Dynamical Susceptibility Research Articles

Gapless spin excitations in the superconducting state of a quasi-one-dimensional spin-triplet superconductor

Majorana zero modes form as intrinsic defects in an odd-orbital one-dimensional superconductor, thus motivating the search for such materials in the pursuit of Majorana physics. Here, we present combined experimental results and first-principles calculations which suggest that quasi-one-dimensional ${\mathrm{K}}_{2}{\mathrm{Cr}}_{3}{\mathrm{As}}_{3}$ may be such a superconductor. Using inelastic neutron scattering we probe the dynamic spin susceptibilities of ${\mathrm{K}}_{2}{\mathrm{Cr}}_{3}{\mathrm{As}}_{3}$ and ${\mathrm{K}}_{2}{\mathrm{Mo}}_{3}{\mathrm{As}}_{3}$ and show the presence of antiferromagnetic spin fluctuations in both compounds. Below the superconducting transition, these fluctuations gap in ${\mathrm{K}}_{2}{\mathrm{Mo}}_{3}{\mathrm{As}}_{3}$ but not in ${\mathrm{K}}_{2}{\mathrm{Cr}}_{3}{\mathrm{As}}_{3}$. Using first-principles calculations, we show that these fluctuations likely arise from nesting on one-dimensional features of the Fermi surface. Considering these results we propose that while ${\mathrm{K}}_{2}{\mathrm{Mo}}_{3}{\mathrm{As}}_{3}$ is a conventional superconductor, ${\mathrm{K}}_{2}{\mathrm{Cr}}_{3}{\mathrm{As}}_{3}$ is likely a spin triplet, and consequently a topological superconductor.

Non-Hertz-Millis scaling of the antiferromagnetic quantum critical metal via scalable Hybrid Monte Carlo

A key component of the phase diagram of many iron-based superconductors and electron-doped cuprates is believed to be a quantum critical point (QCP), delineating the onset of antiferromagnetic spin-density wave order in a quasi-two-dimensional metal. The universality class of this QCP is believed to play a fundamental role in the description of the proximate non-Fermi liquid behavior and superconducting phase. A minimal model for this transition is the O(3) spin-fermion model. Despite many efforts, a definitive characterization of its universal properties is still lacking. Here, we numerically study the O(3) spin-fermion model and extract the scaling exponents and functional form of the static and zero-momentum dynamical spin susceptibility. We do this using a Hybrid Monte Carlo (HMC) algorithm with a novel auto-tuning procedure, which allows us to study unprecedentedly large systems of 80 × 80 sites. We find a strong violation of the Hertz-Millis form, contrary to all previous numerical results. Furthermore, the form that we do observe provides good evidence that the universal scaling is actually governed by the analytically tractable fixed point discovered near perfect “hot-spot’" nesting, even for a larger nesting window. Our predictions can be directly tested with neutron scattering. Additionally, the HMC method we introduce is generic and can be used to study other fermionic models of quantum criticality, where there is a strong need to simulate large systems.

Dynamical Susceptibilities of Confined Water from Room Temperature to the Glass Transition.

We confine water to narrow silica pores, where crystallization is suppressed, and determine the dynamical susceptibilities of the liquid from room temperature down to the glass transition by combining broadband dielectric spectroscopy (BDS) with 1H and 2H nuclear magnetic resonance (NMR), in particular, by establishing NMR field-cycling relaxometry. For the correlation times, derivative analysis reveals Vogel-Fulcher-Tammann and Arrhenius regimes at T ≥ 215 K and T ≤ 160 K, respectively, which are separated by a broad crossover region. The continuous transition in the temperature dependence is accompanied by a gradual change from asymmetric high-temperature shapes of the dynamical susceptibilities to symmetric low-temperature ones and by a steady decrease of the dielectric relaxation strength. In the Arrhenius regime (Ea = 0.48 eV) at T ≤ 160 K, 2D 2H NMR spectra reveal quasi-isotropic water reorientation. We rationalize these results in terms of a crossover to an interface-affected, noncooperative relaxation involving both rotational and translational motions.

Magnetic excitations in the helical Rashba superconductor

We investigate the magnetic excitation spectrum in the helical state of a noncentrosymmetric superconductor with inversion symmetry breaking and strong Rashba spin–orbit coupling. For this purpose we derive the general expressions of the dynamical spin response functions under the presence of strong Rashba splitting of conduction bands, superconducting gap and external field which lead to stabilization of Cooper pairs with finite overall momentum in a helical state. The latter is characterized by momentum space regions of paired and unpaired states with different quasiparticle dispersions. The magnetic response is determined by i) excitations within and between both paired and unpaired regions ii) anomalous coherence factors and iii) additional spin matrix elements due to helical Rashba spin texture of bands. We show that as a consequence typical correlated real space and spin space anisotropies appear in the dynamical susceptibility which would be observable as a characteristic fingerprint for a helical superconducting state in inelastic neutron scattering investigations.

Low-frequency spin dynamics in diluted magnetic semiconductors

The low-frequency dynamical magnetic properties in paramagnetic diluted magnetic semiconductors are addressed in the framework of the dynamical mean-field theory applied for the Kondo lattice model. In the infinite-dimensional limit, a set of self-consistent equations is derived so the single-particle Green's function and its self-energy can be evaluated numerically. In terms of the Green's function and self-energies, the local dynamical spin susceptibility function and then the spin-relaxation rate are explicitly expressed based on the Baym-Kadanoff approach. It is found that the spin fluctuations become dominated, indicated by the sharp peak appearing at the low frequency of the spin dynamical susceptibility function in the case of large magnetic coupling and temperature close to the paramagnetic-ferromagnetic transition point. The low-frequency spin dynamic in the systems is also addressed in the signatures of the spin-relaxation process. In the case of large temperature and small magnetic coupling, the spin-relaxation rate releases the scenario of the Korringa process specifying the weak correlation systems likely normal metals. Otherwise, i.e., at small temperature and large magnetic coupling, we find exponential behavior of the spin-relaxation rate versus temperature. Moreover, at a temperature approaching the paramagnetic-ferromagnetic transition point, one finds sharp suppression of the spin-relaxation rate or speeding up of the spin-relaxation time. These scenarios are attributed to the appearance of the magnetic coherence bound state or the spin clusters in diluted magnetic semiconductors due to the strongly magnetic correlations.

Quantum critical dynamics in the two-dimensional transverse Ising model

In the vicinity of the quantum critical point (QCP), thermodynamic properties diverge toward zero temperature governed by universal exponents. Although this fact is well known, how it is reflected in quantum dynamics has not been addressed. The QCP of the transverse Ising model on a triangular lattice is an ideal platform to test the issue, since it has an experimental realization, the dielectrics being realized in an organic dimer Mott insulator, $\ensuremath{\kappa}\text{\ensuremath{-}}{\mathrm{ET}}_{2}X$, where a quantum electric dipole represents the Ising degrees of freedom. We track the Glauber-type dynamics of the model by constructing a kinetic protocol based on the quantum Monte Carlo method. The dynamical susceptibility takes the form of the Debye function and shows a significant peak narrowing in approaching a QCP due to the divergence of the relaxation timescale. It explains the anomaly of dielectric constants observed in the organic materials, indicating that the material is very near the ferroelectric QCP. We disclose how the dynamical and other critical exponents develop near QCP beyond the simple field theory.

Electron-phonon correlations inducing excitonic excitations in semimetal and semiconducting materials

The influence of phonons on the low-energy excitonic excitations at zero temperature in the extended Falicov-Kimball model has been investigated. In the framework of the unrestricted Hartree-Fock approximation, a set of self-consistent equations for the excitonic condensate order parameter and a lattice distortion is derived when both electron-phonon coupling and electron-hole Coulomb interaction are treated on an equal footing. The low-energy excitation properties of the excitonic condensate are addressed in signatures of the optical conductivity and the dynamical excitonic susceptibility function. The real part of the optical conductivity is evaluated by the Kubo linear response theory and the imaginary part of the dynamical excitonic susceptibility is found by adapting the random phase approximation. In the semimetal state, one always finds a sharp peak in the optical conductivity spectrum indicating the stability of the excitonic condensation in the BCS type if the correlation between electrons and phonons becomes significant. In contrast, the peak is smeared out on the semiconducting side indicating the stability of the BEC-type excitonic condensate. In this semiconducting side, the sharp peak signature appears and the system turns to the BCS-type excitonic condensation state by increasing the electron-phonon correlations. In either the semimetal or the semiconducting normal state, increasing the electron-phonon correlations always reinforces a low-energy sharp peak in the dynamical excitonic susceptibility spectrum, indicating the existence of the tightly bound excitonic excitations before the condensation state. Specifically, on the semiconducting side, the ``halo'' phase with the preformed excitons exiting outside of the BEC-excitonic condensation state has been specified. The halo phase becomes more recognizable by raising the electron-phonon correlations.

Multipartite entanglement in the one-dimensional spin- 12 Heisenberg antiferromagnet

Multipartite entanglement was thought to be intrinsically difficult to measure in solids, but recent work has established connections between multipartite entanglement, dynamic susceptibilities, and neutron scattering data, via the quantum Fisher information. This work focuses on the paradigmatic spin-half chain and shows that there are further simplifications: even static structure factors contain quantitative information about multipartite entanglement at low temperatures. Theory, numerics, and experiment then suggest that a high degree of multipartite entanglement is observable in Heisenberg chain compounds, including KCuF${}_{3}$.

Electron-Hole Asymmetry of Quantum Collective Excitations in High-Tc Copper Oxides

We carry out a systematic study of collective spin- and charge excitations for the canonical single-band Hubbard, $t$-$J$-$U$, and $t$-$J$ models of high-temperature copper-oxide superconductors, both on electron- and hole-doped side of the phase diagram. Recently developed variational wave function approach, combined with the expansion in inverse number of fermionic flavors, is employed. All three models exhibit a substantial electron-hole asymmetry of magnetic excitations, with a robust paramagnon emerging for hole-doping, in agreement with available resonant inelastic $x$-ray scattering data for the cuprates. The $t$-$J$ model yields additional high-energy peak in the magnetic spectrum that is not unambiguously identified in spectroscopy. For all considered Hamiltonians, the dynamical charge susceptibility contains a coherent mode for both hole- and electron doping, with overall bandwidth renormalization controlled by the on-site Coulomb repulsion. Away from the strong-coupling limit, the antiferromagnetic ordering tendency is more pronounced on electron-doped side of the phase diagram.

Dynamical susceptibilities near ideal glass transitions.

Building on the recently derived inhomogeneous mode-coupling theory, we extend the generalized mode-coupling theory of supercooled liquids to inhomogeneous environments. This provides a first-principles-based, systematic, and rigorous way of deriving high-point dynamical susceptibilities from variations of the many-body dynamic structure factors with respect to their conjugate field. This framework allows for a fully microscopic possibility to probe for collective relaxation mechanisms in supercooled liquids near the mode-coupling glass transition. The behavior of these dynamical susceptibilities is then studied in the context of simplified self-consistent relaxation models.

Choice of diameters in a polydisperse model glassformer: Deterministic or stochastic?

In particle-based computer simulations of polydisperse glassforming systems, the particle diameters σ=σ_{1},⋯,σ_{N} of a system with N particles are chosen with the intention to approximate a desired distribution density f with the corresponding histogram. One method to accomplish this is to draw each diameter randomly and independently from the density f. We refer to this stochastic scheme as model S. Alternatively, one can apply a deterministic method, assigning an appropriate set of N values to the diameters. We refer to this method as model D. We show that, for sample-to-sample fluctuations, especially for the glassy dynamics at low temperatures, it matters whether one chooses model S or model D. Using molecular dynamics computer simulations, we investigate a three-dimensional polydisperse nonadditive soft-sphere system with f(s)∼s^{-3}. The swap Monte Carlo method is employed to obtain equilibrated samples at very low temperatures. We show that for model S the sample-to-sample fluctuations due to the quenched disorder imposed by the diameters σ can be explained by an effective packing fraction. Dynamic susceptibilities in model S can be split into two terms: one that is of thermal nature and can be identified with the susceptibility of model D, and another one originating from the disorder in σ. At low temperatures the latter contribution is the dominating term in the dynamic susceptibility. Our study clarifies the pros and cons of the use of models S and D in practice.

Shear-induced diffusion and dynamic heterogeneities in dense granular flows

We study two-dimensional dense granular flows by molecular dynamics simulations. We quantify shear-induced diffusion of granular particles by the transverse component of particle displacements. In long time scales, the transverse displacements are described as normal diffusion and obey Gaussian distributions, where time correlations of particle velocities entirely vanish. In short time scales, the transverse displacements are strongly non-Gaussian if the system is dense and sheared quasistatically though memory effects on the particle velocities are further suppressed. We also analyze spatio-temporal structures of the transverse displacements by self-intermediate scattering functions and dynamic susceptibilities. We find that the relation between the maximum intensity and characteristic time scale for dynamic heterogeneities is dependent on the models of contact damping (which exhibit different rheological properties such as the Newtonian fluids’ behavior and shear thickening). In addition, the diffusion coefficient over the shear rate is linear (sub-linear) in the maximum of dynamic susceptibility if the damping force is not restricted (restricted) to the normal direction between the particles in contact.

Low-Frequency Dynamic Magnetic Susceptibility of Antiferromagnetic Nanoparticles with Superparamagnetic Properties

As is known, the multi-sublattice structure of antiferromagnets (AFMs) entails that, under size diminution to the nanoscale, compensation of the sublattice magnetizations becomes incomplete. Due to that, the nanoparticles acquire small, but finite permanent magnetic moments. An AC field applied to such particles induces their magnetic response, the measurement of which is well within the sensitivity range of the experimental technique. Given the small size of the particles, their magnetodynamics is strongly affected by thermal fluctuations, so that their response bears a considerable superparamagnetic contribution. This specific feature is well-known, but usually is accounted for at the estimation accuracy level. Herein, a kinetic model is proposed to account for the magnetic relaxation of AFM nanoparticles, i.e., the processes that take place in the frequency domain well below the magnetic resonance band. Assuming that the particles possess uniaxial magnetic anisotropy, the expressions for the principal components of the both linear static and dynamic susceptibilities are derived, yielding simple analytical expressions, including those for the case of a random distribution of the particle axes.

Dynamical charge susceptibility in nonequilibrium double quantum dots

Double quantum dots are one of the promising two-state quantum systems for realizing qubits. In the quest of successfully manipulating and reading information in qubit systems, it is of prime interest to control the charge response of the system to a gate voltage, as filled in by the dynamical charge susceptibility. We theoretically study this quantity for a nonequilibrium double quantum dot by using the functional integral approach and derive its general analytical expression. One highlights the existence of two lines of maxima as a function of the dot level energies, each of them being split under the action of a bias voltage. In the low frequency limit, we derive the capacitance and the charge relaxation resistance of the equivalent quantum RC-circuit with a notable difference in the range of variation for $R$ depending on whether the system is connected in series or in parallel. By incorporating an additional triplet state in order to describe the situation of a double quantum dot with spin, we obtain results for the resonator phase response which are in qualitative agreement with recent experimental observations in spin qubit systems. These results show the wealth of information brought by the knowledge of dynamical charge susceptibility in double quantum dots with potential applications for spin qubits.

Dynamical magnetic response in superconductors with finite-momentum pairs

We derive the dynamical magnetic response functions in the Fulde-Ferrell (FF) state of a superconductor with inversion symmetry. The pair momentum 2q is obtained by minimization of the condensation energy and the resulting quasiparticle states and spectral functions exhibit the segmentation into paired and unpaired regions due to the finite q. The dynamical magnetic susceptibility is then calculated in linear response formalism in the FF state with finite-q condensate resulting from s-wave or d-wave pairing. We show that quasiparticle excitations inside as well as between paired and unpaired segments contribute to the dynamical response. We discuss its dependence on frequency and momentum transfer which develops a characteristic symmetry-breaking parallel to q. Furthermore, we investigate the possible influence on Knight shift and in the case of d-wave pairing on the spin resonance formation in the FF state.

Nonlinear contributions to the dynamic magnetic susceptibility of magnetic fluids

• Higher order harmonic susceptibilities of magnetic fluids are obtained theoretically. • Mean spherical approximation is used with field strength expansion of magnetization. • Theoretical prediction is compared to the Langevin and Debye-Weiss limiting cases. • Field amplitude and frequency range of validity of the expanded MSA model is mapped. Based on our earlier analytical results for the magnetization of magnetic fluids with respect to the magnetic field strength, we propose an expansion method within the framework of mean spherical approximation (MSA) to obtain the coefficients of different nonlinear terms. Through a Fourier expansion of the frequency-dependent magnetic susceptibility the harmonic coefficients corresponding to the linear and nonlinear dynamic susceptibilities are calculated from the field expansion of magnetization. The frequency dependence of the higher order susceptibilities is determined on the basis of the Debye relaxation of magnetic dipoles. Our MSA based results are in line with the corresponding limiting case of the Debye-Weiss theory. We mapped the range of applicability of the expansion method concerning the field strength and frequencies. Our results show that under weak fields a 7th order expansion is sufficient to predict the magnitudes of the susceptibility components up to the 4th harmonic relevant for magnetic fluids.

Collective mode excitations and simulated L -edge resonant inelastic x-ray scattering spectra in antiferromagnetic Ca2RuO4

Using the three-orbital Hubbard model, we investigate the low-energy excitation spectra in the antiferromagnetic phase of Ca$_2$RuO$_4$. We calculate the dynamical susceptibilities in the low-energy region by the random phase approximation and find that the anisotropic dispersion of the transverse mode is in good agreement with the spectra recently reported by inelastic neutron scattering experiments. Using the fast collision approximation, we simulate the resonant inelastic x-ray scattering (RIXS) spectra of the Ru $L_3$-edge from the dynamical susceptibilities. We show that the dispersion of the transverse mode is clearly observed in the calculated RIXS spectra and that the polarization dependence of the incident x-rays enables one to distinguish between the excitations of the in-plane transverse mode and out-of-plane transverse mode.

One- and two-particle properties of the weakly interacting two-dimensional Hubbard model in proximity to the van Hove singularity

We study the weak-coupling limit of the $t-t^\prime-U$ Hubbard model on a two-dimensional square lattice using a direct perturbative approach. Aided by symbolic computational tools, we compute the longitudinal density-density correlation functions in the $\chi_{\uparrow \uparrow}$ and $\chi_{\uparrow \downarrow}$ basis from which we can obtain the dynamical spin and charge susceptibilities at arbitrary doping and temperature. We find that for non-zero $t^\prime$, the zero frequency commensurate $\mathbf{q} = (\pi, \pi)$ spin and charge excitations are each strongest at different densities and we observe a clear behavioral change that appears tied to the van Hove singularity of the non-interacting dispersion upon which the perturbative expansion is built. We find a strongly reduced compressibility in the vicinity of the van Hove singularity as well as a behavioral change in the double occupancy. For finite $t^\prime$, the observed van Hove singularity occurs away from half-filling leading us to conclude that that this reduction in compressibility is distinct from Mott insulating physics that one expects in the strong-coupling regime. We compute the full dynamical spin and charge excitations and observe distinct structure for electron and hole doped scenarios in agreement with experiments on cuprate materials. Finally, we observe a peculiar splitting in spin and charge excitations in the vicinity of the van Hove singularity, the origin of which is traced to a splitting near the bottom of the band.

Hot-lines topology and the fate of the spin resonance mode in three-dimensional unconventional superconductors

In the quasi-two-dimensional (quasi-2D) copper- and iron-based superconductors, the onset of superconductivity is accompanied by a prominent peak in the magnetic spectrum at momenta close to the wave-vector of the nearby antiferromagnetic state. Such a peak is well described in terms of a spin resonance mode, i.e., a spin-1 exciton theoretically predicted for quasi-2D superconductors with a sign-changing gap. The same theories, however, indicate that such a resonance mode should be absent in a three-dimensional (3D) system with a spherical Fermi surface. This raises the question of the fate of the spin resonance mode in layered unconventional superconductors that are not strongly anisotropic, such as certain heavy-fermion compounds and potentially the newly discovered nickelate superconductor NdNiO$_2$. Here, we use the random-phase-approximation to calculate the dynamical spin susceptibility of 3D superconductors with a $d_{x^2-y^2}$-wave gap symmetry and corrugated cylindrical-like Fermi surfaces. By varying the out-of-plane hopping anisotropy $t_z/t$, we demonstrate that the appearance of a spin resonance mode is determined by the topology of the hot lines -- i.e. lines on the Fermi surface that are connected by the magnetic wave-vector. For an in-plane antiferromagnetic wave-vector, the hot lines undergo a topological transition from open lines to closed loops at a critical $t_z/t$ value. The closed hot lines cross the nodal superconducting lines, making the spin resonance mode overdamped and incoherent. In contrast, for an out-of-plane antiferromagnetic wave-vector, the hot lines remain open and the spin resonance mode remains sharp. We discuss the experimental implications of our results for the out-of-plane dispersion of the spin resonance mode and, more generally, for inelastic neutron scattering experiments on unconventional superconductors.

Low-energy excitonic condensate excitations in semimetal and semiconducting materials

The low-energy excitation properties of the excitonic condensate in the semimetal and semiconducting materials are inspected in the extended Falicov-Kimball model. In the framework of the unrestricted Hartree-Fock approximation, we have released a set of self-consistent equations so the excitonic condensate order parameter and then the optical conductivity and the dynamical excitonic susceptibility function are evaluated. We find that the optical conductivity becomes significant and shows a sharp peak at a frequency that is twice as of the excitonic condensate order parameter once the system settles in the excitonic condensate. In the meanwhile, out of the excitonic condensation state, the dynamical excitonic susceptibility function in the semimetal state releases a dominant peak at low frequency if Coulomb interaction is sufficiently large. This character indicates the possibility of the resonance bound excitonic condensate even in high-temperature normal semimetals. The resonance is dramatically reinforced inside of the semiconducting state and that specifies the stability of the bound excitonic coherent state of the preformed excitons in the semiconducting materials.