Mid-infrared Femtosecond Laser Pulses Research Articles

Hybrid Photoexcitation in Undoped Diamond by Mid-Infrared Femtosecond Laser Pulses

Direct interband and intragap photoexcitation by intense mid-infrared (4.0 and 4.7 μm) femtosecond (fs) laser pulses was explored in ultrapure chemical-vapor deposited (CVD) diamond via acquisition of characteristic ultraviolet photoluminescence of free excitons and A-band photoluminescence of electrons anchored at deep donor–acceptor or dislocation-related traps, respectively. At lower laser intensities (<10 TW/cm2) the excitonic photoluminescence yields exhibit highly nonlinear dependences with Iλ2-scaling and power slopes N ≈ 17 (4.0 μm) and 14 (4.7 μm), still insufficient to cross over the direct bandgap (≥6.5 eV) by ≈1.2 and 2.8 eV, respectively. Similarly high slope of ≈9 (4.7 μm) for intragap (≥3.5 eV) photo-population of donor–acceptor traps is still insufficient for their direct excitation by ≈1 eV. At the intermediate Iλ2-dependent values of the Keldysh parameter γ ∼ 1 such incomplete multiphoton excitation anticipates the hybrid total “multiphoton + tunneling” photoexcitation generally predicted by the Keldysh theory, but never unambiguously experimentally demonstrated. At higher laser intensities (>10 TW/cm2) both the excitonic and A-band photoluminescence yields exhibit (sub)linear slopes, apparently, indicating formation of more strongly absorbing electron–hole plasma. These findings shed light on the hybrid multiphoton + tunneling character of Keldysh photoexcitation at intermediate values γ and pave the way to defect/impurity band engineering of intragap nonlinear optical properties in bulk dielectrics for their precise fs-laser nanomodification.

Efficient and high-spatiotemporal-quality terawatt-class mid-infrared optical parametric amplifiers by spatially shaped pumping

We propose a method to efficiently generate terawatt (TW)-class mid-infrared (MIR) femtosecond laser pulses with high spatiotemporal quality through optical parametric chirped-pulse amplification (OPCPA). By transforming the pump-beam profile for the OPCPA from Gaussian to flat-top using a designed field mapping optics consisting of two aspherical lenses, we obtain a TW-class femtosecond laser pulse at 2 µm with a conversion efficiency of over 36% according to our simulations. Furthermore, the spatiotemporal coupling effects are greatly suppressed in our method compared to an OPCPA system that is pumped by a widely employed Gaussian profile beam. Our work provides a simple and robust method for developing OPCPA systems with high efficiency and high pulse quality.

Single-shot selective femtosecond and picosecond infrared laser crystallization of an amorphous Ge/Si multilayer stack

Pulsed laser crystallization is an efficient annealing technique to obtain polycrystalline silicon or germanium films on non-refractory substrates. This is important for creating “flexible electronics” and can also be used to fabricate thin-film solar cells. In this work, near- and mid-infrared femtosecond and picosecond laser pulses were used to crystallize a Ge/Si multilayer stack consisting of alternating amorphous thin films of silicon and germanium. The use of infrared radiation at wavelengths of 1030 and 1500 nm with photon energies lower than the optical absorption edge in amorphous silicon allowed obtaining selective crystallization of germanium layers with a single laser shot. The phase composition of the irradiated stack was investigated by the Raman scattering technique. Several non-ablative regimes of ultrashort-pulse laser crystallization were found, from partial crystallization of germanium without intermixing the Ge/Si layers to complete intermixing of the layers with formation of GexSi1-x solid alloys. The roles of single- and two-photon absorption, thermal and non-thermal (ultrafast) melting processes, and laser-induced stresses in selective pico- and femtosecond laser annealing are discussed. It is concluded that, due to a mismatch of the thermal expansion coefficients between the adjacent stack layers, efficient explosive solid-phase crystallization of the Ge layers is possible at relatively low temperatures, well below the melting point.

Selective ultrashort laser annealing of amorphous Ge/Si multilayer stacks

We report on single-short laser crystallization of Ge/Si multilayer stacks consisting of alternating amorphous nanosized films of silicon and germanium using near- and mid-infrared femtosecond and picosecond laser pulses. The phase composition of the irradiated stacks was investigated by the Raman scattering technique. Several non-ablative regimes of crystallization were found, from partial crystallization of germanium without intermixing the Ge/Si layers to complete intermixing of the layers with formation of GexSi1-x solid alloys. The roles of one- and two-photon absorption, thermal and non-thermal (ultrafast) melting processes, and laser-induced stresses in selective pico- and femtosecond laser annealing are analysed based on theoretical estimations and comparison with experimental data. It is concluded that, due to a mismatch of the thermal expansion coefficients between the adjacent stack layers, efficient explosive solid-phase crystallization of the Ge layers is possible at relatively low temperatures, well below the melting point. The possibility of ultrafast non-thermal phase transition in germanium in the studied regimes is also discussed.

Observation of ultrafast impact ionization in diamond driven by mid-infrared femtosecond pulses

We report on the observation of ultrafast impact ionization in monocrystalline diamond driven by high-intensity mid-infrared femtosecond laser pulses. The measurements are based on monitoring the excited carrier population during and after the interaction of the pre-excited sample with a strong infrared pulse by transient transmission spectroscopy and photoluminescence measurements. A twofold increase in the initial carrier population due to impact ionization is observed with the peak infrared intensity of 2.5 TW/cm2. The experimental results are supported by numerical simulations of electron dynamics using time-dependent density functional theory, which show that the electrons in the conduction band reach the energy threshold for impact ionization during the interaction with the infrared pulse.

Ionisation processes and laser induced periodic surface structures in dielectrics with mid-infrared femtosecond laser pulses

Irradiation of solids with ultrashort pulses and laser processing in the mid-Infrared (mid-IR) spectral region is a yet predominantly unexplored field with a large potential for a wide range of applications. In this work, laser driven physical phenomena associated with processes following irradiation of fused silica (SiO2) with ultrashort laser pulses in the mid-IR region are investigated in detail. A multiscale modelling approach is performed that correlates conditions for formation of perpendicular or parallel to the laser polarisation low spatial frequency periodic surface structures for low and high intensity mid-IR pulses (not previously explored in dielectrics at those wavelengths), respectively. Results demonstrate a remarkable domination of tunneling effects in the photoionisation rate and a strong influence of impact ionisation for long laser wavelengths. The methodology presented in this work is aimed to shed light on the fundamental mechanisms in a previously unexplored spectral area and allow a systematic novel surface engineering with strong mid-IR fields for advanced industrial laser applications.

Observation of extremely efficient terahertz generation from mid-infrared two-color laser filaments

Extreme nonlinear interactions of THz electromagnetic fields with matter are the next frontier in nonlinear optics. However, reaching this frontier in free space is limited by the existing lack of appropriate powerful THz sources. Here, we experimentally demonstrate that two-color filamentation of femtosecond mid-infrared laser pulses at 3.9 μm allows one to generate ultrashort sub-cycle THz pulses with sub-milijoule energy and THz conversion efficiency of 2.36%, resulting in THz field amplitudes above 100 MV cm−1. Our numerical simulations predict that the observed THz yield can be significantly upscaled by further optimizing the experimental setup. Finally, in order to demonstrate the strength of our THz source, we show that the generated THz pulses are powerful enough to induce nonlinear cross-phase modulation in electro-optic crystals. Our work paves the way toward free space extreme nonlinear THz optics using affordable table-top laser systems.

Single-Shot Multi-Stage Damage and Ablation of Silicon by Femtosecond Mid-infrared Laser Pulses

Although ultrafast laser materials processing has advanced at a breakneck pace over the last two decades, most applications have been developed with laser pulses at near-IR or visible wavelengths. Recent progress in mid-infrared (MIR) femtosecond laser source development may create novel capabilities for material processing. This is because, at high intensities required for such processing, wavelength tuning to longer wavelengths opens the pathway to a special regime of laser-solid interactions. Under these conditions, due to the λ2 scaling, the ponderomotive energy of laser-driven electrons may significantly exceed photon energy, band gap and electron affinity and can dominantly drive absorption, resulting in a paradigm shift in the traditional concepts of ultrafast laser-solid interactions. Irreversible high-intensity ultrafast MIR laser-solid interactions are of primary interest in this connection, but they have not been systematically studied so far. To address this fundamental gap, we performed a detailed experimental investigation of high-intensity ultrafast modifications of silicon by single femtosecond MIR pulses (λ = 2.7–4.2 μm). Ultrafast melting, interaction with silicon-oxide surface layer, and ablation of the oxide and crystal surfaces were ex-situ characterized by scanning electron, atomic-force, and transmission electron microscopy combined with focused ion-beam milling, electron diffractometry, and μ-Raman spectroscopy. Laser induced damage and ablation thresholds were measured as functions of laser wavelength. The traditional theoretical models did not reproduce the wavelength scaling of the damage thresholds. To address the disagreement, we discuss possible novel pathways of energy deposition driven by the ponderomotive energy and field effects characteristic of the MIR wavelength regime.

Dual-Chirped Optical Parametric Amplification: A Method for Generating Super-Intense Mid-Infrared Few-Cycle Pulses

High-energy infrared (IR) femtosecond laser sources are important for applications in ultrafast and strong-field laser science; thus, considerable effort has recently been made to develop such laser systems. In this paper, we review our recent work on developing TW-class mid-infrared (MIR) femtosecond laser pulses in the 1–4 $\mu$ m region using a dual-chirped optical parametric amplification (DC-OPA) method. By employing a Ti:sapphire laser with sub-joule energy to pump the DC-OPA system, MIR femtosecond pulses with 100-mJ-class energy are demonstrated. Efficient energy scalability and flexible wavelength tunability in DC-OPA are confirmed experimentally. Different features of DC-OPA from those of conventional OPA and narrow-band pumped optical parametric chirped pulse amplification (OPCPA) are observed. By precisely optimizing the chirps of the seed and pump pulses in the DC-OPA system, bandwidth narrowing of amplified pulses can be minimized in an energy-scaling strategy. Moreover, DC-OPA can be universally employed for the energy scaling of near-IR, MIR, and far-IR pulses, regardless of the type of nonlinear crystal, and is helpful for efficiently generating few-cycle carrier-envelope phase stable IR pulses with TW-class peak power.

Supercontinuum generation in the absence and in the presence of color centers in NaCl and KBr

We study supercontinuum generation with femtosecond mid-infrared laser pulses in NaCl and KBr crystals when pumped at the vicinity of their zero group velocity dispersion points. Almost three octave-spanning SC spectra (covering the 0.7–5.4 μm and 0.85–5.4 μm ranges in 5 mm-thick NaCl and KBr samples, respectively) were produced by filamentation of 70 fs, 3.6 μm input pulses in continuously translated samples. In the static setup, we show that rapid formation of persistent color centers (within a few seconds at 500 Hz repetition rate) inside these materials results in a marked decrease (by 40%) of the overall energy transmittance and in significant narrowing of SC spectra. We also demonstrate that the effect of color centers on the SC spectrum could be adequately simulated numerically using a simple phenomenological model which considers color centers as impurities with a certain energy bandgap.

Relativistic Interaction of Long-Wavelength Ultrashort Laser Pulses with Nanowires

We report on experimental results in a new regime of a relativistic light-matter interaction employing mid-infrared (3.9-micrometer wavelength) high-intensity femtosecond laser pulses. In the laser generated plasma, the electrons reach relativistic energies already at rather low intensities due to the fortunate lambda^2-scaling of the kinetic energy with the laser wavelength. The lower intensity suppresses optical field ionization and creation of the pre-plasma at the rising edge of the laser pulse efficiently, enabling an enhanced efficient vacuum heating of the plasma. The lower critical plasma density for long-wavelength radiation can be surmounted by using nanowires instead of flat targets. In our experiments about 80% of the incident laser energy has been absorbed resulting in a long living, keV-temperature, high-charge state plasma with a density of more than three orders of magnitude above the critical value. Our results pave the way to laser-driven experiments on laboratory astrophysics and nuclear physics at a high repetition rate.

Optical transmission during mid-infrared femtosecond laser pulses ablation of fused silica

We report on the optical transmission of near-infrared (1.8 μm) femtosecond laser pulses during multiple pulses laser ablation of fused silica surface. In addition to the previously reported ciliary white light phenomenon (Phys. Rev. Lett. 110, 097601 (2013)), two new optical transmission phenomena were observed for relatively low energy laser pulses. We systemically examined the damage morphologies of the ablation site as a function of laser pulse energy and laser shot number. Laser induced periodic surface structures (LIPSS) with different periods and orientations were observed for different pulse energy regimes. Comparison of the damage morphologies and the optical transmission reveals that the two new optical transmission phenomena origin from the refraction of the incident near-infrared pulses on the LIPSS covered damage surface followed by nonlinear propagation of the beamlets and even filamentation if the laser energy was high enough. We found that the interference of the neighboring white light emissions gives rise to radially orientated optical fringes. Based on this observation, we proposed another interpretation for the ciliary white light phenomenon.

High-order harmonic generations in intense MIR fields by cascade three-wave mixing in a fractal-poled LiNbO3 photonic crystal.

We report on the generation of harmonic-like photon upconversion in a LiNbO3-based nonlinear photonic crystal by mid-infrared (MIR) femtosecond laser pulses. We study below bandgap harmonics of various driver wavelengths, reaching up to the 11th order at 4μm driver with 13% efficiency. We compare our results to numerical simulations based on two mechanisms: cascade three-wave mixing and non-perturbative harmonic generation, both of which include quasi-phase matching. The cascade model reproduces well the general features of the observed spectrum, including a plateau-like harmonic distribution and the observed efficiency. This has the potential for providing a source of tabletop few femtosecond ultraviolet pulses.

Nonperturbative generation of above-threshold harmonics from pre-excited argon atoms in intense mid-infrared laser fields

We experimentally investigate the generation of above-threshold harmonics completely from argon atoms on an excited state using mid-infrared femtosecond laser pulses. The highly nonlinear dependences of the observed signal on the pulse energy and polarization of the probe laser pulses indicate its nonperturbative characteristic.

Publisher's Note: Comment on “Direct photodetachment of F− by mid-infrared few-cycle femtosecond laser pulses” [Phys. Rev. A 94 , 057401 (2016)

Received 19 December 2016DOI:https://doi.org/10.1103/PhysRevA.94.069903©2016 American Physical Society

Comment on “Direct photodetachment of F− by mid-infrared few-cycle femtosecond laser pulses”

Multiphoton detachment of F$^-$ by strong few-cycle laser pulses was studied by Shearer and Monteith using a Keldysh-type approach [Phys. Rev. A 88, 033415 (2013)]. We believe that this work contained errors in the calculation of the detachment amplitude and photoelectron spectra. We describe the necessary corrections to the theory and show that the results, in particular, the interference features of the photoelectron spectra, appear noticeably different.

Single-step sub-200 fs mid-infrared generation from an optical parametric oscillator synchronously pumped by an erbium fiber laser.

We demonstrate the single-step generation of mid-infrared femtosecond laser pulses in a AgGaSe₂ optical parametric oscillator that is synchronously pumped by a 100MHz repetition rate sub-90fs erbium fiber laser. The tuning range of the idler beam in principle covers ∼3.5 to 17μm, only dependent on the choice of cavity and mirror design. As an example, we experimentally demonstrate idler pulse generation from 4.8 to 6.0μm optimized for selective vibrational resonant molecular spectroscopy. We find an oscillation threshold as low as 150mW of pump power. At 300mW pump power and a central wavelength of ∼5.0 μm, we achieve an average infrared power of up to 17.5mW, with a photon conversion efficiency of ∼18%. A pulse duration of ∼180 fs is determined from a nonlinear cross-correlation with residual pump light. The single-step nonlinear conversion leads to a high power stability with <1% average power drift at <0.5% rms noise over 1h.

All-Optical Reconstruction of Crystal Band Structure.

The band structure of matter determines its properties. In solids, it is typically mapped with angle-resolved photoemission spectroscopy, in which the momentum and the energy of incoherent electrons are independently measured. Sometimes, however, photoelectrons are difficult or impossible to detect. Here we demonstrate an all-optical technique to reconstruct momentum-dependent band gaps by exploiting the coherent motion of electron-hole pairs driven by intense midinfrared femtosecond laser pulses. Applying the method to experimental data for a semiconductor ZnO crystal, we identify the split-off valence band as making the greatest contribution to tunneling to the conduction band. Our new band structure measurement technique is intrinsically bulk sensitive, does not require a vacuum, and has high temporal resolution, making it suitable to study reactions at ambient conditions, matter under extreme pressures, and ultrafast transient modifications to band structures.

Super high power mid-infrared femtosecond light bullet

Mid-infrared ultrashort high energy laser sources are opening up new opportunities in science, including keV-class high harmonic generation and monoenergetic MeV-class proton acceleration. As new higher energy sources become available, potential applications for atmospheric propagation can dramatically grow to include stand-off detection, laser communications, shock-driven remote terahertz enhancement and extended long-lived thermal waveguides to transport high power microwave and radiofrequency waves. We reveal a new paradigm for long-range, low-loss, ultrahigh power ultrashort pulse propagation at mid-infrared wavelengths in the atmosphere. Before the onset of critical self-focusing, energy in the fundamental wave continually leaks into shock-driven spectrally broadened higher harmonics. A persistent near-invariant solitonic leading edge on the multi-terawatt pulse waveform transports most of the power over hundred-metre-long distances. Such light bullets are resistant to uncontrolled multiple filamentation and are expected to spark extensive research in optics, where the use of mid-infrared lasers is currently much under-utilized. A mechanism for the propagation of mid-infrared femtosecond laser pulses in air is theoretically investigated. A numerical simulation predicts that the propagation of multiple-terawatt pulses is possible over hundreds of metres.

Photodetachment of Si− by mid-infrared few-cycle femtosecond laser pulses

The Kelydsh model originally developed for infinitely long periodic laser pulses is extended to a spin polarized model to consider direct photodetachment of negative ions with half-filled np3 valence shells by few-cycle laser pulses without taking into account rescattering effects. The theory is applied to study above threshold detachment of Si− negative ions by intense short infrared pulses but is expected to be inherent of any half-filled p subshell negative ion. Photoelectron momentum maps of the direct electrons of Si− are presented. These are found to exhibit a distinctive threshold structure of concentric elliptical rings where the separation of these rings is dependent on the quantized frequency components of the few-cycle laser pulse. Photoelectron angular distributions (PADs) predicted by short duration laser pulses are calculated and threshold effects associated with channel closings are observed as the laser-field frequency and intensity pass through critically induced ponderomotive potential channel closures. Enhanced structures of the PADs in the vicinity near threshold show that the detachment process does not follow the Wigner law. This is a because the photon energy is not conserved in a few-cycle pulse in contrast to a long periodic pulse. In the energy spectra interference effects are observable as multiphoton peaked structures whose positions are dependent on the ponderomotive threshold shifts determined by the nature of the time-dependent vector potential. Additionally we show that carrier envelope phase effects manipulate all emission spectra considered.