High Laser Damage Threshold Research Articles

Effect of annealing on ion-beam-sputtered hafnium oxide thin films properties

HfO2 films are high laser damage-threshold and low-absorption thin-films that can be utilized for a broad range of optoelectronic and optical applications. In this study, HfO2 thin films were prepared via dual ion beam sputtering followed by annealing in the atmosphere at temperatures ranging from 200 to 700 °C. The optical properties, microstructure, film stress, and absorption loss of the HfO2 films at various annealing temperatures were then systematically characterized. The results revealed that the properties of the films were improved after annealing at temperatures below 500 °C. Specifically, at an optimal annealing temperature of 400 °C, the residual stress of the films was minimized close to zero and the absorption loss was as low as 1 ppm. However, at annealing temperatures reaching 600 °C, the films began to crystallize, leading to the deterioration of their optical properties. Optimizing the process parameters for HfO2 thin film deposition is crucial for developing the next generation of high-performance laser optics.

Extending mid-infrared wavelength to 6.84 μm in oxide nonlinear optical crystal via birefringence dispersion management.

Extending lasing wavelengths to the mid-infrared (MIR) spectrum is vital for both civilian and military applications; however, it remains challenging when employing oxide nonlinear optical crystals. In this study, we report the generation of MIR nanosecond pulses via difference frequency generation (DFG) with a near-IR pump using a newly designed langasite (LGS) crystal, La3(Nb0.6Ta0.4)0.5Ga5.5O14 (LGNT0.4), which incorporates birefringence dispersion management techniques with La3Ga5.5Nb0.5O14 (LGN) as a template. Due to the improved effective nonlinear coefficients and the maintained IR cutoff relative to LGN, the tunable DFG laser in LGNT0.4 extended from 4.24 to 6.84 μm, delivering a maximum pulse energy of 16.3 μJ at 5.02 μm. To the best of our knowledge, this is the first known oxide material capable of generating tunable nanosecond pulsed lasers beyond 6 μm at μJ-level energies, demonstrating promising potential for high-intensity MIR laser systems owing to its high laser damage threshold.

Optical properties of hafnium-dioxide derived from reflection electron energy loss spectroscopy spectra

The optical properties of HfO2 have practical applications. As an important gate dielectric material with high-k dielectric, HfO2 is beneficial to reduce the leakage current of the complementary metal-oxide-semiconductor (CMOS) gate and improves the gate structure. HfO2 also plays a key role in optical coating materials field for its high transmittance in the ultraviolet to near-infrared band, and high laser damage threshold. Therefore, it is of practical significance for the accurate knowledge of optical properties of HfO2. Here we present the optical constants and dielectric function of HfO2 based on the energy loss function (ELF) in the energy loss range of 0–200 eV for nanocrystalline film. Our new data are derived from the analysis of the reflected electron energy loss spectra by using the latest version of our reverse Monte Carlo modelling. Sum rules are used to check the reliability of the new data. We have found that up to 30 eV there are three main peaks, and the first-principles calculation also confirms the three peak structures. A comparison with previous results indicates that the ELF peak positions of HfO2 with different crystal structures are similar, but the peak intensity and shape are different. The heterogenicity of the crystal structure of HfO2 leads to different measurement results for different samples.

Bridgman growth and characterizations of nonlinear optical crystal La3Ga5.5Nb0.5O14

La3Ga5.5Nb0.5O14 (LGN) crystal is a promising material for optical parametric chirped-pulse amplification (OPCPA) with high laser damage threshold and wide transmission range which is able to achieve high peak power laser. LGN with a diameter of 25 mm was successfully grown by the vertical Bridgman method for the first time and a series of characterizations were performed. The 1.7 µm absorption peak in transmittance spectra of LGN crystal which was caused by the Czochralski technique can be effectively eliminated by the vertical Bridgman method. LGN crystal possesses a high transmittance of 81.3 % in the range of 0.294 ∼ 7.500 μm. The experimental optical band gap of LGN is 4.16 eV which is positively correlated with laser damage threshold. The experimental laser damage threshold of LGN was determined to 1.416 GW/cm2 by Nd:YAG. The outstanding thermal properties of LGN indicate that it possesses thermal stability in high energy laser field. This work demonstrates that LGN crystal holds great potential for OPCPA applications and the vertical Bridgman method is proved to be a effective and excellent technique to grow high quality LGN crystal.

Defect-controlled fabrication of reduced graphene oxide/ZnO/PMMA-based solid-state optical limiting filters with SA/RSA switching property

A solid-state optical limiting filter was fabricated by noncovalently functionalizing a graphene-based nanocomposite with a polymer. Graphene oxide was reduced by varying reducing agent concentration and functionalized with metal oxide nanoparticles to enhance electronic transitions and third-order nonlinear optical characteristics. The nanocomposite was dispersed over the PMMA polymer framework, and thin films with μm-scale thickness were fabricated using the dip coating method. XRD analysis confirmed the wurtzite crystal structure of ZnO nanoparticles and the amorphous nature of PMMA. The carbon structural integrity was analyzed using Raman spectra. Linear optical studies revealed a redshift in the π-π* transition peak in rGO, suggesting enhanced conjugation. Third-order nonlinear refraction and absorption properties were assessed using the Z-scan technique, revealing a switching behavior in nonlinear absorption at different input intensities. An increase in the relative concentration of sp2 domains enhanced the nonlinear absorption. Optical limiting potential, determined using open aperture Z-scan data, yielded a threshold value of 0.066 GW/cm2. This study aims to develop a solid-state optical filter with a high laser damage threshold by adjusting the reduction rate, tuning defect levels, and analyzing its effect on the optical limiting potential.

Second Harmonic Generation in β-K2TeW3O12: An Acentric Crystal Designed from Centric Phase via Pressure Modulation.

The latent value of nonlinear optical (NLO) crystals applied in solid-state laser equipment necessitates the development of applicable strategies for constructing noncentrosymmetric (NCS) crystals. By modulating the synthetic temperature and pressure to achieve the rearrangement of [TeO3]2- groups, a new NCS tellurium tungstate, β-K2TeW3O12 (β-KTW), with a strong second harmonic generation (SHG) response was synthesized based on its centrosymmetric polymorphic phase α-K2TeW3O12 (α-KTW). Computational calculation reveals that the large SHG response of β-KTW (15 × KH2PO4@1064 and 1.5 × KTiOPO4@1950 nm) could be attributed to the uniform arrangement of the NLO-active [TeO3]2- and [WO6]6- groups. β-KTW also exhibits enlarged birefringence (0.196@1064 nm) and a high laser damage threshold (42.3 MW cm-2), showing great potential as a nonlinear crystalline material. This work also provides a new route for the construction of NLO crystals based on centric structure, i.e., reverse pressure regulation.

Boosted Second Harmonic Generation of a Chiral Hybrid Lead Halide Resonant to Charge Transfer Exciton from Metal Halide Octahedra to Ligand.

Chiral hybrid organic-inorganic metal halides (HOMHs) offer an ideal platform for the advancement of second-order nonlinear optical (NLO) materials owing to their inherent noncentrosymmetric structures. The enhancement of optical nonlinearity of chiral HOMHs could be achieved by matching the free exciton and/or self-trapped exciton energy levels with desired NLO frequencies. However, the current scarcity of resonance modes and low resonance ratio hamper the further improvements of NLO performance. Herein, we propose a new resonant channel of charge transfer (CT) excited states from metal halide polyhedra to organic ligand to boost the second-order optical nonlinearity of chiral HOMHs. The model lead halide (C7H10N)PbBr3 (C7H10N=1-ethylpyridinium) exhibits a drastically enhanced second harmonic generation in resonance to the deep CT exciton energy, with intensity of up to 111.0 times that of KDP and 10.9 times that of urea. The effective NLO coefficient has been determined to be as high as ~40.2 pm V-1, balanced with a large polarization ratio and high laser damage threshold. This work highlights the contribution of organic ligands in the construction of a resonant channel for enhancing second-order NLO coefficients of metal halides, and thus provides guidelines for designing new chiral HOMHs materials for advanced nonlinear photonic applications.

Boosted Second Harmonic Generation of a Chiral Hybrid Lead Halide Resonant to Charge Transfer Exciton from Metal Halide Octahedra to Ligand

AbstractChiral hybrid organic–inorganic metal halides (HOMHs) offer an ideal platform for the advancement of second‐order nonlinear optical (NLO) materials owing to their inherent noncentrosymmetric structures. The enhancement of optical nonlinearity of chiral HOMHs could be achieved by matching the free exciton and/or self‐trapped exciton energy levels with desired NLO frequencies. However, the current scarcity of resonance modes and low resonance ratio hamper the further improvements of NLO performance. Herein, we propose a new resonant channel of charge transfer (CT) excited states from metal halide polyhedra to organic ligand to boost the second‐order optical nonlinearity of chiral HOMHs. The model lead halide (C7H10N)PbBr3 (C7H10N=1‐ethylpyridinium) exhibits a drastically enhanced second harmonic generation in resonance to the deep CT exciton energy, with intensity of up to 111.0 times that of KDP and 10.9 times that of urea. The effective NLO coefficient has been determined to be as high as ~40.2 pm V−1, balanced with a large polarization ratio and high laser damage threshold. This work highlights the contribution of organic ligands in the construction of a resonant channel for enhancing second‐order NLO coefficients of metal halides, and thus provides guidelines for designing new chiral HOMHs materials for advanced nonlinear photonic applications.

Fabrication of double-cladding fluoroindate glass fibers and watt-level 2.7 μm laser application

We report a double-cladding fluoroindate fiber with three layers of step refractive index glass. The gain double-cladding fluoroindate fiber is fabricated by the traditional rob-in-tube method. It possesses a tunable refractive index from 1.46 to 1.51 via modification of glass components. The good thermal–mechanical performance of fluoroindate glass protects fiber against thermal damage. The luminescence characteristics and radiation parameters are studied, and the results indicate enhanced emission with the higher Er3+ doping concentration. The maximum output power and the slope efficiency of heavily erbium-doped fiber laser are about 1.2 W and 16.3 %, respectively. The numerical modeling of a heavily-erbium-doped fluoroindate fiber laser is also carried out and compared with our experimental results. The low phonon energy and high laser damage threshold of fluoroindate glass allow for higher output power and efficiency of fiber lasers. In brief, this is the first study on watt-level 2.7 μm fiber laser in all-solid double-cladding fluoroindate fibers to our knowledge.

Surface damage induced by micropores in transparent ceramics under nanosecond laser irradiation.

The increasing use of transparent ceramics in laser systems presents a challenge; their low damage threshold has become a significant impediment to the development of powerful laser systems. Consequently, it is imperative to undertake research into the damage sustained by these materials. Micropores, the most common structural defects in transparent ceramics, inevitably remain within the material during its preparation process. However, the relationship between the density and size of these micropores and their impact on nanosecond laser damage threshold and damage evolution remains unclear. In this study, we utilize the annealing process to effectively manage the density and size of micropores, establishing a correlation between micropores in relation to damage thresholds. This study confirms for the first time that micropores significantly contribute to laser damage, comparing and analyzing the damage morphology characteristics of both front and rear surfaces of transparent ceramics. It also presents, potential mechanisms that may contribute to these differences in damage. This paper offers guidance for controlling micropores during the preparation and processing of transparent ceramics with high laser damage thresholds. The findings are expected to further improve the anti-nanosecond laser damage capabilities of transparent ceramics.

Few-mode metal-free perovskite optical fiber with second-order optical nonlinearity

Semiconductor core optical fibers are highly desirable for fiber-based photonic and optoelectronic applications as they can combine strong optical nonlinearities, tight light confinement, wide transmission bands, and electronic functionality within a single platform. Perovskites have emerged as particularly exciting materials for semiconductor photonics as they have strong optical nonlinearities and tunable optoelectronic bandgaps. However, lead-based perovskites contain toxic elements and are, therefore, not environmentally friendly. Furthermore, in fiber form, their core-size is prohibitively large, making them unsuitable for nonlinear optics and applications that require single-mode guidance, such as telecommunications. Here, we report a metal-free perovskite core optical fiber where lead has been substituted for an ammonium cation in the perovskite structure. The core material has a wide bandgap greater than 5 eV, a high laser damage threshold, and a core diameter that can be produced as small as 5 µm. At this core size, the fiber supports just six modes, and the fundamental mode can readily be excited and isolated. Moreover, the metal-free perovskite has a second-order susceptibility that is absent in the archetypal lead-based perovskites and many other semiconductor core materials, such as silicon and germanium. The second-order susceptibility is important for many nonlinear optics applications, such as second-harmonic generation and quantum optics.

A Self-Healing Optoacoustic Patch with High Damage Threshold and Conversion Efficiency for Biomedical Applications

HighlightsBased on Fe-Hpdca-PDMS and carbon nanotube composite, an optoacoustic patch is developed, which can recover from the damage induced by cutting or laser irradiation at room temperature.The patch has high laser damage threshold (183.44 mJ cm−2) and optoacoustic energy conversion efficiency (10.66×10−3).The patch has been successfully examined in acoustic flow, thrombolysis, and wireless energy harvesting, which may provide new insights into the field of the design and fabrication of novel ultrasound devices for biomedical applications.

A Ferroelectric Nonlinear Optical Crystal for Deep‐UV Quasi‐Phase‐Matching

AbstractPhase matching is indispensable for high efficiency of second‐order nonlinear optical (NLO) crystals. Thousands of these crystals rely on birefringence phase matching, whereas only a few of them are quasi‐phase matching without the restriction of birefringence. Herein, using oriented seeds inch‐sized LiNH4SO4 (LAS) single crystals are successfully grown. LAS is NLO‐active with a very short deep‐UV absorption edge of 171 nm and high laser damage threshold up to 1.47 GW cm−2 at 1064 nm, 10 ns, but its birefringence is merely 0.0078@532 nm, which is too small to realize birefringence phase matching in deep‐UV region. Fortunately, P−E hysteresis loop, variable‐temperature NLO tests, and ferroelectric domain observations confirm that LAS is ferroelectric. Furthermore, LAS exhibits small refractive index dispersion resulting in a relatively long periodic length of 1.4 µm and its single domain structure can be easily obtained by electrical poling. These attributes make LAS a scarce NLO candidate for deep‐UV quasi‐phase matching. This work highlights the longly overlooked potential of sulfates and provides new opportunities for deep‐UV NLO materials.

A Machine Learning Study on High Thermal Conductivity Assisted to Discover Chalcogenides with Balanced Infrared Nonlinear Optical Performance.

Exploration of novel nonlinear optical (NLO) chalcogenides with high laser-induced damage thresholds (LIDT) is critical for mid-infrared (mid-IR) solid-state laser applications. High lattice thermal conductivity (κL ) is crucial to increasing LIDT yet often neglected in the search for NLO crystals due to lack of accurate κL data. A machine learning (ML) approach to predict κL for over 6000 chalcogenides is hereby proposed. Combining ML-generated κL data and first-principles calculation, a high-throughput screening route is initiated, and ten new potential mid-IR NLO chalcogenides with optimal bandgap, NLO coefficients, and thermal conductivity are discovered, in which Li2 SiS3 and AlZnGaS4 are highlighted. Big-data analysis on structural chemistry proves that the chalcogenides having dense and simple lattice structures with low anisotropy, light atoms, and strong covalent bonds are likely to possess higher κL . The four-coordinated motifs in which central cations show the bond valence sum of +2 to +3 and are from IIIA, IVA, VA, and IIB groups, such as those in diamond-like defect-chalcopyrite chalcogenides, are preferred to fulfill the desired structural chemistry conditions for balanced NLO and thermal properties. This work provides not only an efficient strategy but also interpretable research directions in the search for NLO crystals with high thermal conductivity.

Ultra-precision lapping of H2O(g) plasma-treated CaF2 by porous diamond grits

The calcium fluoride (CaF2) component has excellent light transmission and a high laser damage threshold in the UV band, and thus is a potentially ideal material for high-power laser facility. However, the low-damage surface is difficult to attain via the existing processing technologies due to its brittleness, especially the dissociation property of the (111) surface. We innovatively propose H2O(g) plasma-assisted porous diamond abrasive lapping technology to achieve low-damage and high-precision surface processing of CaF2 component, which means that the CaF2 component is modified first and then the softened modified layer is removed by the porous diamond abrasive lapping. The H2O(g) plasma modification mechanism was elucidated through a combination of molecular dynamics simulation and experiment and comparison with H2O(g) plasma etching. The modification layer including an oxide layer and a phase change layer was produced by adjusting the plasma processing process (power of 25 W and H2O(g) content of 10 ml). Then the modified CaF2 component was lapped by the porous diamond abrasive tool on the ductile domain layer which is more than the modified layer and less than the sum of the modified layer and plastic domain. When the lapping process parameters were 200 rpm platen rotation speed and 20 N lapping pressure, a surface accuracy of 15.34 nm PV, 2.29 nm RMS (φ1 mm) was obtained. This study provides technical support for the low-damage processing of CaF2 component.

Alkaline-earth metal sulfide nanocrystals embedded in oxysulfide glasses

As a wide band gap semiconductor, alkaline-earth metal sulfides (AES) with low phonon energy, high laser damage threshold, and high transmittance in infrared, have wide application prospects in bioimaging, spectral conversion, and solid-state lighting. However, AES nanocrystals (NCs) suffer from the weak chemical-stability and low mechanical-stability, and can be easily oxidized in humidity and oxygen. Incorporation of AES NCs into inorganic glass is expected to overcome those inherent limitations. In this work, a new type of oxysulfide glass-ceramics containing CaS, SrS, BaS, SrxBa1−xS, and CaxSr1−xS NCs is developed, and average diameters of these AES NCs are tuned in the range of 3–18 nm. Precipitation of AES NCs not only improves the mechanical properties of glass, but also maintains high transmittance (˃60%) in the spectral range of 1–4.3 µm. Results reported in this work offer a new pathway for developing novel oxysulfide glass-ceramics for multi-functional optical devices.

Robust Type‐II Band Alignment and Stacking‐Controlling Second Harmonic Generation in GaN/ZnO vdW Heterostructure

AbstractMost traditional 2D materials have small bandgaps, resulting in low laser damage thresholds and limiting their applications in the ultraviolet region. Recently experimentally synthesized 2D GaN and ZnO can be such candidates due to their wide bandgaps, high charge mobilities, and optical transparency. Here, the van der Waals heterostructure GaN/ZnO is predicted that can exhibit both wide bandgap and strong second harmonic generation (SHG) response by compelling simulations. The results show the heterostructure always exhibits type‐II band alignment under all probable stacking configurations. The out‐of‐plane SHG coefficients are up to 90 pm V−1 at 400 nm, comparable to those of MoS2 and MoSe2 and higher than most 3D crystals. Interestingly, the positions are enhanced with localized, symmetric, and stacking‐dependent features in the Brillouin zone. This peculiar momentum space behavior is originated from the relative strength of two distinct mechanisms contributing to the second‐order nonlinear optical (NLO) response, that is, a purely interband transition part and a mixed interband‐intraband contribution. Thus, this study proposes that GaN/ZnO heterostructure may be an efficient and high laser damage thresholds (LDTs) NLO material and an interesting platform for studying NLO optical properties.

Sensitive and high laser damage threshold substrates for surface-enhanced Raman scattering based on gold and silver nanoparticles.

Surface-enhanced Raman scattering (SERS) is a sensitive and fast technique for sensing applications such as chemical trace analysis. However, a successful, high-throughput practical implementation necessitates the availability of simple-to-use and economical SERS substrates. In this work, we present a robust, reproducible, flexible and yet cost-effective SERS substrate suited for the sensitive detection of analytes at near-infrared (NIR) excitation wavelengths. The fabrication is based on a simple dropcast deposition of silver or gold nanomaterials on an aluminium foil support, making the design suitable for mass production. The fabricated SERS substrates can withstand very high average Raman laser power of up to 400mW in the NIR wavelength range while maintaining a linear signal response of the analyte. This enables a combined high signal enhancement potential provided by (i) the field enhancement via the localized surface plasmon resonance introduced by the noble metal nanomaterials and (ii) additional enhancement proportional to an increase of the applicable Raman laser power without causing the thermal decomposition of the analyte. The application of the SERS substrates for the trace detection of melamine and rhodamine 6G is demonstrated, which shows limits of detection smaller than 0.1ppm and analytical enhancement factors on the order of 104 as compared to bare aluminium foil.

Enhancing second harmonic generation response in infrared nonlinear optical material through Pb substitution: A study of Li2PbSiS4compound

The demand for infrared nonlinear optical (IR-NLO) materials is increasing due to their applications in many civil and military fields. However, a critical challenge revolves around achieving a good balance between a large second harmonic generation (SHG) response and a high laser damage threshold (LDT). Based on earlier study on Li2SrSiS4 compound which showed good SHG and high LDT performances, and to afford one new NLO material, we propose, in this work to replace the Sr atom with a P-bloc (Pb) atom in the Li2SrSiS4 compound. According to DFT calculations, the newly designed Li2PbSiS4 compound crystallizes in the stable stannite structure. In addition, it is thermodynamically, dynamically and mechanically stable. The investigated material presents an indirect bandgap of 2.48 eV employing the HSE06 approach, including spin-orbit coupling (SOC) effects. Moreover, the calculated SHG response is 0.85 × AgGaS2, which is larger than the SHG response of Li2SrSiS4. Furthermore, the SHG response increases directly with temperature, allowing using the compound at high temperatures. The obtained results may make the Li2PbSiS4 compound a promising NLO material.

Laser damage properties of LiB3O5 crystal surface under UV laser irradiation.

LiB3O5 (LBO) crystal has a very high bulk laser damage threshold. Laser damage often occurs on the surfaces with a large number of processing defects during application. In this paper, the surface laser damage threshold, damage growth threshold, and damage growth curve of LBO crystal and fused silica under the same processing process have been comparatively studied by using a 355 nm pulsed laser. The surface laser damage performance of LBO crystal has been comprehensive evaluated. The results show that the laser damage threshold and damage growth threshold of LBO are about twice that of fused silica, and the damage growth coefficient is about 0.7 times that of fused silica. The detection and analysis of impurity defects and photothermal weak absorption defects show that the subsurface defects of LBO crystal are less than that of fused silica. Laser damage morphologies show that the damage process is related to strongly bonded chemical structure and anisotropic physical characteristics of LBO crystal. These characteristics together determine the high threshold damage performance of LBO crystal. The results of this study are of great guidance for the application of LBO crystal in high-power laser systems.