Demonstration of a 1 TW peak power, joule-level ultrashort Tm:YLF laser.

We report on the demonstration of a diode-pumped, Tm:YLF-based, chirped pulse amplification laser system operating at λ ≈ 1.9 µm that produces amplified pulse energies exceeding 1.5 J using a single 8-pass power amplifier. The amplified pulses are subsequently compressed to sub-300 fs durations by a diffraction grating pair, producing record >1 TW peak power pulses. To the best of our knowledge, this is the highest peak power demonstrated for any solid-state, near-2 µm laser architecture and illustrates the potential of Tm:YLF for the next generation of high-power, diode-pumped ultrashort lasers.

1 GW peak power and 100 J pulsed operation of a diode-pumped Tm:YLF laser.

We report on the generation of high energy, high power pulses in a tabletop diode-pumped Tm:YLF-based laser system, which delivers amplified pulse energies up to 108 J, as well as GW peak power performance when seeded with nanosecond duration pulses. Furthermore, the high power and efficiency capabilities of operating Tm:YLF in the multi-pulse extraction (MPE) regime were explored by seeding the experimental setup with a multi-kHz burst of pulses exhibiting a low individual pulse fluence, resulting in a 3.6 kW average power train of multi-joule-level pulses with an optical-to-optical efficiency of 19%.

Femtosecond damage experiments and modeling of broadband mid-infrared dielectric diffraction gratings.

High peak and average power lasers with high wall-plug efficiency, like the Big Aperture Thulium (BAT) laser, have garnered tremendous attention in laser technology. To meet the requirements of the BAT laser, we have developed low-dispersion reflection multilayer dielectric (MLD) gratings suitable for compression of high-energy pulses for operations at 2 micron wavelength. We carried out 10000-on-1 damage tests to investigate the fluence damage thresholds of the designed MLD gratings and mirrors, which were found between 100-230 mJ/cm2. An ultrashort pulsed laser (FWHM = 53 fs, λ = 1.9 µm) operating at 500 Hz was used in the serpentine raster scans. The atomic force microscope images of the damage sites show blister formation of the underlying layers at lower fluences but ablation of the grating pillars at higher fluences. We simulated the dynamic electronic excitation in the MLD optics with a finite-difference in the time domain approach in 2D. The simulation results agree well with the LIDT measurements and the observed blister formation. This model is able to evaluate the absolute LIDT of MLD gratings.

Demonstration of a compact, multi-joule, diode-pumped Tm:YLF laser.

We report the demonstration of a diode-pumped Tm:YLF laser operating at 1.88 µm that produces pulse energies up to 3.88 J in 20 ns. The compact system consists of a Q-switched cavity-dumped oscillator generating 18 mJ pulses, which are then amplified in a four-pass power amplifier. Energies up to 38.1 J were obtained with long-pulse amplifier operation. These results illustrate the high energy storage and extraction capabilities of diode-pumped Tm:YLF, opening the path to high peak and average power mid-infrared solid-state lasers.

Temporal prepulse contrast degradation in high-intensity CPA lasers from anisotropy of amplifier gain media.

We present a study of the temporal prepulse contrast degradation of high focused intensity pulses produced in CPA laser systems due to imperfections in amplifier design, alignment of amplifier components, and crystal inhomogeneity. Using an extended cross-polarized imaging technique, we demonstrate the presence of multiple crystal domains inside Ti:sapphire slabs with ≈10cm diameter. The results of our numerical calculations show that crystalline c-axis orientation inhomogeneity caused by these crystal domains can lead to the generation of prepulses with a relative contrast of >10-10 within several picoseconds before the main pulse. In a multiple-slab amplifier head configuration sometimes used in high-repetition-rate systems, the misalignment of the crystalline c-axes of the amplifier slab with respect to each other can lead to the generation of prepulses with relative contrast as high as 10-6, depending on the magnitude of misalignment.

Imaging ultrafast molecular dynamics with laser-induced electron diffraction.

Establishing the structure of molecules and solids has always had an essential role in physics, chemistry and biology. The methods of choice are X-ray and electron diffraction, which are routinely used to determine atomic positions with sub-ångström spatial resolution. Although both methods are currently limited to probing dynamics on timescales longer than a picosecond, the recent development of femtosecond sources of X-ray pulses and electron beams suggests that they might soon be capable of taking ultrafast snapshots of biological molecules and condensed-phase systems undergoing structural changes. The past decade has also witnessed the emergence of an alternative imaging approach based on laser-ionized bursts of coherent electron wave packets that self-interrogate the parent molecular structure. Here we show that this phenomenon can indeed be exploited for laser-induced electron diffraction (LIED), to image molecular structures with sub-ångström precision and exposure times of a few femtoseconds. We apply the method to oxygen and nitrogen molecules, which on strong-field ionization at three mid-infrared wavelengths (1.7, 2.0 and 2.3 µm) emit photoelectrons with a momentum distribution from which we extract diffraction patterns. The long wavelength is essential for achieving atomic-scale spatial resolution, and the wavelength variation is equivalent to taking snapshots at different times. We show that the method has the sensitivity to measure a 0.1 Å displacement in the oxygen bond length occurring in a time interval of ∼5 fs, which establishes LIED as a promising approach for the imaging of gas-phase molecules with unprecedented spatio-temporal resolution.

Broadband extreme ultraviolet probing of transient gratings in vanadium dioxide.

Nonlinear spectroscopy in the extreme ultraviolet (EUV) and soft x-ray spectral range offers the opportunity for element selective probing of ultrafast dynamics using core-valence transitions (Mukamel et al., Acc. Chem. Res. 42, 553 (2009)). We demonstrate a step on this path showing core-valence sensitivity in transient grating spectroscopy with EUV probing. We study the optically induced insulator-to-metal transition (IMT) of a VO(2) film with EUV diffraction from the optically excited sample. The VO(2) exhibits a change in the 3p-3d resonance of V accompanied by an acoustic response. Due to the broadband probing we are able to separate the two features.

Laser-induced electron diffraction for probing rare gas atoms.

Recently, using midinfrared laser-induced electron diffraction (LIED), snapshots of a vibrating diatomic molecule on a femtosecond time scale have been captured [C.I. Blaga et al., Nature (London) 483, 194 (2012)]. In this Letter, a comprehensive treatment for the atomic LIED response is reported, a critical step in generalizing this imaging method. Electron-ion differential cross sections (DCSs) of rare gas atoms are extracted from measured angular-resolved, high-energy electron momentum distributions generated by intense midinfrared lasers. Following strong-field ionization, the high-energy electrons result from elastic rescattering of a field-driven wave packet with the parent ion. For recollision energies ≥100 eV, the measured DCSs are indistinguishable for the neutral atoms and ions, illustrating the close collision nature of this interaction. The extracted DCSs are found to be independent of laser parameters, in agreement with theory. This study establishes the key ingredients for applying LIED to femtosecond molecular imaging.

Redshift in the optical absorption of ZnO single crystals in the presence of an intense midinfrared laser field.

We report time-resolved electroabsorption of a weak probe in a 500 µm thick zinc-oxide crystal in the presence of a strong midinfrared pump in the tunneling limit. We observe a substantial redshift in the absorption edge that scales with the cube root of intensity up to 1 TW/cm(2) (0.38 eV cm(2/3) TW(-1/3)) after which it increases more slowly to 0.4 eV at a maximum applied intensity of 5 TW/cm(2). The maximum shift corresponds to more than 10% of the band gap. The change in scaling occurs in a regime of nonperturbative high-order harmonic generation where electrons undergo periodic Bragg scattering from the Brillouin zone boundaries. It also coincides with the limit where the electric field becomes comparable to the ratio of the band gap to the lattice spacing.

An investigation of harmonic generation in liquid media with a mid-infrared laser.

We present a harmonic generation experiment using liquid H(2)O and D(2)O interrogated by a mid-infrared, 3.66 mum, laser at a maximum intensity of 8x10(13) W/cm(2). The unique aspects of the experiment include the long wavelength and short (9 cycle-110 fs) pulse duration of the laser as well as the near-resonant excitation of the H(2)O and D(2)O vibrational modes. We observe up to the 13th harmonic order in H(2)O and intensity scaling is consistent with a direct perturbative process up to the 9th harmonic order. Phase matching and resonant absorption are unable to account for the observed differences in harmonic yields between samples.

The Role of Super-Atom Molecular Orbitals in Doped Fullerenes in a Femtosecond Intense Laser Field.

The interaction of gas phase endohedral fullerene Ho3N@C80 with intense (0.1-5 × 1014 W/cm2), short (30 fs), 800 nm laser pulses was investigated. The power law dependence of Ho3N@C80q+, q = 1-2, was found to be different from that of C60. Time-dependent density functional theory computations revealed different light-induced ionization mechanisms. Unlike in C60, in doped fullerenes, the breaking of the cage spherical symmetry makes super atomic molecular orbital (SAMO) states optically active. Theoretical calculations suggest that the fast ionization of the SAMO states in Ho3N@C80 is responsible for the n = 3 power law for singly charged parent molecules at intensities lower than 1.2 × 1014 W/cm2.