Solution-phase exfoliation of graphite for ultrafast photonics

We exfoliate graphite in both aqueous and non-aqueous environments through mild sonication followed by centrifugation. The dispersions are enriched with monolayers. We mix them with polymers, followed by slow evaporation to produce optical quality composites. Nonlinear optical measurements show similar to 5% saturable absorption. The composites are then integrated into fiber laser cavities to generate 630 fs pulses at 1.56 mu m. This shows the viability of solution phase processing for graphene based photonic devices. (C) 2010 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Nonlinear optics in Silicon photonic crystal cavities

Silicon is known to be a very good material for the realization of high-Q, low-volume photonic cavities, but at the same it is usually considered as a poor material for nonlinear optical functionalities like second-harmonic generation, because its second-order nonlinear susceptibility vanishes in the dipole approximation. In this work we demonstrate that nonlinear optical effects in silicon nanocavities can be strongly enhanced and even become macroscopically observable. We employ photonic crystal nanocavities in silicon membranes that are optimized simultaneously for high quality factor and efficient coupling to an incoming beam in the far field. Using a low-power, continuous-wave laser at telecommunication wavelengths as a pump beam, we demonstrate simultaneous generation of second- and third harmonics in the visible region, which can be observed with a simple camera. The results are in good agreement with a theoretical model that treats third-harmonic generation as a bulk effect in the cavity region, and second-harmonic generation as a surface effect arising from the vertical hole sidewalls. Optical bistability is also observed in the silicon nanocavities and its physical mechanisms (optical, due to two-photon generation of free carriers, as well as thermal) are investigated. © 2011 IEEE.

Interaction between the intrinsic second- and third-order optical fields in an Al0.53Ga0.47N/GaN heterostructure

We present an experimental demonstration of the interaction between the intrinsic second- and third-order optical fields in an Al0.53Ga0.47N/GaN heterostructure. The sample was deposited by metal-organic chemical vapor deposition on (0001) sapphire. The nonlinear optical coefficients of the sample, which were measured with a Mach-Zehnder interferometer system, quadratically increase with the applied modulating voltage, indicating the existence of the third-order optical field. The third-order signal was then detected by the Z-scan method and we calculated the built-in dc field on the AlGaN/GaN interface to confirm the strong interaction between the intrinsic second- and third-order optical fields. (c) 2008 American Institute of Physics.

Third-order optical nonlinearities of lead-free (Na1-xKx)(0.5)Bi0.5TiO3 thin films

(Na1-xKx)(0.5)Bi0.5TiO3 (NKBT) (x = 0.1, 0.2, and 0.3) thin films with good surface morphology and rhombohedral perovskite structure were fabricated on quartz substrates by a sol-gel process. The fundamental optical constants (the band gaps, linear refractive indices and absorption coefficients) of the films were obtained through optical transmittance measurements. The nonlinear optical properties were investigated by Z-scan technique performed at 532 nm with a picosecond laser. A two-photon absorption effect closely related with potassium-doping content was found in thin films, and the nonlinear refractive index n(2) increases evidently with potassium-doping. The real part of the third-order nonlinear susceptibility chi((3)) is much larger than its imaginary part, indicating that the third-order optical nonlinear response of the NKBT films is dominated by the optical nonlinear refractive behavior. These results show that NKBT thin films have potential applications in nonlinear optics. (C) 2007 Elsevier B.V. All rights reserved.

Study on in-plane optical anisotropy of Si0.75Ge0.25/Si/Si0.5Ge0.5 asymmetric superlattice by reflectance difference spectroscopy - art. no. 071908

Si0.75Ge0.25/Si/Si0.5Ge0.5 trilayer asymmetric superlattices were prepared on Si (001) substrate by ultrahigh vacuum chemical vapor deposition at 500 degrees C. The nonlinear optical response caused by inherent asymmetric interfaces in this structure predicted by theories was verified by in-plane optical anisotropy in (001) plane measured via reflectance difference spectroscopy. The results show Si0.75Ge0.25/Si/Si0.5Ge0.5 asymmetric superlattice is optically biaxial and the two optical eigen axes in (001) plane are along the directions [110] and [-110], respectively. Reflectance difference response between the above two eigen axes can be influenced by the width of the trilayers and reaches as large as similar to 10(-4)-10(-3) in 15-period 2.7 nm-Si0.75Ge0.25/8 nm-Si/1.3 nm-Si0.5Ge0.5 superlattice when the normal incident light wavelength is in the range of 500-1100 nm, which is quite remarkable because the optical anisotropy does not exist in bulk Si.

Optimization and characterization of the guest-host polyetherketone polymer films for application in integrated optical devices

In order to optimize the loading of 3-(1, 1-dicyanothenyl)-1-phenyl-4, 5-dihydro-1H-pryazole (DCNP) in polyetherketone (PEK-c) guest-host polymer films, ten kinds of DCNP/PEK-c thin films, in which the weight per cent of DCNP changes from 5 to 50, were prepared. Their second-order nonlinear optical coefficients chi(33)((2)) at 1064 nm were measured by Using Maker fringe method after poling under the optimal poling condition. Their optical waveguide transmission losses were measured at 632.8 nm. Optimal weight per cent of the chromophore for the DCNP/PEK-c guest-host polymer system has been determined as about 20 for use in the integrated optical devices.

Determination of the macroscopic optical properties for the NAEC/PEK-c guest-host polymer films

The polyetherketone (PEK-c) guest-host polymer films doped with (4'-nitro)-3-azo-9-ethyl-carbazole (NAEC) were prepared. The films were poled by corona-onset poling at elevated temperature (COPET). The orientational order parameter of the chromophores NAEC in poled polymer film was determined by measuring the absorption spectra of the films before and after being poled. By using the two-level model, the measured dispersion of the refractive index of the polymer film, and the dispersion of the first hyperpolarizability of chromophore NAEC, the dispersion of the macroscopic second-order nonlinear optical (NLO) and linear electrooptic (EO) coefficients was evaluated for the NAEC/PEK-c guest-host polymer film. (C) 2001 Elsevier Science Ltd. All rights reserved.

Dielectric relaxation of poled polymer DCNP/PMMA

We have prepared the polymer thin films of a 3-(1,1-dicyanothenyl)-1-phenyl-4,5-dihydro-1H-pyrazole (DChTP)/poly (methyl methacrylate) (PMMA) guest-host system by spin coating. In order to investigate their temporal and temperature stability, we have measured their dielectric relaxation spectra including the frequency dependence of the real and imaginary parts of dielectric constants. The investigated frequency ranged from 50 Hz to 10 MHz. The measured temperature range above the glass transition temperature T-g (95 degrees C) of the DCNP/PMMA system was from 95 degrees C to 1250C. By using the Adam-Gibbs model, the temperature dependence of the characteristic time tau above T-g was fitted, and the values of the characteristic times tau below T-g were estimated. The lifetimes of the polymer were evaluated by the Kohlrausch-Williams Watts (KWW) empirical decay model. (C) 2000 Elsevier Science B.V. All rights reserved.

Intersubband optical absorption in a step asymmetric semiconductor quantum well driven by a terahertz field

The nonlinear optical absorption in a three-subband step asymmetric semiconductor quantum well driven by a strong terahertz (THz) field is investigated theoretically by employing the intersubband semiconductor-Bloch equations. We show that the optical absorption spectrum strongly depends on the intensity, frequency, and phase of the pump THz wave. The strong THz field induces THz sidebands and Autler-Townes splitting in the probe absorption spectrum. Varying the pump frequency can bring not only the new absorption peaks but also the changing of the energy separation of the two higher-energy levels. The dependence of the absorption spectrum on the phase of the pump THz wave is also very remarkable.

Synthesis, characterization, photoluminescent and electroluminescent properties of new conjugated 2,2 '-(arylenedivinylene)bis-8-substituted quinolines

A series of new PPV oligomers containing 8-substituted quinoline, 2,2'-(arylenedivinylene) bis-8-quinoline derivatives, were designed and synthesized via a Knoevenagel condensation reaction of quinaldine, 8-hydroxy-or 8-methoxy-quinaldine with aromatic dialdehydes. These PPV oligomers were characterized by H-1 and C-13-NMR, X-ray diffraction, elemental analysis, UV-visible and fluorescence spectroscopies. The X-ray diffraction investigation showed that there are intermolecular pi...pi interactions in the solid state in 1 and 3. The optical and photoluminescent properties study demonstrated that the emission color of the resulting materials varies from blue to yellow and is dependent on the substituents (pi-donor and pi-acceptor groups) on both sides of the conjugated molecules and the aromatic core in the middle of the conjugated backbones. The electroluminescent devices using compounds 1-4 as the emitters and electron-transporting layers were fabricated with the structure ITO/NPB/emitter/LiF/Al. The best device performance with the maximum brightness of 5530 cd m(-2) and the luminous efficiency of 2.4 cd A(-1) is achieved by using compound 4, with intramolecular charge transfer character, as the emitter; these values represent a more than 5-fold improvement in brightness and efficiency compared to compound 3 without methoxy groups on the phenyl rings.

Effect of hydrogen bonds on optical nonlinearities of inorganic crystals

This work probes the role of hydrogen bonds (such as O-H ... O and N-H ... O) in some inorganic nonlinear optical (NLO) crystals, such as HIO3, NH4H2PO4 (ADP), K[B5O6(OH)(4)] . 2H(2)O (KB5) and K2La(NO3)(5) . 2H(2)O (KLN), from the chemical bond standpoint. Second order NLO behaviors of these four typical inorganic crystals have been quantitatively studied, results show hydrogen bonds play a very important role in NLO contributions to the total nonlinearity. Conclusions derived here concerning the effect of hydrogen bonds on optical nonlinearities of inorganic crystals have important implications with regard to the utilization of hydrogen bonds in the structural design of inorganic NLO crystals. (C) 1999 Elsevier Science B.V. All rights reserved.

Bunching-induced optical nonlinearity and instability in cold atoms [Invited].

We report a new nonlinear optical process that occurs in a cloud of cold atoms at low-light-levels when the incident optical fields simultaneously polarize, cool, and spatially-organize the atoms. We observe an extremely large effective fifth-order nonlinear susceptibility of χ(⁵) = 7.6 × 10⁻¹⁵ (m/V)⁴, which results in efficient Bragg scattering via six-wave mixing, slow group velocities (∼ c/10⁵), and enhanced atomic coherence times (> 100 μs). In addition, this process is particularly sensitive to the atomic temperatures, and provides a new tool for in-situ monitoring of the atomic momentum distribution in an optical lattice. For sufficiently large light-matter couplings, we observe an optical instability for intensities as low as ∼ 1 mW/cm² in which new, intense beams of light are generated and result in the formation of controllable transverse optical patterns.

Designed ultrafast optical nonlinearity in a plasmonic nanorod metamaterial enhanced by nonlocality

All-optical signal processing enables modulation and transmission speeds not achievable using electronics alone(1,2). However, its practical applications are limited by the inherently weak nonlinear effects that govern photon-photon interactions in conventional materials, particularly at high switching rates(3). Here, we show that the recently discovered nonlocal optical behaviour of plasmonic nanorod metamaterials(4) enables an enhanced, ultrafast, nonlinear optical response. We observe a large (80%) change of transmission through a subwavelength thick slab of metamaterial subjected to a low control light fluence of 7 mJ cm(-2), with switching frequencies in the terahertz range. We show that both the response time and the nonlinearity can be engineered by appropriate design of the metamaterial nanostructure. The use of nonlocality to enhance the nonlinear optical response of metamaterials, demonstrated here in plasmonic nanorod composites, could lead to ultrafast, low-power all-optical information processing in subwavelength-scale devices.

Nonlinear optics from an ab initio approach by means of the dynamical Berry phase: Application to second- and third-harmonic generation in semiconductors

We present an ab initio real-time-based computational approach to study nonlinear optical properties in condensed matter systems that is especially suitable for crystalline solids and periodic nanostructures. The equations of motion and the coupling of the electrons with the external electric field are derived from the Berry-phase formulation of the dynamical polarization [Souza et al., Phys. Rev. B 69, 085106 (2004)]. Many-body effects are introduced by adding single-particle operators to the independent-particle Hamiltonian. We add a Hartree operator to account for crystal local effects and a scissor operator to correct the independent particle band structure for quasiparticle effects. We also discuss the possibility of accurately treating excitonic effects by adding a screened Hartree-Fock self-energy operator. The approach is validated by calculating the second-harmonic generation of SiC and AlAs bulk semiconductors: an excellent agreement is obtained with existing ab initio calculations from response theory in frequency domain [Luppi et al., Phys. Rev. B 82, 235201 (2010)]. We finally show applications to the second-harmonic generation of CdTe and the third-harmonic generation of Si. 

Photonic devices for optical and RF signal processing

O presente trabalho tem por objectivo o estudo de novos dispositivos fotónicos aplicados a sistemas de comunicações por fibra óptica e a sistemas de processamento de sinais RF. Os dispositivos apresentados baseiam-se em processamento de sinal linear e não linear. Dispositivos lineares ópticos tais como o interferómetro de Mach-Zehnder permitem adicionar sinais ópticos com pesos fixos ou sintonizáveis. Desta forma, este dispositivo pode ser usado respectivamente como um filtro óptico em amplitude com duas saídas complementares, ou, como um filtro óptico de resposta de fase sintonizável. O primeiro princípio de operação serve como base para um novo sistema fotónico de medição em tempo real da frequência de um sinal RF. O segundo princípio de operação é explorado num novo sistema fotónico de direccionamento do campo eléctrico radiado por um agregado de antenas, e também num novo compensador sintonizável de dispersão cromática. O processamento de sinal é não linear quando sinais ópticos são atrasados e posteriormente misturados entre si, em vez de serem linearmente adicionados. Este princípio de operação está por detrás da mistura de um sinal eléctrico com um sinal óptico, que por sua vez é a base de um novo sistema fotónico de medição em tempo real da frequência de um sinal RF. A mistura de sinais ópticos em meios não lineares permite uma operação eficiente numa grande largura espectral. Tal operação é usada para realizar conversão de comprimento de onda sintonizável. Um sinal óptico com multiplexagem no domínio temporal de elevada largura de banda é misturado com duas bombas ópticas não moduladas com base em processos não lineares paramétricos num guia de ondas de niobato de lítio com inversão periódica da polarização dos domínios ferroeléctricos. Noutro trabalho, uma bomba pulsada em que cada pulso tem um comprimento de onda sintonizável serve como base a um novo conversor de sinal óptico com multiplexagem no domínio temporal para um sinal óptico com multiplexagem no comprimento de onda. A bomba é misturada com o sinal óptico de entrada através de um processo não linear paramétrico numa fibra óptica com parâmetro não linear elevado. Todos os dispositivos fotónicos de processamento de sinal linear ou não linear propostos são experimentalmente validados. São também modelados teoricamente ou através de simulação, com a excepção dos que envolvem mistura de sinais ópticos. Uma análise qualitativa é suficiente nestes últimos dispositivos.