We propose to induce a time crystalline state in a high-$T_c$ superconductor, by optically driving a sum resonance of the Higgs mode and a Josephson plasma mode. The generic cubic process that couples these fundamental excitations converts driving of the sum resonance into simultaneous resonant driving of both modes, resulting in an incommensurate subharmonic motion. We use a numerical implementation of a semi-classical driven-dissipative lattice gauge theory on a three-dimensional layered lattice, which models the geometry of cuprate superconductors, to demonstrate the robustness of this motion against thermal fluctuations. We demonstrate this light-induced time crystalline phase for mono- and bilayer systems and show that this order can be detected for pulsed driving under realistic technological conditions.
Higgs spectroscopy is a new field in which Higgs modes in nonequilibrium superconductors are analyzed to gain information about the ground state. One experimental setup in which the Higgs mode in s-wave superconductors was observed is periodic driving with THz light, which shows resonances in the third-harmonic generation (THG) signal if twice the driving frequency matches the energy of the Higgs mode. We derive expressions of the driven gap oscillations for arbitrary gap symmetry and calculate the THG response. We demonstrate that the possible Higgs modes for superconductors with non-trivial …
In superconductors the Anderson-Higgs mechanism allows for the existence of a collective amplitude (Higgs) mode which can couple to eV-light mainly in a non-linear Raman-like process. The experimental non-equilibrium results on isotropic superconductors have been explained going beyond the BCS theory including the Higgs mode. Furthermore, in anisotropic d-wave superconductors strong interaction effects with other modes are expected. Here we calculate the Raman contribution of the Higgs mode from a new perspective, including many-body Higgs oscillations effects and their consequences in convent…
Anderson-Higgs mechanism of mass generation is a generic concept in high-energy and condensed matter physics. It shows up through the Meissner effect providing the expulsion of static and low-frequency magnetic fields from superconductors. However, it does not affect propagating electromagnetic waves with a spectrum gap determined by the plasma frequency, which is too large to be sensitive to the superconducting transition. Here we demonstrate the spectroscopic manifestation of the Anderson-Higgs mass, showing that it determines the spectrum gap of magnons in superconductor/ferromagnet/superco…
The concept of mass-generation via the Higgs mechanism was strongly inspired by earlier works on the Meissner-Ochsenfeld effect in superconductors. In quantum field theory, the excitations of longitudinal components of the Higgs field manifest as massive Higgs bosons. The analogous Higgs mode in superconductors has not yet been observed due to its rapid decay into particle-hole pairs. Following recent theories, however, the Higgs mode should decrease below the pairing gap $2Δ$ and become visible in two-dimensional systems close to the superconductor-insulator transition (SIT). For experimental…
We investigate theoretically the excitation of Higgs oscillations of the order parameter in superconductors by incoherent short pulses of light with frequency much larger than the superconducting gap. The excitation amplitude of the Higgs mode is controlled by a single parameter which is determined by the total number of quasiparticles excited by the pulse. This fact can be traced back to the universality of the shape of the light-induced quasiparticle cascade at energy below the Debye frequency and above the gap.
Higgs mode in superconducting materials describes slowly-decaying oscillations of the order parameter amplitude. We demonstrate that in magnetic superconductors with built-in spin-splitting field Higgs mode is strongly coupled to the spin degrees of freedom allowing for the generation of time-dependent spin currents. Converting such spin currents to electric signals by spin-filtering elements provides a tool for the second-harmonic generation and the electrical detection of the Higgs mode generated by the external irradiation. The non-adiabatic spin torques generated by these spin currents all…
We reveal that due to the presence of disorder oscillations of the order parameter amplitude called the Higgs mode can be effectively excited by the external electromagnetic radiation in usual BCS superconductors. This mechanism works for superconductors with both isotropic s-wave and anisotropic, such as d-wave, pairings. The non-linear response in the presence of impurities is captured by the quasiclassical formalism. We demonstrate that analytical solutions of the Eilenberger equation with impurity collision integral and external field drive coincide with the exact summation of ladder impur…
The concept of "broken symmetry", that the symmetry of the vacuum may be lower than the Hamiltonian of a quantum theory, plays an important role in modern physics. A manifestation of this phenomena is the Higgs boson in particle physics whose long awaited discovery is imminent. An equivalent mode in superconductors is implicit in the early theories of their collective fluctuations. Spurred by some mysterious experimental results, the theory of the oscillation of the amplitude of superconductivity order parameter, which is the equivalent to the Higgs modes in s-wave superconductors and its iden…
Collective excitation modes are a characteristic feature of symmetry-broken phases of matter. For example, superconductors exhibit an amplitude Higgs mode and a phase mode, which are the radial and angular excitations in the Mexican-hat potential of the free energy. In two-band superconductors there exists in addition a Leggett phase mode, which corresponds to collective fluctuations of the interband phase difference. In equilibrium systems amplitude and phase modes are decoupled, since they are mutually orthogonal excitations. The direct detection of Higgs and Leggett modes by linear-response…
We put forth a mechanism for enhancing the interlayer transport in cuprate superconductors, by optically driving plasmonic excitations along the $c$ axis with a frequency that is blue-detuned from the Higgs frequency. The plasmonic excitations induce a collective oscillation of the Higgs field which induces a parametric enhancement of the superconducting response, as we demonstrate with a minimal analytical model. Furthermore, we perform simulations of a particle-hole symmetric $U(1)$ lattice gauge theory and find good agreement with our analytical prediction. We map out the renormalization of…
Through the Higgs mechanism, the long-range Coulomb interaction eliminates the low-energy Goldstone phase mode in superconductors and transfers spectral weight all the way up to the plasma frequency. Here we show that the Higgs mechanism breaks down for length scales shorter than the superconducting coherence length while it stays intact, even at high energies, in the long-wavelength limit. This effect is a consequence of the composite nature of the Higgs field of superconductivity and the broken Lorentz invariance in a solid. Most importantly, the breakdown of the Higgs mechanism inside the s…
Quantum fluctuations and the emergence of in-gap Higgs mode in superconductors
Max Planck Institute for Solid State Research（马克斯·普朗克固体研究所）；The University of Tokyo（东京大学）；RIKEN Center for Emergent Matter Science (CEMS)（理化学研究所凝聚体物质科学中心）；Trans-Scale Quantum Science Institute, The University of Tokyo（东京大学跨尺度量子科学研究院）
In a recent manuscript Phys. Rev. Lett. 127, 197001 (2021) Puviani et al. claim that the Higgs mode gives an enhancement of the Raman response in the symmetric $A_{1g}$ Raman channel of cuprates. Here we report a series of technical mistakes in their derivation that completely invalidate this conclusion. In particular, the Raman response function contains two renormalized vertices, with a clearly overcounting of diagrams and uncontrolled results for the Higgs-mode contribution.
Type II Lifshitz invariant and optically active Higgs mode in time-reversal symmetry broken superconductors
Institute for Theory of Condensed Matter, Karlsruhe Institute of Technology（卡尔斯鲁厄理工学院凝聚态理论研究所）；Department of Physics, University of Tokyo（东京大学物理学系）；RIKEN Center for Emergent Matter Science (CEMS)（理化学研究所新兴物质科学中心）；Trans-Scale Quantum Science Institute, University of Tokyo（东京大学跨尺度量子科学研究所）
The recent observation of a transmitted Thz pulse oscillating at three times the frequency of the incident light paves the way to a new protocol to access resonant excitations in a superconductor. Here we show that this non-linear optical process is dominated by light-induced excitation of Cooper pairs, in analogy with a standard Raman experiment. The collective amplitude (Higgs) fluctuations of the superconducting order parameter give in general a smaller contribution, unless one designs the experiment by combining properly the light polarization with the lattice symmetry.
Recent studies have emphasized the importance of impurity scattering for the optical Higgs response of superconductors. In the dirty limit, an additional paramagnetic coupling of light to the superconducting condensate arises which drastically enhances excitation. So far, most work concentrated on the periodic driving with light, where the third-harmonic generation response of the Higgs mode was shown to be enhanced. In this work, we additionally calculate the time-resolved optical conductivity of single- and two-band superconductors in a two-pulse quench-probe setup, where we find good agreem…
We report experimental evidences for the observation of the superconducting amplitude mode, so-called `Higgs' mode in the charge density wave superconductor 2H-NbSe2 using Raman scattering. By comparing 2H-NbSe2 and its iso-structural partner 2H-NbS2 which shows superconductivity but lacks the charge density wave order, we demonstrate that the superconducting mode in 2H-NbSe2 owes its spectral weight to the presence of the coexisting charge density wave order. In addition, temperature dependent measurements in 2H-NbSe2 show a full spectral weight transfer from the charge density wave mode to t…
Despite the formal analogy with the Higgs particle, the amplitude fluctuations of the order parameter in weakly-coupled superconductors do not identify a real mode with a Lorentz-invariant dynamics. Indeed, its resonance occurs at $2Δ_0$, which coincides with the threshold $2E_{gap}$ for quasiparticle excitations, that spoil any relativistic dynamics. Here we investigate the fate of the Higgs mode in the unconventional case where $2E_{gap}$ becomes larger than $2Δ_0$, as due to strong coupling or strong disorder. We show that also in this situation the amplitude fluctuations never identify a r…
Ultrafast responses of BCS superconductor Nb1-xTixN films in a nonadiabatic excitation regime were investigated by using terahertz (THz) pump-THz probe spectroscopy. After an instantaneous excitation with the monocycle THz pump pulse, a transient oscillation emerges in the electromagnetic response in the BCS gap energy region. The oscillation frequency coincides with the asymptotic value of the BCS gap energy, indicating the appearance of the theoretically-anticipated collective amplitude mode of the order parameter, namely the Higgs amplitude mode. Our result opens a new pathway to the ultraf…
Using the non-equilibrium Keldysh formalism, we solve the equations of motion for electron-phonon superconductivity, including an ultrafast pump field. We present results for time-dependent photoemission spectra out of equilibrium which probes the dynamics of the superconducting gap edge. The partial melting of the order by the pump field leads to oscillations at twice the melted gap frequency, a hallmark of the Higgs or amplitude mode. Thus the Higgs mode can be directly excited through the nonlinear effects of an electromagnetic field and detected without any additional symmetry breaking.
Higgs oscillations in nonequilibrium superconductors provide an unique tool to obtain information about the underlying order parameter. Several properties like the absolute value, existence of multiple gaps and the symmetry of the order parameter can be encoded in the Higgs oscillation spectrum. Studying Higgs oscillations with time-resolved angle-resolved photoemission spectroscopy (ARPES) has the advantage over optical measurements that a momentum-resolved analysis of the condensate dynamic is possible. In this paper, we investigate the time-resolved spectral function measured in ARPES for d…
Third-harmonic generation (THG) experiments on superconductors can be used to investigate collective excitations like the amplitude mode of the order parameter known as Higgs mode. These modes are visible due to resonances in the THG signal if the driving frequency matches the energy of the mode. In real materials multiple modes can exist giving rise to additional THG contributions, such that it is difficult to unambiguously interpret the results. In this paper, we additionally analyze the phase of the THG signal, which contains microscopic details beyond classical resonances as well as signat…
We develop a microscopic and gauge-invariant theory for collective modes resulting from the phase of the superconducting order parameter in non-centrosymmetric superconductors. Considering various crystal symmetries we derive the corresponding gauge mode $ω_{\rm G}({\bf q})$ and find, in particular, new Leggett modes $ω_{\rm L}({\bf q})$ with characteristic properties that are unique to non-centrosymmetric superconductors. We calculate their mass and dispersion that reflect the underlying spin-orbit coupling and thus the balance between triplet and singlet superconductivity occurring simultane…
We consider the amplitude (Higgs) mode in a superconductor with a condensate flow (supercurrent). We demonstrate that, in this case, the amplitude mode corresponding to oscillations $δ|Δ|_Ω \exp(i Ωt)$ of the superconducting gap is excited by an external ac electric field $\mathbf{E}_Ω \exp(i Ωt)$ already in the first order in $|\mathbf{E}_Ω|$, so that ${δ|Δ|_Ω \propto (\mathbf{v}_{0} \mathbf{E}_Ω)}$, where $\mathbf{v}_{0}$ is the velocity of the condensate. The frequency dependence $δ|Δ|_Ω$ has a resonance shape with a maximum at ${Ω= 2 Δ}$. In contrast to the standard situation without the c…
Nematic superconductivity with spontaneously broken rotation symmetry has recently been reported in doped topological insulators, $M_x$Bi$_2$Se$_3$ ($M$=Cu, Sr, Nb). Here we show that the electromagnetic (EM) response of these compounds provides a spectroscopy for bosonic excitations that reflect the pairing channel and the broken symmetries of the ground state. Using quasiclassical Keldysh theory, we find two characteristic bosonic modes in nematic superconductors: the nematicity mode and the chiral Higgs mode. The former corresponds to the vibrations of the nematic order parameter associated…
A recent Little-Parks experiment on Kagome-structured superconductor CsV_3Sb_5 demonstrated remarkable resistance oscillations with period \phi0/3=hc/6e. Here, we perform analysis based on a theory involving three 2e superconductivity (SC) order parameters associated with the three reciprocal lattice vectors which connect M points of the hexagonal Brillouin zone. In a ring geometry we unveil that, as a series of metastable states, phase of one SC order parameter winds 2πmore or less than the other two ones around the ring, which yields local free energy minima at integer multiples of \phi0/3. …
Recent advances in time-domain terahertz (THz) spectroscopy have unveiled that resonantly-enhanced strong THz third-harmonic generation (THG) mediated by the collective Higgs amplitude mode occurs in s-wave superconductors, where charge-density fluctuations (CDF) have also been shown to contribute to the nonlinear third-order susceptibility. It has been theoretically proposed that the nonlinear responses of Higgs and CDF exhibit essentially different polarization dependences. Here we experimentally discriminate the two contributions by polarization-resolved intense THz transmission spectroscop…
When a continuous symmetry of a physical system is spontaneously broken, two types of collective modes typically emerge: the amplitude and phase modes of the order-parameter fluctuation. For superconductors, the amplitude mode is recently referred to as the ''Higgs mode'' as it is a condensed-matter analogue of a Higgs boson in particle physics. Higgs mode is a scalar excitation of the order parameter, distinct from charge or spin fluctuations, and thus does not couple to electromagnetic fields linearly. This is why the Higgs mode in superconductors has evaded experimental observations over a …
We examine fundamental properties of Green's functions of Nambu-Goldstone and Higgs modes in superconductors with multiple order parameters. Nambu-Goldstone and Higgs modes are determined once the symmetry of the system and that of the order parameters are specified. Multiple Nambu-Goldstone modes and Higgs modes exist when we have multiple order parameters. The Nambu-Goldstone Green function $D(ω,{\bf q})$ has the form $1/(gN(0))^2\cdot (2Δ)^2/(ω^2-c_s^2{\bf q}^2)$ with the coupling constant $g$ and $c_s=v_F/\sqrt{3}$ for small $ω$ and ${\bf q}$, with a pole at $ω=0$ and ${\bf q}=0$ indicatin…
We describe the crystal growth of high quality single crystals of the non-centrosymmetric superconductor, Ru7B3 by the floating zone technique, using an optical furnace equipped with xenon arc lamps. The crystals obtained are large and suitable for detailed measurements, and have been examined using x-ray Laue patterns. The superconducting properties of the crystals obtained have been investigated by magnetisation and resistivity measurements. Crystals have also been grown starting with enriched 11B isotope, making them suitable for neutron scattering experiments.
We theoretically investigate coherent optical excitations of collective modes in two-band BCS superconductors, which accommodate two Higgs modes and one Leggett mode corresponding, respectively, to the amplitude and relative-phase oscillations of the superconducting order parameters associated with the two bands. We find, based on a mean-field analysis, that each collective mode can be resonantly excited through a nonlinear light-matter coupling when the doubled frequency of the driving field coincides with the frequency of the corresponding mode. Among the two Higgs modes, the higher-energy o…
Higgs mode in superconductors, i.e. the collective amplitude mode of the order parameter does not associate with charge nor spin fluctuations, therefore it does not couple to the electromagnetic field in the linear response regime. On the contrary to this common understanding, here, we demonstrate that, if the dc supercurrent is introduced into the superconductor, the Higgs mode becomes infrared active and is directly observed in the linear optical conductivity measurement. We observed a sharp resonant peak at $ω=2Δ$ in the optical conductivity spectrum of a thin-film NbN in the presence of dc…
By applying a microscopic gauge-invariant kinetic theory in $d$-wave superconductors, we analytically derive the energy spectra of the breathing Higgs mode and, in particular, rotating Higgs mode that is unique for the $d$-wave order parameter. Analytical investigation on their dynamic properties is also revealed. We show that the breathing Higgs mode is optically visible in the second-order regime. Whereas the rotating Higgs mode is optically inactive, we show that this mode can be detected in the pseudogap phase by magnetic resonance experiment. It is interesting to find that with a longitud…
We present a unified framework to construct and classify topological crystalline superconductors (TCSCs). The building blocks are one-dimensional topological superconductors (TSCs) protected solely by onsite symmetries, which are arranged and glued by crystalline symmetries in real space. We call this real-space scheme "wire construction", and we show its procedure can be formulated mathematically. For illustration, we treat TCSCs of Altland-Zirnbauer (AZ) class[1] DIII protected by wallpaper group as well as layer group symmetries, with the resulting states by wire construction being TCSCs in…
We show that low-lying excitations of a 2D BCS superconductor are significantly altered when coupled to an externally driven cavity, which induces controllable long-range attractive interactions between the electrons. We find that they combine non-linearly with intrinsic local interactions to increase the Bogoliubov quasiparticle excitation energies, thus enlarging the superconducting gap. The long-range nature of the driven-cavity-induced attraction qualitatively changes the collective excitations of the superconductor. Specifically, they lead to the appearance of additional collective excita…
The $N$-component London $\mathrm{U}(1)$ superconductor is expressed in terms of integer-valued supercurrents. We show that the inclusion of inter-band Josephson couplings introduces monopoles in the current fields, which convert the phase transitions of the charge-neutral sector to crossovers. The monopoles only couple to the neutral sector, and leave the phase transition of the charged sector intact. The remnant non-critical fluctuations in the neutral sector influence the one remaining phase transition in the charged sector, and may alter this phase transition from a $3DXY$ inverted phase t…
Superconductors have the potential to revolutionize technology due to their ability to have zero electrical resistance. However, superconductor materials require either low temperatures or high pressures to function in a superconductive state. Thus, researchers are now on the search for the first-ever room temperature, ambient pressure superconductor. Yet, recent discoveries have only shown superconductors that work at low temperatures with ambient pressure or room temperature with high pressures. The region between these two extremes has not been identified due to the number of variables that…
In multiband superconductors, multiple collective modes exist associated with the multiple order parameters. Oscillations of the amplitude and the relative phase of the order parameters are called Higgs and Leggett modes, respectively. Recently, it has been suggested that nonmagnetic impurity scattering would enhance nonlinear coupling between the Higgs mode and an electromagnetic wave with a frequency located in the superconducting gap region, while its effect on the Leggett mode is still unresolved. Here, we theoretically investigated the nonlinear optical response of multiband Bardeen-Coope…
The Higgs mode in superconductors is a scalar mode without electric or magnetic dipole moment. Thus, it is commonly believed that its excitation is restricted to a nonlinear two-photon Raman process. However, recent efforts have shown that a linear excitation in the presence of a supercurrent is possible, resulting in a new resonant enhancement at $Ω=2Δ$ with the driving light frequency $Ω$ and the energy of the Higgs mode $2Δ$. This is in contrast to the usual $2Ω= 2Δ$ resonance condition found in nonlinear third-harmonic generation experiments. In this communication, we show that such a line…
A superconductor subject to electromagnetic irradiation in the terahertz range can show amplitude oscillations of its order parameter. However, coupling this so-called Higgs mode to the charge current is notoriously difficult. We propose to achieve such a coupling in a particle-hole-asymmetric configuration using a DC-voltage-biased normal-metal--superconductor tunnel junction. Using the quasiclassical Green's function formalism, we demonstrate three characteristic signatures of the Higgs mode: (i) The AC charge current exhibits a pronounced resonant behavior and is maximal when the radiation …
In iron-based superconductors, band inversion of $d$- and $p$-orbitals yields Dirac semimetallic states. We theoretically investigate their topological properties in normal and superconducting phases, based on the tight-binding model involving full symmetry of the materials. We demonstrate that a Cooper pair between electrons with $d$- and $p$-orbitals relevant to the band structure yields odd-parity superconductivity. Moreover, we present the typical surface states by solving the Bogoliubov-de Gennes equation and characterize them by topological invariants defined with crystal symmetry. It is…
We investigate an index theorem for a Bogoliubov-de Gennes Hamiltonian (BdGH) describing a topological superconductor with Yang-Mills-Higgs couplings in arbitrary dimensions. We find that the index of the BdGH is determined solely by the asymptotic behavior of the Higgs fields and is independent of the gauge fields. It can be nonvanishing if the dimensionality of the order parameter space is equal to the spatial dimensions. In the presence of point defects there appear localized zero energy states at the defects. Consistency of the index with the existence of zero energy bound states is examin…
We study the nonlinear optical response in a superconducting NbN thin film with strong terahertz (THz)wave. Besides the expected third harmonic generation, we observe a new transient oscillation which softensin frequency with temperature increasing towards superconducting transition temperatureTc. We identify thisnew mode as the Higgs transient oscillation. To verify this proposal, we introduce a time-frequency resolvedtechnique, named spectrogram for visualizing THz spectrum. The dynamic decaying behavior of the mode isobserved, which is consistent with theoretical expectation about intrinsic…
