The field of attosecond science was first enabled by nonlinear compression of intense laser pulses to a duration below two optical cycles. Twenty years later, creating such short pulses still requires state-of-the-art few-cycle laser amplifiers to most efficiently exploit “instantaneous” optical nonlinearities in noble gases for spectral broadening and parametric frequency conversion. Here, we show that nonlinear compression can be much more efficient when driven in molecular gases by pulses substantially longer than a few cycles because of enhanced optical nonlinearity associated with rotational alignment. We use 80-cycle pulses from an industrial-grade laser amplifier to simultaneously drive molecular alignment and supercontinuum generation in a gas-filled capillary, producing more than two octaves of coherent bandwidth and achieving >45-fold compression to a duration of 1.6 cycles. As the enhanced nonlinearity is linked to rotational motion, the dynamics can be exploited for long-wavelength frequency conversion and compressing picosecond lasers.

Recent developments in ultrafast laser technology have resulted in novel few-cycle sources in the mid-infrared. Accurately characterizing the time-dependent intensities and electric field waveforms of such laser pulses is essential to their applications in strong-field physics and attosecond pulse generation, but this remains a challenge. Recently, it was shown that tunnel ionization can provide an ultrafast temporal “gate” for characterizing high-energy few-cycle laser waveforms capable of ionizing air. Here, we show that tunneling and multiphoton excitation in a dielectric solid can provide a means to measure lower-energy and longer-wavelength pulses, and we apply the technique to characterize microjoule-level near- and mid-infrared pulses. The method lends itself to both all-optical and on-chip detection of laser waveforms, as well as single-shot detection geometries.

Studies of 2s → np autoionization resonances in the neon isoelectronic sequence using relativistic multichannel quantum defect theory (RMQDT) are reported. The relativistic random phase approximation (RRPA) is used to calculate the quantum defect parameters. The autoionization resonances are characterized using Fano resonance parameters. The results are compared with available experimental and theoretical data, and the behavior of the resonances as a function of Z is discussed.

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We probe a new pathway for the formation of smaller anions from the temporary negative ion states (anion resonances) of C n N− (n = 1–3, 5–7) in the circumstellar envelope of IRC+10216. C n N− (n = 1–3, 5–7) anions were collisionally excited to their resonance states and were observed to decay into a variety of smaller anions. The measured kinetic-energy-release distributions for the anionic fragments arising from each of the parent anions indicate a concerted manner of occurrence of these fragments, implying rich dissociation dynamics. and C2N− were found to be dominant fragments of these anions, suggesting their presence in the external layers of IRC+10216 where UV photons penetrate. C n N− (n = 1–3) were also observed to undergo dissociative and nondissociative double-electron detachments, with the former being dominant. The significance of this new pathway in determining the stability and abundance of anions in IRC+10216 is discussed.