We exploit inverse Raman scattering and solvated electron absorption to perform a quantitative characterization of the energy loss and ionization dynamics in water with tightly focused near-infrared femtosecond pulses. A comparison between experimental data and numerical simulations suggests that the ionization energy of water is 8 eV, rather than the commonly used value of 6.5 eV. We also introduce an equation for the Raman gain valid for ultra-short pulses that validates our experimental procedure.
We experimentally demonstrate energy exchange between a delay-tuned femtosecond beam and two delay-fixed ones as they spatiotemporally overlapped and experienced filamentation in air. The energy exchange process in the relative time delay is dramatically elongated up to 40 ps in the presence of plasma grating, indicating that filamentary beams coupling may be an effective method for filament control.
We analyze numerically and experimentally the effect of the input pulse chirp on the nonlinear energy deposition from $5 mu$J fs-pulses at $800$ nm to water. Numerical results are also shown for pulses at $400$ nm, where linear losses are minimized, and for different focusing geometries. Input chirp is found to have a big impact on the deposited energy and on the plasma distribution around focus, thus providing a simple and effective mechanism to tune the electron density and energy deposition. We identify three relevant ways in which plasma features may be tuned.
We report on the nonlinear temporal compression of mJ energy pulses from a Ti:Sa chirped pulse amplifier system in a multipass cell filled with argon. The pulses are compressed from 30 fs down to 5.3 fs, corresponding to two optical cycles. The post-compressed beam exhibits excellent spatial quality and homogeneity. These results pave the way to robust and energy-scalable compression of Ti:Sa pulses down to the few-cycle regime.
We present an analysis of two experimental approaches to controlling the directionality of molecular rotation with ultrashort laser pulses. The two methods are based on the molecular interaction with either a pair of pulses (a double kick scheme) or a longer pulse sequence (a chiral pulse train scheme). In both cases, rotational control is achieved by varying the polarization of and the time delay between the consecutive laser pulses. Using the technique of polarization sensitive resonance-enhanced multi-photon ionization, we show that both methods produce significant rotational directionality. We demonstrate that increasing the number of excitation pulses supplements the ability to control the sense of molecular rotation with quantum state selectivity, i.e. predominant excitation of a single rotational state. We also demonstrate the ability of both techniques to generate counter-rotation of molecular nuclear spin isomers (here, ortho- and para-nitrogen) and molecular isotopologues (here, 14N_2 and 15N_2).
We discuss finite-difference time-domain simulations of femtosecond pulses interacting with silver nanowires and nanoparticles. We show how localized hot spots near the metal surfaces can be generated and controlled in a spatiotemporal manner. The control is made possible by chirping the pulses such that the effective frequency passes through surface plasmon resonances associated with different spatial regions of the nanostructure over the course of time. The response of such nanostructures to chirped pulses could provide a novel means of encoding or decoding optical signals.