No Arabic abstract
Strong-field quantum-state control is investigated, taking advantage of the full---amplitude and phase---characterization of the interaction between matter and intense ultrashort pulses via transient-absorption spectroscopy. A sequence of intense delayed pulses is used, whose parameters are tailored to steer the system into a desired quantum state. We show how to experimentally enable this optimization by retrieving all quantum features of the light-matter interaction from observable spectra. This provides a full characterization of the action of strong fields on the atomic system, including the dependence upon possibly unknown pulse properties and atomic structures. Precision and robustness of the scheme are tested, in the presence of surrounding atomic levels influencing the systems dynamics.
Advances of quantum control technology have led to nearly perfect single-qubit control of nuclear spins and atomic hyperfine ground states. In contrast, quantum control of strong optical transitions, even for free atoms, are far from being perfect. Developments of such quantum control appears to be bottlenecked by available laser technology for generating isolated, sub-nanosecond optical waveforms with sub-THz programming bandwidth. Here we propose a simple and robust method for the desired pulse shaping, based on precisely stacking multiple delayed picosecond pulses. Our proof-of-principal demonstration leads to arbitrarily shapeable optical waveforms with 30~GHz bandwidth and $100~$ps duration. We confirm the stability of the waveforms by interfacing the pulses with laser-cooled atoms, resulting in ``super-resolved spectroscopic signals. This pulse shaping method may open exciting perspectives in quantum optics, and for fast laser cooling and atom interferometry with mode-locked lasers.
We investigate AC Stark-shifted resonances in argon with ultrashort near-infrared pulses. Using 30 fs pulses we observe periodic enhancements of the excitation yield in the intensity regions corresponding to the absorption of 13 and 14 photons. By reducing the pulse duration to 6 fs with only a few optical cycles, we also demonstrate that the enhancements are significantly reduced beyond what is measurable in the experiment. Comparing these to numerical predictions, which are in quantitative agreement with experimental results, we find that even though the quantum-state distribution can be broad, the enhancements are largely due to efficient population of a select few AC Stark-shifted resonant states rather than the closing of an ionization channel. Because these resonances are dependent on the frequency and intensity of the laser field, the broad bandwidth of the 6 fs pulses means that the resonance condition is fulfilled across a large range of intensities. This is further exaggerated by volume-averaging effects, resulting in excitation of the $5g$ state at almost all intensities and reducing the apparent magnitude of the enhancements. For 30 fs pulses, volume averaging also broadens the quantum state distribution but the enhancements are still large enough to survive. In this case, selectivity of excitation to a single state is reduced below 25% of the relative population. However, an analysis of TDSE simulations indicates that excitation of up to 60% into a single state is possible if volume averaging can be eliminated and the intensity can be precisely controlled.
We use classical electron ensembles and the aligned-electron approximation to examine the effect of laser pulse duration on the dynamics of strong-field double ionization. We cover the range of intensities $10^{14}-10^{16} W/cm^2$ for the laser wavelength 780 nm. The classical scenario suggests that the highest rate of recollision occurs early in the pulse and promotes double ionization production in few-cycle pulses. In addition, the purely classical ensemble calculation predicts an exponentially decreasing recollision rate with each subsequent half cycle. We confirm the exponential behavior by trajectory back-analysis.
High-order harmonics generated by bicircular laser field have helicities which alternate between $+1$ and $-1$. In order to generate circularly polarized high-harmonic pulses, which are important for applications, it is necessary to achieve asymmetry in emission of harmonics having opposite helicities. We theoretically investigated a wide range of bicircular field component intensities and found areas where both the harmonic intensity is high and the helicity asymmetry is large. We investigated the cases of $omega$--$2omega$ and $omega$--$3omega$ bicircular fields and atoms having the $s$ and $p$ ground states, exemplified by He and Ne atoms, respectively. We have shown that for He atoms strong high harmonics having positive helicity can be generated using $omega$--$3omega$ bicircular field with a much stronger second field component. For Ne atoms the helicity asymmetry can be large in a wider range of the driving field component intensities and for higher harmonic orders. For the stronger second field component the harmonic intensity is higher and the helicity asymmetry parameter is larger for higher harmonic orders. The results for Ne atoms are illustrated with the parametric plots of elliptically polarized attosecond high-harmonic field.
A nonlinear interferometry scheme is described theoretically to induce and resolve electron wave- function beating on time scales shorter than the optical cycle of the time-delayed pump and probe pulses. By employing two moderately intense few-cycle laser fields with a stable carrier-envelope phase, a large range of the entire electronic level structure of a quantum system can be retrieved. In contrast to single-photon excitation schemes, the retrieved electronic states include levels that are both dipole- and non-dipole-accessible from the ground electronic state. The results show that strong-field interferometry can reveal both high-resolution and broad-band spectral information at the same time with important consequences for quantum-beat spectroscopy on attosecond or even shorter time scales.