High-order harmonic generation from a thin film crystal perturbed by a quasi-static terahertz field.

Studies of laser-driven strong field processes subjected to a (quasi-)static field have been mainly confined to theory. Here we provide an experimental realization by introducing a bichromatic approach for high harmonic generation (HHG) in a dielectric that combines an intense 70 femtosecond duration mid-infrared driving field with a weak 2 picosecond period terahertz (THz) dressing field. We address the physics underlying the THz field induced static symmetry breaking and its consequences on the efficient production/suppression of even-/odd-order harmonics, and demonstrate the ability to probe the HHG dynamics via the modulation of the harmonic distribution. Moreover, we report a delay-dependent even-order harmonic frequency shift that is proportional to the time derivative of the THz field. This suggests a limitation of the static symmetry breaking interpretation and implies that the resultant attosecond bursts are aperiodic, thus providing a frequency domain probe of attosecond transients while opening opportunities in precise attosecond pulse shaping.

Two-dimensional retrieval methods for ultrafast imaging of molecular structure using laser-induced electron diffraction.

Molecular structural retrieval based on electron diffraction has been proposed to determine the atomic positions of molecules with sub-angstrom spatial and femtosecond temporal resolutions. Given its success on small molecular systems, in this work, we point out that the accuracy of structure retrieval is constrained by the availability of a wide range of experimental data in the momentum space in all molecular systems. To mitigate the limitations, for laser-induced electron diffraction, here we retrieve molecular structures using two-dimensional (energy and angle) electron momentum spectra in the laboratory frame for a number of small molecular systems, which have previously been studied with 1D methods. Compared to the conventional single-energy or single-angle analysis, our 2D methods effectively expand the momentum range of the measured data. Besides utilization of the 2D data, two complementary methods are developed for consistency check on the retrieved results. The 2D nature of our methods also offers a way of estimating the error from retrieval, which has never been explored before. Comparing with results from prior experiments, our findings show evidence that our 2D methods outperform the conventional 1D methods. Paving the way to the retrieval of large molecular systems, in which their tunneling ionization rates are challenging to obtain, we estimate the error of using the isotropic model in place of including the orientation-dependent ionization rate.

Diffractive Imaging of C_{60} Structural Deformations Induced by Intense Femtosecond Midinfrared Laser Fields.

Theoretical studies indicated that C_{60} exposed to linearly polarized intense infrared pulses undergoes periodic cage structural distortions with typical periods around 100 fs (1 fs=10^{-15} s). Here, we use the laser-driven self-imaging electron diffraction technique, previously developed for atoms and small molecules, to measure laser-induced deformation of C_{60} in an intense 3.6 µm laser field. A prolate molecular elongation along the laser polarization axis is determined to be (6.1±1.4)% via both angular- and energy-resolved measurements of electrons that are released, driven back, and diffracted from the molecule within the same laser field. The observed deformation is confirmed by density functional theory simulations of nuclear dynamics on time-dependent adiabatic states and indicates a nonadiabatic excitation of the h_{g}(1) prolate-oblate mode. The results demonstrate the applicability of laser-driven electron diffraction methods for studying macromolecular structural dynamics in four dimensions with atomic time and spatial resolutions.

Femtosecond laser damage of germanium from near- to mid-infrared wavelengths.

Femtosecond laser-induced damage and ablation (fs-LIDA) is a rich field in extreme non-perturbative nonlinear optics with wide ranging applications, including laser micro- and nano-machining, waveguide writing, and eye surgery. Our understanding of fs-LIDA, however, is limited mostly to visible and near-infrared wavelengths. In this work, we systematically study single-shot, fs-laser ablation (fs-LIA) of single-crystal germanium from near- to mid-infrared wavelengths, and compare the fs-LIA wavelength scaling with two widely used models. We show that these models are inadequate, particularly at mid-infrared wavelengths. Instead, a hybrid model is proposed involving Keldysh ionization rates, a constant free-carrier density threshold, and multi-band effects, which yields good agreement with experimental observations. Aspects of this model may be applied to understanding other strong-field non-perturbative phenomena in solids.

The roles of photo-carrier doping and driving wavelength in high harmonic generation from a semiconductor.

High-harmonic generation from gases produces attosecond bursts and enables high-harmonic spectroscopy to explore electron dynamics in atoms and molecules. Recently, high-harmonic generation from solids has been reported, resulting in novel phenomena and unique control of the emission, absent in gas-phase media. Here we investigate high harmonics from semiconductors with controllable induced photo-carrier densities, as well as the driving wavelengths. We demonstrate that the dominant generation mechanism can be identified by monitoring the variation of the harmonic spectra with the carrier density. Moreover, the harmonic spectral dependence on the driving wavelength is reported and a different dependence from the well-known one in gas-phase media is observed. Our study provides distinct control of the harmonic process from semiconductors, sheds light on the underlying mechanism and helps optimize the harmonic properties for future solid-state attosecond light sources.

Tunable mid-infrared source of light carrying orbital angular momentum in the femtosecond regime.

We report on a tunable intense femtosecond mid-infrared (mid-IR) light source carrying orbital angular momentum (OAM). Our setup is based on an optical parametric amplification system with an 800 nm pump shaped with a spiral phase plate. We confirm the anisotropic OAM transfer from the pump to the idler through stimulated difference frequency generation by measuring the diffraction patterns of a triangular aperture illuminated by the signal, pump, and idler beams. The tunability of the setup is demonstrated by performing measurements at 3.0 and 3.6 µm idler wavelengths. This result provides a robust method of controlling OAM in strong field physics and designing secondary sources carrying OAM in the extreme ultraviolet spectral range through high-order harmonics generation.

Laser induced periodic surface structure formation in germanium by strong field mid IR laser solid interaction at oblique incidence.

Laser induced periodic surface structures (LIPSS or ripples) were generated on single crystal germanium after irradiation with multiple 3 µm femtosecond laser pulses at a 45° angle of incidence. High and low spatial frequency LIPSS (HSFL and LSFL, respectively) were observed for both s- and p-polarized light. The measured LSFL period for p-polarized light was consistent with the currently established LIPSS origination model of coupling between surface plasmon polaritons (SPP) and the incident laser pulses. A vector model of SPP coupling is introduced to explain the formation of s-polarized LSFL away from the center of the damage spot. Additionally, a new method is proposed to determine the SPP propagation length from the decay in ripple depth. This is used along with the measured LSFL period to estimate the average electron density and Drude collision time of the laser-excited surface. Finally, full-wave electromagnetic simulations are used to corroborate these results while simultaneously offering insight into the nature of LSFL formation.

Diffraction using laser-driven broadband electron wave packets.

Directly monitoring atomic motion during a molecular transformation with atomic-scale spatio-temporal resolution is a frontier of ultrafast optical science and physical chemistry. Here we provide the foundation for a new imaging method, fixed-angle broadband laser-induced electron scattering, based on structural retrieval by direct one-dimensional Fourier transform of a photoelectron energy distribution observed along the polarization direction of an intense ultrafast light pulse. The approach exploits the scattering of a broadband wave packet created by strong-field tunnel ionization to self-interrogate the molecular structure with picometre spatial resolution and bond specificity. With its inherent femtosecond resolution, combining our technique with molecular alignment can, in principle, provide the basis for time-resolved tomography for multi-dimensional transient structural determination.

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.

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.