Laser-induced Damage Threshold Research Articles

Optical properties of Ba-impurity defect clusters in KH2PO4 crystals

Potassium dihydrogen phosphate (KDP) is widely used in electro-optical switches and inverter crystals in inertial confinement fusion (ICF). The early studies suggested that defect clusters are one of the main reasons why the laser-induced damage threshold (LIDT) is far lower than the theoretical value. However, it is not clear what type of defect clusters cause this phenomenon. The BaK defect cluster models have been determined by simulation using General Utility Lattice Programs (GULP). We found that BaK+VH and BaK+VK cause a dramatic distortion on H-O bonds with maximum values of 29.5 % and 27.12 %, respectively. By analyzing the configuration coordinate diagram and optical spectra, we believe that both defect clusters can promote ionization through defect-assisted "2+1" photon absorption, which leads to free electrons more easily exceeding the critical value for electron avalanche breakdown. Our study will offer insight into the effects of defect clusters in KDP crystals.

Comparing the laser-induced damage distribution in POFs with raytracing simulations

The understanding of the laser-induced damage behavior in polymer optical materials is of high interest to prevent their damage and to increase the laser damage resistance of optical components. Moreover, compared with optical components made from high-quality glass materials, nanosecond laser-induced damage for wavelengths in the visible and near-infrared (NIR) occurs inside the bulk material of PMMA and not at its surface. This phenomenon complicates the determination of the laser-induced damage threshold (LIDT) in PMMA fibers. Since the bulk material itself determines the LIDT, knowledge of the intensity distribution in the multimode fiber is of utmost importance. Our fibers were irradiated at a wavelength of 532 nm with an ns-pulsed laser system with a 10 Hz repetition rate. To investigate the damage behavior in polymer optical fibers, we applied different imaging and analysis techniques. To our knowledge, those techniques are used here for the first time in order to study damaged polymer materials. With the help of a Nomarski microscope, axial and radial damage distributions within the multimode PMMA fibers were determined and compared with ray-tracing simulations of the intensity distribution within the optical fiber. Moreover, extruded PMMA plates were irradiated with the aim of comparing the damage behavior of materials with different manufacturing. In addition, the planar geometry of the plates allows for a more reliable application of the different measurement methods. Overall, investigations with a thermal imaging camera and EDX analysis indicate that the damage behavior of polymer optical material is thermally driven during the ns-pulsed irradiation. Furthermore, voids are formed during the damaging process within the polymer optical fibers and plates, as indicated by both SEM images and X-ray computed microtomography (µ-CT) investigations. Finally, we investigated the damages in fiber preforms and PMMA plates using two photon-microscopy. By doing this, we detected fluorescence signals from the damaged material, indicating that the damage process leads to a major modification of the polymer.

Delivery of nanosecond laser pulses by multi-mode anti-resonant hollow core fiber at 1 µm wavelength

In this paper we explore the application of low-loss multimode anti-resonant hollow-core fiber (MM-AR-HCF) in the delivery of nanosecond laser pulses at 1 µm wavelength. MM-AR-HCF with large core offers a rich content of low-loss higher-order modes which plays a key role in the efficient coupling and transmission of high-power laser of low beam quality. In the experiment, laser pulses of an average pulse energy of 21.8 mJ with 14.6 ns pulse width (corresponding a peak power of 1.49 MW) are transmitted through MM-AR-HCF of 9.8 m length without damage. 85% transmission efficiency is achieved where the incident laser beam suffers a low beam quality with M2x and M2y of 2.18 and 1.99 respectively. Laser-induced damage threshold (LIDT) of MM-AR-HCF was measured to be 22.6 mJ for 85% transmission efficiency, which is 7 times higher than that for a multimode silica optical fiber with a large core of 200 µm.

Design of Pentanary Mixed-Chalcogenides Ag2In2SiS6-xSex (x = 1, 2) Based on the Bucket Effect: Local Structural Difference and High-Performance Nonlinear-Optical Properties Realized by Partial Congener Substitution.

Noncentrosymmetric chalcogenides are promising candidates for infrared nonlinear-optical (NLO) crystals, and exploring high-performance ones is a hot topic and challengeable. Herein, the combination of AgQ4, InQ4, and SiQ4 (Q = S, Se) units with different S/Se ratios resulted in the discovery of the tetrahedral chalcogenides Ag2In2SiS4Se2 (1) and Ag2In2SiS5Se (2). They both crystallize in the monoclinic Cc space group with different local structures. Co-occupied S/Se sites only exist in 2, and the arrangement of [In2SiQ3] six-membered rings builds different helical chains and 3D [(In2SiQ6)2-]n polyanionic frameworks in 1 and 2. They show balanced NLO performances, including phase-matchable moderate NLO responses (0.7 and 0.5 × AGS) and enhanced laser-induced damage thresholds (4.5 and 5.1 × AGS). Theoretical calculations reveal that their NLO responses are predominantly contributed by the AgQ4 and InQ4 units.

Vacancy‐Induced Extraordinary Second Harmonic Generation Response for Diamond‐Like Cu3PS4

AbstractImproving polarizability is an important strategy for designing high‐performance mid‐infrared (mid‐IR) nonlinear optical (NLO) materials. The substitution of equivalent or aliovalent atoms can manipulate the polarizability by adjusting the symmetry of the polyhedron. Herein, the Li+ and Cd2+ are introduced into the Cu3PS4 as the equivalent and aliovalent dopants for the Cu site. As a result, Li+ can significantly improve the bandgap (Eg) of LixCu3−xPS4 from 2.38 to 2.88 eV, leading to a higher laser‐induced damage threshold (LIDT) of 4.9 times than AgGaS2 (AGS) with a comparable second harmonic generation (SHG) response of AGS (26−45 µm). Interestingly, Cd2+ can improve the SHG response and enlarge the Eg simultaneously. As a result, Cd0.4Cu2.2PS4 has a large SHG response of 10 × AGS at 2050 nm (26−45 µm) and a LIDT of 2.6 × AGS. Theoretical calculations reveal that lattice vacancies induced by Cd2+ significantly boost polarizability compared to LixCu3−xPS4 with no vacancy, leading to a strong NLO response.

LaMg6Ga6S16: a chemical stable divalent lanthanide chalcogenide

Divalent lanthanide inorganic compounds can exhibit unique electronic configurations and physicochemical properties, yet their synthesis remains a great challenge because of the weak chemical stability. To the best of our knowledge, although several lanthanide monoxides epitaxial thin films have been reported, there is no chemically stable crystalline divalent lanthanide chalcogenide synthesized up to now. Herein, by using octahedra coupling tetrahedra single/double chains to construct an octahedral crystal field, we synthesized the stable crystalline La(II)-chalcogenide, LaMg6Ga6S16. The nature of the divalent La2+ cations can be identified by X-ray photoelectron spectroscopy, X-ray absorption near-edge structure and electron paramagnetic resonance, while the stability is confirmed by the differential thermal scanning, in-situ variable-temperature powder X-ray diffraction and a series of solid-state reactions. Owing to the particular electronic characteristics of La2+(5d1), LaMg6Ga6S16 displays an ultrabroad-band green emission at 500 nm, which is the inaugural instance of La(II)-based compounds demonstrating luminescent properties. Furthermore, as LaMg6Ga6S16 crystallizes in the non-centrosymmetric space group, P−6, it is the second-harmonic generation (SHG) active, possessing a comparable SHG response with classical AgGaS2. In consideration of its wider band gap (Eg = 3.0 eV) and higher laser-induced damage threshold (5×AgGaS2), LaMg6Ga6S16 is also a promising nonlinear optical material.

A congruent-melting rubidium zinc vanadium oxychloride exhibiting strong mid-infrared second-harmonic generation and high laser-induced damage threshold

A novel mid-infrared (MIR) nonlinear optical (NLO) crystal Rb4ZnV5O15Cl (RZVC) has been designed and sythesized by the aliovalent substitution strategy based on the parent structure Rb2(VO)(V2O7). Modification of square pyramidal VO5 units through introduction of chlorine ion and zinc metal caion significantly enhanced the dipole moments in a unit cell from 1.653 D for Rb2(VO)(V2O7) to 6.559 D for RZVC. Consequently, polycrystalline RZVC exhibits strong SHG responses of 12.5 × KDP @1064nm and 1.2 × AGS @2 μm. Furthermore, RZVC features a congruent melting property, an ultra-high LIDT value (62 × AGS @1064nm), and a deep IR transparency cutoff edge (10 μm). Most importantly, RZVC can achieve full-wavelength phase matching in a very wide MIR transparency range of 1.6910 μm, completely covering the important atmospheric window (35 μm) through NLO processes. Because of its many outstanding properties, RZVC can be a highly desirable candidate for practical MIR NLO applications.

Infrared nonlinear optical materials with multiple strongly ionic cations

Infrared nonlinear optical (IR-NLO) crystals with excellent properties are in extensive demand due to their important role in IR laser technology. Currently, it remains a great challenge to obtain IR-NLO materials with both high second harmonic generation (SHG) response and large laser-induced damage thresholds (LIDTs). Some structural design strategies such as ‘structural/functional regions’ have been adopted to develop new high-performance NLO materials. The covalent structural region producing SHG signals has been extensively investigated, whereas the hard cations (alkali, alkaline-earth, and rare-earth metal ions) which are responsible for improving LIDTs, have been relatively neglected. Utilizing the concept of structural/functional regions, we focus on the relation between structural regions and SHG properties in chalcogenides. Combining different kinds of hard cations can change the dimension of structures and affect the stacking of NLO-active groups. Introducing more hard cations and constructing more complex ion regions help to increase the laser damage threshold. Based on the mentioned structural strategies, guidance will be provided for developing high-performance multiple-cation materials for IR NLO applications.

Effect of metal doping on the laser induced damage of KDP crystals: A first-principles study

KH2PO4 (KDP) crystal is a kind of widely used nonlinear optical material, but its manufacturing process produces various defects which influence the laser induced damage threshold (LIDT) of the KDP crystal. This work studies the influence of the metal doping defects (Na, Cr, Co, Ni, Zn and Pb) on the stability, electronic structure, optical and mechanical properties of KDP crystal by the density functional theory (DFT) calculation. Results show that the change of lattice parameters and bond lengths, and the formation energies of the metal doped KDP have close relationship with the radius of the doped metal atoms. The electronic and optical calculations show that the Na doping defects have little effect on the energy band and optical properties of KDP crystals, but Cr, Zn and Pb doping defects show large optical absorption peaks. Meanwhile, the Cr, Co, Ni and Pb atoms have great influence on the mechanical properties of the KDP. Therefore, the KDP synthesis process needs to pay particular attention to control Cr and Pb doping defects to avoid decreasing the LIDT of KDP. This work explains the effect of metal doping on the laser damage resistance of KDP crystals and provides a theoretical basis for enhancing the performance of KDP crystals.

Nano-imprint lithography of broad-band and wide-angle antireflective structures for high-power lasers.

We demonstrate efficient anti reflection coatings based on adiabatic index matching obtained via nano-imprint lithography. They exhibit high total transmission, achromaticity (99.5% < T < 99.8% from 390 to 900 nm and 99% < T < 99.5% from 800 to 1600 nm) and wide angular acceptance (T > 99% up to 50 degrees). Our devices show high laser-induced damage thresholds in the sub-picosecond (>5 J/cm2 at 1030 nm, 500 fs), nanosecond (>150 J/cm2 at 1064 nm, 12 ns and >100 J/cm2 at 532 nm, 12 ns) regimes, and low absorption in the CW regime (<1.3 ppm at 1080 nm), close to those of the fused silica substrate.

Barium Chalcogenide Crystals: A Review

In recent decades, new nonlinear optical materials have been actively developed to create coherent tunable light sources in the mid-infrared (mid-IR) part of the spectrum used in a variety of scientific fields. In the present review, the main attention is focused on barium chalcogenide crystals, including their linear and nonlinear optical properties, laser-induced damage threshold (LIDT), and frequency down-conversion.

Anhydrous Aluminum Iodate: Strong Second Harmonic Generation Effect Contributed by Unbonded and Antibonding Orbitals.

Exploring materials that balance the second harmonic generation (SHG) effect and laser-induced damage threshold (LIDT) is the frontier of nonlinear optical (NLO) crystal research at present. In this work, the NLO property of anhydrous aluminum iodate is extensively explored and discussed first. It exhibits a strong SHG intensity of 18.3 × KH2PO4 (KDP) and a high-powder LIDT of 1.4 × KDP at 1064 nm. Combining experimental and theoretical studies at the atomic level and electronic levels, it is found that the cations in the structure are replaced by cations with small radius and high valence, enabling the production of materials with large SHG responses. Unbonded and antibonding orbitals play a crucial positive role in the SHG response of the structure, whereas bonding orbitals produce a large negative contribution. This provides a scarce example of materials in which bonding orbitals make significant negative contributions.

Nanosecond laser damage of 532 nm thin film polarizers evaluated by different testing protocols

Different laser damage testing protocols, including 1-on-1, S-on-1, and Raster Scan, were conducted on 532 nm polarizers to evaluate the damage resistance and mechanisms. A comparison of the laser-induced damage thresholds (LIDTs) revealed different damage characteristics and major contributions to film failure for different polarizations. For P polarization, the LIDTs for the three test protocols were nearly the same because of the stabilization of two typical damage morphologies of flat-bottomed pits and mussel damage pits. For S polarization, the LIDTs for multiple pulses were lowest, where absorptive defect-induced damage was revealed. The damage characteristics of 532 nm polarizers and 1064 nm polarizers have been also compared. The mussel damage pits, which are similar to the typical damage morphologies of ultraviolet (UV) laser damage to fused silica, were observed for the first time in coatings of 532 nm polarizers. This suggests that, the polishing-induced subsurface damage of fused silica substrates may tend to be excited by a short-wavelength laser rather than the fundamental wavelength.

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.

Laser induced damage threshold of GaSe with antireflection microstructures at a wavelength of 5 µm.

Large GaSe crystals were grown and various antireflection microstructures (ARMs) were fabricated on their cleaved surfaces using optimized femtosecond laser ablation, which provided the antireflection effect in a wide wavelength range of 4-16µm. The influence of ARMs created on the GaSe surface on the change of the laser-induced damage threshold (LIDT) of the crystal at a wavelength of 5 μm was evaluated. The 5-µm Fe:ZnMgSe laser with the pulse duration of 135 ns was used for the LIDT test in conditions close to single pulse exposure. The measured values of LIDT of 56 ± 6MW/cm2 and 51 ± 9 MW/cm2 for two GaSe substrates, respectively, were comparable with the known data of single pulse LIDT of GaSe. The average LIDT intensities of 54 ± 6MW/cm2 and 52 ± 7 MW/cm2 for the ARMs at two GaSe plates, respectively, were close to LIDT intensities for the corresponding GaSe substrates. The ARMs with lower structural quality had lower LIDT (50-52 MW/cm2) in comparison with the high-quality ARMs (58-60 MW/cm2). High LIDT for high-quality ARMs can be caused by increased selenium content in the ARMs. In any case, all the tested ARMs on the GaSe plates with different surface quality are workable for development of widely tunable mid-infrared nonlinear optical converters.

KREP2S6 (RE = Sm, Gd, Tb, Dy): A Series of Polar Rare-Earth Thiophosphates with High Laser-Induced Damage Thresholds and Moderate Nonlinear-Optical Responses Synergistically Contributed by Isolated P2S6 Units and {[RE2S15]24-}∞ Layers.

As one of the potential candidates of nonlinear-optical (NLO) materials, rare-earth chalcophosphates have demonstrated promising properties. Here, KREP2S6 (RE = Sm, Gd, Tb, Dy) were synthesized using the facile RE2O3-B-S solid-state method. They crystallize with a monoclinic chiral P21 structure, and their layer structures are built by isolated ethane-like P2S6 dimers and RES8 bicapped trigonal prisms built {[RE2S15]24-}∞ layers. By comparing the structures with related ones, the change of the alkali metal or RE3+ ions can cause structural transformation. Their band gaps are tunable between 2.58 and 3.79 eV, and their powder samples exhibit good NLO properties. Theoretical calculations suggest that the NLO properties are mainly contributed by P2S6 units and {[RE2S15]24-}∞ layers synergistically, in which {[RE2S15]24-}∞ layers and P2S6 units dominate the contribution to the band gap and second-harmonic-generation response, respectively. This work enriches the application of rare-earth chalcophosphates as NLO materials.

Hg3Se(SeO3)(SO4): A Mixed-Valent Selenium Compound with Mid-Infrared Transmittance Obtained by In Situ Reaction.

Exploring new material systems is a highly significant task in the field of inorganic chemistry. A new mixed-valent selenium compound, Hg3Se(SeO3)(SO4), was successfully synthesized through in situ reactions. This compound exhibits a novel three-dimensional structure composed of Hg3Se(SO4) layers bridged by SeO3 trigonal pyramids. It is the first structure containing (SeO3)2-, (SO4)2-, and Se2- simultaneously. In addition, Hg3Se(SeO3)(SO4) possesses a wide bandgap (3.5 eV), moderate birefringence (Cal:0.064@546 nm, Exp:0.069@546 nm), a high laser-induced damage threshold (23.35 MW cm-2), and a wide transmittance window (0.28-6.6 μm). Our work demonstrates that mixed-valent (+4, -2) selenite selenide can be potential optical materials for the mid-infrared region.

Modeling of the femtosecond pulsed laser-induced damage of multi-layer dielectric gratings

The laser damage resistance of multi-layer dielectric gratings (MDGs) and metal multi-layer dielectric gratings (MMDGs) for femtosecond lasers directly determines the performance and life span of the high-energy laser system. It remains a significant challenge to predict the laser-induced damage threshold (LIDT) of MDGs and MMDGs for femtosecond lasers. Based on the nonlinear ionization and electric field intensity model, an effective method is proposed to calculate the LIDT of MDGs and MMDGs by introducing the dual temperature model. We take into account the evolutions of thermophysical parameters including the absorption coefficient, heat capacity, and thermal conductivity of the dielectric material as a function of the free-electron density and temperature. The free electron density of the conduction band combined with the electric field strength inside the grating can be calculated by the laser-induced ionization theory, more importantly, the transient distribution of the lattice temperature field generated by femtosecond laser irradiated grating excitation is obtained by the two-temperature model (TTM). This work is beneficial for guiding the design and fabrication of MDGs and MMDGs with high-LIDTs for ultra-short ultra-intense laser systems.

Na12(NbO)3(PO4)7: A Congruent Melting Nonlinear Optical Crystal with Large NbO6 Distortion and High Laser-Induced Damage Threshold.

A new noncentrosymmetric crystal Na12(NbO)3(PO4)7 was successfully synthesized in the niobium phosphate system. Its structure characterizes isolated and highly distorted NbO6 octahedra joining with isolated PO4 groups to form a unit of a (Nb6P6O12) hexagonal star by sharing O atoms. In (Nb6P6O12) hexagonal stars, all Nb and P atoms are in a hexagonal star-like arrangement and all Na atoms are also in a hexagonal star-like arrangement, except for Na(3) and Na(10) atoms. Notably, it exhibits a strong phase-matched second harmonic response: 3 × KDP, which is rare in known niobium phosphate systems. Meanwhile, it also has a wide optically transparent window (0.29-4.44 μm) and a high laser-induced damage threshold (3.5 GW/cm2). More importantly, Na12(NbO)3(PO4)7 is a congruent melting compound that has the potential to be grown into large-sized single crystals by the Czochralski method. These excellent properties make it a promising candidate as a mid-infrared nonlinear optical crystal.

Striated composite layers of silica and hafnia offering advantageous properties for short-pulse optical coatings.

Monolayers containing subnanometer striations of silica and hafnia to form composite materials at varying ratios are explored as a method to develop high-index dielectric layers with increased laser-induced-damage thresholds (LIDTs). These layers can then be used in multilayer dielectric coatings for short-pulse, high-peak-power laser applications, particularly in regions of the highest electric-field intensity. Fabrication is achieved by means of exposure to two different evaporant vapor plumes, where local exposure to each plume is controlled via shielding to prevent simultaneous exposure. The LIDT of the resulting layers has been evaluated at 1053 nm with 600-fs pulses. The results indicate that such hafnia/silica layers exhibit LIDTs similar to silica for a refractive index of ≤1.65. These results suggest that the use of these layers in locations subjected to high electric-field intensity within multilayer dielectric coatings may significantly improve the LIDT, with this deposition process providing particular benefit for scaling to large-aperture, high-fluence components.