Ultrafast dynamics in the presence of antiferromagnetic correlations in electron-doped cuprate La2−x_{2-x}Cex_xCuO4±δ_{4\pm\delta}

We used femtosecond optical pump-probe spectroscopy to study the photoinduced change in reflectivity of thin films of the electron-doped cuprate La$_{2-x}$Ce$_x$CuO$_4$ (LCCO) with dopings of x$=$0.08 (underdoped) and x$=$0.11 (optimally doped). Above T$_c$, we observe fluence-dependent relaxation rates which onset at a similar temperature that transport measurements first see signatures of antiferromagnetic correlations. Upon suppressing superconductivity with a magnetic field, it is found that the fluence and temperature dependence of relaxation rates is consistent with bimolecular recombination of electrons and holes across a gap (2$\Delta_{AF}$) originating from antiferromagnetic correlations which comprise the pseudogap in electron-doped cuprates. This can be used to learn about coupling between electrons and high-energy ($\omega>2\Delta_{AF}$) excitations in these compounds and set limits on the timescales on which antiferromagnetic correlations are static

High Harmonic Generation in SF6_{6}: Raman-excited Vibrational Quantum Beats

In a recent experiment (N. Wagner et al., PNAS v103, p13279) on SF$_{6}$, a high-harmonic generating laser pulse is preceded by a pump pulse which stimulates Raman-active modes in the molecule. Varying the time delay between the two pulses modulates high harmonic intensity, with frequencies equal to the vibration frequencies of the Raman-active modes. We propose an explanation of this modulation as a quantum interference between competing pathways that occur via adjacent vibrational states of the molecule. The Raman and high harmonic processes act as beamsplitters, producing vibrational quantum beats among the Raman-active vibrational modes that are excited by the first pulse. We introduce a rigorous treatment of the electron-ion recombination process and the effect of the ionic Coulomb field in the electron propagation outside the molecule, improving over the widely-used three-step model.Comment: submitted to PR