UV-induced two-photon absorption in BiB3O6 single crystals

We show that BiB₃O₆ (BiBO) crystals, well known for their excellent second harmonic generation (SHG) properties, may also be of interest for third-order optical phenomena, particularly for two-photon absorption (TPA). Photoinduced TPA measurements were performed under illumination of excimer Xe–F laser (λ = 217 nm) as a photoinducing (pumping) beam. It created a thin surface layer (about 85 nm) that was a source of the observed photoinduced TPA. Raman shifted Nd-YAG laser radiation (λ = 1.9 μm) as well as its second and fourth harmonics (λ = 950 and λ = 475 nm, respectively) were used as fundamental (probing) beams of the TPA. The highest values of the TPA β coefficient were achieved for a polarization of the pumping light directed along crystallographic axis b. Quantum chemical simulations indicate on substantial contribution of UV-induced electron–phonon anharmonicity to the observed TPA. The obtained values of TPA coefficients indicate a possibility of using BiBO crystals as UV-operated optical limiters in a wide spectral range.     

Manifestation of nano-sized effects in photoinduced nonlinear optics of CdI2–Cu layered single crystals

The infrared (IR) induced second harmonic generation in the thin CdI₂–Cu crystalline layers was discovered. With decreasing thickness of the CdI₂–Cu crystals up to several nanometers value of second-order nonlinear optical susceptibility d₁₄ (at wavelength λ=2.76 μm) for the output IR-induced SHG significantly increases. For the Cu content about 0.4% the output SHG signal achieves its maximum at the sample thickness below 2 nm. It is important that for the samples with larger film thickness the corresponding changes have substantially different properties. Limitation of the d₁₄ at the larger concentration is probably caused by formation of the Cu clusters limiting the enhancement of the hyperpolarizability for particular cluster as well as total nonlinear dielectric susceptibility.     

Manifestation of hexagonal-like structure in the second-order nonlinear effects in the GaN nanocrystallites

Contribution of the hexagonal-like structural components to the photoinduced second harmonic generation (SHG) in GaN large-sized nanocrystallites (with sizes about the 10–30 nm) incorporated into the polyvinylalcohol photopolymer matrices is revealed. The SHG measurements were done using pulsed Nd:YAG laser beam (λ=1.06 μm; pulse duration τ=15–50 ps, laser power about 30 MW) as a fundamental ones and a picosecond nitrogen pulsed laser (P=10 MW; λ=0.377 μm; pulse time duration τ=10–25 ps) as a photoinducing one. We have found that with increasing pumping power density the SHG output signal increases and achieves its maximum value for the power density about 2.6 GW/cm² per pulse. The maximal output photoinduced SHG signal was achieved for parallel directions of the pumping and fundamental beam polarizations. The maximal values of the second-order nonlinear susceptibilities were equal to about 1.09 pm/V. We have observed an increase of the output SHG below 30 K and for pump-probe delaying time about 18 ps. Substantial contribution to the SHG of wurtzite-like (hexagonal) structural fragments is shown.     

Second harmonic generation in In2O3–SiON films doped by Al and Sn

Photoinduced optical and second-order non-linear optical effects in the interfaces separating In₂O₃–SiON (O/N ratio equals 1) films doped with A1, Sn and glass substrates were investigated using the photoinduced optical second harmonic generation. The photoinduced effective second-order optical susceptibility d_eff (at λ=1.76 μm) shows a good correlation with the linear optical susceptibility, particularly with the shift of the absorption edge. The maximal response of the photoinduced optical response signal was observed for the pump–probe delaying time of 34 ps. The performed experimental measurements indicate that the observed effects are mainly caused by the interface potential gradients on the border glass–In₂O₃–SiON film and by additional polarization due to insertion of the Al and Sn atoms. The observed phenomenon may be proposed as a sensitive tool for investigation of thin semiconducting interfacial layers and simultaneously such films may be used as materials for non-linear optical devices.     

Nanometer-scale probing of optical and thermal near-fields with an apertureless NSOM

We have used a home-made apertureless near-field scanning optical microscope (ANSOM) for mapping nanometric steps between SiC and gold regions under visible (λ=655 nm) and infrared (λ=10.6 μm) illumination. The images, obtained with a signal demodulation at the tip oscillation frequency and at higher harmonics, clearly show optical contrasts with a subwavelength resolution of about 30 nm. Other images recorded in the visible on a YBa₂Cu₃O₇ crystal indicate that the tip used in our experiments is able to reveal polarization effects. We also present a near-field thermal optical microscope (NTOM) which operates without any external illumination. In this new kind of microscope, the laser source which is usually used to excite the evanescent waves, is replaced by a simple heating of the sample. The electromagnetic radiation locally scattered by the tip comes from the thermal radiation. Our results with this new technique prove a 200 nm lateral resolution.     

A DFG spectrometer at 3 μm for high resolution molecular spectroscopy and trace gas detection

We report the realization and characterization of a spectrometer based on difference frequency generation using a periodically poled lithium niobate crystal. As signal and pump lasers we used a diode-pumped Nd–YAG laser (λ=1.064 μm) and an extended cavity semiconductor diode laser (λ=0.785 μm), respectively. The mid-infrared coherent radiation was produced at 3 μm with a maximum power of about 160 nW obtained with 340 mW of signal and only 3.4 mW of pump. That corresponds to an efficiency of 0.01%/Wcm, which is in good agreement with other data available in literature. The generated radiation around 3 μm has allowed us to study fundamental absorption bands of molecules of great atmospheric and physical interest such as water vapor and the hydroxyl free radical. In this work we report preliminary spectroscopic results concerning the ν₁ 5₄₁→6₅₂ H₂O line at 2.968 μm. In particular, for this line we provide the first experimental estimation of self-, N₂- and O₂-broadening coefficients.     

Photoinduced non-linear optical diagnostic of SiNxOy/Si111 interfaces

Anisotropic (elliptically polarized) photoinduced second harmonic generation (PISHG) in SiN_xO_y/Si1 1 1 films was proposed for contact-less monitoring of specimens with different nitrogen to oxygen (N/O) ratios. As a source for the photoinducing light, we used a nitrogen Q-switched pulse laser at wavelengths of 315, 337 and 354 nm as well as doubled frequency YAG–Nd laser wavelength (λ=530 nm). The YAG : Nd pulse laser (λ=1.06 μm; W=30 MW; τ=10–50 ps) was used to measure the PISHG. All measurements were done in a reflected light regime. We found that the output PISHG signal was sensitive to the N/O ratio and the film thickness. Measurements of the PISHG versus pumping wavelengths, powers, incident angles as well as independent measurements of the DC-electric field induced second harmonic generation indicate the major role played in this process by axially symmetric photoexcited electron–phonon states. The SiN_xO_y films were synthesized using a technique of chemical evaporation at low pressures. Films with thickness varying between 10 and 30 nm and with an N/O ratio between 0 and 1 were obtained. Electrostatic potential distribution at the Si1 1 1–SiN_xO_y interfaces was calculated. Comparison of the experimentally obtained and quantum chemically calculated PISHG data are presented. High sensitivity of anisotropic PISHG to the N/O ratio and film thickness is revealed. The role of the electron–phonon interactions in the dependencies observed is discussed. We have shown that the PISHG method has higher sensitivity than the traditional extended X-ray absorption fine structure spectroscopic and linear optical method for films with the N/O ratio higher than 0.50.     

Dynamic moiré patterns produced by sinusoidal gratings superposition in the Bi12 TiO20 crystal

In the present note a real-time holographic moire-like pattern is shown. It is produced by the superposition of two rotated sinusoidal phase gratings and the result represents a promising technique for possible metrological applications. The experiments were performed in a diffusion-only recording mechanism in a photorefractive Bi₁₂TiO₂₀ crystal illuminated by λ = 0.633 μm from a HeNe laser light source.     

Angular distribution of intensity of reflected radiation investigations of the influence of CO2 laser treatment on optical properties of hydrogenated amorphous silicon

Thin films of hydrogenated amorphous silicon (a-Si:H) were annealed using CO₂ laser radiation (λ=10.6 μm). Changes of optical properties of the treated a-Si:H were investigated using optical transmittance spectroscopy and the angular distribution of intensity of reflected radiation (ADIRR). The CO₂ laser annealing influences the spectral characteristics of the real part of refractive index n and absorption coefficient α of light in a-Si:H. This treatment increases the n and α values as well as the Urbach energy of a-Si:H. Simultaneously it decreases the optical energy gap of this material. The changes of optical parameters at the interfaces of a-Si:H–glass substrate and a-Si:H–air were established.     

Spectroscopic and laser properties of Nd:Gd0.8La0.2VO4 crystal

The polarised absorption and fluorescence spectra of Nd:Gd_0.8La_0.2VO₄ crystal are measured and compared to those of Nd:GdVO₄. CW laser properties of diode-pumped Nd:Gd_0.8La_0.2VO₄ crystal operating at fundamental wavelengths of 1.06 and 1.34 μm, as well as when intracavity frequency-doubled to 532 and 670 nm, have been studied. The maximum output powers at 1.06 μm, 1.34 μm, 532 nm and 670 nm are 1.18 W, 671 mW, 206 mW and 42 mW respectively, at a diode-launched pump power of 2.9 W. The threshold pump powers are 80, 267, 7 and 15 mW respectively.     

Photoinduced second-order optical susceptibilities of Er2O3 doped TeO2-GeO2-PbO glasses

Second-order optical susceptibilities were established in the optically poled erbium doped tellurite glasses near the melting temperature. The non-linear optical susceptibility was formed by bicolor coherent optical treatment performed by two coherent laser beams originated from 50 ps Nd-YAG laser (λ = 1.32 μm) exciting the high pressure hydrogen laser cell emitting at 1907 nm. The non-centrosymmetric grating of the medium was created by coherent superposition of the fundamental laser illumination at 1907 nm and the doubled frequency one at 953.5 nm. The maximally all-optically poled SHG occurs for 2% doped Er₂O₃ (in weighting units) TeO₂-GeO₂-PbO glass. It was found that the photoinduced SHG demonstrates a saturation during the photo-treatment of 9-10 min using the two beams polarized at angle about 45° between them. During the coherent bicolor optical treatment it was achieved the value of second-order susceptibility up to 3.6 pm/V at 1907 nm. The optimal ratio between the fundamental beam with power density about 1.1 GW/cm² and writing doubled frequency seeding beam about 0.015 GW/cm² corresponds to the maximal of photoinduced SHG. For glasses with lower concentration of Er₂O₃, the relaxation of the second-order optical susceptibility is substantially longer and achieves SHG value that corresponds to 80% of the maximal ones. It is necessary to emphasize that efficient optically-poled grating exists only within the narrow temperature range near the glassing temperature. Possible physical mechanisms of the phenomenon observed are discussed. Generally the used glasses possess better parameters than early investigated germinate glasses.     

High repetition rate mid-infrared laser source

An efficient, high-power mid-infrared laser source based on ZnGeP₂ (ZGP) optical parametric oscillator (OPO) is presented. Using a Q-switched Ho:YAG laser as the pump source a total output power of 10.6 W was obtained in the 3–5 μm band at 10 kHz and 8.5 W at 20 kHz. The Ho:YAG laser was pumped by two diode-pumped polarization coupled Tm:YLF lasers. Optical-to-optical efficiency achieved is >8.8% (laser-diode 792 nm to mid-IR 3–5 μm). With a commercial PtSi infrared camera (256×256 pixel focal plane array, 24 μm pitch) the pointing stability of Ho pump, signal and idler beam was measured to be better than 30 μrad. Whilst propagating the OPO beams over 100 m, little absorption for the idler beam was observed, resulting in a significant higher peak-to-peak value of ±22%, whereas the peak-to-peak stability of the signal pulses remained unchanged (±13%). To cite this article: M. Schellhorn et al., C. R. Physique 8 (2007).     

Study on nonlinear optical absorption properties of [(CH3)4N]2[Cu(dmit)2] by Z-scan technique

The third-order optical nonlinearities of an organo-metallic compound, [(CH₃)₄N]₂[Cu(dmit)₂] (dmit²⁻=4,5-dithiolate-1,3-dithiole-2-thione), abbreviated as MeCu, dissolved in acetone are characterized by Z-scan technique with picosecond and nanosecond laser pulses in the near-infrared region. Two-photon absorption has been found when the sample solution is irradiated by 40 ps pulse width at 1064 nm and the two-photon absorption (TPA) coefficient β_TPA is 4×10⁻¹³ m/W. While excited by 15 ns laser pulses at 1053 nm, the Z-scan spectra reveal strong reverse saturable absorption (RSA) and the nonlinear absorption coefficient β_RSA is estimated to be as high as 7.07×10⁻¹¹ m/W which is much larger than β_TPA. An explanation for this enhancement is given. All the results suggest that MeCu may be a promising candidate for the application to optical limiting in the near-infrared region.     

Intra-cavity second harmonic generation with Nd:YVO4/BIBO laser at 542 nm

We report, for the first time, an efficient intra-cavity second-harmonic generation (SHG) at 1084 nm in a nonlinear optical crystal, BiB₃O₆(BIBO) at the direction of (θ, ?) = (170.1°, 90°), performed with a LD end-pumped cw Nd:YVO₄ laser. With 590 mW diode pump power, a continuous-wave (cw) SHG output power of 19 mW at 542 nm yellow-green color has been obtained using a 1.5 mm-thick BIBO crystal. The optical conversion efficiency was 3.22%. It was found that the output wavelength could be 532 nm, 537 nm or 542 nm according to regulating the angle of BIBO.     

The optical properties and laser characteristics of Cr and Nd co-doped Y3Al5O12 ceramics

We have fabricated Cr³⁺ and Nd³⁺ co-doped YAG (Cr;Nd:YAG) ceramics, and investigated their optical properties and laser characteristics. The Cr;Nd:YAG has two broad absorption bands at around 440 nm (⁴A₂→⁴T₁) and 600 nm (⁴A₂→⁴T₂) respectively, caused by Cr³⁺ ions. In the case of pumping at 440 nm, the maximum effective lifetime of the Cr;Nd:YAG was 737 μs with a 0.1 at% Cr³⁺ and 1.0 at% Nd³⁺ co-doped YAG sample. Cr³⁺ ions take a role of an effective sensitizer to convert the UV light of flashlamp. For single-shot laser operation, a 10.4 J output energy at 1064 nm was obtained with 0.1 at% Cr³⁺ and 1.0 at% Nd³⁺ co-doped YAG ceramic rod with a laser efficiency of 4.9%. The laser efficiency was found to be more than twice that of a 1.0 at % Nd³⁺:YAG ceramic rod.     

Efficient diode-pumped Nd:YVO4 continuous-wave laser at 1.34 μm

We report a high-power continuous-wave(cw) diode-pumped efficient 1.34 μm Nd:YVO₄ laser. The laser properties of a low Nd³⁺-doped concentration of the Nd:YVO₄ crystal operating at 1.34 μm formed with a simple plane-concave cavity have been demonstrated. With the incident pump power of 22 W, an output power of 8.24 W was obtained, giving an optical conversion efficiency of 37.5% and slope efficiency of 40%. The thermal effects of cw end-pumped solid-state lasers were studied.     

Preparation and optical constants of the nano-crystal and polymer composite Bi4Ti3O12/PMMA thin films

Bismuth titanate, Bi₄Ti₃O₁₂ (BTO), is a typical ferroelectric material with useful properties for optical memory, piezoelectric and electro-optic devices. Its nano-crystals were compounded by the chemical solution decomposition technique. Its structure and size were analyzed by X-ray diffraction and transmissive electron microscopy. The composite thin film of BTO nano-crystals and high transparency polymethylmethacrylate (PMMA) polymer was prepared by spin coating. The transmitted spectrum of BTO/PMMA composite thin film in 300–1500 nm was measured. The film thickness d and the optical constants of the film, such as the refractive index n, the absorption coefficient α, and the extinction coefficient κ were obtained using the data from the transmitted spectrum.     

Compact eye-safe laser sources based on OPOs with KTP or PPKTP crystals

We report on compact eye-safe nanosecond laser sources emitting in the 1.5 μm wavelength range based on non-critically phase-matched parametric interaction in optical parametric oscillators (OPOs) with KTP and periodically poled KTP (PPKTP) crystals, pumped by the fundamental frequency of Nd:YAG lasers. As much as 250 μJ signal pulse energy at 1.5 μm wavelength, 6.5 ns FWHM pulse-width, has been obtained in a PPKTP-OPO, extracavity pumped by a Nd:YAG microlaser oscillator–amplifier at 650 μJ pump pulse energy, 8 ns pulse-width. A single signal pulse of 2.7-mJ output energy at 1.57 μm wavelength, less than 5 ns pulse-width, was generated in a KTP-OPO, intracavity pumped by a passively Q-switched Nd:YAG laser.     

Resonant-cavity-enhanced photodetectors and LEDs in the mid-infrared

In this paper we outline the use of resonant-cavity enhancement for increasing the exterior coupling efficiency of photodetectors and light-emitting diodes (LEDs) in the mid-infrared (MIR) spectral region. This method is potentially very important in the MIR because encapsulation is not presently feasible due to the lack of suitable materials. Among other potential applications, resonant-cavity-enhanced (RCE) photodetectors and LEDs could be particularly suitable for greenhouse gas detection because of their ‘pre-tunable’ spectrally narrowed resonantly enhanced peaks. We also present the optical characterization of an InAs RCE photodetector aimed at the detection of methane gas (λ≈3.3 μm), and an InAs/InAs_0.91Sb_0.09 resonant-cavity LED (RCLED) aimed at carbon dioxide gas (λ≈4.2 μm). The high peak responsivity of the RCE photodetector was 34.7 A/W at λ=3.14 μm, and the RCLED peaked at λ=3.96 μm. These are among the longest operating wavelengths for III–V RCE photodetectors and RCLEDs reported in the literature.     

A novel CO2 gas analyzer based on IR absorption

Carbon dioxide (CO₂) gas analyzer can be widely used in many fields. A novel CO₂ gas analyzer based on infrared ray (IR) absorption is presented sufficiently in this paper. Applying Lambert–Beer Law, a novel space-double-beam optical structure is established successfully. The optical structure includes an IR source, a gas cell, a bandpass filter with a transmission wavelength at 4.26 μm, another bandpass filter with a transmission wavelength at 3.9 μm, and two IR detectors. Based on Redial Basic Function (RBF) artificial neural network, the measuring model of IR CO₂ analyzer is established with a high accuracy. A dynamic compensation filter is effectively designed to improve the dynamic characteristic of the IR CO₂ analyzer without gas pump. The IR CO₂ analyzer possesses the advantages of high accuracy and mechanical reliability with small volume, lightweight, and low-power consumption. Therefore, it can be used in such relevant fields as environmental protection, processing control, chemical analysis, medical diagnosis, and space environmental and control systems.