Laser ablation of GaAs in liquids: structural, optical, and nonlinear optical characteristics of colloidal solutions

We investigated the optical, structural, and nonlinear optical properties of GaAs nanoparticles prepared by laser ablation in various liquids at the wavelengths of 795 nm and 1,054 nm. The slow-thermal-effect-induced self-defocusing processes were dominating both in the cases of high pulse repetition rate and nanosecond pulses. The two-photon absorption was observed in these colloidal solutions in the case of low pulse repetition rate of picosecond and femtosecond radiation. The nonlinear susceptibility of GaAs nanoparticles ablated in water was measured to be 2× 10^–9 esu.     

Experimental studies of the second-order nonlinear optical response of a novel class of tricyanovinylated thiophene compounds

We measured the second-order nonlinear optical response of a novel class of tricyanovinylated thiophene compounds using electric-field-induced second-harmonic generation. Very large second-order nonlinearity was observed for these compounds. The results indicate that the combination of the tricyanovinyl acceptor and the thiophene conjugating moiety offers excellent molecular second-order optical nonlinearity.     

Femtosecond Third-Order Optical Nonlinearity of Au：Bi203 Nanocomposite Films

Ultrafast third-order optical nonlinearities of the as-deposited and annealed Au：Bi2O3 nanocomposite films deposited by magnetron cosputtering are investigated by using femtosecond time-resolved optical Kerr effect （OKE） and pump probe techniques. The third-order optical nonlinear susceptibility is estimated to be 2.6Ф×10^- 10 esu and 1.8 × 10.9 esu at wavelength of 800nm, for the as-deposited and the annealed film, respectively. The OKE signal of the as-deposited film is nearly temporally symmetrical with a peak centred at zero delay time, which indicates the dominant contribution from intraband transition of conduction electrons. For the annealed film, the existence of a decay process in OKE signal implies the important contribution of hot electrons. These characteristics are in agreement with the hot electron dynamics observed in pump probe measurement.     

Optical beams in sub-strongly non-local nonlinear media: A variational solution

Discussed is the propagation of optical beams in non-local nonlinear media modelled by 1 + 1D non-local nonlinear Schrödinger equation (NNLSE). In the sub-strongly non-local case, an approximate analytical solution is obtained for an arbitrary response function by a variational approach. Described by a combination of the Jacobian elliptic functions, the solution is periodic, and its period depends on not only the input power but also the initial beam width, which is confirmed by the numerical simulation of the NNLSE.     

Large Third-Order Optical Nonlinearity of a Novel Copper Phthalocyanine--Ferrocene Dyad

Third-order optical nonlinearity of a novel copper phthalocyanine-ferrocene dyad is measured by femtosecond forward degenerate four-wave mixing （DFWM） technique at 800 nm. The second-order hyperpolarizability of the novel copper phthalocyanine-ferrocene dyad is measured to be 1.74 ×10^-30 esu. This large and ultrafast thirdorder optical nonlinear response is mainly enhanced by the formation of intramolecular charge-transfer which can enhance the delocalized movements of the large π-electrons in the molecules.     

Third-Order Optical Nonlinearity in Novel Porphyrin Dimers

We investigate the third-order optical nonlinearities in four novel porphyrin dimers （dimers A to D） and a monomeric porphyrin H2 CPTPP measured by using the single-beam z-scan technique with a pulsed Q-switched Nd：YAG nanosecond laser at 532nm. All the samples show strong excited state absorption （ESA） and high value of Х^（3） in the ns domain at this wavelength. We perform a comparison between dimer A and its monomer H2 CPTPP in their third-order optical nonlinearity, and discuss the relationships between the values of Х^（3） and the different bridging groups for all the dimers.     

Nonlinear Optical Properties of Novel Polymeric Rare Earth Phthalocyanine Studied Using Picosecond Z-Scan Technique

Three novel tri-dimensional phthalocyanine polymers, with lanthanum （LaPPc）, gadolinium （GdPPc） and ytterbium （YbPPc） as centric atoms, have been synthesized from a tetranuclear phthalonitrile. Third-order optical nonlinearities of these compounds in DMF solution are measured by a picosecond Z-sacn technique at 532 nm. It is found that all the compounds show reverse saturation absorption and nonlinear self-focus refraction effect. The second-order molecular hyperpolarizabilities are calculated to be 1.82×10^-23, 1.48×10^-23 and 1.45×10^-23 esu for LaPPc, GdPPc and YbPPc, respectively. The differences among their nonlinear optical properties are attributed to the special tri-dimensional structure and the variation in rare earth atoms.     

Optical beams in lossy non-local Kerr media

It is discussed that optical beams propagate in non-local Kerr medium waveguides with losses. A variational principle is carried out for the 1 + 1-D non-local non-linear Schrödinger equation in the presence of the losses. In the strongly non-local case, the approximate analytical solutions are obtained. The lossy soliton solution shows that, Unlike its local counterpart, such lossy strongly non-local soliton does not possess the adiabatic property anymore. In addition, the general approximate results for non-soliton cases are gained. The comparisons between our approximate analytic solutions and numerical simulations confirm our variational approximate solutions.     

Third-Order Nonlinear Optical Properties of a Series of Polythiophenes

The third-order nonlinear optical properties of a series of polythiophenes are investigated with the Z-scan method under picosecond pulse laser irradiation at 532nm. The copolymers exhibit a good nonlinear response： large nonlinear refraction coefficients without nonlinear absorption. The signs of nonlinear refraction coefficients are positive, which are opposite to the negative signs of the polythiophene reported before. The mechanism accounting for the process of nonlinear refraction under pulse laser excitation is analyzed from the viewpoint of the electrondonor/acceptor units of polythiophenes. Moreover, changes of nonlinearity according to the lengths of main chains in polythiophene molecules are discussed.     

Internal vibrations of nonlocal nonlinear Schrödinger soliton

We prove that the nonlocality is a source of the internal mode generation in a bright soliton of the nonlocal nonlinear Schrödinger equation, at least in the weak nonlocality limit. The internal mode bifurcates from the edge of the continuous spectrum of the linearized eigenvalue problem into the gap of this spectrum. A dependence of the internal mode propagation constant position in the gap on the nonlocality rate is established. It is shown that the vibration amplitude of the soliton decays inversely proportional to the propagation distance, as in the local models.     

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.     

Optical limiting with higher fullerenes

Optical limiting has been investigated for higher fullerenes and compared with C₆₀. The transmission through an aperture placed after solutions of C₇₆, C₇₈, and C₈₄ in tetrahydronaphthalene was measured using Q-switched laser pulses with a wavelength of 532 nm and a pulse width of 8 ns FWHM. Unlike C₆₀, the transmission for these higher fullerene solutions decreased linearly with increasing optical pulse energy. We attribute the linearized optical limiting response to self-defocusing of the optical beam and the absence of excited-state absorption. The ground state absorption spectra for the higher fullerenes suggest their use for optical limiting in the near infrared, and the C₈₄-tetrahydronaphthalene solution was found to be an optical limiter at 1.064 m.     

Probing interface properties of nanocomposites by third-order nonlinear optics

We describe the exploitation of third-order nonlinear optical response — particularly nonlinear absorption and the nonlinear index of refraction — to probe interface dynamics, modifications and relaxation processes in granular materials consisting of metal quantum dots embedded in such dielectrics as fused silica and sapphire. Many features of these materials can be interpreted in terms of the quantum-mechanical model of the particle-in-a-box. Electronic and thermal relaxation processes in these novel nanocomposites are dominated by interactions of conduction-band electrons at the boundary between the quantum dot and its surrounding host material. Experimental examples presented include measurements of thermal and electronic relaxation rates, dephasing due to electron collisions at the nanocluster surface, effects of local structural order, changes in the saturation parameter due to chemical modification of the substrate, and one-and two-dimensional heat-transfer effects.Paper presented at the 129th WE-Heraeus-Seminar on Surface Studies by Nonlinear Laser Spectroscopies, Kassel, Germany, May 30 to June 1, 1994.     

Determination of nonlinear absorption and refraction by single Z-scan method

We report a simplified Z-scan technique based on a study on the symmetric features of a typical Z-scan curve. The contributions from the two-photon absorption (TPA) and the nonlinear refraction (NLR) are easily separated from a closed-aperture Z-scan curve using this method. And the determination of the two nonlinearities is simplified and unambiguous. We demonstrate this method on ZnSe, CdS, and ZnTe semiconductors with 120-fs laser pulses. And the influence from the uncertainty of the focal plane (Z=0) position is discussed. It is also found that the TPA coefficient can be obtained independently without knowing the exact location of the focal point. Received: 8 July 1999 / Published online: 3 November 1999     

(1 + 2)-Dimensional sub-strongly nonlocal spatial optical solitons: Perturbation method

By extending the (1 + 1)-dimensional [(1 + 1)-D] perturbation method suggested by Ouyang et al. [S. Ouyang, Q. Guo, W. Hu, Phys. Rev. E. 74 (2006) 036622] to the (1 + 2)-D case, we obtain a fundamental soliton solution to the (1 + 2)-D nonlocal nonlinear Schrödinger equation (NNLSE) with a Gaussian-type response function for the sub-strongly nonlocal case. Numerical simulations show that the soliton solution obtained in this paper can describe the soliton states in both the sub-strongly nonlocal case and the strongly nonlocal case. It is found that the phase constant and the power of the (1 + 2)-D strongly nonlocal spatial optical soliton with a Gaussian-type response function are both in inverse proportion to the 4th power of its beam width.     

Formation of periodic structures by the space-selective precipitation of Ge nanoparticles in channel waveguides

Thermally stabilized channel waveguides with Bragg gratings were fabricated by the space-selective precipitation technique of crystalline Ge nanoparticles using KrF excimer laser irradiation. The periodic structures consisting of Ge nanoparticles were formed in Ge-B-SiO₂ thin glass films after exposure to an interference pattern of the laser followed by annealing at 600 °C. The channel waveguides with the periodic structures were fabricated by the cladding of the patterned Cr layers on the films. The diffraction peak for the TE-like mode of 11.8 dB depth was observed clearly at a wavelength of 1526.4 nm, indicating that the periodic structure also served as the optical band-pass filter in optical communication wavelength. The spectral shape, diffraction efficiency, and diffraction wavelength remained unchanged even after annealing at 400 °C. Furthermore, a low temperature dependence of the diffraction wavelength - as low as 8.1 pm/°C - was achieved. The diffraction efficiency was further enhanced after subsequent annealing at 600 °C. The space-selective precipitation technique is expected to be useful for the fabrication of highly reliable optical filters or durable sensing devices operating at high temperature.     

Dispersion of second-order nonlinear optical coefficient

A simple, approximate relation between the dispersion of the second-order nonlinear optical (SNLO) coefficient and first-order susceptibility has been derived using the well-known results of density-matrix calculation of quantum-mechanical theory. A new tensor of SNLO coefficient has been defined, which retains symmetries when the input beams are in the spectral range of transparency while the generated beam can also be in the spectral range of absorption. The validity of the relation has been checked for three ferroelectric crystals, KTP, LiNbO₃ and KNbO₃, which are transparent in the visible and near infrared, and for two semiconductors, GaP and GaAs, which absorb in the visible. Contrary to Miller’s law, the presented relation is in good agreement with measurements. Received: 8 February 2001 / Revised version: 2 July 2001 / Published online: 10 October 2001     

Optical nonlinearity enhancement for an anisotropic semiconductor–insulator composite

We investigate the effect of geometric anisotropy on the optical nonlinearity enhancement for a periodic composite with a rectangular array of elliptic semiconducting cylinders in an insulating host. By using a series expression of the space-dependent electric field obtained by a simple Fourier method in a periodic composite, we calculate the frequency dependence of the effective third-order nonlinear susceptibility as a function of anisotropy. The results show that the height of the nonlinearity enhancement peak may be increased by several orders of magnitude as the aspect ratio of the ellises is decreased or the lattice edge length ratio is increased. At resonance frequency, there exists a strong anomalous dispersion. We also investigate the effect of the volume fraction of the semiconductor phase for composites with a square array of circular semiconducting cylinders. Received: 23 November 2000 / Accepted: 2 August 2001 / Published online: 17 October 2001     

Z-scan study of optical nonlinearities in two fullerene derivatives

The third-order nonlinear optical properties of two fullerene derivatives under picosecond laser excitation have been investigated by Z-scan technique. The experimental results reveal that all the derivatives have very large nonlinear absorption coefficient under 532 nm pulses excitation and great third-order nonlinear refraction index under 1064 nm pulses excitation. The molecular second hyperpolarizabilities have been obtained from the experimental results.