Ultrafast entropy production in pump-probe experiments

The ultrafast control of materials has opened the possibility to investigate non-equilibrium states of matter with striking properties, such as transient superconductivity and ferroelectricity, ultrafast magnetization and demagnetization, as well as Floquet engineering. The characterization of the ultrafast thermodynamic properties within the material is key for their control and design. Here, we develop the ultrafast stochastic thermodynamics for laser-excited phonons. We calculate the entropy production and heat absorbed from experimental data for single phonon modes of driven materials from time-resolved X-ray scattering experiments where the crystal is excited by a laser pulse. The spectral entropy production is calculated for SrTiO₃ and KTaO₃ for different temperatures and reveals a striking relation with the power spectrum of the displacement-displacement correlation function by inducing a broad peak beside the eigenmode-resonance.