Michael Chini

Tailoring a 67 attosecond pulse through advantageous phase-mismatch

A single isolated attosecond pulse of 67 as was composed from an extreme UV supercontinuum covering 55-130 eV generated by the double optical gating technique. Phase mismatch was used to exclude the single-atom cutoff of the spectrum that possesses unfavorable attochirp, allowing the positive attochirp of the remaining spectrum to be compensated by the negative dispersion of a zirconium foil. Two algorithms, PROOF and FROG-CRAB, were employed to retrieve the pulse from the experimental spectrogram, yielding nearly identical results.

Characterizing ultrabroadband attosecond lasers.

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.

Sub-cycle Oscillations in Virtual States Brought to Light

Understanding and controlling the dynamic evolution of electrons in matter is among the most fundamental goals of attosecond science. While the most exotic behaviors can be found in complex systems, fast electron dynamics can be studied at the fundamental level in atomic systems, using moderately intense (≲103 W/cm2) lasers to control the electronic structure in proof-of-principle experiments. Here, we probe the transient changes in the absorption of an isolated attosecond extreme ultraviolet (XUV) pulse by helium atoms in the presence of a delayed, few-cycle near infrared (NIR) laser pulse, which uncovers absorption structures corresponding to laser-induced “virtual” intermediate states in the two-color two-photon (XUV+NIR) and three-photon (XUV+NIR+NIR) absorption process. These previously unobserved absorption structures are modulated on half-cycle (~1.3 fs) and quarter-cycle (~0.6 fs) timescales, resulting from quantum optical interference in the laser-driven atom.

Extreme ultraviolet supercontinua supporting pulse durations of less than one atomic unit of time

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.

Practical issues of retrieving isolated attosecond pulses

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.

Generation of high-flux attosecond extreme ultraviolet continuum with a 10 TW laser

We report a laser system that delivers 15 fs pulses with 200 mJ energy at a 10 Hz repetition rate. The broadband spectrum extending from 700 nm to 900 nm was obtained by seeding a two-stage Ti:sapphire chirped-pulse power amplifier with sub-mJ white-light pulses from a gas-filled hollow-core fiber. With this laser, an extreme ultraviolet (XUV) super-continuum supporting 230 as isolated attosecond pulses at 35 eV was generated using the generalized double optical gating technique. The XUV pulse energy was ∼100 nJ at the exit of the argon gas target.

Delay control in attosecond pump-probe experiments.

The time delay between the pump and probe pulses in attosecond time-resolved experiments, such as attosecond streaking, is commonly introduced by splitting and recombining the two pulses in an interferometer. This technique suffers from instability in the optical path lengths of the two arms due to mechanical vibration of the optical elements and fluctuating environmental conditions. We present a technique with which the instability of the unconventional interferometer is suppressed while at the same time the time delay is controlled to within 20 as RMS using a feedback loop. Using this scheme, the streaked spectrogram of an attosecond pulse was measured.

53-attosecond X-ray pulses reach the carbon K-edge

The motion of electrons in the microcosm occurs on a time scale set by the atomic unit of time—24 attoseconds. Attosecond pulses at photon energies corresponding to the fundamental absorption edges of matter, which lie in the soft X-ray regime above 200 eV, permit the probing of electronic excitation, chemical state, and atomic structure. Here we demonstrate a soft X-ray pulse duration of 53 as and single pulse streaking reaching the carbon K-absorption edge (284 eV) by utilizing intense two-cycle driving pulses near 1.8-μm center wavelength. Such pulses permit studies of electron dynamics in live biological samples and next-generation electronic materials such as diamond.Isolated attosecond pulses are produced using high harmonic generation and sources of these pulses often suffer from low photon flux in soft X-ray regime. Here the authors demonstrate efficient generation and characterization of 53 as pulses with photon energy near the water window.

Resonance effects and quantum beats in attosecond transient absorption of helium

We present theoretical simulations of the attosecond transient absorption of singly-excited states of helium atoms in the presence of a dressing near-infrared or infrared laser. In particular, we aim to address several unresolved questions in the transient absorption of helium and to resolve the remaining discrepancies between theory and experiment. We initially focus on the forklike structures in the Autler–Townes splitting of the 1s2p state and the effects of resonant coupling to the 1s2s and 1s3s states. We find that the delay-dependent features of the Autler–Townes doublet depend strongly on both the laser frequency detuning from resonance and on the laser pulse duration, and explain the lack of such structures in current experimental data. Next, we identify the interference mechanism which causes the half-cycle oscillations in the absorption spectrum below the excited state manifold. Finally, we observe for the first time the presence of quantum beating in the simulated transient absorption spectrogram, and discuss the conditions under which such wavepacket dynamics could be observed experimentally.

Coupling between energy and phase in hollow-core fiber based f-to-2f interferometers

The dependence of the carrier-envelope (CE) phase of the pulses from a hollow-core fiber on the input laser energy was studied using two f-to- 2f interferometers. The CE phase in the in-loop f-to-2f interferometer was measured with the octave spanning white-light spectrum from the hollow-core fiber, whereas the out-of-loop interferometer was based on a sapphire plate. By modulating the input power of the in-loop interferometer and measuring the out-of-loop CE phase at the same time, the coupling coefficient between the measured CE phase and the laser energy for the hollow-core fiber was determined to be 128 mrad per 1% energy change .