Fourth Harmonic Generation Research Articles

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.

Designing Strong Polarity and High Configurational Entropy Flexible Units toward Excellent Ultraviolet Nonlinear Optical Materials

AbstractPolar materials play a crucial role in numerous essential fields; however, efficiently synthesizing them remains a significant challenge. In this study, a viable approach is proposed to enhance the probability of discovering polar materials by developing new functional basic units (FBUs) with strong polarity and high configurational entropy. To validate this approach, a site‐modification strategy is applied to the high configurational entropy flexible (C3H2O4)2− FBU, resulting in the development of four new polar‐enhancing FBUs: (C3(CH3)2O4)2−, (C3F2O4)2−, (C3H(OH)O4)2−, and (C3HFO4)2−. Moreover, 11 new compounds through temperature‐driven conformational changes in FBUs are successfully synthesized. Among these, the proportion of polar structures reaches an impressive 54%. Remarkably, all of these novel polar compounds exhibit outstanding nonlinear optical (NLO) properties. The [Li2C3(CH3)2O4]2·3H2O demonstrates the rare coexistence of a moderate birefringence (0.071@514 nm), short UV cutoff edge (210 nm), and the strongest second harmonic generation (SHG) effect (6.5 × KDP) among ionic‐organic fourth harmonic generation crystals. Preliminary laser experiments have also proven its potential practical value as a fourth harmonic generation crystal. This research not only discovers a variety of exceptional UV NLO crystals but also provides a feasible method to increase the likelihood of finding polar materials.

Improving fourth harmonic generation performance by elevating the operation temperature of ADP crystal.

In current inertial confinement fusion (ICF) facilities, potassium dihydrogen phosphate (KH2PO4, KDP) type crystals are the only nonlinear optical (NLO) materials that can satisfy the aperture requirement of the ICF laser driver. Ammonium dihydrogen phosphate (NH4H2PO4, ADP) crystal is a typical isomer of KDP crystal, with a large nonlinear optical coefficient, high ultraviolet transmittance, and large growth sizes, which is an important deep ultraviolet (UV) NLO material. In this paper, we investigated the effect of ADP temperature on its fourth-harmonic-generation (FHG) performance. When the temperature of the ADP crystal was elevated to 48.9 °C, the 90° phase-matched FHG of the 1064 nm laser was realized. Compared with the 79° phase-matched FHG at room temperature (23.0 °C), the output energy at 266 nm, conversion efficiency, angular acceptance, and laser-induced damage threshold (LIDT) increased 113%, 71%, 623%, 19.6%, respectively. It shows that elevating ADP temperature is an efficient method to improve its deep UV frequency conversion properties, which may also be available to other NLO crystals. This discovery provides a very valuable technology for the future development of UV, deep UV lasers in ICF facilities.

High-efficiency fourth harmonic generation and polarization smoothing based on an orthogonal cascade of DKDP crystals: publisher's note.

This publisher's note corrects an error in Appl. Opt.63, 1411 (2024)APOPAI0003-693510.1364/AO.512229.

High-efficiency fourth harmonic generation and polarization smoothing based on an orthogonal cascade of DKDP crystals.

Because of the high efficiency of frequency conversion and beam-target coupling, a fourth harmonic (4ω) laser has a splendid application prospect in a high-power laser facility. The polarization smoothing (PS) crystal is preferably after the frequency conversion crystal to flexibly obtain the best uniformity illumination of the target. However, as a high irradiance 4ω laser beam propagates through the PS crystal, the transverse stimulated Raman scattering (TSRS) effect of the PS crystal will be stronger, resulting in significant energy dissipation and crystal damage. This paper proposes a novel, to the best of our knowledge, fourth harmonic generation (FHG) scheme based on an orthogonal cascade of the DKDP crystals. This orthogonal cascaded FHG (OC-FHG) scheme employs two cascaded FHG crystals with orthogonal optical axes, and the PS crystal is in the middle. The PS crystal can rotate the polarization direction of the 2ω laser by 90°, while the polarization direction of the 4ω laser is maintained to a great extent. This OC-FHG scheme realizes the FHG by two steps, and the laser intensity at the PS crystal cuts down nearly 50%. The output intensity of the 4ω laser can be increased from 1.8G W/c m 2 to about 3.6G W/c m 2 under the condition of effectively inhibiting the TSRS effect. Meanwhile, the output 4ω laser contains two orthogonal polarized beams realizing in-beam polarization smoothing instantaneously. In addition, the novel FHG scheme can also have a high conversion efficiency and bandwidth tolerance.

Tunable Harmonics Generation from Low Average Power Mode-Locked Er-Fiber Laser Using Periodic Poled Nonlinear Crystals

Abstract: Sufficient second, third, and fourth harmonic generation of mode-locked Er-doped fiber laser (ML - EDFL) was experimentally demonstrated. This was achieved by using periodically poled KTiOPO4 (PPKTP) and PP LiNbO3 (PPLN) PPLN nonlinear crystals. Harmonic generation in both crystals depended on the direction of polarization. The highest conversion efficiency was obtained by using a half-wave plate to rotate the polarization before the crystals. When using the PPKTP nonlinear crystal, conversion efficiencies of 4.88%, 0.02%, and 0.002% were obtained for second, third, and fourth harmonics generation at wavelengths of 980, 520, and 390 nm, respectively. For the PPLN nonlinear crystal, temperature and polarization direction were optimized for each harmonic generation wavelength. As a result, conversion efficiencies of 8.6%, 0.1%, and 0.007% were obtained for second, third, and fourth harmonic generation at the same respective wavelengths. Tunable wavelength ranges and their SHGs, as well as the multi-wavelength output and their corresponding SHG wavelengths, were also reported. Keywords: Er-fiber laser, Passive mode-locked fiber laser, Nonlinear polarization rotation, PPKTP, PPLN, SHG, THG, FHG. PACS: Fiber lasers, 42.55.Wd, Mode locking, 42.60.Fc.

High repetition-rate photoinjector laser system for S3FEL

The photoinjector laser system of Shenzhen Superconducting Soft X-Ray Free Electron Laser (S3FEL) is reported in this paper. This laser system operates at up to 1 MHz and produces more than 50 μJ infrared (IR) laser pulses. With a customized fourth harmonic generation (FHG) module, more than 2 μJ ultraviolet (UV) laser pulses were obtained. The power standard deviations of the IR laser and the UV laser are 0.093% and 0.395% respectively. While the pulse energy standard deviations are 1.087% and 1.746% correspondingly. We implemented the pulse stacking scheme to generate flat-top pulses. With four birefringent uniaxial crystals, the Gaussian pulses were converted to flat-top shape, featuring 10 ps pulse width and 0.5 ps rising and falling edges. A cut-Gaussian transverse profile with very sharp rising and falling edges can be produced after the spatial pulse shaper.

206 nm deep ultraviolet laser generated from fifth harmonic of femtosecond fiber laser

Deep ultraviolet (DUV) femtosecond laser, which combines the advantages of high single-photon energy of DUV laser with high peak power of femtosecond laser, is widely used in scientific research, biomedicine, material processing and so on. However, in the process of generating DUV femtosecond laser based on nonlinear frequency conversion is encountered a problem that the group velocity mismatch caused by dispersion makes the temporal walk-off of the nonlinear frequency conversion larger than the pulse duration of the femtosecond laser, thus making the generation of the DUV femtosecond laser very difficult. In this work, based on a Yb-doped fiber femtosecond laser, the delay line is optimized to precisely compensate for the spatial and temporal walk-off, so DUV femtosecond laser possesses the following performances: the center wavelength is 206 nm, the repetition rate is 1 MHz, the maximum output power is 102 mW, the maximum conversion efficiency is 4.25% from near infrared to DUV, the root mean square (RMS) power stability is 0.88% within 3 h, and the peak-to-peak power stability is 3.75%. The evolution of laser spectra and beam quality in the process of second harmonic generation (SHG), fourth harmonic generation (FHG) and sum-frequency generation (SFG) are also systematically studied. The experimental results provide a basis for generating DUV femtosecond laser from femtosecond fiber lasers.

Wave theory-based fourth harmonic generation of Bessel–Gauss beam by total internal reflection-quasi phase matching in a rectangular slab of beta barium borate

This work presents a theoretical approach to a highly multimode-guided wave-based fourth harmonic (FH) generation method by exploiting a zero-order Bessel–Gauss beam through the total internal reflection quasi phase-matching technique. An anisotropic crystal featuring a rectangular structure of beta barium borate has been used to carry out this analysis. In contrast to the conventional frequency conversion scheme using a Gaussian beam, the projected scheme yields a maximum six times superior efficiency of 6.9547% in a crystal length of nearly 6.3 mm, corresponding to a 266-nm FH wavelength. The analysis has also taken into account optical losses, such as absorption, Goos–Hänchen-shift, surface roughness, and the effect of the nonlinear law of reflection. Finally, a systematic study has been performed to describe the influence of parametric modification, such as variations in slab length and thickness, to provide a more comprehensive picture of the overall analysis.

Growth and characterizations of a new nonlinear optical crystal for 266 nm laser generation: LiSr3Be3B3O9F4

The LiSr3Be3B3O9F4 (LSBBF) single crystal with dimensions of 30 × 20 × 15 mm3 was grown from a LiF-NaBF4-B2O3-SrF2 flux system using a top-seeded solution growth method with a seed perpendicular to the (011) plane. The X-ray rocking curve, transmission spectra, refractive indices and laser-induced damage threshold have also been studied. The Sellmeier equations were derived from the measured refractive indices for the first time. According to the Sellmeier equations, the limits of type-I and type-II phase-matching (PM) frequency doubling wavelengths are 241 and 318 nm, respectively. It indicates that LSBBF is a potential UV nonlinear optical crystal for the fourth harmonic generation of Nd:YAG laser at 266 nm.

220 nm deep-UV coherent source based on fifth-harmonic generation in ADP and DKDP crystals

Based on the 1.1 μm laser radiation obtained by parametrically amplifying Yb:YAG laser using frequency doubling of Nd:YAG laser, a 220 nm deep-UV coherent source was systematically presented via the efficient fifth-harmonic generation (FiHG) in NH4H2PO4 (ADP) and KD2PO4 (DKDP) crystals. In ADP crystals, noncritical phase-matching (NCPM) fourth-harmonic generation (FHG) and FiHG were realized at 109.4 and 31.6 °C, respectively. For DKDP crystals, we demonstrated the critical phase-matching FHG at 57.5 °C and verified that NCPM FiHG can be achieved at 38.7 °C, which was the first demonstration of the FiHG using the DKDP crystal to our knowledge. The energy-dependent conversion efficiencies, angular acceptances, and temperature acceptances of these nonlinear processes were systematically measured. The highest total conversion efficiencies from 1.1 μm to the fifth harmonic in ADP and DKDP crystals were 17.5% and 23.6%, respectively. Owing to the large-aperture availability of KDP-family crystals, this work paves the way for the generation and application of high-energy and high-peak-power deep-UV laser radiation.

Femtosecond two-photon LIF imaging of atomic hydrogen in high-pressure methane-air flames

Atomic hydrogen (H) imaging studies in combustion systems have been limited thus far to atmospheric- or low-pressure flames. The commonly used excitation scheme for two-photon laser-induced fluorescence (TPLIF) of H involves 205-nm deep-ultra-violet (DUV) laser pulses generated using nanosecond (ns), picosecond (ps), or femtosecond (fs) laser systems. Ultrashort pulse, fs excitation schemes are more attractive because of the efficient two-photon excitation and interference-free kHz-rate imaging capability. In this work, we implemented a home-built, direct fourth harmonic generation (FHG) laser system to generate high-energy fs pulses for H imaging in CH4/air flames at pressures up to 10 bar. The high-energy FHG output was capable of overcoming transmission losses of DUV laser pulses through thick optical windows of the pressure vessel. Signal interferences such as photoionization, photolytic production, amplified spontaneous emission, and background chemiluminescence were avoided or minimized during data acquisition and subsequent data processing steps. A quadratic dependence of the H TPLIF signal on the laser energy was observed. The increase in the pressure from 1 to 10 bar showed a rapid decay of the fs H TPLIF signal although it should scale linearly with increasing H number density with pressure ideally at equilibrium conditions. Besides a detailed quenching correction, laser absorption and fluorescence signal trapping remain major issues at elevated pressures. The measured fluorescence signals are compared with the equilibrium H number densities and local H concentrations calculated using the Cantera (0D) and UNICORN (2D) flame codes, respectively, for a range of equivalence ratios, and possible reasons for discrepancies are discussed. Experimentally obtained 1D and 2D spatial distributions of H are well predicted by the UNICORN flame model. Steps towards quantitative single-shot H TPLIF imaging measurements in high-pressure flames are also discussed. Overall, the fs TPLIF imaging technique coupled with a high-efficiency home-built FHG system is a promising diagnostic approach for H imaging in high-pressure flames.

Noncollinear frequency mixing and fourth-harmonic generation of oppositely chirped laser pulses

Highly efficient fourth-harmonic generation of 60 µJ, 25 ps chirped (compressible down to 340 fs FWHM) Yb:KGW laser pulses was demonstrated experimentally utilizing noncollinear opposite chirp frequency mixing in Type I beta-barium borate (BBO) and lithium triborate (LBO) crystals as second-harmonic generators followed by collinear frequency doubling in another BBO crystal as a fourth-harmonic generator. Second-harmonic spectral narrowing by a factor over 100 and output UV pulse energy of 10 µJ were achieved.

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.

New solid state laser system for SPES: Selective Production of Exotic Species project at Laboratori Nazionali di Legnaro.

The Selective Production of Exotic Species project is under construction at Laboratori Nazionali di Legnaro-INFN. The aim of the collaboration is to produce highly pure Radioactive Ion Beams (RIBs) from fission fragments of a uranium carbide (UCx) target activated by a cyclotron proton beam. In order to select a specific atomic species, the main tool to be applied is the resonant laser ionization technique. We have just completed the installation of a dedicated all solid state laser system whose elements are tunable to transitions of all the elements/isotopes of interest for the project. The new laser system is based on three Titanium:sapphire laser sources, independently pumped by three Nd:YLF pump lasers, and it can be coupled to two high harmonic generation (second harmonic generation, third harmonic generation, and fourth harmonic generation) setups. The power, wavelength, and position of the laser beams are continuously monitored and stabilized by using automated active systems to improve the beam production stability of RIBs. This paper presents the main features of the laser system and examples of application of a laser ion source, including a first demonstration of photoionization of stable silver, one of the most requested elements for RIB application.

Research on the Nonlinear Absorption Coefficient of 98% Deuterated DKDP Crystal at Fourth-Harmonic-Generation Wavelength

A series of 98% deuterated DKDP crystals were grown in solutions with different pD values (2.9, 3.3, 3.8, and 4.3) using the rapid growth method. Samples were cut along the z-direction and fourth-harmonic-generation (FHG) direction which contained both pyramidal and prismatic regions. The nonlinear absorption (NLA) coefficient β of 98% deuterated DKDP crystals was obtained using the Z-scan method operated at the FHG wavelength (266 nm) of a picosecond Nd:YAG laser. According to the results, the nonlinear absorption at 266 nm could be identified as two-photon absorption. The β values of crystal grown in the solution with 3.3 pD value were higher than those of crystals grown in solutions with other pD values under higher laser fluence. The results also indicated that FHG device samples should be prepared from the pyramidal region due to its lower β value. This work will help optimizing the application of 98% DKDP crystals as FHG elements in high-power laser systems.

Second and cascaded harmonic generation of pulsed laser in a lithium niobate on insulator ridge waveguide.

Nonlinear crystalline ridge waveguides, e.g., lithium niobate-on-insulator ridge waveguides, feature high index contrast and strong optical confinement, thus dramatically enhancing nonlinear interaction and facilitating various nonlinear effects. Here, we experimentally demonstrate efficient second-harmonic generation (SHG) and cascaded fourth-harmonic generation (FHG) in a periodically poled lithium niobate (PPLN) ridge waveguide pumped with pulsed laser at the quasi-phase matching (QPM) wavelength, as well as simultaneous SHG and cascaded third-harmonic generation (THG) waves when pumped at the non-QPM wavelength. Furthermore, the ridge waveguide achieves an efficient single-pass SHG conversion efficiency of picosecond pulsed laser at ∼62%. These results may be beneficial for on-chip nonlinear frequency conversion.

Ultrafast time- and angle-resolved photoemission spectroscopy with widely tunable probe photon energy of 5.3-7.0eV for investigating dynamics of three-dimensional materials.

Time- and angle-resolved photoemission spectroscopy (TrARPES) is a powerful technique for capturing the ultrafast dynamics of charge carriers and revealing photo-induced phase transitions in quantum materials. However, the lack of widely tunable probe photon energy, which is critical for accessing the dispersions at different out-of-plane momentum kz in TrARPES measurements, has hindered the ultrafast dynamics investigation of 3D quantum materials, such as Dirac or Weyl semimetals. Here, we report the development of a TrARPES system with a highly tunable probe photon energy from 5.3 to 7.0eV. The tunable probe photon energy is generated by the fourth harmonic generation of a tunable wavelength femtosecond laser source by combining a β-BaB2O4 crystal and a KBe2BO3F2 crystal. A high energy resolution of 29-48meV and time resolution of 280-320fs are demonstrated on 3D topological materials ZrTe5 and Sb2Te3. Our work opens up new opportunities for exploring ultrafast dynamics in 3D quantum materials.

High-power, high-efficiency, all-fiberized-laser-pumped, 260-nm, deep-UV laser for bacterial deactivation

We report a 5.8-W deep-ultraviolet (DUV) laser obtained from frequency-quadrupling of an all-fiberized ytterbium-doped fiber (YDF) master oscillator power amplifier (MOPA). The MOPA system delivers 585 ps pulses at 1040 nm with a maximum available output power of 23.5 W for nonlinear frequency conversion. A lithium triborate (LBO) crystal and a beta barium borate (BBO) crystal are employed for second- and fourth-harmonic generation (FHG), respectively. At a repetition rate of 1.6 MHz, a maximum DUV output power of 5.8 W is obtained at 260 nm with a corresponding pulse energy of 3.6 μJ and maximum peak power of at least 6.9 kW. A 1μm-to-260nm conversion efficiency of 26.4% is achieved at a DUV output power of 5.8 W. To the best of our knowledge these results represent the highest-average-power fiberized-laser-pumped DUV laser, as well as the most efficient DUV generation based on BBO crystals to date. We further demonstrate application of the pulsed DUV laser in bacterial disinfection achieving an inactivation efficiency of 99.999% for E-coli bacteria at a DUV exposure of 7 mJ/cm2.

Nd:YAG fourth harmonic (266-nm) generation for corneal reshaping procedure: An ex-vivo experimental study.

Corneal reshaping is a common medical procedure utilized for the correction of different vision disorders relying on the ablation effect of the UV pulsed lasers, especially excimer lasers (ArF) at 193 nm. This wavelength is preferred in such medical procedures since laser radiation at 193 nm exhibits an optimum absorption by corneal tissue. However, it is also significantly absorbed by the water content of the cornea resulting in an unpredictability in the clinical results, as well as the high service and operation cost of the commercial ArF excimer laser device. Consequently, other types of solid-state UV pulsed lasers have been introduced. The present work investigates the ablation effect of solid-state laser at 266 nm in order to be utilized in corneal reshaping procedures. Different number of pulses has been applied to Polymethyl Methacrylate (PMMA) and ex-vivo rabbit cornea to evaluate the ablation effect of the produced laser radiation. PMMA target experienced ellipse-like ablated areas with a conical shape in the depth. The results revealed an almost constant ablation area regardless the number of laser pulses, which indicates the stability of the produced laser beam, whereas the ablation depth increases only with increasing the number of laser pulses. Examination of the ex-vivo cornea showed a significant tissue undulation, minimal thermal damage, and relatively smooth ablation surfaces. Accordingly, the obtained 266-nm laser specifications provide promising alternative to the traditional 193-nm excimer laser in corneal reshaping procedure.