Kavli Affiliate: Frank Wise | Summary:Raman scattering underlies a broad range of spectroscopic and light-generation techniques, yet its conventional description, based on the Raman gain spectrum, accurately describes only long-pulse, steady-state dynamics. We employ a time-domain theoretical approach to account for spectrotemporal aspects of continuous frequency-shifting, which are not addressed by prior theories. In particular, […]

Kavli Affiliate: Frank Wise | Summary:Raman scattering underlies a broad range of spectroscopic and light-generation techniques, yet its conventional description, based on the Raman gain spectrum, accurately describes only long-pulse, steady-state dynamics. We present a time-domain theoretical approach that provides a unified and physically-transparent description of Raman interactions across all temporal regimes. It enables direct […]

Kavli Affiliate: Frank Wise | Summary:Raman scattering underlies a broad range of spectroscopic and light-generation techniques, yet its conventional description, based on the Raman gain spectrum, accurately describes only long-pulse, steady-state dynamics. We present and develop a time-domain theoretical approach that provides a unified and physically-transparent description of Raman interactions across all temporal regimes. It […]

Kavli Affiliate: Darrell Schlom | Summary:The prototypical Mott-Hubbard insulator LaVO3 undergoes a structural phase transition accompanied by the onset of spin and orbital ordering below 140 K. By combining ultrafast optical pump-probe spectroscopy and two-dimensional electronic spectroscopy, we investigate the interplay between fluctuations of the local spin and orbital order parameter and the lifetime of […]