Interlayer transport in high-$T_C$ cuprates is mediated by superconducting tunneling across the CuO$_2$ planes. For this reason, the terahertz frequency optical response is dominated by one or more Josephson plasma resonances and becomes highly nonlinear at fields for which the tunneling supercurrents approach their critical value, $I_C$. These large terahertz nonlinearities are in fact a hallmark of superconducting transport. Surprisingly, however, they have been documented in La$_{2-x}$Ba$_x$CuO$_4$ also above $T_C$ for doping values near $x=1/8$, and interpreted as an indication of superfluidity in the stripe phase. Here, Electric Field Induced Second Harmonic (EFISH) is used to study the dynamics of time-dependent interlayer voltages when La$_{2-x}$Ba$_x$CuO$_4$ is driven with large-amplitude terahertz pulses, in search of other characteristic signatures of Josephson tunnelling in the normal state. We show that this method is sensitive to the voltage anomalies associated with 2$pi$ Josephson phase slips, which near $x=1/8$ are observed both below and above $T_C$. These results document a new regime of nonlinear transport that shares features of sliding charge-density-waves and superconducting phase dynamics.
Resonant optical excitation of certain molecular vibrations in $kappa$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Br has been shown to induce transient superconducting-like optical properties at temperatures far above equilibrium $T_c$. Here, we report experiments across the bandwidth-tuned phase diagram of this class of materials, and study the Mott insulator $kappa$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Cl and the metallic compound $kappa$-(BEDT-TTF)$_2$Cu(NCS)$_2$. We find non-equilibrium photoinduced superconductivity only in $kappa$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Br, indicating that the proximity to the Mott insulating phase and possibly the presence of preexisting superconducting fluctuations are pre-requisites for this effect.
Superconductivity in organic conductors is often tuned by the application of chemical or external pressure. With this type of tuning, orbital overlaps and electronic bandwidths are manipulated, whilst the properties of the molecular building blocks remain virtually unperturbed.Here, we show that the excitation of local molecular vibrations in the charge-transfer salt $kappa-(BEDT-TTF)_2Cu[N(CN)_2]Br$ induces a colossal increase in carrier mobility and the opening of a superconducting-like optical gap. Both features track the density of quasi-particles of the equilibrium metal, and can be achieved up to a characteristic coherence temperature $T^* approxeq 50 K$, far higher than the equilibrium transition temperature $T_C = 12.5 K$. Notably, the large optical gap achieved by photo-excitation is not observed in the equilibrium superconductor, pointing to a light induced state that is different from that obtained by cooling. First-principle calculations and model Hamiltonian dynamics predict a transient state with long-range pairing correlations, providing a possible physical scenario for photo-molecular superconductivity.
Optical excitation of stripe-ordered La$_{2-x}$Ba$_x$CuO$_4$ has been shown to transiently enhance superconducting tunneling between the CuO$_2$ planes. This effect was revealed by a blue-shift, or by the appearance of a Josephson Plasma Resonance in the terahertz-frequency optical properties. Here, we show that this photo-induced state can be strengthened by the application of high external magnetic fields oriented along the c-axis. For a 7-Tesla field, we observe up to a ten-fold enhancement in the transient interlayer phase correlation length, accompanied by a two-fold increase in the relaxation time of the photo-induced state. These observations are highly surprising, since static magnetic fields suppress interlayer Josephson tunneling and stabilize stripe order at equilibrium. We interpret our data as an indication that optically-enhanced interlayer coupling in La$_{2-x}$Ba$_x$CuO$_4$ does not originate from a simple optical melting of stripes, as previously hypothesized. Rather, we speculate that the photo-induced state may emerge from activated tunneling between optically-excited stripes in adjacent planes.
Superconductivity often emerges in proximity of other symmetry-breaking ground states, such as antiferromagnetism or charge-density-wave (CDW) order. However, the subtle inter-relation of these phases remains poorly understood, and in some cases even the existence of short-range correlations for superconducting compositions is uncertain. In such circumstances, ultrafast experiments can provide new insights, by tracking the relaxation kinetics following excitation at frequencies related to the broken symmetry state. Here, we investigate the transient terahertz conductivity of BaPb1-xBixO3 - a material for which superconductivity is adjacent to a competing CDW phase - after optical excitation tuned to the CDW absorption band. In insulating BaBiO3 we observed an increase in conductivity and a subsequent relaxation, which are consistent with quasiparticles injection across a rigid semiconducting gap. In the doped compound BaPb0.72Bi0.28O3 (superconducting below Tc=7K), a similar response was also found immediately above Tc. This observation evidences the presence of a robust gap up to T=40 K, which is presumably associated with short-range CDW correlations. A qualitatively different behaviour was observed in the same material fo T>40 K. Here, the photo-conductivity was dominated by an enhancement in carrier mobility at constant density, suggestive of melting of the CDW correlations rather than excitation across an optical gap. The relaxation displayed a temperature dependent, Arrhenius-like kinetics, suggestive of the crossing of a free-energy barrier between two phases. These results support the existence of short-range CDW correlations above Tc in underdoped BaPb1-xBixO3, and provide new information on the dynamical interplay between superconductivity and charge order.
We report on an investigation of the redistribution of interlayer coherence in the trilayer cuprate Bi2Sr2Ca2Cu3O10. The experiment is performed under the same apical-oxygen phonon excitation discussed in the past for the bilayer cuprate YBa2Cu3O6.5. In Bi2Sr2Ca2Cu3O10, we observe a similar spectral weight loss at the transverse plasma mode resonance seen in YBa2Cu3O6.5. However, this feature is not accompanied by light-enhanced interlayer coherence that was seen in YBa2Cu3O6+x, for which the transverse plasma mode is observed at equilibrium even in the normal state. These new observations offer new experimental perspective in the context of the physics of light-enhanced interlayer coupling in various cuprates.
We comment on the model proposed by Orenstein and Dodge in arXiv:1506.06758v1, which describes time-domain terahertz measurements of transiently generated, high-electron-mobility (or superconducting) phases of solids. The authors main conclusion is that time-domain terahertz spectroscopy does not measure a response function that is mathematically identical to the transient optical conductivity. We show that although this is correct, the difference between the measured response function and the microscopic optical conductivity is small for realistic experimental parameters. We also show that for the experiments reported by our group on light-induced superconducting-like phases in cuprates and in organic conductors, the time-domain terahertz yields a very good estimate for the optical conductivity.
The control of non-equilibrium phenomena in complex solids is an important research frontier, encompassing new effects like light induced superconductivity. Here, we show that coherent optical excitation of molecular vibrations in the organic conductor K3C60 can induce a non-equilibrium state with the optical properties of a superconductor. A transient gap in the real part of the optical conductivity and a low-frequency divergence of the imaginary part are measured for base temperatures far above equilibrium Tc=20 K. These findings underscore the role of coherent light fields in inducing emergent order.
We analyze the pump wavelength dependence for the photo-induced enhancement of interlayer coupling in La1.885Ba0.115CuO4, which is promoted by optical melting of the stripe order. In the equilibrium superconducting state (T < Tc = 13 K), in which stripes and superconductivity coexist, time-domain THz spectroscopy reveals a photo-induced blue-shift of the Josephson Plasma Resonance after excitation with optical pulses polarized perpendicular to the CuO2 planes. In the striped, non-superconducting state (Tc < T < T_SO = 40 K) a transient plasma resonance similar to that seen below Tc appears from a featureless equilibrium reflectivity. Most strikingly, both these effects become stronger upon tuning of the pump wavelength from the mid-infrared to the visible, underscoring an unconventional competition between stripe order and superconductivity, which occurs on energy scales far above the ordering temperature.
We address the kinetic competition between charge striped order and superconductivity in La$_{1.675}$Eu$_{0.2}$Sr$_{0.125}$CuO$_{4}$. Ultrafast optical excitation is tuned to a mid-infrared vibrational resonance that destroys charge order and promptly establishes transient coherent interlayer coupling in this material. This effect is evidenced by the appearance of a longitudinal plasma mode reminiscent of a Josephson plasma resonance. We find that coherent interlayer coupling can be generated up to the charge order transition $T_{CO} approx$ 80 K, far above the equilibrium superconducting transition temperature of any lanthanide cuprate. Two key observations are extracted from the relaxation kinetics of the interlayer coupling. Firstly, the plasma mode relaxes through a collapse of its coherence length and not its density. Secondly, two distinct kinetic regimes are observed for this relaxation, above and below spin order transition $T_{SO} =$ 25 K. Especially, the temperature independent relaxation rate observed below $T_{SO}$ is anomalous and suggests coexistence of superconductivity and stripes rather than competition. Both observations support arguments that a low temperature coherent stripe (or pair density wave) phase suppresses c-axis tunnelling by disruptive interference rather than by depleting the condensate.
