We demonstrated a novel optical switch to control the high-order harmonic generation process so that single attosecond pulses can be generated with multiple-cycle pulses. The technique combines two powerful optical gating methods: polarization gating and two-color gating. An extreme ultraviolet supercontinuum supporting 130 as was generated with neon gas using 9 fs laser pulses. We discovered a unique dependence of the harmonic spectra on the carrier-envelope phase of the laser fields, which repeats every 2 pi radians.

Isolated attosecond pulses are powerful tools for exploring electron dynamics in matter. So far, such extreme ultraviolet pulses have only been generated using high power, few-cycle lasers, which are very difficult to construct and operate. We propose and demonstrate a technique called generalized double optical gating for generating isolated attosecond pulses with 20 fs lasers from a hollow-core fiber and 28 fs lasers directly from an amplifier. These pulses, generated from argon gas, are measured to be 260 and 148 as by reconstructing the streaked photoelectron spectrograms. This scheme, with a relaxed requirement on laser pulse duration, makes attophysics more accessible to many laboratories that are capable of producing such multicycle laser pulses.

Recent progress in sub-laser-cycle gating of high-order harmonic generation promises to push the limits on optical pulse durations below the atomic unit of time, 24 as, which corresponds to a bandwidth broader than 75 eV. However, the available techniques for attosecond pulse measurement are valid only for narrow-bandwidth spectra, due to one of the key approximations made in the phase retrieval. Here we report a new technique for characterizing attosecond pulses, whereby the spectral phase of the attosecond pulse is extracted from the oscillation component with the dressing laser frequency in the photoelectron spectrogram. This technique, termed PROOF (Phase Retrieval by Omega Oscillation Filtering), can be applied to characterizing attosecond pulses with ultrabroad bandwidths.

Helium atoms in the presence of extreme ultraviolet light pulses can lose electrons through direct photoionization or through two-electron excitation followed by autoionization. Here we demonstrate that, by combining attosecond extreme ultraviolet pulses with near infrared femtosecond lasers, electron dynamics in helium autoionization can be not only monitored but also controlled. Furthermore, the interference between the two ionization channels was modified by the intense near infrared laser pulse. To the best of our knowledge, this is the first time that double excitation and autoionization were studied experimentally by using isolated attosecond pulses.

High-order-harmonic-generation yield is remarkably sensitive to driving laser ellipticity, which is interesting from a fundamental point of view as well as for applications. The most well-known example is the generation of isolated attosecond pulses via polarization gating. We develop an intuitive semiclassical model that makes use of the recently measured initial transverse momentum of tunneling ionization. The model is able to predict the dependence of the high-order-harmonic yield on driving laser ellipticity and is in good agreement with experimental results and predictions from a numerically solved time-dependent Schrödinger equation.

Double optical gating of high-harmonic generation was used to obtain supercontinuous spectra in the extreme UV (XUV) region including the water window. The spectra supported a 16 as pulse duration that is below one atomic unit of time (24 as). The dependence of the gated spectra on the carrier-envelope phase of the laser provided evidence that isolated attosecond pulses were generated. In addition, to ensure the temporal coherence of the XUV light, the pulse shape and phase of isolated 107 as XUV pulses using a portion of the spectrum were characterized by attosecond streaking.

The attosecond streaking technique is used for the characterization of isolated extreme ultraviolet (XUV) attosecond pulses. This type of measurement suffers from low photoelectron counts in the streaked spectrogram, and is thus susceptible to shot noise. For the retrieval of few-or mono-cycle attosecond pulses, high-intensity streaking laser fields are required, which cause the energy spectrum of above-threshold ionized (ATI) electrons to overlap with that of the streaked photoelectrons. It is found by using the principal component generalized projections algorithm that the XUV attosecond pulse can accurately be retrieved for simulated and experimental spectrograms with a peak value of 50 or more photoelectron counts. Also, the minimum streaking intensity is found to be more than 50 times smaller than that required by the classical streaking camera for retrieval of pulses with a spectral bandwidth supporting 90 as transform-limited pulse durations. Furthermore, spatial variation of the streaking laser intensity, collection angle of streaked electrons and time delay jitter between the XUV pulse and streaking field can degrade the quality of the streaked spectrogram. We find that even when the XUV and streaking laser focal spots are comparable in size, the streaking electrons are collected from a 4π solid angle, or the delay fluctuates by more than the attosecond pulse duration, the attosecond pulses can still be accurately retrieved. In order to explain the insusceptibility of the streaked spectrogram to these factors, the linearity of the streaked spectrogram with respect to the streaking field is derived under the saddle point approximation.

Single isolated attosecond pulses can be extracted from a pulse train with an ultrafast gate in the generation target. By setting the gate width sufficiently narrow with the generalized double optical gating, we demonstrate that single isolated attosecond pulses can be generated with any arbitrary carrier-envelope phase value of the driving laser. The carrier-envelope phase only affects the photon flux, not the pulse duration or contrast. Our results show that isolated attosecond pulses can be generated using carrier-envelope phase unstabilized 23 fs pulses directly from chirped pulse amplifiers.