Optical excitation in the cuprates has been shown to induce transient superconducting correlations above the thermodynamic transition temperature TC, as evidenced by the terahertz-frequency optical properties in the nonequilibrium state. In YBa2Cu3O6tx, this phenomenon has so far been associated with the nonlinear excitation of certain lattice modes and the creation of new crystal structures. In other compounds, like La2?xBaxCuO4, similar effects were reported also for excitation at near-infrared frequencies, and were interpreted as a signature of the melting of competing orders. However, to date, it has not been possible to systematically tune the pump frequency widely in any one compound, to comprehensively compare the frequency-dependent photosusceptibility for this phenomenon. Here, we make use of a newly developed nonlinear optical device, which generates widely tunable high-intensity femtosecond pulses, to excite YBa2Cu3O6.5 throughout the entire optical spectrum (3–750 THz). In the far-infrared region (3–24 THz), signatures of nonequilibrium superconductivity are induced only for excitation of the 16.4- and 19.2-THz vibrational modes that drive c-axis apical oxygen atomic positions. For higher driving frequencies (25–750 THz), a second resonance is observed around the charge transfer band edge at approximately 350 THz. These findings highlight the importance of coupling to the electronic structure of the CuO2 planes, mediated either by a phonon or by charge transfer.
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