Enhancing high-order harmonic generation in light molecules by using chirped pulses

One of the current challenges in high-harmonic generation is to extend the harmonic cutoff to increasingly high energies while maintaining or even increasing the efficiency of the high-harmonic emission. Here we show that the combined effect of down-chirped pulses and nuclear dynamics in light molecules allows one to achieve this goal, provided that long enough IR pulses are used to allow the nuclei to move well outside the Franck-Condon region. We also show that, by varying the duration of the chirped pulse or by performing isotopic substitution while keeping the pulse duration constant, one can control the extension of the harmonic plateauWe gratefully acknowledge fruitful discussions with Y.Mairesse. This work has been accomplished with a generous allocation of computer time from Mare Nostrum BSC and CCC-UAM and has been partially supported by the European Research Council Advanced Grant No. XCHEM 290853, MINECO Project No. FIS2013-42002-R, ERA-Chemistry Project No. PIM2010EEC-00751, European Grant No. MC-ITN CORINF, European COST Action XLIC CM1204, and the CAM project NANOFRONTMAG. R. E. F. S. acknowledges FCT—Fundação para a Ciência e Tecnologia, Portugal, Grant No. SFRH/BD/84053/201

Following the Nonthermal Phase Transition in Niobium Dioxide by Time-Resolved Harmonic Spectroscopy

Photoinduced phase transitions in correlated materials promise diverse applications from ultrafast switches to optoelectronics. Resolving those transitions and possible metastable phases temporally are key enablers for these applications, but challenge existing experimental approaches. Extreme nonlinear optics can help probe phase changes, as higher-order nonlinearities have higher sensitivity and temporal resolution to band structure and lattice deformations. Here the ultrafast transition from the semiconducting to the metallic phases in polycrystalline thin-film NbO2 is investigated by time-resolved harmonic spectroscopy. The emission strength of all harmonic orders shows a steplike suppression when the excitation fluence exceeds a threshold (∼11-12 mJ/cm2), below the fluence required for the thermal transition - a signature of the nonthermal emergence of a metallic phase within 100 ± 20 fs. This observation is backed by full ab initio simulations as well as a 1D chain model of high-harmonic generation from both phases. Our results demonstrate femtosecond harmonic probing of phase transitions and nonthermal dynamics in solids.</p