Ginzburg-Landau Free Energy Research Articles

D-wave charge-4e superconductivity from fluctuating pair density waves

We present a theory for charge-4e superconductivity as a leading low-temperature instability with a nontrivial d-wave symmetry. We show that in several microscopic models for the pair-density-wave (PDW) state, when the PDW wave vectors connect special parts of the Fermi surface, the predominant interaction is in the bosonic pairing channel mediated by exchanging low-energy fermions. This bosonic pairing interaction is repulsive in the s-wave channel but attractive in the d-wave one, leading to a d-wave charge-4e superconductor. By analyzing the Ginzburg-Landau free energy including higher-order fluctuation effects of PDW, we find that the charge-4e superconductivity emerges as a vestigial order of PDW, and sets in via a first-order transition. Both the gap amplitude and the transition temperature decay monotonically with increasing superfluid stiffness of the PDW order. Our work provides a microscopic mechanism of higher-charge condensates with unconventional ordering symmetry in strongly-correlated materials.

Classification of Lifshitz invariant in multiband superconductors: An application to Leggett modes in the linear response regime in Kagome lattice models

Multiband superconductors are sources of rich physics arising from multiple order parameters, which show unique collective dynamics including Leggett mode as relative phase oscillations. Previously, it has been pointed out that the Leggett mode can be optically excited in the linear response regime, as demonstrated in a one-dimensional model for multiband superconductors [T. Kamatani , ]. Here we identify the linear coupling term in the Ginzburg-Landau free energy to be the so-called Lifshitz invariant, which takes the form of d·(Ψi*∇Ψj−Ψj*∇Ψi), where d is a constant vector and Ψi and Ψj(i≠j) represent superconducting order parameters. We classify all pairs of irreducible representations of order parameters in the crystallographic point groups that allow for the existence of the Lifshitz invariant. We emphasize that the Lifshitz invariant can appear even in systems with inversion symmetry. The results are applied to a model of s-wave superconductors on a Kagome lattice with various bond orders, for which in some cases we confirm that the Leggett mode appears as a resonance peak in a linear optical conductivity spectrum based on microscopic calculations. We discuss a possible experimental observation of the Leggett mode by a linear optical response in multiband superconductors. Published by the American Physical Society 2024

Drastic magnetic-field-induced chiral current order and emergent current-bond-field interplay in kagome metals.

In kagome metals, the chiral current order parameter [Formula: see text] with time-reversal-symmetry-breaking is the source of various exotic electronic states, while the method of controlling the current order and its interplay with the star-of-David bond order [Formula: see text] are still unsolved. Here, we reveal that tiny uniform orbital magnetization [Formula: see text] is induced by the chiral current order, and its magnitude is prominently enlarged under the presence of the bond order. Importantly, we derive the magnetic-field ([Formula: see text])-induced Ginzburg-Landau (GL) free energy expression [Formula: see text], which enables us to elucidate the field-induced current-bond phase transitions in kagome metals. The emergent current-bond-[Formula: see text] trilinear coupling term in the free energy, [Formula: see text], naturally explains the characteristic magnetic-field sensitive electronic states in kagome metals, such as the field-induced current order and the strong interplay between the bond and current orders. The GL coefficients of [Formula: see text] derived from the realistic multiorbital model are appropriate to explain various experiments. Furthermore, we discuss the field-induced loop current orders in the square lattice models that have been studied in cuprate superconductors.

Ions and dipoles in electric field: nonlinear polarization and field-dependent chemical reaction.

We investigate electric-field effects in dilute electrolytes with nonlinear polarization. As a first example of such systems, we add a dipolar component with a relatively large dipole moment [Formula: see text] to an aqueous electrolyte. As a second example, the solvent itself exhibits nonlinear polarization near charged objects. For such systems, we present a Ginzburg-Landau free energy and introduce field-dependent chemical potentials, entropy density, and stress tensor, which satisfy general thermodynamic relations. In the first example, the dipoles accumulate in high-field regions, as predicted by Abrashikin et al.[Phys.Rev.Lett. 99, 077801 (2007)]. Finally, we consider the case, where Bjerrum ion pairs form a dipolar component with nonlinear polarization. The Bjerrum dipoles accumulate in high-field regions, while field-induced dissociation was predicted by Onsager [J. Chem. Phys.2, 599 (1934)]. We present an expression for the field-dependent association constant K(E), which depends on the field strength nonmonotonically.

Free-energy-based lattice Boltzmann model for emulsions with soluble surfactant

We propose a diffuse interface model to simulate a system of two immiscible liquids with surfactant. This model is based on a modified Ginzburg-Landau free energy functional to account for non-ionic soluble surfactants and couples the Navier-Stokes equations with two Cahn-Hilliard transport equations to represent immiscible fluids and surfactant concentration. The governing equations are solved using a lattice Boltzmann framework. The proposed model is validated for Langmuir and Frumkin adsorption isotherms when applied to simulate a planar interface and a spherical drop equilibration. The model ensures numerical stability and accurate results for low and high surfactant concentrations, and the diffuse interface thickness remains constant even for high surfactant loads. The model also allows achieving a surface tension reduction of 45-50% compared to the clean system, even at low surfactant concentrations. The appropriate surfactant mobility and solubility values are recommended for different values of the strength of nonlinear surfactant coupling.

Dynamics of surfactant-laden drops in shear flow by lattice Boltzmann method

We developed and applied a diffuse interface lattice Boltzmann method for simulating immiscible liquids with soluble surfactants using a modified Ginzburg–Landau free energy functional. We first validated the approach through simulations of planar interfaces and drop equilibration in quiescent fluid. The proposed method accurately captures the phase and surfactant fields with diminishing spurious velocities of 10−6. We systemically examined the effects of capillary number, comparing viscous to surface forces, the combined effect of surfactant and viscosity ratio (λ) of the drop to the continuous phase, and the bulk surfactant load on the deformation and breakage in a shear flow. At a given capillary number (0.05<Ca<0.32), drop behavior is influenced by reduced surface tension, tip-stretching, Marangoni stresses, and surface dilution. These effects either promote (by tip-stretching) or hinder (via Marangoni stresses, surface dilution) the surfactant distribution at the interface, consequently affecting the final drop morphology. As Ca increases, the competition between the viscosity ratio and the presence of surfactant determines drops' topological changes. The presence of surfactants can overcome the effect of viscosity ratio (when 0.05≤λ≤1.7) and promote drop breakup, whereas highly viscous drops (either λ<0.05 or λ>1.7) do not break. Furthermore, high surfactant loads result in higher drop deformation and earlier drop breakup. In brief, our method successfully captures the dynamics of surfactant-laden drops in shear flow, elucidating the complex interplay between flow hydrodynamics and surfactant transport with 3D quantitative phase and surfactant concentration fields.

The supercurrent diode effect and nonreciprocal paraconductivity due to the chiral structure of nanotubes

The phenomenon that critical supercurrents along opposite directions become unequal is called the supercurrent diode effect (SDE). It has been observed in various systems and can often be understood by combining spin-orbit coupling and Zeeman field, which break the spatial-inversion and time-reversal symmetries, respectively. Here, we theoretically investigate another mechanism of breaking these symmetries and predict the existence of the SDE in chiral nanotubes without spin-orbit coupling. The symmetries are broken by the chiral structure and a magnetic flux through the tube. With a generalized Ginzburg-Landau theory, we obtain the main features of the SDE in its dependence on system parameters. We further show that the same Ginzburg-Landau free energy leads to another important manifestation of the nonreciprocity in superconducting systems, i.e., the nonreciprocal paraconductivity (NPC) slightly above the transition temperature. Our study suggests a new class of realistic platforms to investigate nonreciprocal properties of superconducting materials. It also provides a theoretical link between the SDE and the NPC, which were often studied separately.

Landau-Ginzburg theory of charge density wave formation accompanying lattice and electronic long-range ordering

We propose an analytical Landau-Ginzburg theory of the charge density waves coupled with lattice and electronic long-range order parameters. Examples of long-range order include electronic wave function of superconducting Cooper pairs, structural distortions, electric polarization, and magnetization. We formulate the Landau-Ginzburg free energy density as power expansion with respect to the charge density and other long-range order parameters, as well as their spatial gradients, and biquadratic coupling terms. We introduced a biquadratic coupling between the charge density gradient and long-range order parameters, as well as nonlinear higher gradients of the long-range order parameters. The biquadratic gradient coupling is critical to the appearance of different spatially-modulated phases in charge-ordered ferroics and high-temperature superconductors. We derived the thermodynamic conditions for the stability of the spatially-modulated phases, which are the intertwined spatial waves of charge density and lattice/electronic long-range order. The analytical expressions for the energies of different phases, corresponding order parameters, charge density waves amplitudes and modulation periods, obtained in this work, can be employed to guide the comprehensive physical explanation, deconvolution and Bayesian analysis of experimental data on quantum materials ranging from charge-ordered ferroics to high-temperature superconductors.

Cahn–Hilliard equations on random walk spaces

In this paper, we study a nonlocal Cahn–Hilliard equation (CHE) in the framework of random walk spaces, which includes as particular cases, the CHE on locally finite weighted connected graphs, the CHE determined by finite Markov chains or the Cahn–Hilliard Equations driven by convolution integrable kernels. We consider different transitions for the phase and the chemical potential, and a large class of potentials including obstacle ones. We prove existence and uniqueness of solutions in [Formula: see text] of the Cahn–Hilliard Equation. We also show that the Cahn–Hilliard equation is the gradient flow of the Ginzburg–Landau free energy functional on an appropriate Hilbert space. We finally study the asymptotic behavior of the solutions.

A higher degenerated invasive‐invaded species interaction

Invasive‐invaded species problems are of relevance in mathematics applied to population dynamics. In this paper, the mentioned dynamics is introduced based on a fourth‐order parabolic operator, together with coupled non‐linear reaction terms. The fourth‐order operator allows us to model a heterogeneous diffusion, as introduced by the Landau–Ginzburg free energy approach. The reaction terms are given by a coupled non‐linear effect in the invasive species, to account for the action of the invaded species and limited resources, and by a non‐Lipschitz term in the invaded species, to account for possible sprouts, once the invasion occurs. The analysis starts by the proof of existence and uniqueness of solutions, making use of the semi‐group theory and a fixed point argument. Asymptotic solutions to the invasive species are explored with an exponential scaling. Afterward, the problem is analyzed with traveling wave profiles, for which a region of positive solutions is explored.

Rigorous formalism for unconventional symmetry breaking in Fermi liquid theory and its application to nematicity in FeSe

Unconventional symmetry breaking due to nonlocal order parameters has attracted considerable attention in many strongly correlated metals. Famous examples are the nematic order in Fe-based superconductors and the star-of-David charge density order in kagome metals. Such exotic symmetry breaking in metals is a central issue of modern condensed matter physics, while its theoretical foundation is still unclear in comparison with the well-established theory of superconductivity. To overcome this difficulty, here we introduce the "form factor" that generalizes the nonlocal order parameter into the Luttinger-Ward (LW) Fermi liquid theory. We then construct a rigorous formalism of the "density-wave equation" that gives the thermodynamically stable form factor, similarly to the superconducting-gap equation. In addition, a rigorous expression of the Ginzburg-Landau free-energy for the unconventional order is presented to calculate various thermodynamic properties. In the next stage, we apply the derived formalism to a typical Fe-based superconductor FeSe, by using the one-loop LW function that represents the free-energy gain due to the interference among paramagnons. The following key experiments are naturally explained: (i) Lifshitz transition (=disappearance of an electron-pocket) due to the bond+orbital order below $T_c$. (ii) Curie-Weiss behavior of the nematic susceptibility at higher T, and the deviation from the Curie-Weiss behavior at lower T near the nematic quantum-critical-point. (iii) Scaling relation of the specific heat jump at $T_c$, $\Delta C/T_c \propto T_c^b$ with $b \sim 3$. (Note that b=0 in the BCS theory.) These results lead to a conclusion that the nematicity in FeSe is the bond+orbital order due to the "paramagnon interference mechanism". The present theory paves the way for solving various unconventional phase transition systems.

Proximity of superconducting LaCoSi to a ferromagnetic quantum critical point.

The physical characteristics of the 4 K superconductor LaCoSi are studied using first-principles density functional theory inside the local density approximation (LDA) framework. We discover that LDA predicts a ferromagnetic ground state for LaCoSi, which is in disagreement with the experiments. Even though LDA rarely overestimates the local magnetic moment associated with the magnetic ion in itinerant systems, such occurrences highlight the significance of spin fluctuations in the system. In this view, the Ginzburg-Landau free energy expansion and its variation as a function of pressure are used to calculate the amplitude of the zero-point fluctuations. Based on our calculations, we contend that the superconductivity associated with LaCoSi is closely related to a ferromagnetic quantum critical point, making it an intriguing candidate for the category of quantum materials.

Unconditionally strong energy stable scheme for Cahn–Hilliard equation with second‐order temporal accuracy

We propose an unconditionally gradient stable scheme for solving the Cahn–Hilliard equation with second‐order accuracy in time using the effective time‐step analysis. The conventional convex splitting scheme is one of the most well‐known methods for solving gradient flows, and it guarantees both energy stability and first‐order accuracy in time. Recently, there are some researches, which are extended to the second‐order accuracy; however, most of results provide the proof of energy stability for a modified (pseudo) energy or in a weak sense. In this paper, we prove the energy stability of the proposed method with respect to the Ginzburg–Landau free energy functional. Moreover, the unique solvability, mass conservation, and accuracy of the proposed scheme are also proven based on the convex splitting approach. The numerical experiments are presented to show convergence rate, mass conservation, energy stability, and phase separation are in good agreement with the theory.

Anisotropic Vortex Squeezing in Synthetic Rashba Superconductors: A Manifestation of Lifshitz Invariants

Most of 2D superconductors are of type II, i.e., they are penetrated by quantized vortices when exposed to out-of-plane magnetic fields. In presence of a supercurrent, a Lorentz-like force acts on the vortices, leading to drift and dissipation. The current-induced vortex motion is impeded by pinning at defects, enabling the use of superconductors to generate high magnetic fields without dissipation. Usually, the pinning strength decreases upon any type of pair-breaking. Here we show that in Rashba superconductors the application of an in-plane field leads, instead, to an unexpected enhancement of pinning. When rotating the in-plane component of the field with respect to the current direction, the vortex inductance turns out to be highly anisotropic. We explain this phenomenon as a manifestation of Lifshitz invariant terms in the Ginzburg-Landau free energy, which are enabled by inversion and time-reversal symmetry breaking and lead to an elliptic squeezing of vortex cores. Our experiment provides access to a fundamental property of Rashba superconductors and offers an entirely new approach to vortex manipulation.

Nodeless time-reversal symmetry breaking in the centrosymmetric superconductor Sc5Co4Si10 probed by muon-spin spectroscopy

We investigate the superconducting properties of Sc$_{5}$Co$_{4}$Si$_{10}$ using low-temperature resistivity, magnetization, heat capacity, and muon-spin rotation and relaxation ($\mu$SR) measurements. We find that Sc$_{5}$Co$_{4}$Si$_{10}$ {exhibits type-II} superconductivity with a superconducting transition temperature $T_\mathrm{C}= 3.5 (1)$\,K. The temperature dependence of the superfluid density obtained from transverse-field $\mu$SR spectra is best modeled using an isotropic Bardeen-Cooper-Schrieffer type $s$-wave gap symmetry with $2\Delta/k_\mathrm{B}T_\mathrm{C} = 2.84(2)$. However, the zero-field muon-spin relaxation asymmetry reveals the appearance of a spontaneous magnetic field below $T_\mathrm{C}$, indicating that time-reversal symmetry (TRS) is broken in the superconducting state. Although this behavior is commonly associated with non-unitary or mixed singlet-triplet pairing, our group-theoretical analysis of the Ginzburg-Landau free energy alongside density functional theory calculations indicates that unconventional mechanisms are pretty unlikely. Therefore, we have hypothesized that TRS breaking may occur via a conventional electron-phonon process.

Superfluid transition temperature and fluctuation theory of spin-orbit- and Rabi-coupled fermions with tunable interactions

We obtain the superfluid transition temperature of equal Rashba-Dresselhaus spin-orbit- and Rabi-coupled Fermi superfluids, from the Bardeen-Cooper-Schrieffer (BCS) to Bose-Einstein condensate (BEC) regimes in three dimensions for tunable $s$-wave interactions. In the presence of Rabi coupling, we find that spin-orbit coupling enhances (reduces) the critical temperature in the BEC (BCS) limit. For fixed interactions, we show that spin-orbit coupling can convert a first-order (discontinuous) phase transition into a second-order (continuous) phase transition, as a function of Rabi coupling. We derive the Ginzburg-Landau free energy to sixth power in the superfluid order parameter to describe both continuous and discontinuous phase transitions as a function of spin-orbit and Rabi couplings. Lastly, we develop a time-dependent Ginzburg-Landau fluctuation theory for an arbitrary mixture of Rashba and Dresselhaus spin-orbit couplings at any interaction strength.

P -wave superconductivity in Luttinger semimetals

We consider the three-dimensional spin-orbit-coupled Luttinger semimetal of ``spin'' $3/2$ particles in presence of weak attractive interaction in the $l=1$ ($p$-wave) channel, and determine the low-temperature phase diagram for both particle- and hole dopings. The phase diagram depends crucially on the sign of the chemical potential, with two different states (with total angular momentum $j=0$ and $j=3$) competing on the hole-doped side, and three (one $j=1$ and two different $j=2$) states on the particle-doped side. The ground-state condensates of Cooper pairs with the total angular momentum $j=1,2,3$ are selected by the quartic, and even sextic terms in the Ginzburg-Landau free energy. Interestingly, we find that all the $p$-wave ground states appearing in the phase diagram, while displaying different patterns of reduction of the rotational symmetry, preserve time reversal. The resulting quasiparticle spectrum is either fully gapped or with point nodes, with nodal lines being absent.

Instability analysis and geometric perturbation theory to a mutual beneficial interaction between species with a higher order operator

<abstract><p>The higher order diffusion can be understood as a generalization to the classical fickian diffusion. To account for such generalization, the Landau-Ginzburg free energy concept is applied leading to a fourth order spatial operator. This kind of diffusion induces a set of instabilities in the proximity of the critical points raising difficulties to study the convergence of Travelling Waves (TW) solutions. This paper aims at introducing a system of two species driven by a mutual interaction towards prospering and with a logistic term in their respective reactions. Previous to any analytical finding of TW solutions, the instabilities of such solutions are studied. Afterwards, the Geometric Perturbation Theory is applied to provide means to search for a linearized hyperbolic manifold in the proximity of the equilibrium points. The homotopy graphs for each of the flows to the hyperbolic manifolds are provided, so that analytical solutions can be obtained in the proximity of the critical points. Additionally, the set of eigenvalues in the homotopy graphs tend to cluster and synchronize for increasing values of the TW-speed.</p></abstract>

Symmetry and polarity of antiphase boundaries in PbZrO3

The polar properties of antiphase boundaries (APBs) in PbZrO$_3$ are analyzed in detail using a recently developed layer group approach in order parameter space and compared with the results from Landau-Ginzburg free energy description. It is shown that the former approach reveals the microscopic APBs' properties, and predicts polar APB structures at particular positions inside the unit cell, which agree very well with recent experimental obsevations [Wei, et.~al. \cite{Wei2014,Wei2015}]. The systematic usage of the method is developed. In contrast with it the commonly used free energy description obscures the microscopic features but still can reflect the macroscopic properties of the APBs by taking into account the bilinear coupling of polarization and order parameter gradients. The relation between the layer group approach and the Landau-Ginzburg free energy description is discussed and two mechanisms of polarization switching inside the APBs are distinguished. It is illustrated that the polar APBs observed in PbZrO$_3$ are consistently and naturally explained by the layer group approach. This analysis is expected to have a significant impact also in other materials.

The absence of superconductivity in the next-to-leading order Ginzburg–Landau functional for Bardeen–Cooper–Schrieffer superconductor

Shortly after the Gor’kov microscopic derivation of the Ginzburg–Landau (GL) model via a small order parameter expansion in Bardeen–Cooper–Schrieffer theory of superconductivity, the derivation was carried to next-to-leading order in that parameter and its spatial derivatives. The aim was to obtain a generalized GL free energy that approximates the microscopic model better. Since 1960s, multiple works have claimed or implicitly assumed that this extended GL model corresponds to the free energy and has solutions in the form of local minima describing superconductivity, such as vortex solutions. In contrast to this, we prove that this extended GL functional does not represent free energy since it does not have any solutions in the form of minima. Accordingly, it cannot be used to describe superconducting states.