Research progress of third-order optical nonlinearity of chalcogenide glasses

Chalcogenide glasses(ChGs) are a promising candidate for applications in nonlinear photonic devices. In this paper,we review the research progress of the third-order optical nonlinearity(TONL) of ChGs from the following three aspects:chemical composition, excitation condition, and post processing. The deficiencies in previous studies and further research of the TONL property of ChGs are also discussed.     

External influence on third-order optical nonlinearity of transparent chalcogenide glass-ceramics

Transparent 90GeS₂⋅10Ga₂S₃(G10) chalcogenide glass-ceramics containing β-GeS₂ nanocrystals was successfully fabricated through controllable crystallization based on the knowledge of its nucleation-rate-like curve. Using the conventional Z-scan method, both large spectral dependence and crystallinity dependence of optical nonlinear parameters were learned under the excitation of different wavelengths that in proximity of the half-bandgap. In particular, a large value of figure of merit (FOM≈11.64) was obtained in the crystallized sample after the heat-treatment at 466°C for 40 h. Although it is not a straightforward process to select an appropriate medium for a specific application, this work opens a new way to construct suitable optical nonlinear properties (e.g., large FOM) though modifying the microstructure of chalcogenide glass-ceramics.     

Linearity and nonlinearity of quantum-dot semiconductor optical amplifiers

Linearity and nonlinearity of quantum-dot semiconductor optical amplifiers (QD-SOAs) are analyzed in this paper using numerical and analytical solutions. The basic formulas are derived from rate equations of multiple-states QD-SOAs. The solutions reveal that linearity and nonlinearity of QD-SOAs, which is quantificationally characterized by the maximal linear output power and the nonlinear factor, are strongly dependent on injected current, modal gain and spontaneous radiative lifetime. Additionally, the solutions also provide some useful suggestions in designing and using of QD-SOAs, either be used in linear or nonlinear operational region.     

Slow decay dynamics of visible photoluminescence from nanometer-size silicon crystallites

We have studied the decay dynamics of visible photoluminescence (PL) from nanometer-sized Si crystallites fabricated by electrochemical etching of single crystalline Si and laser-breakdown of SiH₄ gas. In two types of Si crystallites, the slow decay behavior of red PL is characterized by a stretched exponential function. The temperature dependence of the PL decay rate is similar to that of variable-range hopping of carriers in two-dimensional systems. It is concluded that the slow decay PL is caused by the hopping-limited recombination in surface states of nanocrystallines.PACS: 73.20.Dx; 78.66.-w; 78.90.+t     

Intersubband optical nonlinearity and bistable behavior of semiconductor superlattices

The optical nonlinearity and bistability (OB) induced by intersubband transitions (ISBTs) in semiconductor superlattices are studied by means of the Kronig–Penney model and the density-matrix method. The OB state equation in a Fabry–Perot configuration is derived. It is shown that the ISBT-induced OB can be realized over a wide frequency range, and its bistable domain and hysteresis loop are much larger than those of a two-level system. Numerical illustration of the OB behavior in a GaAs/Al_xGa_1−xAs superlattice is also given.     

Ultrafast third-order optical nonlinearity of several sandwich-type phthalocyaninato and porphyrinato europium complexes

The third-order optical nonlinearity of two sandwich-type phthalocyaninato and porphyrinato europium com- plexes, including double- and triple-deckers （Eu[Pc（OC5H11）8]2, Eu2（Pc）（TPP）2, Pc=phthalocyanine, TPP=5, 10, 15, 20- tetraphenylporphyrinate）, was investigated by using the femtosecond time-resolved optical Kerr gate method at 830 nm wavelength. Their second-order hyperpolarizability is estimated to be 0.74× 10^-30esu and 3.0× 10^-3esu respectively. This exhibits an evident enhancement in comparison with 0.47×10^-30esu for one-decker Eu（Pc）（acac） （acac=acetylacetonate）, which is also measured under the same conditions. The enhancement is attributed to the introduction of lanthanide metal to the large π-conjugated system, intermacrocycle interaction and two-photon resonance etc.     

Modulating the molecular third-order optical nonlinearity by curved surface of carbon skeleton

Curved π bowl compounds represent another class of the completely conjugated materials with quantum dot nature. Non-equivalent hybridisation type from rim to hub carbon atoms in curved π bowl compound triggers anisotropic physical properties. With density functional method (CAM-B3LYP) and response theory calculations, curved π bowl compounds exhibit large radial and axial component ratio for its polarisability and the second hyperpolarisability. More importantly, they possess larger effective mass second hyperpolarisability (γ^mass) and nondiagonal components (γ_xxyy) compared to C₆₀. Except the static properties, the dispersion characters of dynamic cubic response of curved π bowl compounds have been analysed in large frequency range.     

Ultrashort pulse breaking in optical fiber with third-order dispersion and quintic nonlinearity

The optical wave breaking （OWB） characteristics in terms of the pulse shape, spectrum, and frequency chirp, in the normal dispersion regime of an optical fiber with both the third-order dispersion （TOD） and quintic nonlinearity （QN） are numerically calculated. The results show that the TOD causes the asymmetry of the temporal- and spectral-domain, and the chirp characteristics. The OWB generally appears near the pulse center and at the trailing edge of the pulse, instead of at the two edges of the pulse symmetrically in the case of no TOD. With the increase of distance, the relation of OWB to the TOD near the pulse center increases quickly, leading to the generation of ultra-short pulse trains, while the OWB resulting from the case of no TOD at the trailing edge of the pulse disappears gradually. In addition, the positive （negative） QN enhances （weakens） the chirp amount and the fine structures, thereby inducing the OWB phenomena to appear earlier （later）. Thus, the TOD and the positive （negative） QN are beneficial （detrimental） to the OWB and the generation of ultra-short pulse trains.     

Z-scan determination of third-order nonlinear optical nonlinearity of three azobenzenes doped polymer films

The third-order nonlinear response of methyl red (MR), methyl orange (MO) and p-dimethylamino benzene arsenic acid (PDBAA) doped polyvinyl alcohol (PVA) films are studied by using the Z-scan technique under 532 nm and 1064 nm excitations. The larger third-order nonlinear refractive index of PDBAA doped PVA film is discussed in terms of fall of the energy level in excited state for the effect of heavy-atom arsenic. At the end, the second hyperpolarizabilities of the films are estimated and the figures of merit are evaluated for their value of applications in ultra-fast all-optical devices.     

Calculation of the dispersion of the third-order optical nonlinearity in C60 films

Using wave functions determined from ground-state local-density calculations, we have calculated the wave-dispersed free response of the optical nonlinear polarizability ⁽³⁾(–3;,,), for the C₆₀ molecule and ⁽³⁾(–3;,,) i.e. Third-Harmonic Generation (THG) for films using a sum-over-states approach. The influence of screening was determined by applying an external static electric field in separate selfconsistent calculations to evaluate induced dipole moments which was used to determine the static linear and nonlinear polarizabilities. The polarizabilities calculated in the static limit were used to determine an effective screening parameter which was, in turn, used together with an RPA approach to calculate screened wave-dispersed, third-order nonlinear optical properties such as ⁽³⁾(–3;,,) and ⁽³⁾(–3;,,). Comparing evaluated polarizabilities with experimental values we found that the non-resonant free polarizability compares well in absolute magnitude with experimental results. Inclusion of screening results in a polarizability about two orders of magnitude below the experimental values.Paper presented at the 129th WE-Heraeus-Seminar on Surface Studies by Nonlinear Laser Spectroscopies, Kassel, Germany, May 30 to June 1, 1994     

Z-scan determination of the third-order optical nonlinearity of L-asparaginium picrate (LASP) crystal

The NLO properties of L-asparaginium picrate (LASP) crystals have been measured. The measurements were performed using a SHG diode-pumped laser at 532-nm wavelengths by employing the Z-scan technique. The nonlinear refractive index is found to be on the order of 10^?8 cm²/W. The magnitude of the third-order susceptibility is on the order of 10^?5 esu.     

Charge-separated-state enhancement of the third-order optical nonlinearity of a photosensitizer-electron acceptor triad assembly

′ ,4^′′,4^′′′-tetrasulfonato-phthalocyanine/N-butyl-N^′-methylanthraquinone-4,4^′-bipyridinum dibromide assembly (ZnTsPc-V-AQ), was observed to be enhanced by ten times when the sample was optically pumped by a 355 nm pump beam. The enhancement of the nonlinearity was found to be due predominantly to the charge transfer between the two monomers of the supramolecule after optical excitation. Received: 2 July 1996     

Investigation of third-order optical nonlinearity in KBe2BO3F2 crystal by Z-scan

The third-order optical nonlinearity of deep-ultraviolet (DUV) nonlinear optical (NLO) crystal KBe₂BO₃F₂ (KBBF) was investigated using single-beam Z-scan technique for the first time. The Z-scans were performed on a c-cut KBBF crystal and a KBBF prism-coupling device (PCD) with picosecond pulses at 355?nm. No two-photon absorption was observed in the experiment. The measured nonlinear refraction index n ₂ showed positive signs, indicating self-focusing Kerr effects. The n ₂ values were estimated to be (1.75±0.35)×10^?15?cm²/W with the c-cut sample and (1.85±0.37)×10^?15?cm²/W with the PCD, corresponding to the third-order nonlinear optical susceptibilities $\chi_{\mathrm{eff}}^{(3)}$ of (0.99±0.20)×10^?13?esu and (0.94±0.19)×10^?13?esu, respectively. The results are expected to promote the investigation of frequency conversion processes with ultra-short laser in KBBF crystal.     

Ge-Ga-Cd硫化物玻璃的超快三阶非线性光学性质与结构关系研究

本文采用飞秒时间分辨光学克尔门技术测量了GeS2-Ga2S3-CdS硫化物玻璃体系的超快三阶非线性光学响应，所用激光波长分别为820nm和640nm。?实验结果证明了GeS2-Ga2S3-CdS组分玻璃具有很大的飞秒超快三阶非线性光学响应，另外，其Kerr信号随摩尔组分的不同呈显著变化。通过拉曼光谱结构分析，探讨了此系列硫化物玻璃的三阶非线性光学性质与结构的关系，结果表明构成玻璃网络的四面体结构单元[GeS4]([GaS4])对其超快三阶光学非线性起重要作用。实验还表明了此硫化物玻璃体系的超快三阶非线性不符合半经验的Miller定律。     

The third-order optical nonlinearity and upconversion luminescence of CdTe quantum dots under femtosecond laser excitation

The aqueous CdTe quantum dots (QDs) were synthesized by the electrostatic reaction method. The optical properties of CdTe QDs were investigated by femtosecond Z-scan and time-resolved luminescence technique in nonresonant spectral region. The nonlinear absorption and refraction are ascribed to two-photon absorption, and time-resolved upconversion photoluminescence produces biexponential decay pattern at infrared femtosecond laser excitation. Upconversion luminescence is composed of a band-edge excitonic state and a photoinduced trapping state. The short-lived band-edge excitonic emission is independent of the detection wavelengths, and long-lived species becomes even longer with the increase of detection wavelengths, which indicates the size dependence of surface excitonic emission. Electronic supplementary material  The online version of this article (doi:) contains supplementary material, which is available to authorized users.     

用光波导方法测量Ⅱ—Ⅵ族半导体的光学非线性和光学双稳

本文报道利用光波导方法在ＧａＡｓ衬底上制备的Ⅱ－Ⅵ族半导体单晶薄膜和超晶格中所观测到的光学吸收,光学非线性和瞬态光学双稳的实验结果。     

Enhancement of third-order nonlinearity in Ag-nanoparticles-contained chalcohalide glasses

Ag-nanoparticles were embedded in 56GeS₂?C24Ga₂S₃?C20KBr chalcohalide glass with average size varying from 100 to 300 nm. A large femtosecond optical Kerr effect indicated an enhancement of third-order optical nonlinearity due to Ag-nanoparticles observed by AFM images. Among these Ag-nanoparticles-embedded chalcohalide glass samples, the sample (c) with the second largest implanting dose 1 × 10¹⁷ ions/cm² showed the largest value of ??⁽³⁾ 5.34 × 10^?13 esu, which was ten times larger than that of the substrate. The nonlinear relation between the implanted dose and third-order optical nonlinearity is strongly related to the intrinsic local field and Ag-nanoparticles interaction in the glasses.