Modification of chirped laser pulses via delayed rotational nonlinearity.

To interpret single-shot measurements of rotational revival patterns in molecular gases excited by an ultrashort laser pulse, an analytical description of the probe pulse modulation by the impulsively excited medium is developed. A femtosecond pump laser pulse prepares a rotational wavepacket in a gas-phase sample, and the resulting periodic revivals are mapped into the frequency domain by using a substantially chirped continuum probe pulse. Since the standard approximate descriptions of probe pulse propagation are inapplicable (such as the slowly varying envelope approximation and the slowly evolving wave approximation), we propose an approach capable of incorporating both the substantial chirp of the pulse and the temporal dispersion of the medium response. Theory is presented for the case where the frequency change of the probe during the probe pulse duration is comparable with the carrier frequency. Analytical expressions are obtained for the probe signal modulation over the pump-probe interaction region and for the resulting heterodyned transient birefringence spectra. The approach is illustrated using the case of nitrogen gas.

Control of spectral interference patterns in broad Rabi sidebands toward quasi-comb structures.

The pattern of spectral interference fringes in broad dynamic Rabi sidebands allows for a considerable degree of control by shaping the picosecond driving pulse. We demonstrate experimental evidence of such control and report an analytic and numerical investigation of possibilities to control the fringe pattern to produce a comb-like optical structure. The temporal phase and amplitude shaping of a picosecond driving pulse influence the spectrum envelope, fringe contrast, and fringe spacing variation in the sideband spectra. The sideband spectrum envelope depends on the sharpness of the driving pulse, that is, on the rate at which the temporal distance between the leading and trailing edges grows away from the pulse maximum. Increasing this parameter reduces the variation of the envelope amplitude across the sideband. The fringe contrast, defined by the maximum-to-minimum difference, depends strongly on the asymmetry of the driving pulse. The imbalance between the leading and trailing edges leads to a decrease of the contrast. The variation of interpeak distance within a sideband was controlled using the temporal shape of the driving pulse. In the particular case of a blue-shifted sideband emitted by excited oxygen atoms driven by a picosecond pulse of 800 nm carrier wavelength and ∼5×10¹° W cm⁻² intensity, a Gaussian pulse shape results in an interpeak distance increasing almost five times over the interval from 1.60 to 1.66 eV, whereas a super-Gaussian shape leads to almost equidistant fringes producing a comb-like spectrum.

Ionization-grating-induced nonlinear phase accumulation in spectrally resolved transient birefringence measurements at 400 nm.

We report experimental confirmation of the ionization-grating-induced transient birefringence predicted by Wahlstrand and Milchberg [Opt. Lett. 36, 3822 (2011)] and discuss its impact on the higher-order Kerr effect interpretation by Loriot et al. of pump-probe transient birefringence measurements made at 800 nm [Opt. Express 17, 13429 (2009)]. Measurement of the transient birefringence in air at 400 nm shows a negative contribution to the index of refraction at zero delay for frequencies within the pump bandwidth, the degenerate case, and no negative contribution for frequencies exceeding the pump bandwidth, the nondegenerate case. Our findings suggest that a reevaluation of the higher-order Kerr effect hypothesis of Loriot et al. is necessary.

Spatial-spectral distribution of Rabi radiation generated in plasma.

We report observation and control of the spatial-spectral distributions of coherent, dynamic Rabi sideband radiation. The Rabi sidebands result from the interaction of a shaped picosecond probe laser of intensity 10(10) W cm(-2), with neutral excited atomic oxygen generated in a laser-induced microplasma. The spatial-spectral distribution is measured and compared for picosecond laser pulses having either an asymmetric temporal shape or a Gaussian temporal shape. The resulting spatial-spectral distributions are in quantitative agreement with theoretical predictions that account for the radial intensity distribution of the picosecond probe pulse.

Origin of the spectral coherence in dynamically broadened Rabi sidebands.

We demonstrate the coherent nature of dynamic Rabi-shifted sidebands arising when a picosecond probe laser interacts with a weakly ionized laser-generated microplasma. The coherence is manifested as spectral fringes observed in the sideband spectra. A model is presented that quantitatively predicts both the spectral phase and the spectral interference measured in the sidebands.

Self-shortening dynamics measured along a femtosecond laser filament in air.

The filamentation-induced temporal shortening of a 40 femtosecond pulse propagating in air is traced using impulsive vibrational Raman scattering and measurement of the power spectrum as a function of position along the propagation axis. The N2, O2, and H2O vibrational Raman responses reveal self-shortening of pulse features to 14 fs during the first filamentation cycle and to at least 9 fs in the second cycle. Spectral measurements further demonstrate that the coherent bandwidth generated in the region from 470 to 330 nm during the self-shortening process forms the ∼9 fs pulse.

Selective bond dissociation and rearrangement with optimally tailored, strong-field laser pulses.

We used strong-field laser pulses that were tailored with closed-loop optimal control to govern specified chemical dissociation and reactivity channels in a series of organic molecules. Selective cleavage and rearrangement of chemical bonds having dissociation energies up to approximately 100 kilocalories per mole (about 4 electron volts) are reported for polyatomic molecules, including (CH3)2CO (acetone), CH3COCF3 (trifluoroacetone), and C6H5COCH3 (acetophenone). Control over the formation of CH(3)CO from (CH3)2CO, CF3 (or CH3) from CH3COCF3, and C6H5CH3 (toluene) from C6H5COCH3 was observed with high selectivity. Strong-field control appears to have generic applicability for manipulating molecular reactivity because the tailored intense laser fields (about 10(13) watts per square centimeter) can dynamically Stark shift many excited states into resonance, and consequently, the method is not confined by resonant spectral restrictions found in the perturbative (weak-field) regime.

Postionization medium evolution in a laser filament: A uniquely nonplasma response.

Theoretical consideration of the optical response of nascent free electrons in the process of laser filamentation reveals that the initial microscopically inhomogeneous charge distribution causes a transient electromagnetic response of the medium that differs drastically from that of a homogeneous plasma with the same degree of ionization. An analytical model, describing the forced oscillations of virtually isolated and expanding electron clouds, predicts considerable enhancement of these oscillations caused by transient resonance with the laser field. The transient resonance processes should play a role in the currently accepted picture of filament formation dynamics.

Impact-ionization cooling in laser-induced plasma filaments.

The ionization rates and subsequent electron dynamics for laser-induced plasma channels are measured for the noble gas series He, Ne, Ar, Kr, and Xe at 1.0 atm. The cw fluorescence emission increases superlinearly in the series from He to Xe in agreement with Ammosov-Delone-Krainov tunnel ionization calculations. The electron temperature after laser-induced plasma formation, measured by four-wave mixing, evolves from >20 eV to <1 eV kinetic energies with time constants ranging from 1 ns for He to 100 ps for Xe in agreement with an impact-ionization cooling model.

Rovibrational wave-packet dispersion during femtosecond laser filamentation in air.

An impulsive, femtosecond filament-based Raman technique producing high quality Raman spectra over a broad spectral range (1554.7-4155 cm(-1)) is presented. The temperature of gas phase molecules can be measured by temporally resolving the dispersion of impulsively excited vibrational wave packets. Application to laser-induced filamentation in air reveals that the initial rovibrational temperature is 300 K for both N2 and O2. The temperature-dependent wave-packet dynamics are interpreted using an analytic anharmonic oscillator model. The wave packets reveal a 1/e dispersion time of 3.9 ps for N2 and 2.8 ps for O2. Pulse self-compression of temporal features to 8 fs within the filament is directly measured by impulsive vibrational excitation of H2.

Elucidating the spectral and temporal contributions from the resonant and nonresonant response to femtosecond coherent anti-Stokes Raman scattering.

A theoretical expression is developed for femtosecond coherent anti-Stokes Raman scattering (CARS) to quantitatively account for the vibrational line shape in the presence of nonresonant signal. The contributions of the resonant and nonresonant components are extracted from the emitted signal line shape as a function of Stokes wavelength and as a function of the temporal overlap of the two pump pulses (for spectrally resolved femtosecond CARS). The theory is compared to the measured spectra of the oxygen vibrational transition DeltaG(01)=1556.4 cm(-1) for temporal detunings of 0 and 700 fs.