FFLO State Research Articles

Constructing the Fulde-Ferrell-Larkin-Ovchinnikov State in a CrOCl/NbSe2 van der Waals Heterostructure.

Time reversal symmetry breaking in superconductors, resulting from external magnetic fields or spontaneous magnetization, often leads to unconventional superconducting properties. In this way, an intrinsic phenomenon called the Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) state may be realized by the Zeeman effect. Here, we construct the FFLO state in an artificial CrOCl/NbSe2 van der Waals (vdW) heterostructure by utilizing the superconducting proximity effect of NbSe2 flakes. The proximity-induced superconductivity demonstrates a considerably weak gap of about 0.12 meV, and the in-plane upper critical field reveals the behavior of the FFLO state. First-principles calculations uncover the origin of the proximitized superconductivity, which indicates the importance of Cr vacancies or line defects in CrOCl. Moreover, the FFLO state could be induced by the inherent large spin splitting in CrOCl. Our findings not only provide a practical scheme for constructing the FFLO state but also inspire the discovery of an exotic FFLO state in other two-dimensional vdW heterostructures.

Magnetically tunable supercurrent in dilute magnetic topological insulator-based Josephson junctions

A superconductor, when exposed to a spin-exchange field, can exhibit spatial modulation of its order parameter, commonly referred to as the Fulde–Ferrell–Larkin–Ovchinnikov state. Such a state can be induced by controlling the spin-splitting field in Josephson junction devices, allowing access to a wide range of the phase diagram. Here we demonstrate that a Fulde–Ferrell–Larkin–Ovchinnikov state can be induced in Josephson junctions based on the two-dimensional dilute magnetic topological insulator (Hg,Mn)Te. We do this by observing the dependence of the critical current on the magnetic field and temperature. The substitution of Mn dopants induces an enhanced Zeeman effect, which can be controlled with high precision by using a small external magnetic field. We observe multiple re-entrant behaviours of the critical current as a response to an in-plane magnetic field, which we assign to transitions between ground states with a phase shifted by π. This will enable the study of the Fulde–Ferrell–Larkin–Ovchinnikov state in much more accessible experimental conditions.

Superconducting Quasicrystals

AbstractDan Shechtman's discovery of quasicrystals in 1982 introduced the scientific world to aperiodic crystals with unique rotational symmetries, redefining traditional crystallography. Although superconductivity in related periodic approximants has since been observed, true bulk superconductivity in quasicrystals was confirmed only in 2018. This recent discovery opens a new horizon not only for the study of correlated quasicrystals but more generally for the study of superconductivity with nontrivial spatial order. The theoretical understanding of superconducting quasicrystals poses challenges due to their lack of periodicity. Notably, they exhibit non‐BCS type superconductivity and distinct electromagnetic responses, reminiscent of the so‐called FFLO state. In this review, we provide an overview of superconducting quasicrystals, along with some “behind‐the‐scenes” information.

Effect of Fermi surface topology change on the Kagome superconductor CeRu2 under pressure

The cubic Laves phase compound CeRu2 with a Kagome substructure of Ru has been investigated to understand myriad fascinating phenomena resulting from competition among its various physical and geometric features. Such phenomena include flat bands, van Hove singularities, Dirac cones, reentrant superconductivity, magnetism, the Fulde–Ferrell–Larkin–Ovchinnikov state, valence fluctuations, time-irreversible anisotropic s-state superconductivity, etc. Extensive studies have thus been carried out since 1958 when the highly unusual coexistence of superconductivity and ferromagnetism was proposed for the mixed compounds (Ce,Gd)Ru2. Activity has accelerated in recent years due to increasing interest in topological states in superconductors. However, there has been little investigation of the mutual influence of these fascinating states. Therefore, we systematically investigated the superconductivity and possible Fermi surface topological change in CeRu2via magnetic, resistivity, and structural measurements under pressure up to ∼168 GPa. An unusual phase diagram that suggests an intriguing interplay between the compound's superconducting order and Fermi surface topological order has been constructed. A resurgence in its superconducting transition temperature was observed above 28 GPa. Our experiments have identified a structural transition above 76 GPa and a few tantalizing phase transitions driven by high pressure. Our high-pressure results further suggest that superconductivity and Fermi surface topology in CeRu2 are strongly intertwined.

Reentrant Proximity-Induced Superconductivity for GeTe Semimetal

We experimentally investigate charge transport in In–GeTe and In–GeTe–In proximity devices, which are formed as junctions between superconducting indium leads and thick single crystal flakes of α-GeTe topological semimetal. We observe nonmonotonic effects of the applied external magnetic field, including reentrant superconductivity in In–GeTe–In Josephson junctions: supercurrent reappears at some finite magnetic field. For a single In–GeTe Andreev junction, the superconducting gap is partially suppressed in zero magnetic field, while the gap is increased nearly to the bulk value for some finite field before its full suppression. We discuss possible reasons for the results obtained, taking into account spin polarization of Fermi arc surface states in topological semimetal \\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\alpha $$\\end{document}-GeTe with a strong spin–orbit coupling. In particular, the zero-field surface state spin polarization partially suppresses the superconductivity, while it is recovered due to the modified spin-split surface state configuration in finite fields. As an alternative possible scenario, the transition into the Fulde–Ferrell–Larkin–Ovchinnikov state is discussed. However, the role of strong spin–orbit coupling in forming the nonmonotonic behavior has not been analyzed for heterostructures in the Fulde–Ferrell–Larkin–Ovchinnikov state, which is crucial for junctions involving GeTe topological semimetal.

Multiple-q current states in a multicomponent superconducting channel

It is well-established that multicomponent superconductors can host different nonstandard phenomena such as broken-time reversal symmetry (BTRS) states, exotic Fulde–Ferrell–Larkin–Ovchinnikov phases, the fractional Josephson effect as well as plenty of topological defects like phase solitons, domain walls and unusual vortex structures. We show that in the case of a two-component superconducting quasi-one-dimensional channel this catalogue can be extended by a novel inhomogeneous current state, which we have termed as a multiple-q state, characterized by the coexistence of two different interpenetrating Cooper pair condensates with different total momenta. Within the Ginzburg–Landau formalism for a dirty two-band superconductor with sizable impurity scattering treated in the Born-approximation we reveal that under certain conditions, the occurrence of multiple-q states can induce a cascade of transitions involving switching between them and the homogeneous BTRS (non-BTRS) states and vice versa leading this way to a complex interplay of homogeneous and inhomogeneous current states. We find that hallmarks of such a multiple-q state within a thin wire or channel can be a saw-like dependence of the depairing current and the existence of two distinct stable branches on it (a bistable current state).

Generation and decay of Higgs mode in a strongly interacting Fermi gas

We investigate the life cycle of the large amplitude Higgs mode in strongly interacting superfluid Fermi gas. Through numerical simulations with time-dependent density functional theory and the technique of the interaction quench, we verify the previous theoretical predictions on the mode’s frequency. Next, we demonstrate that the mode is dynamically unstable against external perturbation and qualitatively examine the emerging state after the mode decays. The post-decay state is characterized by spatial fluctuations of the order parameter and density at scales comparable to the superfluid coherence length scale. We identify similarities with FFLO states, which become more prominent at higher dimensionalities and nonzero spin imbalances.

The superconducting FFLO state induced by orbital effect of in-plane magnetic field

The superconducting FFLO state induced by orbital effect of in-plane magnetic field

Quantum geometric effect on Fulde-Ferrell-Larkin-Ovchinnikov superconductivity

Quantum geometry characterizes the geometric properties of Bloch electrons in the wave space, represented by the quantum metric and the Berry curvature. Recent studies have revealed that the quantum geometry plays a major role in various physical phenomena, from multipole to non-Hermitian physics. For superconductors, the quantum geometry is clarified to appear in the superfluid weight, an essential quantity of superconductivity. Although the superfluid weight was considered to be determined by the Fermi-liquid contribution for a long time, the geometric contribution is not negligible in some superconductors such as artificial flat-band systems and monolayer FeSe. While the superfluid weight is essential for many superconducting phenomena related to the center of mass momenta of Cooper pairs (CMMCP), the full scope of the quantum geometric effect on superconductivity remains unresolved. In this paper, we study the quantum geometric effect on the Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) state acquiring a finite CMMCP in equilibrium. As a benchmark, the phase diagrams of effective models for monolayer FeSe in an in-plane magnetic field are calculated. In the case of the isotropic $s$-wave pairing, the quantum geometry stabilizes the BCS state, and a metastable BCS state appears in the high-magnetic-field region. In addition, the quantum geometry induces the phase transition from the FFLO state to the BCS state with increasing temperature. However, for the intersublattice pairing, the quantum geometry gives a negative contribution to the superfluid weight; this can induce the FFLO superconductivity in particular parameter sets.

Emergent anisotropy in the Fulde–Ferrell–Larkin–Ovchinnikov state

Exotic superconductivity is formed by unconventional electron pairing and exhibits various unique properties that cannot be explained by the basic theory. The Fulde–Ferrell–Larkin–Ovchinnikov (FFLO) state is known as an exotic superconducting state in that the electron pairs have a finite center-of-mass momentum leading to a spatially modulated pattern of superconductivity. The spatial modulation endows the FFLO state with emergent anisotropy. However, the anisotropy has never been experimentally verified despite numerous efforts over the years. Here, we report detection of anisotropic acoustic responses depending on the sound propagation direction appearing above the Pauli limit. This anisotropy reveals that the two-dimensional FFLO state has a center-of-mass momentum parallel to the nesting vector on the Fermi surface. The present findings will facilitate our understanding of not only superconductivity in solids but also exotic pairings of various particles.

Feasibility of a Fulde-Ferrell-Larkin-Ovchinnikov superfluid Fermi atomic gas

We theoretically explore a promising route to achieve the Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) state in a spin-imbalanced ultracold Fermi gas. In the current stage of cold atom physics, search for this exotic Fermi superfluid is facing two serious difficulties: One is the desperate destruction of the FFLO long-range order by FFLO pairing fluctuations, which precludes entering the phase through a second-order transition, even in three dimension. The other is the fierce competition with the phase separation into the BCS (Bardeen-Cooper-Schrieffer) state and the spin-polarized normal state. Including strong FFLO pairing fluctuations within the framework of the strong-coupling theory developed by Nozi\`eres and Schmitt-Rink, we show that the anisotropy of Fermi surface introduced by an optical lattice makes the FFLO state stable against the paring fluctuations. This stabilized FFLO state is also found to be able to overcome the competition with the phase separation under a certain condition. Since the realization of unconventional Fermi superfluids is one of the most exciting challenges in cold atom physics, our results would contribute to the further development of this field.

Orbital-induced crossover of the Fulde-Ferrell-Larkin-Ovchinnikov phase into Abrikosov-like states

The Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) state can emerge in superconductors for which the orbital critical field exceeds the Pauli limit. Here, we present angular-resolved specific-heat data of the quasi-two-dimensional organic superconductor $\kappa$-(ET)$_2$Cu(NCS)$_2$, with a focus on high fields in the regime of the FFLO transition. For an increasing out-of-plane tilt of the applied magnetic field, which leads to an increase of orbital contributions, we found that the nature of the superconducting transition changes from second to first order and that a further transition appears within the high-field superconducting phase. However, the superconducting state above the Pauli limit is stable for field tilt of several degrees. Since any finite perpendicular component of the magnetic field necessarily leads to quantization of the orbital motion, the resulting vortex lattice states compete with the modulated order parameter of the FFLO state leading to complex high-field superconducting phases. By solving the linearized self-consistency equation within weak-coupling BCS theory, we show that our results are clear experimental evidence of an orbital-induced transformation of the FFLO order-parameter into Abrikosov-like states of higher Landau levels.

Competition between orbital effects, Pauli limiting, and Fulde–Ferrell–Larkin–Ovchinnikov states in 2D transition metal dichalcogenide superconductors

We compare the upper critical field of bulk single-crystalline samples of the two intrinsic transition metal dichalcogenide superconductors, 2H-NbSe2 and 2H-NbS2, in high magnetic fields where their layer structure is aligned strictly parallel and perpendicular to the field, using magnetic torque experiments and a high-precision piezo-rotary positioner. While both superconductors show that orbital effects still have a significant impact when the layer structure is aligned parallel to the field, the upper critical field of NbS2 rises above the Pauli limiting field and forms a Fulde–Ferrell–Larkin–Ovchinnikov (FFLO) state, while orbital effects suppress superconductivity in NbSe2 just below the Pauli limit, which excludes the formation of the FFLO state. From the out-of-plane anisotropies, the coherence length perpendicular to the layers of 31 Å in NbSe2 is much larger than the interlayer distance, leading to a significant orbital effect suppressing superconductivity before the Pauli limit is reached, in contrast to the more 2D NbS2.

Superconducting spin smecticity evidencing the Fulde-Ferrell-Larkin-Ovchinnikov state in Sr2RuO4.

Translational symmetry breaking is antagonistic to static fluidity but can be realized in superconductors, which host a quantum-mechanical coherent fluid formed by electron pairs. A peculiar example of such a state is the Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) state, induced by a time-reversal symmetry-breaking magnetic field applied to spin-singlet superconductors. This state is intrinsically accompanied by the superconducting spin smecticity, spin density-modulated fluidity with spontaneous translational-symmetry breaking. Detection of such spin smecticity provides unambiguous evidence for the FFLO state, but its observation has been challenging. Here, we report the characteristic "double-horn" nuclear magnetic resonance spectrum in the layered superconductor Sr2RuO4 near its upper critical field, indicating the spatial sinusoidal modulation of spin density that is consistent with superconducting spin smecticity. Our work reveals that Sr2RuO4 provides a versatile platform for studying FFLO physics.

FFLO state driven by quasiperiodic Zeeman field and its transition to localized states

We numerically study the ground-state properties of a one-dimensional lattice model in the presence of a quasiperiodic Zeeman field, by means of the density matrix renormalization group algorithm. We map out a global phase diagram, which encloses a Bardeen-Cooper-Schrieffer (BCS) phase, a Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) phase where the Cooper pairs obtain a finite center-of-mass momentum, and a localized phase. The FFLO phase is promoted by the quasiperiodic Zeeman field, which demonstrates a power-law pairing correlation with a critical exponent ${\ensuremath{\eta}}_{\mathrm{FFLO}}<1$ decaying much slower than the charge density and spin density correlations. By tuning the interaction and the filling factor, we find the FFLO phase is suppressed in the strong interaction and low filling regions. A large Zeeman field destroys the FFLO state and drives a superconductor-insulator transition. Furthermore, we propose this FFLO phase and the superconductor-insulator transition could be observed in the optical lattice experiment.

FFLO Phase in Layered Organic Superconductors

FFLO Phase in Layered Organic Superconductors

Quasiparticle Nodal Plane in the Fulde-Ferrell-Larkin-Ovchinnikov State of FeSe.

The Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) state, characterized by Cooper pairs condensed at finite momentum, has been a long-sought state that remains unresolved in many classes of fermionic systems, including superconductors and ultracold atoms. A fascinating aspect of the FFLO state is the emergence of periodic nodal planes in real space, but its observation is still lacking. Here we investigate the superconducting order parameter at high magnetic fields H applied perpendicular to the ab plane in a high-purity single crystal of FeSe. The heat capacity and magnetic torque provide thermodynamic evidence for a distinct superconducting phase at the low-temperature/high-field corner of the phase diagram. Despite the bulk superconductivity, spectroscopic-imaging scanning tunneling microscopy performed on the same crystal demonstrates that the order parameter vanishes at the surface upon entering the high-field phase. These results provide the first demonstration of a pinned planar node perpendicular to H, which is consistent with a putative FFLO state.

Fermi Surface Structure and Isotropic Stability of Fulde-Ferrell-Larkin-Ovchinnikov Phase in Layered Organic Superconductor β″-(BEDT-TTF)2SF5CH2CF2SO3

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.

Disorder-robust high-field superconducting phase of FeSe single crystals

When exposed to high magnetic fields, certain materials manifest an exotic superconducting (SC) phase that has attracted considerable attention. A proposed explanation for the origin of the high-field SC phase is the Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) state. This state is characterized by inhomogeneous superconductivity, where the Cooper pairs have finite center-of-mass momenta. Recently, the high-field SC phase was observed in FeSe, and it was deemed to originate from the FFLO state. Here, we synthesize FeSe single crystals with different levels of disorder. The level of disorder is expressed by the ratio of the mean free path to the coherence length and ranges between 35 and 1.2. The upper critical field \textit{B}$_{\rm{c}2}$ was obtained by both resistivity and magnetic torque measurements over a wide range of temperatures, which went as low as $\sim$0.5 K, and magnetic fields, which went up to $\sim$38 T along the \textit{c} axis and in the \textit{ab} plane. In the high-field region parallel to the \textit{ab} plane, an unusual SC phase was confirmed in all the crystals, and the phase was found to be robust against disorder. This result suggests that the high-field SC phase in FeSe is not a conventional FFLO state.

Thermodynamic evidence for the formation of a Fulde-Ferrell-Larkin-Ovchinnikov phase in the organic superconductor λ−(BETS)2GaCl4

In this work, the thermodynamic properties of the organic superconductor $\lambda$-(BETS)$_2$GaCl$_4$ 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 $H_{\rm FFLO}$ $\sim$ 10~T, which corresponds to the Pauli limiting field $H_{\rm P}$. This anomaly probably originates from a transition from a uniform superconducting state to the FFLO state. $H_{\rm FFLO}$ does not show a strong field-angular dependence due to a quasi-isotropic paramagnetic effect in $\lambda$-(BETS)$_2$GaCl$_4$. The thermodynamic anomaly at $H_{\rm FFLO}$ is smeared out and low-temperature upper critical field $H_{\rm c2}$ changes significantly if fields are not parallel to the conducting plane even for a deviation of $\sim$0.5$^{\circ}$. 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)$_2$GaCl$_4$ from a thermodynamic point of view.