Signatures of Multiband Effects in High-Harmonic Generation in Monolayer MoS_{2}.

High-harmonic generation (HHG) in solids has been touted as a way to probe ultrafast dynamics and crystal symmetries in condensed matter systems. Here, we investigate the polarization properties of high-order harmonics generated in monolayer MoS_{2}, as a function of crystal orientation relative to the mid-infrared laser field polarization. At several different laser wavelengths we experimentally observe a prominent angular shift of the parallel-polarized odd harmonics for energies above approximately 3.5 eV, and our calculations indicate that this shift originates in subtle differences in the recombination dipole strengths involving multiple conduction bands. This observation is material specific and is in addition to the angular dependence imposed by the dynamical symmetry properties of the crystal interacting with the laser field, and may pave the way for probing the vectorial character of multiband recombination dipoles.

Polarization Dependent Excitation and High Harmonic Generation from Intense Mid-IR Laser Pulses in ZnO.

The generation of high order harmonics from femtosecond mid-IR laser pulses in ZnO has shown great potential to reveal new insight into the ultrafast electron dynamics on a few femtosecond timescale. In this work we report on the experimental investigation of photoluminescence and high-order harmonic generation (HHG) in a ZnO single crystal and polycrystalline thin film irradiated with intense femtosecond mid-IR laser pulses. The ellipticity dependence of the HHG process is experimentally studied up to the 17th harmonic order for various driving laser wavelengths in the spectral range 3-4 µm. Interband Zener tunneling is found to exhibit a significant excitation efficiency drop for circularly polarized strong-field pump pulses. For higher harmonics with energies larger than the bandgap, the measured ellipticity dependence can be quantitatively described by numerical simulations based on the density matrix equations. The ellipticity dependence of the below and above ZnO band gap harmonics as a function of the laser wavelength provides an efficient method for distinguishing the dominant HHG mechanism for different harmonic orders.

Strong Light-Field Driven Nanolasers.

Einstein established the quantum theory of radiation and paved the way for modern laser physics including single-photon absorption by charge carriers and finally pumping an active gain medium into population inversion. This can be easily understood in the particle picture of light. Using intense, ultrashort pulse lasers, multiphoton pumping of an active medium has been realized. In this nonlinear interaction regime, excitation and population inversion depend not only on the photon energy but also on the intensity of the incident pumping light, which can be still described solely by the particle picture of light. We demonstrate here that lowering significantly the pump photon energy further still enables population inversion and lasing in semiconductor nanowires. The extremely high electric field of the pump bends the bands and enables tunneling of electrons from the valence to the conduction band. In this regime, the light acts by the classical Coulomb force and population inversion is entirely due to the wave nature of electrons, thus the excitation becomes independent of the frequency but solely depends on the incident intensity of the pumping light.

Single-shot nanosecond-resolution multiframe passive imaging by multiplexed structured image capture.

The Multiplexed Structured Image Capture (MUSIC) technique is used to demonstrate single-shot multiframe passive imaging, with a nanosecond difference between the resulting images. This technique uses modulation of light from a scene before imaging, in order to encode the target's temporal evolution into spatial frequency shifts, each of which corresponds to a unique time and results in individual and distinct snapshots. The resulting images correspond to different effective imaging gate times, because of the optical path delays. Computer processing of the multiplexed single-shot image recovers the nanosecond-resolution evolution. The MUSIC technique is used to demonstrate imaging of a laser-induced plasma. Simultaneous single-shot measurements of electron numbers by coherent microwave scattering were obtained and showed good agreement with MUSIC characterization. The MUSIC technique demonstrates spatial modulation of images used for passive imaging. This allows multiple frames to be stacked into a single image. This method could also pave the way for real-time imaging and characterization of ultrafast processes and visualization, as well as general tracking of fast objects.

Disentangling Intracycle Interferences in Photoelectron Momentum Distributions Using Orthogonal Two-Color Laser Fields.

We use orthogonally polarized two-color (OTC) laser pulses to separate quantum paths in the multiphoton ionization of Ar atoms. Our OTC pulses consist of 400 and 800 nm light at a relative intensity ratio of 10∶1. We find a hitherto unobserved interference in the photoelectron momentum distribution, which exhibits a strong dependence on the relative phase of the OTC pulse. Analysis of model calculations reveals that the interference is caused by quantum pathways from nonadjacent quarter cycles.

Resonance-enhanced multi-octave supercontinuum generation in antiresonant hollow-core fibers.

Ultrafast supercontinuum generation in gas-filled waveguides is an enabling technology for many intriguing applications ranging from attosecond metrology towards biophotonics, with the amount of spectral broadening crucially depending on the pulse dispersion of the propagating mode. In this study, we show that structural resonances in a gas-filled antiresonant hollow core optical fiber provide an additional degree of freedom in dispersion engineering, which enables the generation of more than three octaves of broadband light that ranges from deep UV wavelengths to near infrared. Our observation relies on the introduction of a geometric-induced resonance in the spectral vicinity of the ultrafast pump laser, outperforming gas dispersion and yielding a unique dispersion profile independent of core size, which is highly relevant for scaling input powers. Using a krypton-filled fiber, we observe spectral broadening from 200 nm to 1.7 µm at an output energy of ∼ 23 µJ within a single optical mode across the entire spectral bandwidth. Simulations show that the frequency generation results from an accelerated fission process of soliton-like waveforms in a non-adiabatic dispersion regime associated with the emission of multiple phase-matched Cherenkov radiations on both sides of the resonance. This effect, along with the dispersion tuning and scaling capabilities of the fiber geometry, enables coherent ultra-broadband and high-energy sources, which range from the UV to the mid-infrared spectral range.

Duration of an intense laser pulse can determine the breakage of multiple chemical bonds.

Control over the breakage of a certain chemical bond in a molecule by an ultrashort laser pulse has been considered for decades. With the availability of intense non-resonant laser fields it became possible to pre-determine femtosecond to picosecond molecular bond breakage dynamics by controlled distortions of the electronic molecular system on sub-femtosecond time scales using field-sensitive processes such as strong-field ionization or excitation. So far, all successful demonstrations in this area considered only fragmentation reactions, where only one bond is broken and the molecule is split into merely two moieties. Here, using ethylene (C2H4) as an example, we experimentally investigate whether complex fragmentation reactions that involve the breakage of more than one chemical bond can be influenced by parameters of an ultrashort intense laser pulse. We show that the dynamics of removing three electrons by strong-field ionization determines the ratio of fragmentation of the molecular trication into two respectively three moieties. We observe a relative increase of two-body fragmentations with the laser pulse duration by almost an order of magnitude. Supported by quantum chemical simulations we explain our experimental results by the interplay between the dynamics of electron removal and nuclear motion.

Generation of multi-millijoule red-shifted pulses for seeding stimulated Raman backscattering amplifiers.

The efficient generation of redshifted pulses from chirped femtosecond joule level Bessel beam pulses in gases is studied. The redshift spans from a few 100 cm⁻¹ to several 1000 cm⁻¹ corresponding to a shift of 50-500 nm for Nd:glass laser systems. The generated pulses have an almost perfect Gaussian beam profile insensitive of the pump beam profile, and are much shorter than the pump pulses. The highest measured energy is as high as 30 mJ, which is significantly higher than possible with solid state nonlinear frequency shifters.

Subcycle control of electron-electron correlation in double ionization.

Double ionization of neon with orthogonally polarized two-color (OTC) laser fields is investigated using coincidence momentum imaging. We show that the two-electron emission dynamics in nonsequential double ionization can be controlled by tuning the subcycle shape of the electric field of the OTC pulses. We demonstrate experimentally switching from correlated to anticorrelated two-electron emission, and control over the directionality of the two-electron emission. Simulations based on a semiclassical trajectory model qualitatively explain the experimental results by a subcycle dependence of the electron recollision time on the OTC field shape.

Selective control over fragmentation reactions in polyatomic molecules using impulsive laser alignment.

We investigate the possibility of using molecular alignment for controlling the relative probability of individual reaction pathways in polyatomic molecules initiated by electronic processes on the few-femtosecond time scale. Using acetylene as an example, it is shown that aligning the molecular axis with respect to the polarization direction of the ionizing laser pulse does not only allow us to enhance or suppress the overall fragmentation yield of a certain fragmentation channel but, more importantly, to determine the relative probability of individual reaction pathways starting from the same parent molecular ion. We show that the achieved control over dissociation or isomerization pathways along specific nuclear degrees of freedom is based on a controlled population of associated excited dissociative electronic states in the molecular ion due to relatively enhanced ionization contributions from inner valence orbitals.

Attosecond probe of valence-electron wave packets by subcycle sculpted laser fields.

We experimentally and theoretically demonstrate a self-referenced wave-function retrieval of a valence-electron wave packet during its creation by strong-field ionization with a sculpted laser field. Key is the control over interferences arising at different time scales. Our work shows that the measurement of subcycle electron wave-packet interference patterns can serve as a tool to retrieve the structure and dynamics of the valence-electron cloud in atoms on a sub-10-as time scale.

White light generation over three octaves by femtosecond filament at 3.9 µm in argon.

We report the first (to our knowledge) experimental results and numerical simulations on mid-IR femtosecond pulse filamentation in argon using 0.1 TW peak-power, 80 fs, 3.9 µm pulses. A broadband supercontinuum spanning the spectral range from 350 nm to 5 µm is generated, whereby about 4% of the mid-IR pulse energy is converted into the 350-1700 nm spectral region. These mid-IR-visible coherent continua offer a new, unique tool for time-resolved spectroscopy based on a mid-IR filamentation laser source.

Attosecond-recollision-controlled selective fragmentation of polyatomic molecules.

Control over various fragmentation reactions of a series of polyatomic molecules (acetylene, ethylene, 1,3-butadiene) by the optical waveform of intense few-cycle laser pulses is demonstrated experimentally. We show both experimentally and theoretically that the responsible mechanism is inelastic ionization from inner-valence molecular orbitals by recolliding electron wave packets, whose recollision energy in few-cycle ionizing laser pulses strongly depends on the optical waveform. Our work demonstrates an efficient and selective way of predetermining fragmentation and isomerization reactions in polyatomic molecules on subfemtosecond time scales.

High energy proton ejection from hydrocarbon molecules driven by highly efficient field ionization.

We investigated the ejection of energetic protons from a series of polyatomic hydrocarbon molecules exposed to 790 nm 27 fs laser pulses. Using multiparticle coincidence imaging we were able to decompose the observed proton energy spectra into the contributions of individual fragmentation channels. It is shown that the molecules can completely fragment already at relatively low peak intensities of a few 10(14) W/cm(2), and that the protons are ejected in a concerted Coulomb explosion from unexpectedly high charge states. The observations are in agreement with enhanced ionization taking place at many C-H bonds in parallel.

Two-proton migration in 1,3-butadiene in intense laser fields.

Ultrafast proton migration in 1,3-butadiene in an intense laser field (40 fs, 4.5 × 10(14) W cm(-2)) is investigated by using Coulomb explosion coincidence momentum imaging. The spatial distribution maps of a migrating proton reconstructed for the two three-body Coulomb explosion pathways, C(4)H(6)(3+)→ H(+) + CH(3)(+) + C(3)H(2)(+) and C(4)H(6)(3+)→ H(+) + C(2)H(+) + C(2)H(4)(+), reveal that two protons migrate within a 1,3-butadiene molecule, prior to the three body decomposition.

Optical detection of tunneling ionization.

We have experimentally detected optical harmonics that are generated due to a tunneling-ionization-induced modulation of the electron density. The optical signature of electron tunneling can be isolated from concomitant optical responses by using a noncollinear pump-probe setup. Whereas previously demonstrated tools for attosecond metrology of gases, plasmas, and surfaces rely on direct detection of charged particles, detection of the background-free time-resolved optical signal, which uniquely originates from electron tunneling, offers an interesting alternative that is especially suited for systems in which free electrons cannot be directly measured.