Ultrahigh Nonlinear Responses from MXene Plasmons in the Short-Wave Infrared Range.

Surface plasmons in 2D materials such as graphene exhibit exceptional field confinement. However, the low electron density of majority of 2D materials, which are semiconductors or semimetals, has limited their plasmons to mid-wave or long-wave infrared regime. This study demonstrates that a 2D Ti3C2Tx MXene with high electron density can not only support strong plasmon confinement with an acoustic plasmon mode in the short-wave infrared region, but also provide ultrahigh nonlinear responses. The acoustic MXene plasmons (AMPs) in the MXene (Ti3C2Tx)-insulator (SiO2)-metal (Au) nanostructure generate in the 1.5-6.0 µm wavelength range, exhibiting a two orders of magnitude reduction in wavelength compared to wavelength in free space. Furthermore, AMP resonators with patterned Au rods exhibit a record-high nonlinear absorption coefficient of 1.37 × 10-2 m W-1 at wavelength of 1.56 µm, ≈3 orders of magnitude greater than the highest value recorded for other 2D materials. These results indicate that MXenes can overcome fundamental plasmon wavelength limitations of previously studied 2D materials, providing groundbreaking opportunities in nonlinear optical applications, including all-optical processing and ultrafast optical switching.

Synthesis, Physicochemical and Third Order Nonlinear Optical Properties of Bis-Chalcone (BBDP) as Donor-pi Acceptor Chromophore in Organize Medium.

Bis-Chalcone (BBDP) has been prepared by condensation of N, N-dimethyl benzaldehyde and 1,1'-([1,1'-biphenyl]-4,4'-diyl) di (ethan-1-one), and structure of BBDP was characterized by Mass Spectra, 13C-NMR, 1H-NMR, and IR. Physicochemical properties including Dipole-moments, Stoke-Shifts, Oscillator-strength, dielectric constant and quantum-yields of fluorescence of BBDP were investigated by the emission and absorbances in different solvents. Compound (BBDP) displayed bathochromic shift upon increasing the solvent polarity (from n-Hexane to DMSO). Furthermore, we have exploited third-order nonlinear optical characteristics of the bisChalone were invigilated by the Z-scan techniques in Chloroform. The measurements were taken with a continuous-wave (CW) diode laser having a wavelength of 520 nm in CHCl3 solvent. The third-order nonlinear optical properties, such as the nonlinear refractive index (NLRI) n2, nonlinear absorption coefficient (NLAC) ß, and nonlinear susceptibility χ(3), were measured at various solution concentrations and laser powers. The obtained values of n2, ß, and χ(3) were estimated to be high, of the order of 10-7(cm2/W), 10-3 (cm/W), and 10-6 (esu), respectively. As a result, bis-chalcone (BBDP) is considered as a promising candidate for applications in nonlinear optical (NLO) devices and optical limiting (OL).

Polarization Z-Scan Studies Revealing Plasmon Coupling Enhancement Due to Dimer Formation of Gold Nanoparticles in Nematic Liquid Crystals.

We investigate the plasmon coupling of gold nanoparticle (AuNP) dimers dispersed in a nematic liquid crystal matrix using the polarization z-scan technique. Our experimental setup includes the precise control of incident light polarization through polarization angles of 0°, 45°, and 90°. Two distinct cell orientations are examined: parallel and twisted nematic cells. In parallel-oriented cells, where liquid crystal molecules and AuNPs align with the rubbing direction, we observe a remarkable 2-3-fold increase in the nonlinear absorption coefficient when the polarization of the incident light is parallel to the rubbing direction. Additionally, a linear decrease in the third-order nonlinear absorption coefficient is noted as the polarization angle varies from 0° to 90°. In the case of twisted nematic cells, the NPs do not have any preferred orientation, and the enhancement remains consistent across all polarization angles. These findings conclusively establish that the observed enhancement in the nonlinear absorption coefficient is a direct consequence of plasmon coupling, shedding light on the intricate interplay between plasmonic nanostructures and liquid crystal matrices.

Cubic Nonlinearity of Graphene-Oxide Monolayer.

The cubic nonlinearity of a graphene-oxide monolayer was characterized through open and closed z-scan experiments, using a nano-second laser operating at a 10 Hz repetition rate and featuring a Gaussian spatial beam profile. The open z-scan revealed a reverse saturable absorption, indicating a positive nonlinear absorption coefficient, while the closed z-scan displayed valley-peak traces, indicative of positive nonlinear refraction. This observation suggests that, under the given excitation wavelength, a two-photon or two-step excitation process occurs due to the increased absorption in both the lower visible and upper UV wavelength regions. This finding implies that graphene oxide exhibits a higher excited-state absorption cross-section compared to its ground state. The resulting nonlinear absorption and nonlinear refraction coefficients were estimated to be approximately ~2.62 × 10-8 m/W and 3.9 × 10-15 m2/W, respectively. Additionally, this study sheds light on the interplay between nonlinear absorption and nonlinear refraction traces, providing valuable insights into the material's optical properties.

Two-photon absorption in colloidal semiconductor nanocrystals: a review.

Large two-photon absorption (2PA) cross-section combined with high emission quantum efficiency and size-tunable bandgap energy has put colloidal semiconductor nanocrystals (NCs) on the vanguard of nonlinear optical materials. After nearly two decades of intense studies on the nonlinear optical response in quantum-confined semiconductors, this is still a vibrant field, as novel nanomaterials are being developed and new applications are being proposed. In this review, we examine the progress of 2PA research in NCs, highlighting the impact of quantum confinement on the magnitude and spectral characteristics of this nonlinear response in semiconductor materials. We show that for NCs with three-dimensional quantum confinement, the so-called quantum dots, 2PA cross-section grows linearly with the nanoparticle volume, following a universal volume scaling. We overview strategies used to gain further control over the nonlinear optical response in these structures by shape and heterostructure engineering and some applications that might take advantage of the series of unique properties of these nanostructures.

Investigations on the Nonlinear Optical Properties of 0D, 1D, and 2D Boron Nitride Nanomaterials in the Visible Spectral Region.

In recent years, boron nitride nanomaterials have attracted increasing attention due to their unique properties such as high temperature stability and high thermal conductivity. They are structurally analogous to carbon nanomaterials and can also be generated as zero-dimensional nanoparticles and fullerenes, one-dimensional nanotubes and nanoribbons, and two-dimensional nanosheets or platelets. In contrast to carbon-based nanomaterials, which have been extensively studied during recent years, the optical limiting properties of boron nitride nanomaterials have hardly been analysed so far. This work summarises a comprehensive study on the nonlinear optical response of dispersed boron nitride nanotubes, boron nitride nanoplatelets, and boron nitride nanoparticles using nanosecond laser pulses at 532 nm. Their optical limiting behaviour is characterised by means of nonlinear transmittance and scattered energy measurements and a beam profiling camera is used to analyse the beam characteristics of the transmitted laser radiation. Our results show that nonlinear scattering dominates the OL performance of all measured boron nitride nanomaterials. Boron nitride nanotubes show a large optical limiting effect, much stronger than the benchmark material, multi-walled carbon nanotubes, which makes them promising for laser protection applications.

Excellent ultraviolet optical limiting properties of Se nanosheets.

Selenium (Se) is located in the fourth period of the periodic table in group VIA (element 34). In this experiment, three different solvents (isopropyl alcohol, N-methyl-2-pyrrolidone, and ethanol) were used to prepare the two-dimensional Se nanosheets, which were manufactured by the liquid phase exfoliation method with a thickness of 3.35-4.64 nm and a transverse scale of several hundred nanometers. The nonlinear absorption properties at 355, 532, and 1064 nm were studied using the open apertureZ-scan technique. Final results showed that Se nanosheets exhibited optical limiting (OL) effect in all three wavebands and three solvents, and had large two-photon absorption coefficients, especially in ultraviolet (UV) waveband. Which proved that Se nanosheets had great potential application as excellent OL materials in UV waveband. Our research broadens the path for the semiconductor field of Se, inspires the application of Se in nonlinear optics field.

Fabrication, Characterization of Basic Blue 7 Dye-Doped PVA Films and Their Third-Order Nonlinear Optical Properties.

In this work, we report on the fabrication, characterization and the third-order nonlinear optical (NLO) properties of basic blue 7 (BB 7) dye‒doped polyvinyl alcohol (PVA) polymer thin films. The absorption spectra of BB 7 dye‒PVA films were measured by UV‒visible absorption studies. The functional groups of BB 7‒PVA films have been identified by FT‒IR spectroscopic analysis. The surface morphology was examined by AFM and SEM analysis which shows that the BB 7 dye‒doped PVA films have a homogenous and smooth surface. The nonlinear absorption and refraction of BB 7‒PVA films were respectively explored by open aperture and closed aperture Z‒scan technique using a 5 mW semiconductor diode laser of 635 nm wavelengths. The BB 7‒PVA films exhibit the reverse saturable absorption (RSA) and self-defocusing effect and the measured third‒order nonlinear susceptibility χ(3) values of these films were found to be of the order of 10- 5 esu. The present experimental results show that BB 7‒PVA films may have potential applications in future photonic and NLO devices.

Siloxene Nanosheets and Their Hybrid Gel Glasses for Broad-Band Optical Limiting.

With the development of laser technology, the research of novel laser protection materials is of great significance. In this work, dispersible siloxene nanosheets (SiNSs) with a thickness of about 1.5 nm are prepared by the top-down topological reaction method. Based on the Z-scan and optical limiting testing under the visible-near IR ranges nanosecond laser, the broad-band nonlinear optical properties of the SiNSs and their hybrid gel glasses are investigated. The results show that the SiNSs have outstanding nonlinear optical properties. Meanwhile, the SiNSs hybrid gel glasses also exhibit high transmittance and excellent optical limiting capabilities. It demonstrates that SiNSs are promising materials for broad-band nonlinear optical limiting and even have potential applications in optoelectronics.

Nonlinear absorption-based analysis of energy deposition in melanosomes for 532-nm short-pulsed laser skin treatment.

BACKGROUND AND OBJECTIVES: The clinical use of 532-nm short-pulsed lasers has provided effective treatment of epidermal pigmented lesions. However, the detection of significant differences in treatment effects between picosecond and nanosecond lasers has still varied among clinical studies. For robust evaluation of the differences based on the treatment mechanism, this study presents a nonlinear absorption-based analysis of energy deposition in melanosomes for 532-nm short-pulsed laser treatment. STUDY DESIGN/MATERIALS AND METHODS: Nonlinear absorption by melanin is modeled based on sequential two-photon absorption. Absorption cross-sections and nonradiative lifetimes of melanin, which are necessary for the nonlinear absorption-based analysis, are determined from transmittance measurement. Using the model and parameters, energy deposition in melanosomes was calculated with varying fluence and pulse width settings, including actual clinical parameters. RESULTS: The energy deposition in melanosomes increased with shorter laser pulses, and subnanosecond laser pulses were found to be most efficient. The comparison of energy deposition calculated using clinical parameters demonstrated the differences in treatment effects between picosecond and nanosecond lasers reported in clinical studies. CONCLUSION: The nonlinear absorption-based analysis provides quantitative evidence for the safety and efficacy evaluation of short-pulsed laser treatments, which may lead to the establishment of numerical indices for determining treatment conditions. Future studies considering the effects of the surrounding tissue on energy deposition in melanosomes will be needed.

Nonlinear Optical Properties of Zinc Oxide Nanoparticle Colloids Prepared by Pulsed Laser Ablation in Distilled Water.

The nonlinear optical properties of zinc oxide nanoparticles (ZnONPs) in distilled water were measured using a femtosecond laser and the Z-scan technique. The ZnONPs colloids were created by the ablation of zinc bulk in distilled water with a 532 nm Nd: YAG laser. Transmission electron microscopy, an ultraviolet-visible spectrophotometer, and atomic absorption spectrophotometry were used to determine the size, shape, absorption spectra, and concentration of the ZnONPs colloids. The nonlinear absorption coefficient and nonlinear refractive index were measured at different excitation wavelengths and intensities. The nonlinear absorption coefficient of the ZnONPs colloids was found to be positive, caused by reverse saturable absorption, whereas the nonlinear refractive index was found to be negative due to self-defocusing in the ZnONPs. Both laser parameters, such as excitation wavelength and input intensity, and nanoparticle features, such as concentration and size, were found to influence the nonlinear optical properties of the ZnONPs.

Using Femtosecond Laser Pulses to Explore the Nonlinear Optical Properties of Au NP Colloids That Were Synthesized by Laser Ablation.

In this study, we experimentally investigated the nonlinear optical properties of Au nanoparticles (Au NPs) that were prepared in pure distilled water using the laser ablation method. The Au NPs were prepared using a nanosecond Nd:YAG laser with an ablation time of 5 or 10 min at a constant laser energy of 100 mJ. The structure and the linear optical properties of the Au NPs were investigated using a transmission electron microscope (TEM) and UV-visible spectrophotometer analysis, respectively. The TEM measurements showed that the average size of the Au NPs varied from 20.3 to 14.1 nm, depending on the laser ablation time. The z-scan technique was used to investigate the nonlinear refractive index (n2) and nonlinear absorption coefficient (γ) of the Au NPs, which were irradiated at different excitation wavelengths that ranged from 740 to 820 nm and at different average powers that ranged from 0.8 to 1.6 W. The Au NP samples exhibited a reverse saturable absorption (RSA) behavior that increased when the excitation wavelength and/or incident laser power increased. In addition, the Au NPs acted as a self-defocusing material whenever the excitation wavelength or incident power were modified.

Synthesis, Linear and Nonlinear Optical Properties of Ag/Al2O3 Nanocomposites.

This work reports a detailed study of the synthesis, characterization and third-order nonlinear optical properties of Ag and Al2O3 nanoparticles and their polymer nanocomposites. Ag and Al2O3 nanoparticles were prepared by the chemical precipitation method. The X-ray diffraction studies confirmed the purity and the crystalline nature of the sample and revealed the crystallite size. The linear optical properties and the structural morphology of the nanoparticles were confirmed using UV-visible spectroscopy and SEM analysis. The prepared nanoparticles were introduced into the polymer matrix by the spin-coating technique. Open-aperture and closed-aperture Z-scan technique was used to study the nonlinear absorption and nonlinear refraction of the samples under a Q-switched Nd:YAG laser at 532 nm. The observed third-order nonlinear optical susceptibility (χ(3)) was on the order of 10-6 esu, which indicates that these materials are potential candidates for photonic applications.

Femtosecond Laser-Induced Anisotropic Structure and Nonlinear Optical Response of Yttria-Stabilized Zirconia Single Crystals with Different Planes.

Nonlinear optical properties have been extensively studied due to their promising nonlinear effects and various applications. With ultrashort duration and ultrahigh intensity, a femtosecond laser can fabricate various superior-quality micro-/nanostructures to improve the nonlinearity of materials, which are promising for stable and high-performance nonlinear devices. In this contribution, yttria-stabilized zirconia (YSZ) with fs laser-induced micro-/nanostructures is demonstrated to exhibit unique anisotropic light-material interaction and nonlinear optical response on [100], [110], and [111] planes. Time-resolved reflectivity of YSZ after fs laser excitation is investigated by a pump-probe experiment, which is consistent with simulations through the plasma model combined with a two-temperature model. These results indicate two early ablation mechanisms: Coulomb explosion and melting. Anisotropic crack structures are formed due to thermal stress, which is always ignored in fs laser fabrication and is verified by Raman mapping and analysis of slip systems on different crystal planes. Through the z-scan measurement, the nonlinear absorption (NLA) of crack structures is effectively improved, and a nearly 18 times enhancement of the NLA coefficient is acquired in [100] samples, while a 2 times enhancement in [110] and [111] samples. Such great enhancement of NLA is mainly due to the abundant presence of crack structures and the increase of fs laser-induced oxygen vacancies in [100] YSZ. These results provide a potential way of utilizing fs laser to improve the nonlinearity for the technological development in nonlinear devices.

Nonlinear Optical Activities in Two-Dimensional Gallium Sulfide: A Comprehensive Study.

The nonlinear optical (NLO) properties of two-dimensional (2D) materials are fascinating for fundamental physics and optoelectronic device development. However, relatively few investigations have been conducted to establish the combined NLO activities of a 2D material. Herein, a study of numerous NLO properties of 2D gallium sulfide (GaS), including second-harmonic generation (SHG), two-photon excited fluorescence (TPEF), and NLO absorption are presented. The layer-dependent SHG response of 2D GaS identifies the noncentrosymmetric nature of the odd layers, and the second-order susceptibility (χ2) value of 47.98 pm/V (three-layers of GaS) indicates the superior efficiency of the SHG signal. In addition, structural deformation induces the symmetry breaking and facilitates the SHG in the bulk samples, whereas a possible efficient symmetry breaking in the liquid-phase exfoliated samples results in an enhancement of the SHG signal, providing prospective fields of investigation for researchers. The generation of TPEF from 800 to 860 nm depicts the two-photon absorption characteristics of 2D GaS material. Moreover, the saturable absorption characteristics of 2D GaS are realized from the largest nonlinear absorption coefficient (ß) of -9.3 × 103, -91.0 × 103, and -6.05 × 103 cm/GW and giant modulation depths (Ts) of 24.4%, 35.3%, and 29.1% at three different wavelengths of 800, 1066, and 1560 nm, respectively. Hence, such NLO activities indicate that 2D GaS material can facilitate in the technical advancements of future nonlinear optoelectronic devices.

Broad-Band Ultrafast All-Optical Switching Based on Enhanced Nonlinear Absorption in Corrugated Indium Tin Oxide Films.

Ultrafast all-optical switches based on epsilon-near-zero (ENZ)-enhanced nonlinear refraction in transparent conducting oxides have achieved exciting results in realizing large absolute modulations. However, broad-band, polarization-independent, and wide-angle ultrafast all-optical switches have been challenging to produce, due to the inherent narrow band, polarization-dependent, and angle-dependent characteristics of the ENZ effect. To this end, we propose an ultrafast all-optical switch based on the enhanced nonlinear absorption of corrugated indium tin oxide (ITO) thin films. Taking advantage of the perfect absorption and localized field enhancement of the ENZ and localized surface plasmon resonance modes, we significantly enhanced the nonlinear absorption of the corrugated ITO film in the 1450-1650 nm telecom band. The experimental results show that the nonlinear saturable absorption coefficient of the corrugated ITO film at 1450 nm was as high as -1.5 × 105 cm GW-1, enabling all-optical switching to obtain an extinction ratio of 14.32 dB and an ultrafast switching time of 350 fs at a pump fluence of 18.51 mJ cm-2. Furthermore, the all-optical switch achieved an extinction ratio of over 15 dB and an insertion loss of approximately 2.6 dB within the 200 nm absorption band and exhibited polarization-independent and wide-angle features. The ultrafast temporal response can be attributed to intraband transient bleaching of the corrugated ITO film. Our findings demonstrate that corrugated ENZ films can overcome the inherent narrow-band, polarization-dependent, and angle-dependent problems of natural ENZ materials without increasing the response time, making them a potential ENZ ultrafast all-optical switching material platform.

Multi-Foci Laser Separation of Sapphire Wafers with Partial Thickness Scanning.

With multi-foci laser cutting technology for sapphire wafer separation, the entire cross-section is generally scanned with single or multiple passes. This investigation proposes a new separation technique through partial thickness scanning. The energy effectivity and efficiency of the picosecond laser were enhanced through a two-zone partial thickness scanning by exploiting the internal reflection at the rough exit surface. Each zone spanned only one-third thickness of the cross-section, and only two out of three zones were scanned consecutively. A laser beam of 0.57 W and 50 kHz pulse repetition rate was split into 9 foci, each with a 2.20 µm calculated focused spot diameter. By only scanning the top two-thirds sample thickness, first its middle section then upper section, a cleavable sample could result. This was achieved with the lowest energy deposition at the fastest scanning speed of 10 mm/s investigated. Although with partial thickness scanning only, counter intuitively, the cleaved sample had a previously unattained uniform roughened sidewall profile over the entire thickness. This is a desirable outcome in LED manufacturing. As such, this proposed scheme could attain a cleavable sample with the desired uniformly roughened sidewall profile with less energy usage and faster scanning speed.

Investigation of Nonlinear Optical Processes in Mercury Sulfide Quantum Dots.

The authors report the third-harmonic generation, nonlinear refraction, and nonlinear absorption in HgS quantum dot (QD) suspensions and films using the nanosecond and femtosecond pulses. High conversion efficiency (7 × 10-4) towards the third harmonic (TH) of the 900-1700 nm, 150 fs laser in the thin (70 nm) films containing HgS QDs deposited on the glass substrates is obtained. The authors analyze spectral dependencies of the TH, nonlinear refractive indices, and nonlinear absorption coefficients of QDs in the 500-1700 nm range and discuss the relation between the TH process and the low-order nonlinear optical properties of these quantum dots.

Record Aluminum Molecular Rings for Optical Limiting and Nonlinear Optics.

Crystalline cluster materials, a class of functional motif aggregations, provide a great opportunity for tuning the properties stemming from the flexible and accurate variation of inorganic and organic compositions. In this study, we demonstrate the effects of functional ligand and ring size regulation on the structures and third-order nonlinear optical (NLO) properties. Revealed by the single-crystal X-ray analysis results, aluminum molecular ring expansion is achieved by 2×9 and 3×6 strategies. In terms of the given organic shells, we further tuned the aluminum molecular ring sizes from 3.0 nm to 1.7 nm. The picosecond Z-scan measurements results revealed that the third-order NLO performances do not only depend on the general conjugate interactions but are also related to hydrogen bonding, polarizability, and ring sizes. The large nonlinear absorption coefficient and onset prove that the observed samples are promising candidates for the field of nonlinear optics.

Interfacial Charge Transfer and Ultrafast Photonics Application of 2D Graphene/InSe Heterostructure.

Interface interactions in 2D vertically stacked heterostructures play an important role in optoelectronic applications, and photodetectors based on graphene/InSe heterostructures show promising performance nowadays. However, nonlinear optical property studies based on the graphene/InSe heterostructure are insufficient. Here, we fabricated a graphene/InSe heterostructure by mechanical exfoliation and investigated the optically induced charge transfer between graphene/InSe heterostructures by taking photoluminescence and pump-probe measurements. The large built-in electric field at the interface was confirmed by Kelvin probe force microscopy. Furthermore, due to the efficient interfacial carrier transfer driven by the built-in electric potential (~286 meV) and broadband nonlinear absorption, the application of the graphene/InSe heterostructure in a mode-locked laser was realized. Our work not only provides a deeper understanding of the dipole orientation-related interface interactions on the photoexcited charge transfer of graphene/InSe heterostructures, but also enriches the saturable absorber family for ultrafast photonics application.