_x$. We show that the magnetically ordered state in the parent compound is clearly distinguished from the paramagnetic state by the oscillation period in t…
We show that layered quenched randomness in planar magnets leads to an unusual intermediate phase between the conventional ferromagnetic low-temperature and paramagnetic high-temperature phases. In this intermediate phase, which is part of the Griffiths region, the spin-wave stiffness perpendicular to the random layers displays anomalous scaling behavior, with a continuously variable anomalous exponent, while the magnetization and the stiffness parallel to the layers both remain finite. Analogous results hold for superfluids and superconductors. We study the two phase transitions into the anom…
Here we report the magnetic properties of the layered cobalt oxide system, LixCoO2, in the whole range of Li composition, 0 <= x <= 1. Based on dc-magnetic susceptibility data, combined with results of 59Co-NMR/NQR observations, the electronic phase diagram of LixCoO2 has been established. As in the related material NaxCoO2, a magnetic critical point is found to exist between x = 0.35 and 0.40, which separates a Pauli-paramagnetic and a Curie-Weiss metals. In the Pauli-paramagnetic regime (x <= 0.35), the antiferromagnetic spin correlations systematically increase with decreasing x. Neverthele…
We consider the problem of the orbital upper critical magnetic field, parallel to the most conducting axis of a quasi-one-dimensional layered superconductor. It is shown that superconductivity can be destroyed through orbital effects at fields much higher than the so-called Clogston-Chandrasekhar paramagnetic limiting field, $H_p$, provided that superconducting pairing of electrons are of a triplet nature. We demonstrate that the superconducting state of the quasi-one-dimensional layered conductor, $\mathrm{Li_{0.9}Mo_6O_{17}}$, is well described by the suggested theory. To this end, we consid…
The phase diagram of the layered organic superconductor $κ$-(ET)$_{2}$Cu[N(CN)$_{2}$]Cl has been accurately measured from a combination of $^{1}$H NMR and AC susceptibility techniques under helium gas pressure. The domains of stability of antiferromagnetic and superconducting long-range orders in the pressure {\it vs} temperature plane have been determined. Both phases overlap through a first-order boundary that separates two regions of inhomogeneous phase coexistence. The boundary curve is found to merge with another first order line related to the metal-insulator transition in the paramagnet…
The phase diagram of non-hydrated Na(x)CoO(2) has been determined by changing the Na content x using a series of chemical reactions. As x increases from 0.3, the ground state goes from a paramagnetic metal to a charge-ordered insulator (at x=1/2) to a `Curie-Weiss metal' (around 0.70), and finally to a weak-moment magnetically ordered state (x>0.75). The unusual properties of the state at 1/2 (including particle-hole symmetry at low T and enhanced thermal conductivity) are described. The strong coupling between the Na ions and the holes is emphasized.
We propose that a new state with a fully gapless Fermi surface appears in quasi-2D multiband superconductors in magnetic field applied parallel to the plane. It is characterized by a paramagnetic moment caused by a finite density of states on the open Fermi surface. We calculate thermodynamic and magnetic properties of the gapless state for both s-wave and d-wave cases, and discuss the details of the 1-st order metamagnetic phase transition that accompanies the appearance of the new phase in s-wave superconductors. We suggest possible experiments to detect this state both in the s-wave (2-H Nb…
