Deep-ultraviolet Pulses Research Articles

Generation of sub-10-fs deep and extreme ultraviolet pulses for time-resolved photoemission spectroscopy.

We present a light source capable of generating sub-10-fs deep UV (DUV) and extreme UV (EUV) pulses for use in time-resolved photoemission spectroscopy. The fundamental output of a Ti:sapphire laser was compressed using the multi-plate method and mixed with the uncompressed second harmonic in a filamentation four-wave mixing process to generate sub-10-fs DUV pulses. Sub-10-fs EUV pulses were generated via high-order harmonic generation driven by the second harmonic pulses that were compressed using Ar gas and chirped mirrors. The minimum cross correlation time between 267 and 57 nm (corresponding to 21.7 eV) was measured to be 10.6 ± 0.4 fs.

Ultra-low threshold deep ultraviolet generation in a hollow-core fiber.

Tunable ultrashort pulses in the ultraviolet spectral region are in great demand for a wide range of applications, including spectroscopy and pump-probe experiments. While laser sources capable of producing such pulses exist, they are typically very complex. Notably, resonant dispersive-wave (RDW) emission has emerged as a simple technique for generating such pulses. However, the required pulse energy used to drive the RDW emission, so far, is mostly at the microjoule level, requiring complicated and expensive pump sources. Here, we present our work on lowering the pump energy threshold for generating tuneable deep ultraviolet pulses to the level of tens of nanojoules. We fabricated a record small-core antiresonant fiber with a hollow-core diameter of just 6 μm. When filled with argon, the small mode area enables higher-order soliton propagation and deep ultraviolet (220 to 270 nm) RDW emission from 36 fs pump pulses at 515 nm with the lowest pump energy reported to date (tens of nanojoules). This approach will allow the use of low-cost and compact laser oscillators to drive nonlinear optics in gas-filled fibers for the first time to our knowledge.

Generation of high-energy, sub-20 fs deep-UV pulses in a twin-crystal third harmonic generation scheme.

Ultrashort deep ultraviolet (DUV) pulses serve as indispensable tools for investigating molecular dynamics on the femtosecond scale. Nonlinear frequency upconversion of near-infrared (NIR) light sources in a sequence of nonlinear crystals is a common method for their generation. However, preserving the temporal duration of the starting source encounters challenges owing to phase-matching bandwidth limitations within the harmonic generation process. Here we propose an approach for circumventing this limitation and demonstrate it for the case of generation of the third harmonic of 800 nm pulses in a two-stage scheme (second harmonic generation succeeded by sum-frequency mixing of the fundamental and second harmonic pulses). Expanding the bandwidth of the DUV pulse involves the utilization for the last mixing process of two nonlinear crystals, detuned to convert opposite sides of the spectrum. The implementation of this approach yields 20 µJ, 263 nm DUV pulses as short as 19 fs after compression. The setup is very compact and extremely stable due to the common-path scheme, which makes it very interesting for a variety of advanced ultrafast spectroscopy applications.

Efficient Composite Colorization of Copper by Spatially Controlled Oxidation with Deep‐UV Ultrafast Lasers

AbstractColorizing metals using micrometer and nanometer scale surface modifications has been vastly investigated and presents many advantages for applications across scientific and technological fields. By tuning the surface chemical composition or controlling its morphology, it is possible to produce a wide range of chromatic effects. Ultrafast laser processing presents here an interesting asset, as it allows to simultaneously provide chemical and morphological modifications at the micro‐scale in a single step. In this article, the composite colorization of copper surfaces with mW‐class average power deep ultraviolet (DUV) femtosecond laser pulses is demonstrated. The advantages of this setup are twofold: first, thanks to the increased absorption of copper in the DUV, the technique allows scaling down the requirement for laser power. Second, under ultrafast short‐wavelength illumination molecular oxygen bond‐breaks occur, enhancing the oxidation rate of the copper. The technique allows for highly controllable and efficient copper oxidation with the irradiation parameters. Taking these two effects into account, the generation of a wide spectrum of colors—from dark blue to shiny red—is demonstrated, and the role of the surface oxidation rate, the laser fluence, and laser scanning strategies in the colorization of copper surfaces employing DUV lasers is discussed.

Efficient and compact source of tuneable ultrafast deep ultraviolet laser pulses at 50 kHz repetition rate.

Deep ultraviolet (DUV) laser pulses with tuneable wavelength and very short duration are a key enabling technology for next-generation technology and ultrafast science. Their generation has been the subject of extensive experimental effort, but no technique demonstrated thus far has been able to meet all requirements in one light source. Here we demonstrate a bright, efficient, and compact source of tuneable DUV ultrafast laser pulses based on resonant dispersive wave emission in hollow capillary fiber. In a total footprint of only 120cm×75cm, including the ytterbium-based drive laser, we generate pulses between 208nm and 363nm at 50kHz repetition rate with a total efficiency of up to 3.6%. Down-scaling of the DUV generation reduces the required energy sufficiently to enable the generation of two-color few-femtosecond DUV pulses.

A novel common-path scheme for fourth harmonic generation by ultrashort laser pulses

A new compact common-path scheme for Fourth-Harmonic Generation (FHG) of femtosecond laser pulses is proposed here. Guidelines for selection of non-linear crystals and birefringent crystals used for delay pre-compensation are derived based on approximation of non-saturated sum-frequency mixing of Gaussian pulses. We experimentally demonstrate the scheme and study its performance for a different combinations of BBO nonlinear crystals for the case of generation of sub-200 nm deep ultraviolet pulses by FHG of pulses delivered by a Ti:Sapphire ultrafast laser. Pulses with duration between 130 fs and 370 fs and pulse energy of 19 to 85 μJ were generated. It is shown, that in addition to its compactness and intrinsic stability, the scheme allows a superior spectrum and pulse quality.

Generation of 12 W 257 nm laser pulses by sum-frequency generation based on LBO crystals

We have generated high-power deep ultraviolet laser pulses from a Yb-doped rod-type fiber laser through sum-frequency generation (SFG) based on lithium triborate (LBO) crystals. The 1030 nm nanosecond laser pulses from the fiber laser are frequency-tripled to 343 nm pulses with two LBO crystals, and the residual 1030 nm fundamental laser pulses are mixed with the 343 nm pulses in an LBO crystal for the generation of 257 nm pulses. The maximum 257 nm radiation power is 12 W with a repetition rate of 500 kHz, and the conversion efficiency from 1030 nm to 257 nm is 12%. It is observed that the power of 257 nm radiation is limited by the temperature increase in the LBO crystal used for the SFG.

Generation and compression of 10-fs deep ultraviolet pulses at high repetition rate using standard optics: erratum.

We present an erratum regarding the calculated phase matching bandwidths for achromatic second harmonic generation presented in our paper [Opt. Express29, 25593 (2021)10.1364/OE.425053].

Pathways towards break even for low convergence ratio direct-drive inertial confinement fusion

Following indirect-drive experiments which demonstrated promising performance for low convergence ratios (below 17), previous direct-drive simulations identified a fusion-relevant regime which is expected to be robust to hydrodynamic instability growth. This paper expands these results with simulated implosions at lower energies of 100 and 270 kJ, and ‘hydrodynamic equivalent’ capsules which demonstrate comparable convergence ratio, implosion velocity and in-flight aspect ratio without the need for cryogenic cooling, which would allow the assumptions of one-dimensional-like performance to be tested on current facilities. A range of techniques to improve performance within this regime are then investigated, including the use of two-colour and deep ultraviolet laser pulses. Finally, further simulations demonstrate that the deposition of electron energy into the hotspot of a low convergence ratio implosion through auxiliary heating also leads to significant increases in yield. Results include break even for 1.1 MJ of total energy input (including an estimated 370 kJ of short-pulse laser energy to produce electron beams for the auxiliary heating), but are found to be highly dependent upon the efficiency with which electron beams can be created and transported to the hotspot to drive the heating mechanism.

Sum-frequency generation of 133 mJ, 270 ps laser pulses at 266 nm in LBO crystals.

We demonstrate the generation of high-energy (133 mJ) and sub-nanosecond (∼270 ps) deep ultraviolet (DUV) pulses at 266 nm by sum-frequency mixing in LiB3O5 (LBO) crystals. The highest 133 mJ pulse energy ever reported corresponds to a peak power of 0.49 GW and an energy conversion efficiency of 13.3% from the infrared at 1064 nm to DUV at 266 nm. This is the highest output energy ever reported for the DUV sub-nanosecond pulses to the best of our knowledge. Higher energy efficiency of 25.7% can be achieved from 1064 nm to 266 nm when the fundamental energy was reduced to 346 mJ. Furthermore, the DUV generations using LBO and typical β-BaB2O4 (BBO) crystals were compared regarding the energy efficiency, and the effects of the nonlinear absorption are discussed.

Deep- to near-ultraviolet Raman frequency conversion pumped by femtosecond pulses in a hollow-core waveguide.

Broadband vibrational/rotational Raman generation ranging from deep ultraviolet (DUV) to blue wavelengths is demonstrated by using molecular hydrogen in a hollow-core waveguide as a Raman-active medium pumped by a femtosecond DUV laser. We find the high-order transient stimulated Raman scattering is drastically enhanced for input beams including a circularly polarized component; a circularly polarized input beam achieves the highest conversion efficiency. Coherent vibrational anti-Stokes Raman emission is observed only for a circularly polarized pump beam, indicating that the waveguide effect also contributes to the upconversion of a DUV pulse via transient stimulated Raman scattering.

Generation and compression of 10-fs deep ultraviolet pulses at high repetition rate using standard optics.

The generation and characterization of ultrashort laser pulses in the deep ultraviolet spectral region is challenging, especially at high pulse repetition rates and low pulse energies. Here, we combine achromatic second harmonic generation and adaptive pulse compression for the efficient generation of sub-10 fs deep ultraviolet laser pulses at a laser repetition rate of 200 kHz. Furthermore, we simplify the pulse compression scheme and reach pulse durations of ≈10 fs without the use of adaptive optics. We demonstrate straight-forward tuning from 250 to 320 nm, broad pulse spectra of up to 63 nm width, excellent stability and a high robustness against misalignment. These features make the approach appealing for numerous spectroscopy and imaging applications.

Characterization of vacuum and deep ultraviolet pulses via two-photon autocorrelation signals.

Characterization of ultrashort vacuum and deep ultraviolet pulses is important in view of applications of those pulses for spectroscopic and dynamical imaging of atoms, molecules, and materials. We present an extension of the autocorrelation technique, applied for measurement of the pulse duration via a single Gaussian function. Analytic solutions for two-photon ionization of atoms by Gaussian pulses are used along with an expansion of the pulse to be characterized using multiple Gaussians at multi-color central frequencies. This approach allows one to use two-photon autocorrelation signals to characterize isolated ultrashort pulses and pulse trains, i.e., the time-dependent amplitude and phase variation of the electric field. The potential of the method is demonstrated using vacuum and deep ultraviolet pulses and pulse trains obtained from numerical simulations of macroscopic high harmonic spectra.

Advanced time-resolved absorption spectroscopy with an ultrashort visible/near IR laser and a multi-channel lock-in detector

Ultrashort visible-near infrared (NIR) pulse generation and its applications to ultrafast spectroscopy are discussed. Femtosecond pulses of around 800 nm from a Ti:sapphire laser are used as a pump of an optical parametric amplifier (OPA) in a non-collinear configuration to generate ultrashort visible (500–780 nm) pulses and deep-ultraviolet (DUV, 259–282 nm) pulses. The visible-NIR pulses and DUV pulses were compressed to 3.9 fs and 10.4 fs, respectively, and used to elucidate various ultrafast dynamics in condensed matter with a sub-10 fs resolution by pump-probe measurements. We have also developed a 128-channel lock-in amplifier. The combined system of the world-shortest visible pulse from the OPA and the lock-in amplifier with the world-largest channel-number can clarify the sub-10 fs-dynamics in condensed matter. This system clarified structural changes in an excited state, reaction intermediate, and a transition state. This is possible even during molecular vibration and reactions via a real-time-resolved vibronic spectrum, which provides molecular structural change information. Also, ultrafast dynamics in exotic materials like carbon nanotubes, topological insulators, and novel solar battery systems have been clarified. Furthermore, the carrier-envelope phase in the ultrashort pulse has been controlled and measured.

Low-energy-threshold deep-ultraviolet generation in a small-mode-area hollow-core fiber

We demonstrate the generation of wavelength-tunable deep-ultraviolet pulses in a small-mode-area hollow-core fiber fabricated by tapering a nodeless tubular-type hollow-core fiber. Down-scaling of the cross-sectional geometry reduces the pump energy requirement for inducing sufficient nonlinear effects, presenting a unique opportunity for staging low-energy-threshold gas-based nonlinear optics. We report the onset of the ultraviolet light with the pump pulse energy as low as 125 nJ. Our numerical analysis shows that the frequency conversion arises due to soliton phase matching, and therefore shot-to-shot coherence of the ultraviolet emission is well-preserved. It offers a promising platform for a compact ultraviolet frequency comb source.

Development of a deep-ultraviolet pulse laser source operating at 234 nm for direct cooling of Al+ ion clocks.

We report on the development of a 250-MHz 234 nm deep-ultraviolet pulse source based on a flexible wavelength-conversion scheme. The scheme is based on a frequency-doubled optical parametric oscillator (FD-OPO) together with a cascaded frequency conversion process. We use a χ(2) nonlinear envelope equation to guide the design of an intra-cavity OPO crystal, demonstrating a flexible broadband tunable feature and providing as high as watt-level of a frequency-doubled signal output centered at 850 nm, which is served as an input wave for the cascaded frequency conversion process. As much as 3.0 mW of an average power at 234 nm is obtained, with an rms power stability of better than 1% over 20 minutes. This deep-ultraviolet pulse laser source can be used for many applications in quantum optics and for direct laser cooling of Al+ ion clocks.

Generation of broadband circularly polarized deep-ultraviolet pulses in hollow capillary fibers.

We demonstrate an efficient scheme for the generation of broadband, high-energy, circularly polarized femtosecond laser pulses in the deep ultraviolet through seeded degenerate four-wave mixing in stretched gas-filled hollow capillary fibers. Pumping and seeding with circularly polarized 35 fs pulses centered at 400 nm and 800 nm, respectively, we generate idler pulses centered at 266 nm with 27 µJ of energy and over 95% spectrally averaged ellipticity. Even higher idler energies and broad spectra (27 nm bandwidth) can be obtained at the cost of reduced ellipticity. Our system can be scaled in average power and used in different spectral regions, including the vacuum ultraviolet.

20 W, 2 mJ, sub-ps, 258 nm all-solid-state deep-ultraviolet laser with up to 3 GW peak power.

We demonstrate an all-solid-state deep-ultraviolet (DUV) laser based on the frequency-quadrupling of a 1 µm, 1.2 ps, Yb: YAG Innoslab solid-state laser at a 10 kHz repetition rate, using LBO and BBO as second-harmonic generation and fourth-harmonic generation crystals, respectively. The DUV laser delivers 20 W, 2.0 mJ, 665 fs, 258 nm DUV pulses, with an overall conversion efficiency of ∼8.7% from 1 µm to DUV. The corresponding peak power of DUV pulses is up to 3 GW, which, to the best of our knowledge, is highest in reported kHz-rate all-solid-state DUV sources driven at 1 µm wavelength.

High-power DUV picosecond pulse laser with a gain-switched-LD-seeded MOPA and large CLBO crystal.

We report the generation of a 266 nm deep ultraviolet (DUV) picosecond pulse with an average output power of 14 W by the fourth-harmonic generation (FHG) from two consecutive frequency-doubling stages of a 1064 nm pulse based on a gain-switched-laser-diode (LD)-seeded hybrid fiber/solid-state master oscillator and power amplifier (MOPA) system. Through the gain-switched operation of a narrow-spectral-linewidth distributed-feedback laser diode and by using a Yb-doped fiber and a two-stage ${\rm Nd}:{{\rm YVO}_4}$Nd:YVO4 solid-state amplifier, we achieved an average power of 46.5 W near the Fourier transform limit for a 13 ps pulse with a repetition rate of 200 kHz. The narrow linewidth pulse characteristics enabled highly efficient frequency conversion, and the efficiency of conversion from 532 to 266 nm was 54%, and from 1064 to 266 nm was 31%. The beam quality factor ${M^2}$M2 of the generated DUV pulse was below 1.2. The highly efficient FHG process resulted in appeasing thermal stress caused by nonlinear absorption in the crystal, and more than 5000 h of continuous operation were achieved without any power down or beam profile degradation.

Three-photon-excited laser-induced fluorescence detection of atomic hydrogen in flames.

In many recent studies, ultrashort femtosecond (fs) two-photon (2p) laser-induced fluorescence (LIF) of atomic hydrogen (H) has been demonstrated using a 205 nm excitation. However, 205-nm- deep ultraviolet (UV) pulses can be problematic in practical devices containing thick transmissive optics and can also be susceptible to photolytic production at high laser energies. In this Letter, we investigate the three-photon (3p) excitation scheme of H by using red-shifted 307.7 nm fs laser pulses. Efficient 3p excitation resulting from fs laser pulses enable the 3pLIF detection of H, which was previously unattainable in most flame conditions using ns or ps pulses. Measurements are reported in CH4/O2/N2 Bunsen jet flames and premixed CH4/air flames and compared to similar 2pLIF schemes with fs pulses. Saturation effects, photolytic interferences, and stimulated emissions effects are studied, as well as the benefits of 3pLIF in diagnostic hardware with thick optical windows.