By exciting high-temperature K3C60 with mid-infrared pulses, a large increase in carrier mobility is obtained, accompanied by the opening of a gap in the optical conductivity; these same signatures are observed at equilibrium when cooling K3C60 below the superconducting transition temperature of 20 kelvin, which could be an indication of light-induced high-temperature superconductivity. The use of light to control the properties of condensed-matter materials is a promising area of research, with the long-term prospect that it might lead to the development of quantum devices driven by light. In particular, it was shown recently that nonlinear excitation of certain phonons in bilayer copper oxides induces superconducting-like optical properties at temperatures far above the material's superconducting transition temperature (Tc). This effect was accompanied by the disruption of competing charge-density-wave correlations, explaining some, but not all, of the experimental results. Andrea Cavalleri and colleagues now report that by exciting metallic K3C60 with mid-infrared optical pulses, they can induce a large increase in carrier mobility, accompanied by the opening of a gap in the optical conductivity. Strikingly, these same signatures are observed at equilibrium when K3C60 cools below its Tc of 20 K. The non-equilibrium control of emergent phenomena in solids is an important research frontier, encompassing effects such as the optical enhancement of superconductivity1. Nonlinear excitation2,3 of certain phonons in bilayer copper oxides was recently shown to induce superconducting-like optical properties at temperatures far greater than the superconducting transition temperature, Tc (refs 4, 5, 6). This effect was accompanied by the disruption of competing charge-density-wave correlations7,8, which explained some but not all of the experimental results. Here we report a similar phenomenon in a very different compound, K3C60. By exciting metallic K3C60 with mid-infrared optical pulses, we induce a large increase in carrier mobility, accompanied by the opening of a gap in the optical conductivity. These same signatures are observed at equilibrium when cooling metallic K3C60 below Tc (20 kelvin). Although optical techniques alone cannot unequivocally identify non-equilibrium high-temperature superconductivity, we propose this as a possible explanation of our results.
Excitation of high-Tc cuprates and certain organic superconductors with intense far-infrared optical pulses has been shown to create non-equilibrium states with optical properties that are consistent with transient high-temperature superconductivity. These non-equilibrium phases have been generated using femtosecond drives, and have been observed to disappear immediately after excitation, which is evidence of states that lack intrinsic rigidity. Here we make use of a new optical device to drive metallic K3C60 with mid-infrared pulses of tunable duration, ranging between one picosecond and one nanosecond. The same superconducting-like optical properties observed over short time windows for femtosecond excitation are shown here to become metastable under sustained optical driving, with lifetimes in excess of ten nanoseconds. Direct electrical probing, which becomes possible at these timescales, yields a vanishingly small resistance with the same relaxation time as that estimated by terahertz conductivity. We provide a theoretical description of the dynamics after excitation, and justify the observed slow relaxation by considering randomization of the order-parameter phase as the rate-limiting process that determines the decay of the light-induced superconductor.
Photo-excitation at terahertz and mid-infrared frequencies has emerged as an effective way to manipulate functionalities in quantum materials, in some cases creating non-equilibrium phases that have no equilibrium analogue. In K3C60, a metastable zero-resistance phase was observed that has optical properties, nonlinear electrical transport and pressure dependencies compatible with non-equilibrium high-temperature superconductivity. Here we demonstrate a two-orders-of-magnitude increase in photo-susceptibility near 10 THz excitation frequency. At these drive frequencies, a metastable superconducting-like phase is observed up to room temperature. The discovery of a dominant frequency scale sheds light on the microscopic mechanism underlying photo-induced superconductivity. It also indicates a path towards steady-state operation, limited at present by the availability of a suitable high-repetition-rate optical source at these frequencies.
1 September 2019 in Microporous and Mesoporous Materials