Studies of third-order nonlinear optical properties of C60 by the optical Kerr effect

60 at 1.064 μm is determined by the optical Kerr effect in toluene solution. Values of -6.5×10^-33 esu and 2.0×10^-32 esu for the real and imaginary parts of γ, respectively, are obtained. Based on the experimental results and symmetry constraint, it is concluded that a three-level model is not adequate to describe the third-order nonlinearity of C₆₀. It is also inferred that the non-resonant γ of C₆₀ should be positive in sign, which is in agreement with reported off-resonant measurements of γ of C₆₀ by third-harmonic generation. Received: 3 September 1997/Revised version: 1 December 1997     

Third-order nonlinear optical response of Au-core CdS-shell composite nanoparticles embedded in BaTiO<Subscript>3</Subscript> thin films

Au-core CdS-shell composite nanoparticles were synthesized by a direct self-assembly process and integrated into BaTiO₃ thin films. Characterization by transmission electron microscopy showed that the average diameter of these composite nanoparticles was about 8 nm. Using the femtosecond time-resolved optical Kerr effect method, we investigated the third-order nonlinear optical response of the Au@CdS nanoparticles embedded in the BaTiO₃ thin films at a wavelength of 800 nm. An ultrafast nonlinear response and a large effective third-order nonlinear susceptibility of χ⁽³⁾=7.7×10^-11 esu were observed. We attributed the enhancement of the third-order optical nonlinearity to a localized electric field effect originating from the core-shell structure under off-surface-plasmon resonance conditions. Received: 13 May 2002 / Revised version: 23 October 2002 / Published online: 3 April 2003 RID="*" ID="*"Corresponding author. Fax: +86-21/6510-4949, E-mail: sxqian@fudan.ac.cn     

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.     

Optical study of dye-containing fluorinated polyimide thin films

Thin films of dye-containing fluorinated polyimide have been obtained by adding the dye powder to the polyamic acid resin and by spin coating the resulting solution on silica and silicon substrates. 6FDA (4,4’-hexafluoroisopropylidene diphthalic anhydride) and DAB (diaminobenzophenone) have been used as precursor monomers and rhodamine B as dye. The influence of the rhodamine-B molecule on the completeness of the imidization process has been studied by coupled thermogravimetric and mass-spectrometric analyses (TG-MS) of pure and doped polyamic acid resin and by FT-IR analysis of samples before and after curing. Optical emission, excitation and absorption spectra have been collected in order to study spectroscopic and aggregation characteristics of rhodamine as a function of the deposition parameters. Received: 2 March 2000 / Accepted: 24 July 2000 / Published online: 9 November 2000     

Characterization of nonlinear optical parameters of polymethine dyes

We investigated nonlinear refraction, nonlinear absorption, and saturable absorption of polymethine dyes by the Z-scan technique (λ=1064 nm). The analysis of simultaneous appearance of several nonlinear optical processes in dye solutions excited by picosecond pulses was carried out. The saturable absorption was analyzed taking into account various models. Nonlinear refractive indices, nonlinear absorption coefficients, and saturation intensities of various polymethine dyes were measured. Received: 27 December 2002 / Revised version: 6 March 2003 / Published online: 5 May 2003 RID="*" ID="*"Corresponding author. Fax: +81-471/363-366, E-mail: r_ganeev@issp.u-tokyo.ac.jp RID="**" ID="**"Present address: The Institute for Solid State Physics, The Tokyo University, 5-1-5 Kashiwanoha, Kashiwa, Chiba 277-8581, Japan     

Chemical-bond analysis of the nonlinear optical properties of the borate crystals LiB3O5, CsLiB6O10, and CsB3O5

The second-order nonlinear optical properties of practical borate crystals, LiB₃O₅, CsLiB₆O₁₀, and CsB₃O₅, which all contain the identical basic structural unit [the (B₃O₇)^5- group], have been quantitatively studied from the chemical-bond viewpoint. Differences in the nonlinear optical properties among these three borate crystals arise from the contributions of the different cations, i.e., the different interaction between the cation and the (B₃O₇)^5- anionic group. The chemical-bond method quantitatively expresses this important difference. At the same time, the current calculation also shows that the B₃O₇ group is a very important crystallographic frame in the crystalline borate solids; it offers different cations an excellent coordination environment. Received: 20 February 2001 / Accepted: 14 June 2001 / Published online: 30 August 2001     

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.     

On thickness dependence of electrical and optical properties of Te thin films

Received: 1 July 1997/Accepted: 6 August 1997     

Dispersion of the third-order susceptibility of a cyanine dye measured by coherent anti-Stokes Raman scattering

The dispersion of the third-order susceptibility of the cyanine dye bis-(dimethylamino)-heptamethinium chloride was measured by Coherent Anti-Stokes Raman Scattering (CARS) over a wide wavelength range from 530 to 830 nm. Large negative values of the real part of the second-order hyperpolarizability are observed. The data are analyzed with the help of theoretical calculations based on a perturbative approach for the nonlinearities. The dispersion behavior of the third-order susceptibility is governed by the resonant enhancement due to vibrational transitions of the first excited electronic state and, to lesser extent, by an electronic two-photon resonance around 600 nm.     

Microgeometry and effective permittivity of discontinuous metal films

This work deals with the investigation of dielectric and optical properties of discontinuous metal films over a wide range of filling factors each side of the percolation threshold. A phenomenological two-parameter representation is used for the effective permittivity &εtilde; of such systems. In order to test the proposed approach, we have taken for gold films on a glass substrate the transmittance spectra in the visible and near-IR regions. It is shown that the representation used for the effective permittivity enables us to adequately describe the experimental transmittance spectra. The parameters entering the above representation are determined and the relationship between them and film microgeometry is discussed. Received: 6 November 2000 / Accepted: 30 May 2001 / Published online: 25 July 2001     

Size effect in optical spectra of microcrystalline diamond powders and CVD films

Received: 24 March 1997/Accepted: 27 May 1997     

Structural and magnetic properties of Co-C composite films and Co/C multilayer films

CoC composite films and Co/C multilayer films have been prepared by a method incorporating ion beam sputtering and plasma chemical vapor deposition. It has been found that the structure and magnetic properties of both the Co-C composite and the Co/C multilayer films depend strongly on the substrate temperature during deposition. The Co-C composite film deposited at room temperature is amorphous, with relatively low saturation magnetization and coercivity. On the other hand, the film deposited at 250 °C is composed of fine Co crystallites separated by amorphous C or Co-C phase. As a result, both the saturation magnetization and coercivity are increased compared with the film deposited at room temperature. When deposited at room temperature, the Co/C multilayer film exhibits good periodicity, with a period of 70 nm (Co: 40 nm, C: 30 nm) and sharp and flat Co-C interfaces. High magnetization (602 emu/cm³) and low coercivity (1.6 Oe) are obtained for such a film. However, increasing the substrate temperature to 250 °C was found to be detrimental to the magnetic properties due to the formation of cobalt carbide at the Co-C interface. Received: 11 July 2000 / Accepted: 13 July 2000 / Published online: 30 November 2000     

Photoluminescence characteristics of neodymium oxide nanocrystal/titania/ormosil composite sol-gel thin films

Neodymium (III) oxide nanocrystal/titania/organically-modified silane (ormosil) composite thin films have been prepared using a chemical approach consisting of a combination of inverse microemulsion and sol-gel techniques at low temperature. Transmission electron microscopy shows that the neodymium (III) oxide nanoparticles have a needle-like nanocrystal structure. A strong room temperature emission at 1064 nm, corresponding to the ⁴ F _3/2?⁴ I _11/2 transition, has been observed as a function of the heat treatment temperature used for the production of the composite thin films. In addition to this emission, two other main emissions at 890 nm and at 1336 nm have also been observed. In particular, there was a clear shoulder peak at 1145 nm, probably be due to the host matrix, which was observed in all the measured samples and this shoulder peak gave a maximum intensity after heat treatment at 300 °C. Received: 6 September 2000 / Accepted: 15 November 2000 / Published online: 20 June 2001     

Optical and non-linear optical properties of vanadium oxide phthalocyanine films

The optical and non-linear optical properties of peripheral-substituted vanadium oxide phthalocyanine (VOPc) film and substituted VOPc/polymer composite film were investigated using stationary and transient spectroscopy techniques. The absorption Q band of the VOPc/polymer composite film shows a red shift relative to that of the peripheral-substituted VOPc film, revealing the monomeric characteristics of VOPc molecules. Effective quenching of PL emission was observed for the VOPc/polymer composite film and could be assigned to the efficient VOPc–polymer interaction. From pump-probe and optical Kerr effect (OKE) measurements, two decay components were obtained by fitting the transients for both VOPc films. The fast component, in a femtosecond time domain, originates from the electron–phonon interaction, and the difference in their slow decay is an indication of an efficient ISC process in the VOPc/polymer composite film. The third-order non-linear optical susceptibilities of these films were determined to be in the order of 10^-11 esu. Received: 25 October 2001 / Revised version: 8 January 2002 / Published online: 7 February 2002     

Second-harmonic spectroscopy of Ge/Si(001) and Si1-xGex(001)/Si(001)

0.9 Ge_0.1(001)/Si(001) films with SH photon energies 3.1<2hν<3.5 eV near the bulk E₁ critical point of Si(001) or Si_0.9Ge_0.1(001). Ge was deposited on Si(001) by using atomic layer epitaxy cycles with GeH₄ or Ge₂H₆ deposition at 410 K followed by hydrogen desorption. As Ge coverage increased from 0 to 2 monolayers the SH signal increased uniformly by a factor of seven with no detectable shift in the silicon E₁ resonant peak position. SH signals from Si_0.9Ge_0.1(001)/Si(001) were also stronger than those from intrinsic Si(001). Hydrogen termination of the Si_0.9Ge_0.1(001) and Ge/Si(001) surfaces strongly quenched the SH signals, which is similar to the reported trend on H/Si(001). We attribute the stronger signals from Ge-containingsurfaces to the stronger SH polarizability of asymmetric Ge-Si and Ge-Ge dimers compared to Si-Si dimers. Hydrogen termination symmetrizes all dimers, thus quenching the SH polarizability of all of the surfaces investigated. Received: 13 October 1998 / Revised version: 18 January 1999     

Large third—order optical nonlinearity in Au nanomeytre particle doped BaTiO3 composite films near the resonant frequency

Nanometre-sized gold particles embedded in BaTiO₃ composite thin films (Au/BaTiO₃) were fabricated by the pulsed laser deposition technique. The films were grown on MgO (100) substrates at 700℃. The crystalline property of the films was studied with x-ray diffraction. X-ray photoelectron spectroscopy was used to check the Au composition and chemical nature for the deposited films. The absorption peak due to the surface plasmon resonance of Au particles was observed at the wavelength of about 570 nm, which increased as the metal particle size was increased. The nonlinear optical properties of the Au/BaTiO₃ films were determined using the z-scan method at the wavelength of 532 nm, which was close to the resonant frequency. The real and imaginary parts of the third-order nonlinear susceptibility χ⁽³⁾ at an Au concentration of about 6.7 at.% were determined to be 6.62×10^-7 esu and -6.24×10^-8 esu, respectively. The films showed a very large absorption, masking the nonlinear refraction effect at high metal concentrations.     

Study of optical waveguide of barium sodium niobate films on potassium titanyl phosphate

Barium sodium niobate (BSN) optical waveguide films were grown on potassium titanyl phosphate (KTP) substrate by pulsed laser deposition (PLD). X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray pole spectroscopy, and X-ray photoelectron spectroscopy (XPS) showed that the as-grown BSN films are epitaxially smooth, fine-particled and show small constituent deviation. Both m lines of the waveguided TE and TM modes were recorded. Lattice match between the BSN(110) and both the KTP(001) and KTP(100) planes is examined with mismatch less than 3%. Effective refractive indices as a function of incident wavelength and order of the waveguided modes are studied. A phase matching relationship of k ⁽¹⁾−2k ⁽⁰⁾=0 is established between the first-order and fundamental modes in the BSN/KTP waveguided system. Effective thicknesses for TE and TM modes were obtained to be equal to 0.76 and 0.72 μm, respectively, larger than the thickness of the as-grown BSN film of 0.60 μm. A constituent ratio of Ba:Na:Nb in the BSN film measured was equal to 2:0.82:5.14, slightly deviating from the stoichiometric ratio of 2:1:5, which is attributed to higher relative asymptotic velocity for Nb species and higher evaporation pressure for Na species. Finally, the main factors affecting quality of the as-grown BSN films are also discussed. Received: 26 March 1999 / Accepted: 30 March 1999 / Published online: 19 August 1999     

Influence of predelay between interacting picosecond pulses on the nonlinear optical processes of frequency conversion

Received: 7 October 1996     

Distinct correlation between CeO2 and YSZ in out-of-plane and in-plane mosaic dispersions of heteroepitaxial CeO2/YSZ/Si(001) films

The structural correlations including the lattice constants and the mosaic dispersions between CeO₂ and yttria-stabilized ZrO₂ (YSZ) in CeO₂/YSZ/Si(001) heteroepitaxial films have been investigated by out-of-plane and in-plane X-ray-diffraction techniques. The distinct linear correlations of the full width at half-maximum (FWHM) of the ω scan between CeO₂ and YSZ have been found in both directions. CeO₂ always has a 0.7° lower FWHM of the ω scan than YSZ in the out-of-plane direction, but has a 2.6° higher FWHM in the in-plane direction. A possible relationship between the out-of-plane and in-plane FWHMs of the ω scans has been demonstrated with a lattice-rotation model. Besides, the lattice constants of CeO₂ are dependent on the FWHMs of the YSZ ω scans: as the FWHM is below 3.5°, CeO₂ has a tetragonal distortion, and as the FWHM is higher than 3.5°, CeO₂ exhibits a cubic structure without distortion. The results are of great interest, both for the fundamental understanding of the film-growth mechanisms and for potential applications. Received: 11 September 2000 / Accepted: 5 June 2001 / Published online: 30 August 2001     

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