Ultrashort Mid-infrared Laser Pulses Research Articles

Few-cycle laser pulse characterization on-target using high-harmonic generation from nano-scale solids.

We demonstrate high-harmonic generation for the time-domain observation of the electric field (HHG-TOE) and use it to measure the waveform of ultrashort mid-infrared (MIR) laser pulses interacting with ZnO thin-films or WS2 monolayers. The working principle relies on perturbing HHG in solids with a weak replica of the pump pulse. We measure the duration of few-cycle pulses at 3200 nm, in reasonable agreement with the results of established pulse characterization techniques. Our method provides a straightforward approach to accurately characterize femtosecond laser pulses used for HHG experiments right at the point of interaction.

Unraveling the ultrafast dynamics of thermal-energy chemical reactions.

In this perspective, we discuss how one can initiate, image, and disentangle the ultrafast elementary steps of thermal-energy chemical dynamics, building upon advances in technology and scientific insight. We propose that combinations of ultrashort mid-infrared laser pulses, controlled molecular species in the gas phase, and forefront imaging techniques allow to unravel the elementary steps of general-chemistry reaction processes in real time. We detail, for prototypical first reaction systems, experimental methods enabling these investigations, how to sufficiently prepare and promote gas-phase samples to thermal-energy reactive states with contemporary ultrashort mid-infrared laser systems, and how to image the initiated ultrafast chemical dynamics. The results of such experiments will clearly further our understanding of general-chemistry reaction dynamics.

Ultrafast Infrared Laser Crystallization of Amorphous Ge Films on Glass Substrates.

Amorphous germanium films on nonrefractory glass substrates were annealed by ultrashort near-infrared (1030 nm, 1.4 ps) and mid-infrared (1500 nm, 70 fs) laser pulses. Crystallization of germanium irradiated at a laser energy density (fluence) range from 25 to 400 mJ/cm2 under single-shot and multishot conditions was investigated using Raman spectroscopy. The dependence of the fraction of the crystalline phase on the fluence was obtained for picosecond and femtosecond laser annealing. The regimes of almost complete crystallization of germanium films over the entire thickness were obtained (from the analysis of Raman spectra with excitation of 785 nm laser). The possibility of scanning laser processing is shown, which can be used to create films of micro- and nanocrystalline germanium on flexible substrates.

Coherently enhanced microwave pulses from midinfrared-driven laser plasmas.

Ultrafast ionization of a gas medium driven by ultrashort midinfrared laser pulses provides a source of bright ultrabroadband radiation whose spectrum spans across the entire microwave band, reaching for the sub-gigahertz range. We combine multiple, mutually complementary detection techniques to provide an accurate polarization-resolved characterization of this broadband output as a function of the gas pressure. At low gas pressures, the lowest-frequency part of this output is found to exhibit a drastic enhancement as this field builds up its coherence, developing a well-resolved emission cone, dominated by a radial radiation energy flux. This behavior of the intensity, coherence, and polarization of the microwave output is shown to be consistent with Cherenkov-type radiation by ponderomotively driven plasma currents.

Chirp-controlled high-harmonic and attosecond-pulse generation via coherent-wake plasma emission driven by mid-infrared laser pulses.

Coherent-wake plasma emission induced by ultrashort mid-infrared laser pulses on a solid target is shown to give rise to high-brightness, high-order harmonic radiation, offering a promising source of attosecond pulses and a probe for ultrafast subrelativistic plasma dynamics. With 80-fs, 0.2-TW pulses of 3.9-μm radiation used as a driver, optical harmonics up to the 34th order are detected, with their spectra stretching from the mid-infrared region to the extreme ultraviolet region. The harmonic spectrum is found to be highly sensitive to the chirp of the driver. Particle-in-cell analysis of this effect suggests, in agreement with the generic scenario of coherent-wake emission, that optical harmonics are radiated as trains of extremely short, attosecond ultraviolet pulses with a pulse-to-pulse interval varying over the pulse train. A positive chirp of the driver pulse can partially compensate for this variation in the interpulse separation, allowing harmonics of the highest orders to be generated in the plasma emission spectrum.

Ultraviolet-to-millimeter-band supercontinua driven by ultrashort mid-infrared laser pulses

Combined optical nonlinearity of bound and free electrons in a fast-ionizing medium driven by ultrashort, mid-infrared (mid-IR) pulses gives rise to a vast variety of ultrafast nonlinear-optical scenarios, producing bright, broadband radiation in spectral ranges as different as ultraviolet (UV) and terahertz (THz). Given its enormous bandwidth, a quantitative experimental analysis of this type of nonlinear response is anything but simple. Here, we confront this challenge by ultrabroadband spectral measurements performed across the spectral range from the UV to the millimeter-wave (MMW) band jointly with beam profile analysis in the THz-to-MMW band and direct time-domain field waveform characterization. As one of the most striking results, the nonlinear response of a fast-ionizing gas driven by a two-color field, consisting of a high-peak-power sub-100-fs mid-IR pulse and its second harmonic, is shown to provide a source of a bright multiband supercontinuum (SC) radiation, whose spectrum spans over about 14 octaves, stretching from below 300 nm all the way beyond 4.3 mm. The MMW-to-THz part of this SC is emitted, as direct measurements show, in the form of half-cycle field waveforms that can be focused to yield a field strength of ≈ 5 M V / c m . At least 1.5% of the MMW–THz supercontinuum energy is emitted in the MMW range, giving rise to MMW field strengths up to 100 kV/cm in the beam waist region.

Accurate characterization of mid-infrared ultrashort pulse based on second-harmonic-generation frequency-resolved optical gating

We demonstrate a second-harmonic-generation frequency-resolved optical gating (SHG-FROG) apparatus, which can be used to accurately characterize ultrashort mid-infrared laser pulses. An initial guess with constraint both in time and frequency domain is first proposed in principal components generalized projections algorithm (PCGPA), and it outperforms other guesses for the data errors analysis in these SHG-FROG apparatus. A mid-infrared pulse at 3580 nm from our home-built optical parametric amplifier (OPA) system is measured with a good agreement between the retrieved and measured spectrum. Different initial guesses are studied and a further verification is made to compare the measured spectral phase difference with the calculated one by inserting a dispersion plate. The excellent phase agreement verifies the accuracy of the measurement and high reliability of the device.

Adaptive control of laser-wakefield accelerators driven by mid-IR laser pulses.

There has been growing interest both in studying high intensity ultrafast laser plasma interactions with adaptive control systems as well as using long wavelength driver beams. We demonstrate the coherent control of the dynamics of laser-wakefield acceleration driven by ultrashort (∼ 100 fs) mid-infrared (∼ 3.9 μm) laser pulses. The critical density at this wavelength is 7.3 × 1019 cm-3, which is achievable with an ordinary gas target system. Interactions between mid-infrared laser pulses and such near-critical-density plasma may be beneficial due to much higher absorption of laser energy. In addition, the normalized vector potential of the laser field a0 increases with longer laser wavelength, lowering the required peak laser intensity to drive non-linear laser-wakefield acceleration. Here, MeV level, collimated electron beams with non-thermal, peaked energy spectra are generated. Optimization of electron beam qualities are realized through adaptive control of the laser wavefront. A genetic algorithm controlling a deformable mirror improves the electron total charge, energy spectra, beam pointing and stability at various plasma density profiles. Particle-in-cell simulations reveal that the optimal wavefront causes an earlier injection on the density up-ramp and thus higher energy gain as well as less filamentation during the interaction, which leads to the improvement in electron beam collimation and energy spectra.

Laser wakefield acceleration with mid-IR laser pulses

We report on, to the best of our knowledge, the first results of laser plasma wakefield acceleration driven by ultrashort mid-infrared (IR) laser pulses (λ=3.9 μm, 100fs, 0.25TW), which enable near- and above-critical density interactions with moderate-density gas jets. Relativistic electron acceleration up to ∼12 MeV occurs when the jet width exceeds the threshold scale length for relativistic self-focusing. We present scaling trends in the accelerated beam profiles, charge, and spectra, which are supported by particle-in-cell simulations and time-resolved images of the interaction. For similarly scaled conditions, we observe significant increases in the accelerated charge, compared to previous experiments with near-infrared (λ=800 nm) pulses.

Mapping anomalous dispersion of air with ultrashort mid-infrared pulses

We present experimental studies of long-distance transmission of ultrashort mid-infrared laser pulses through atmospheric air, probing air dispersion in the 3.6–4.2-μm wavelength range. Atmospheric air is still highly transparent to electromagnetic radiation in this spectral region, making it interesting for long-distance signal transmission. However, unlike most of the high-transmission regions in gas media, the group-velocity dispersion, as we show in this work, is anomalous at these wavelengths due to the nearby asymmetric-stretch rovibrational band of atmospheric carbon dioxide. The spectrograms of ultrashort mid-infrared laser pulses transmitted over a distance of 60 m in our experiments provide a map of air dispersion in this wavelength range, revealing clear signatures of anomalous dispersion, with anomalous group delays as long as 1.8 ps detected across the bandwidth covered by 80-fs laser pulses.

Co2amp: a software program for modeling the dynamics of ultrashort pulses in optical systems with CO(2) amplifiers.

A computer code for simulating the amplification of ultrashort mid-infrared laser pulses in CO2 amplifiers and their propagation through arbitrary optical systems is described. The code is based on a comprehensive model that includes an accurate consideration of the CO2 active medium and a physical optics propagation algorithm, and takes into account the interaction of the laser pulse with the material of the optical elements. The application of the code for optimizing an isotopic regenerative amplifier is described.

A Reaction Accelerator: Mid-infrared Strong Field Dissociation Yields Mode-Selective Chemistry.

Mode-selective chemistry has been a dream of chemists since the advent of the laser in the 1970s. Despite intense effort, this goal has remained elusive due to efficient energy randomization in polyatomic molecules. Using ab initio molecular dynamics calculations, we show that the interaction of molecules with intense, ultrashort mid-infrared laser pulses can accelerate and promote reactions that are energetically and entropically disfavored, owing to efficient kinetic energy pumping into the corresponding vibrational mode(s) by the laser field. In a test case of formyl chloride ion photodissociation, the reactions are ultimately complete under field-free conditions within 500 fs after the laser pulse, which effectively overcomes competition from intramolecular vibrational energy redistribution (IVR). The approach is quite general and experimentally accessible using currently available technology.

Ultrabroadband, highly flexible amplifier for ultrashort midinfrared laser pulses based on aperiodically poled Mg:LiNbO_3

We present an amplification medium for optical parametric chirped-pulse amplification that allows for ultrabroadband gain in a collinear configuration. Our approach is based on aperiodic quasi-phase-matching (QPM). For the first demonstration of this method in a mid-IR optical parametric chirped-pulse amplifier, we chose a QPM grating design with a linear chirp of its associated spatial frequencies. The resulting 7.4-mm-long, aperiodically poled Mg:LiNbO(3) amplification crystal has a chirp rate of kappa'=-250 cm(-2) and provides gain over the 800 nm bandwidth centered at 3.4 microm. We were able to generate pulses as short as 75 fs and the pulse energy at the output of the optical parametric amplifier before compression was 1.5 microJ. Low thermal load on the amplification medium allows for operation at a high repetition rate, 100 kHz in our case, and high average power limited only by the available pump power.

Special issue “Advances in Chiroptical Methods”

Special issue “Advances in Chiroptical Methods”

Resonant two-photon photoemission in quantum-well infrared photodetectors

We report the nonlinear behavior of quantum-well infrared photodetectors with three energetically equidistant energy levels. The giant resonant nonlinearity leads to a quadratic power dependence of the photocurrent down to excitation power densities as low as 0.1W∕cm2. Using these highly sensitive two-photon detectors, second-order autocorrelation measurements of ultrashort midinfrared laser pulses in the pJ regime are demonstrated. The dynamical behavior is studied by a numerical analysis of these measurements. At high bias voltages we observe a dominating linear contribution to the photocurrent arising from tunneling processes.

Ultrafast infrared spectroscopy in biomolecules: Active site dynamics of heme proteins

Rapid advances in the generation of intense tunable ultrashort mid-infrared (IR) laser pulses allow the use of ultrafast IR pump-probe and vibrational echo experiments to investigate the dynamics of the fundamental vibrational transition of CO bound to the active site of heme proteins. The studies were performed using a free-electron laser (FEL) and an experimental set up at the Stanford University FEL Center. These novel techniques are discussed in some detail. Pump-probe experiments on myoglobin-CO (MbCO) measure CO vibrational relaxation (VR). The VR process involves loss of vibrational excitation from CO to the protein and solvent. Infrared vibrational echoes measure CO vibrational dephasing. The quantum mechanical treatment of the force-correlation function description of vibrational dynamics in condensed phases is described briefly. A quantum mechanical treatment is needed to explain the temperature dependence of VR in Mb-CO from 10 to 300 K. A molecular-level description including elements of heme protein structure in the treatment of vibrational dynamics is also discussed. Vibrational relaxation of CO in Mb occurs on the 10−11-s time scale. VR was studied in proteins with single-site mutations, proteins from different species, and model heme compounds. A roughly linear relationship between carbonyl stretching frequency and VR rate has been observed. The dominant VR pathway is shown to involve anharmonic coupling from CO through the π-bonded network of the porphyrin, to porphyrin vibrations with frequencies > 400 cm−1. The heme protein influences VR of bound ligands at the active site primarily via altering the through π-bond coupling between CO and heme. Preliminary vibrational echo studies of the effects of protein conformational relaxation dynamics on ligand dephasing are also reported. © 1996 John Wiley & Sons, Inc.

Direct autocorrelation measurements of mid-infrared picosecond pulses by quantum-well devices

We report the direct autocorrelation of ultrashort mid-infrared laser pulses, using an unbiased GaAsy/GaAlAs quantum-well device as a nonlinear photovoltaic medium. Using this method, we autocorrelate ultrashort (3-ps) low-energy (~500-nJ) pulses of 10.6-microm light. This approach should permit the autocorrelation of subpicosecond infrared pulses.