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Register a new userExtreme nonlinear Raman interaction of an ultrashort nitrogen ion laser with an impulsively excited molecular wavepacket
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We report generation of cascaded rotational Raman scattering up to 58th orders in coherently excited CO_2 molecules. The high-order Raman scattering, which produces a quasiperiodic frequency comb with more than 600 sidebands, is obtained using an intense femtosecond laser to impulsively excite rotational coherence and the femtosecond-laser-induced N_2^+ lasing to generate cascaded Raman signals. The novel configuration allows this experiment to be performed with a single femtosecond laser beam at free-space standoff locations. It is revealed that the efficient spectral extension of Raman signals is attributed to the specific spectra-temporal structures of N_2^+ lasing, the ideal spatial overlap of femtosecond laser and N2+ lasing, and the guiding effect of molecular alignment. The Raman spectrum extending above 2000 cm^-1 naturally corresponds to a femtosecond pulse train due to the periodic revivals of molecular rotational wavepackets.
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Dynamics of femtosecond pulses with the telecom carrier wavelength is investigated numerically in a subwavelength layer of an indium tin oxide (ITO) epsilon-near-zero (ENZ) material with high dispersion and high nonlinearity. Due to the subwavelength thickness of the ITO ENZ material, and the fact that the pulses propagation time is shorter than its temporal width, multiple reflections give rise to self-interaction in both spectral and temporal domains, especially at wavelengths longer than the ENZ point, at which the reflections are significantly stronger. A larger absolute value of the pulses chirp strongly affects the self-interaction by redistributing energy between wavelengths, while the sign of the chirp affects the interaction in the temporal domain. It is also found that, when two identical pulses are launched simultaneously from both ends, a subwavelength counterpart of a standing-wave state can be established. It shows robust energy localization in the middle of the sample, in terms of both the spectral and temporal intensity distributions.
We compute molecular continuum orbitals in the single center expansion scheme. We then employ these orbitals to obtain molecular Auger rates and single-photon ionization cross sections to study the interaction of N2 with Free-Electron-Laser (FEL) pulses. The nuclei are kept fixed. We formulate rate equations for the energetically allowed molecular and atomic transitions and we account for dissociation through additional terms in the rate equations. Solving these equations for different parameters of the FEL pulse, allows us to identify the most efficient parameters of the FEL pulse for obtaining the highest contribution of double core hole states (DCH) in the final atomic ion fragments. Finally we identify the contribution of DCH states in the electron spectra and show that the DCH state contribution is more easily identified in the photo-ionization rather than the Auger transitions.
We report on an investigation of simultaneous generation of several narrow-bandwidth laser-like coherent emissions from nitrogen molecular ions ( ) produced in intense mid-infrared laser fields. With systematic examinations on the dependences of coherent emissions on gas pressure as well as several laser parameters including laser intensity, polarization and wavelength of the pump laser pulses, we reveal that the multiple coherent emission lines generated in originate from a series of nonlinear processes beginning with four-wave mixing, followed with stimulated Raman scattering. Our analyses further show that the observed nonlinear processes are greatly enhanced at the resonant wavelengths, giving rise to high conversion efficiencies from the infrared pump laser pulses to the coherent emission lines near the transition wavelengths between the different vibrational energy levels of ground X and that of the excited B states.
Quantum cascade lasers (QCL) have revolutionized the generation of mid-infrared light. Yet, the ultrafast carrier transport in mid-infrared QCLs has so far constituted a seemingly insurmountable obstacle for the formation of ultrashort light pulses. Here, we demonstrate that careful quantum design of the gain medium and control over the intermode beat synchronization enable transform-limited picosecond pulses from QCL frequency combs. Both an interferometric radio-frequency technique and second-order autocorrelation shed light on the pulse dynamics and confirm that mode-locked operation is achieved from threshold to rollover current. Being electrically pumped and compact, mode-locked QCLs pave the way towards monolithically integrated non-linear photonics in the molecular fingerprint region beyond 6 $mu$m wavelength.
A quasi-classical model (QCM) of molecular dynamics in intense femtosecond laser fields has been developed, and applied to a study of the effect of an ultrashort `control pulse on the vibrational motion of a deuterium molecular ion in its ground electronic state. A nonadiabatic treatment accounts for the initial ionization-induced vibrational population caused by an ultrashort `pump pulse. In the QCM, the nuclei move classically on the molecular potential as it is distorted by the laser-induced Stark shift and transition dipole. The nuclei then adjust to the modified potential, non-destructively shifting the vibrational population and relative phase. This shift has been studied as a function of control pulse parameters. Excellent agreement is observed with predictions of time-dependent quantum simulations, lending confidence to the validity of the model and permitting new observations to be made. The applicability of the QCM to more complex multi-potential energy surface molecules (where a quantum treatment is at best difficult) is discussed.
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