Enhancing strong-field induced molecular vibration with femtosecond pulse shaping

TL;DR

This paper demonstrates that femtosecond pulse shaping can significantly enhance Raman excitation efficiency in molecules under strong-field conditions, surpassing traditional transform-limited pulses, with experimental and theoretical insights into different excitation schemes.

Contribution

It introduces the use of femtosecond pulse shaping to improve strong-field Raman excitation, comparing adiabatic and non-adiabatic methods for the first time.

Findings

Pulse shaping increases Raman signal strength beyond transform-limited pulses.

Both adiabatic and non-adiabatic schemes can enhance excitation efficiency.

Experimental and theoretical analysis confirms the effectiveness of pulse shaping in strong fields.

Abstract

This work investigates the utility of femtosecond pulse shaping in increasing the efficiency of Raman excitation of molecules in the strong-field interaction regime. We study experimentally and theoretically the effect of pulse shaping on the strength of non-resonant coherent anti-Stokes Raman scattering in iodine vapor at laser intensities exceeding $10^{13}$ W/cm$^2$. We show that unlike the perturbative case, shaping strong non-resonant laser pulses can increase the signal strength beyond that observed with the transform-limited excitation. Both adiabatic and non-adiabatic schemes of excitation are explored, and the differences of their potential in increasing the excitation efficiency are discussed.