Ultrashort Ultraviolet Pulses Research Articles

Inline UV pulse synthesizer

We demonstrated an inline synthesizer for generating ultrashort pulses in the ultraviolet (UV) range. The inline UV pulse synthesizer comprised three nonlinear crystals located in the propagation path of the fundamental driving laser pulse. Second-harmonic signals with central wavelengths of 420, 375, and 345 nm were generated in turn in the three BBO crystals, resulting in a synthesized UV pulse subsequent to the final nonlinear crystal. Its temporal amplitude and phase could be manipulated easily by changing the relative positions of the crystals, allowing for flexibility of the waveform. The minimum pulse duration of the synthesized UV pulse was 4.7 fs, which was close to the Fourier-transform-limited pulse duration. This ultrashort UV pulse with 19 μ\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\upmu$$\\end{document}J energy can be utilized in various applications such as high harmonic generation and frustrated tunneling ionization.

UV 30 fs laser pulse generation using a multi-pass cell.

Ultrashort ultraviolet (UV) pulses are pivotal for resolving ultrafast electron dynamics. However, their efficient generation is strongly impeded by material dispersion and two-photon absorption, in particular, if pulse durations around a few tens of femtoseconds or below are targeted. Here, we present a new (to our knowledge) approach to ultrashort UV pulse generation: using the fourth-harmonic generation output of a commercial ytterbium laser system delivering 220 fs UV pulses, we implement a multi-pass cell (MPC) providing 5.6 µJ pulses at 256 nm, compressed to 30.5 fs. Our results set a short-wavelength record for MPC post-compression while offering attractive options to navigate the trade-off between upconversion efficiency and acceptance bandwidth for UV pulse production.

High-Throughput Screening for Ultrafast Photochemical Reaction Discovery.

High-repetition-rate lasers present an opportunity to extend ultrafast spectroscopy from a detailed probe of singular model photochemical systems to a routine analysis technique in training machine learning models to aid the design cycle of photochemical syntheses. We bring together innovations in line scan cameras and micro-electro-mechanical grating modulators with sample delivery via high-pressure liquid chromatography pumps to demonstrate a transient absorption spectrometer that can characterize photoreactions initiated with ultrashort ultraviolet pulses in a time scale of minutes. Furthermore, we demonstrate that the ability to rapidly screen an important class of photochemical system, pyrimidine nucleosides, can be used to explore the effect of conformational modification on the evolution of excited-state processes.

Broadband Photoconductive Sampling in Gallium Phosphide (Advanced Optical Materials 9/2023)

Photoconductive sampling of optical light fields in gallium phosphide is performed by Nicholas Karpowicz, Matthias F. Kling, and co-workers (article number 2202994). Ultrashort ultraviolet pulses (blue line) generate electrons (blue cloud) and holes (red cloud) that are accelerated towards electrodes with the optical field (red line). The measured current in the material enables sampling of the waveform of the optical field.

Laser interference ablation by ultrashort UV laser pulses via diffractive beam management

Abstract The fabrication of periodic surface patterns on various materials by ultrashort ultraviolet (UV) laser pulses is reviewed. Laser interference ablation using two or more coherent beams leads to deterministic, strictly periodic patterns. The generation of the interfering beams is accomplished by diffractive optical elements like gratings, grating systems or computer-generated holograms. The recombination of the diffracted beams is performed by optical imaging or diffractive beam management. Ultrashort UV pulses are especially suited for generating micron- to submicron-sized deterministic periodic patterns on metals and semiconductors.

Ultraviolet picosecond conversion efficiency improvement system at 355 nm based on fundamental frequency laser amplified

In recent years, picosecond laser in ultraviolet (UV) has manifested great importance for applications both in science and industry, such as biomedical research, micro machining, etc. Now, the well proven approach to generating ultra-short UV pulses is extra-cavity frequency conversion based on nonlinear optical (NLO) crystal, due to the lack of suitable laser sources directly generating UV laser. In this process of harmonic generation, the length of nonlinear crystal is an important factor affecting the conversion efficiency and beam-quality. The optimal length of the nonlinear crystal is influenced by incident laser parameters and crystal absorption coefficient. At present, for the UV 355 nm picosecond laser generated from extra-cavity sum frequency, published are few reports about detailed analysis and research on the influence of photon ratio of the incident laser beams and nonlinear crystal absorption on optimal length of sum frequency crystal. In this paper, the steady-state solutions with the highest conversion efficiency under different incident conditions are obtained by theoretical analysis and numerical simulation of the three waves coupling equations. The effects of different photon ratios and absorption effect of the sum frequency crystal on the optimum crystal length are analyzed. We propose a solution based on the fundamental frequency laser amplified to shorten crystal length and improve conversion efficiency. In this scheme, the 532 nm second harmonic laser with a high conversion efficiency over 65% can be achieved by LiB<sub>3</sub>O<sub>5</sub> crystal. After that, the 1064 nm fundamental frequency laser is separated from the second harmonic laser, and then it is amplified by the Nd:YVO<sub>4</sub> laser crystal pumped by an 808 nm laser diode. Finally, the ultraviolet 355 nm picosecond laser is obtained by combining the 1064 nm fundamental frequency laser with the 532 nm second harmonic laser in the LiB<sub>3</sub>O<sub>5</sub> crystal. The simulation results show that the incident photon ratio of the sum frequency reaction can be changed by amplifying the residual fundamental frequency laser, and the optimum length of the sum-frequency crystal corresponding to the highest conversion efficiency can be shortened. Meanwhile, the absorption and walk-away effect of the sum frequency crystal can be also reduced. The final 355 nm laser output power can be increased more than 40 percent compared with the traditional scheme of early reports. In consequence, the high sum frequency conversion efficiency of the UV 355 nm picosecond laser can be obtained by changing the photo ratio of the incident laser beams through amplifying the fundamental frequency laser.

Ultraviolet Transient Absorption Spectrometer with Sub-20-fs Time Resolution

We describe a transient absorption (TA) spectroscopy system in the ultraviolet (UV) spectral range, for the study of the ultrafast optical response of biomolecules. After reviewing the techniques for the generation and characterization of ultrashort UV pulses, we describe the experimental setup of our ultrabroadband UV TA spectrometer. The setup combines sub-20-fs UV pump pulses tunable between 3.35 and 4.7 eV, with broadband white-light-continuum probe pulses in the 1.7–4.6 eV range. Thanks to the broad tunability of the pump pulses in the UV spectral range, the extremely high temporal resolution and the broad spectral coverage of the probe, this TA system is a powerful and versatile tool for the study of many biomolecules. As an example of its potential, we apply the TA spectrometer to track ultrafast internal conversion processes in pyrene after excitation in the UV, and to resolve an impulsively excited molecular vibration with 85-fs period.

Generation of microjoule pulses in the deep ultraviolet at megahertz repetition rates

Although ultraviolet (UV) light is important in many areas of science and technology, there are very few if any lasers capable of delivering wavelength-tunable ultrashort UV pulses at MHz repetition rates. Here we report the generation of deep-UV laser pulses at MHz repetition rates and \mu J-energies by means of dispersive wave (DW) emission from self-compressed solitons in gas-filled single-ring hollow-core photonic crystal fiber (SR-PCF). Pulses from an ytterbium fiber laser (~300 fs) are first compressed to ~25 fs in a SR-PCF-based nonlinear compression stage, and subsequently used to pump a second SR-PCF stage for broadband DW generation in the deep UV. The UV wavelength is tunable by selecting the gas species and the pressure. At 100 kHz repetition rate, a pulse energy of 1.05 \mu J was obtained at 205 nm (average power 0.1 W), and at 1.92 MHz, a pulse energy of 0.54 \mu J was obtained at 275 nm (average power 1.03 W).

Multifunctional optical correlator for picosecond ultraviolet laser pulse measurement.

A compact multifunctional optical correlator system for pulse width measurement of ultrashort ultraviolet (UV) pulses has been designed and experimentally demonstrated. Both autocorrelation and cross-correlation functions are measured using a single nonlinear crystal, and the switching between two measurements requires no adjustment of phase matching and detector. The system can measure UV pulse widths from sub-picoseconds to 100ps, and it involves no auxiliary pulse in the measurement. The measurement results on a burst-mode picosecond UV laser show a high-quality performance on speed, accuracy, resolution, and dynamic range. The proposed correlator can be applied to measure any ultrashort UV pulses produced through sum-frequency generation or second-harmonic generation.

Harmonic Extension and Enhancement Using a Two-Color Chirped Pulse and an Ultrashort Ultraviolet Pulse

ABSTRACT A promising method to both extend the harmonic energy and enhance the harmonic intensity is presented when a He atom is exposed to the combination of a two-color chirped pulse and an ultrashort ultraviolet pulse. It is found that: (1) with the introduction of the two chirps, the harmonic energy has been remarkably extended; (2) by properly adding an ultrashort ultraviolet pulse to this synthesized two-color chirped pulse, the harmonic yield is enhanced by 3 orders of magnitude compared with the two-color chirped case; (3) the harmonic spectrum higher than the 96th order shows an ultrabroad supercontinuum with a 395 eV bandwidth, and the proper superposition over the harmonics directly produced a series of intense 40 as pulses which is 3 orders of magnitude higher than that in the two-color chirped case.

Molecular alignment induced ultraviolet femtosecond pulse modulation

Ultrashort ultraviolet pulses at 267 nm were generated through four-wave mixing processes in dual-color femtosecond filaments. The generated ultrashort ultraviolet pulses experienced intensity modulation due to molecular-alignment-induced spatial (de)focusing effects, and the output beam profiles were shown to vary observably at different molecular alignment revivals, facilitating all-optical field-free and ultrafast spatial shaping and profile optimization of the ultraviolet pulses.

Ultrafast Evolution of the Excited-State Potential Energy Surface ofTiO2Single Crystals Induced by Carrier Cooling

We investigate the influence of carrier cooling dynamics in TiO(2) on the excited-state potential energy surface along the A(1g) optical phonon coordinate after above band-gap excitation using ultrashort ultraviolet pulses. The large amplitude coherent oscillation observed in a pump-probe transient reflectivity measurement shows a phase shift of -0.2π with respect to a purely instantaneous displacive excitation. The dynamic evolution of the potential energy surface minimum of the coherent phonon coordinate is explored using accurate density functional theory calculations, which confirm a shift of the potential energy surface minimum upon resonant laser excitation and reveal a significant positive contribution to the displacive force due to the cooling of the excited hot electron-hole plasma. We show that this noninstantaneous effect can quantitatively explain the experimentally observed phase using reasonable assumptions for the parameters characterizing the excited carriers. Our work demonstrates that the fast equilibration dynamics of laser-excited nonequilibrium carrier populations can have a pronounced effect on the initial structural response of crystalline solids.

Spectral phase transfer to ultrashort UV pulses through four-wave mixing

Transfer of spectral phase from near infrared ultrashort pulses to deep ultraviolet (UV) sub-30-fs pulses through four-wave mixing process is demonstrated. Micro joule UV pulses at 237 nm were generated by nonlinear mixing of second harmonic pulses of Ti:sapphire laser output and near infrared pulses from a noncollinear optical parametric amplifier. Chirp of the near infrared pulse was transferred to the UV pulse with the opposite sign. A positively chirped near infrared pulse was used for generating a negatively chirped UV pulse, which was compressed down to 25 fs by a magnesium fluoride window.

Spectrum broadening of ultrashort ultraviolet pulse in dual-color laser field

When collinear dual-color intense laser pulses are overlapped in time, a strong coupling interaction occurs between their plasma filaments. Due to the cross phase modulation, strong non-linear effects are generated and the spectrum width of the ultrafast ultraviolet (UV) pulse is further broadened. The original UV pulse with a bandwidth of 15 nm and energy of 045 mJ is obtained by tripling the frequency of a Ti:sapphire laser system. The UV pulse and the near inferred pulse of 71 mJ can induce plasma filaments separately after focusing within an argon gas cell, leading to an obvious modulation of the UV spectrum. The full width at half maximum of UV spectrum increases to 64 nm which is 4 times the width of spectrum before focusing and 25 times the width of single ultraviolet filament broadening. In this experiment, we mainly study the frequency spectrum evolution of dual-color co-filament in argon gas under the condition of different time delays, coupling locations and gas pressures. Optimizing these factors can yield a valid approach to achieving extremely ultrafast pulses in the range of ultraviolet.

Generation of phase-controlled ultraviolet pulses and characterization by a simple autocorrelator setup

A versatile femtosecond ultraviolet (UV) pulse generation, a phase modulation, and a characterization setup for coherent control applications are demonstrated. For high-performance phase control of ultrashort pulses direct in the UV a microelectromechanical-system-based 2D mirror array is applied. Multiple examples for successful phase control of ultrashort UV pulses are given, such as arbitrarily phase tailoring and pulse recompression in open and closed loop schemes. For simple and effective characterization of the generated pulses, a UV autocorrelator based on two-photon absorption in a solar blind photomultiplier is constructed. The effects of space-time coupling on split mirror autocorrelation measurements are addressed and minimized.

Spectral and temporal analysis of ultrashort ultraviolet pulses generated by high-intensity laser radiation in the atmosphere

We report direct spectral and temporal characterization of ultrashort ultraviolet (UV) pulses resulting from third-harmonic generation by high-intensity Ti: sapphire laser radiation in the atmosphere. The experimental technique implemented in this work enables the measurement of the pulse width and the chirp of the UV field, as well as the electron density of the plasma produced by laser pulses. The bandwidth of the third harmonic generated in our experiments by laser pulses with an initial pulse width of 45 fs supports transform-limited UV pulses as short as 30 fs.

Collinear Generation of Ultrashort UV and XUV Pulses for Pump/probe Spectroscopy

AbstractThe collinear generation of sub-4 fs ultraviolet (UV) and attosecond extreme ultraviolet (XUV) pulses via subsequent third-harmonic and high harmonic generation in noble gases is demonstrated. The ultrashort coherent light bursts are produced by focusing a sub-1.5 cycle near-infrared/visible (NIR) laser pulse in two subsequent quasi-static noble gas targets. With this simple approach, inherently synchronized UV pulsed radiation with a photon energy of ˜5 eV and a pulse energy of ˜1 μJ, and XUV pulses with a cut-off photon energy of more than 120 eV and up to ˜107 XUV photons can be generated. This source represents a novel tool for future UV pump/XUV probe experiments with unprecedented time-resolution.

Generation of intense 11-fs ultraviolet pulses using phase modulation by two types of coherent molecular motions

The use of two types of phase modulations arising from the coherent rotations of ortho-hydrogen and para-hydrogen to generate an intense ultrashort ultraviolet pulse without substantial generation of sub-pulses was demonstrated. This technique allows use of a high-energy long-probe pulse in the pump-probe regime for generating a high-energy compressed pulse. A 100-fs ultraviolet pulse was compressed to 11-fs by the phase modulation followed by dispersion compensation with chirped mirrors.

Cell Design for Picosecond Time-Resolved Infrared Spectroscopy in High-Pressure Liquids and Supercritical Fluids

The design of a new high-pressure infrared (IR) cell for carrying out picosecond time-resolved infrared (ps-TRIR) spectroscopy in supercritical fluids is described. We have employed thin (2 mm) MgF(2) windows in order to overcome possible undesirable nonlinear optical effects caused by the extremely high peak powers of ultrashort ultraviolet (UV)/visible pulses. The design of our cell allows for the study of systems at pressures of up to 5500 psi at temperatures of up to approximately 50 degrees C. The MgF(2) windows enable the excitation of samples with both UV and visible light pulses and these windows are transparent across much of the mid-infrared region. We have demonstrated the use of this cell by examining the photochemistry of Fe(CO)(5) in supercritical Kr (sc Kr).

19 fs shaped ultraviolet pulses

We report the generation of shaped tunable ultrashort ultraviolet pulses with full control over the spectral phase and amplitude. The output of a noncollinearly phase-matched optical parametric amplifier is shaped in phase and amplitude by a liquid-crystal spatial light modulator. The resulting structured visible pulses are transferred into the ultraviolet by sum-frequency mixing with strongly chirped 775 nm pulses. Single, double, and triple pulses at 344 nm with subpulses as short as 19 fs are explicitly demonstrated. The method can easily be adapted to arbitrarily shaped pulses throughout the 295-370 nm range.