Novel solitons in parametric amplifiers and atom lasers

We review recent developments in quantum and classical soliton theory, leading to the possibility of observing both classical and quantum parametric solitons in higher-dimensional environments. In particular, we consider the theory of three bosonic fields interacting via both parametric (cubic) and quartic couplings. In the case of photonic fields in a nonlinear optical medium this corresponds to the process of sum frequency generation (via chi((2)) nonlinearity) modified by the chi((3)) nonlinearity. Potential applications include an ultrafast photonic AND-gate. The simplest quantum solitons or energy eigenstates (bound-state solutions) of the interacting field Hamiltonian are obtained exactly in three space dimensions. They have a point-like structure-even though the corresponding classical theory is nonsingular. We show that the solutions can be regularized with the imposition of a momentum cut-off on the nonlinear couplings. The case of three-dimensional matter-wave solitons in coupled atomic/molecular Bose-Einstein condensates is discussed.

Multidimensional quantum solitons with nondegenerate parametric interactions: Photonic and Bose-Einstein condensate environments

We consider the quantum theory of three fields interacting via parametric and repulsive quartic couplings. This can be applied to treat photonic chi((2)) and chi((3)) interactions, and interactions in atomic Bose-Einstein condensates or quantum Fermi gases, describing coherent molecule formation together with a-wave scattering. The simplest two-particle quantum solitons or bound-state solutions of the idealized Hamiltonian, without a momentum cutoff, are obtained exactly. They have a pointlike structure in two and three dimensions-even though the corresponding classical theory is nonsingular. We show that the solutions can be regularized with a momentum cutoff. The parametric quantum solitons have much more realistic length scales and binding energies than chi((3)) quantum solitons, and the resulting effects could potentially be experimentally tested in highly nonlinear optical parametric media or interacting matter-wave systems. N-particle quantum solitons and the ground state energy are analyzed using a variational approach. Applications to atomic/molecular Bose-Einstein condensates (BEC's) are given, where we predict the possibility of forming coupled BEC solitons in three space dimensions, and analyze superchemistry dynamics.

Infrared seeded parametric four-wave mixing for sensitive detection of molecules

We have developed a sensitive resonant four-wave mixing technique based on two-photon parametric four-wave mixing with the addition of a phase matched ''seeder'' field. Generation of the seeder field via the same four-wave mixing process in a high pressure cell enables automatic phase matching to be achieved in a low pressure sample cell. This arrangement facilitates sensitive detection of complex molecular spectra by simply tuning the pump laser. We demonstrate the technique with the detection of nitric oxide down to concentrations more than 4 orders of magnitude below the capability of parametric four-wave mixing alone, with an estimated detection threshold of 10(12) molecules/cm(3).

Molecular Lego (R): non-centrosymmetric alignment within interdigitating layers

(E)-N-Hexadecyl-4-[2-(4-octadecyloxynaphthyl) ethenyl] quinolinium bromide, which has a wide-bodied chromophore and terminal n-alkyl groups, adopts a U-shape when spread at the air-water interface but a stretched conformation when compressed to ca. 35 mN m(-1). The high-pressure phase has a narrow stability range prior to collapse but may be extended from 40 to 60 mN m(-1) by co-spreading the dye in a 1 : 1 ratio with docosanoic acid. The mixed Langmuir-Blodgett (LB) film has a monolayer thickness of 4.6 +/- 0.2 nm which decreases to 2.5 +/- 0.1 nm layer(-1) in the bulk, the reduction arising from an interdigitating layer arrangement, both top and bottom. It is the first example of LB-Lego(R) and, in addition, represents the only fully interdigitating structure with non-centrosymmetrically aligned chromophores. They are tilted 38 degrees from the substrate normal. The second-harmonic intensity increases quadratically with the number of layers, i.e. as I-(N)(2 omega) = (I(1)N2)-N-2 omega, with a second-order susceptibility of chi ((2))(zzz) = 30 pm V-1 at 1064 nm for refractive indices of n(omega) = 1.55 and n(2 omega) = 1.73, d = 2.5 nm layer(-1) and phi = 38 degrees. Angle resolved X-ray photoelectron spectra (XPS) of these films provide no evidence of the bromide counterion, which suggests that it is replaced by OH 2 or HCO3-, which occur naturally in the aqueous subphase, or C21H43COO- from the co-deposited fatty acid. This probably applies to all cationic dyes deposited by the LB technique.

Critical quantum fluctuations in the degenerate parametric oscillator

We develop a systematic theory of critical quantum fluctuations in the driven parametric oscillator. Our analytic results agree well with stochastic numerical simulations. We also compare the results obtained in the positive-P representation, as a fully quantum-mechanical calculation, with the truncated Wigner phase-space equation, also known as the semiclassical theory. We show when these results agree and differ in calculations taken beyond the linearized approximation. We find that the optimal broadband noise reduction occurs just above threshold. In this region where there are large quantum fluctuations in the conjugate variance and macroscopic quantum superposition states might be expected, we find that the quantum predictions correspond very closely to the semiclassical theory.

Synthesis of new Fe(II) and Ru(II) eta(5)-monocyclopentadienyl compounds showing significant second order NLO properties

A series of new ruthenium(II) complexes of the general formula [Ru(eta(5)-C5H5)(PP)(L)][PF6] (PP = DPPE or 2PPh(3), L = 4-butoxybenzonitrile or N-(3-cyanophenyl)formamide) and the binuclear iron(II) complex [Fe(eta(5)-C5H5)(PP)(mu-L)(PP)(eta(5)-C5H5)Fe][PF6](2) (L = (E)-2-(3-(4-nitrophenyl)allylidene)malononitrile, that has been also newly synthesized) have been prepared and studied to evaluate their potential in the second harmonic generation property. All the new compounds were fully characterized by NMR, IR and UV-Vis spectroscopies and their electrochemistry behaviour was studied by cyclic voltammetry. Quadratic hyperpolarizabilities (beta) of three of the complexes have been determined by hyper-Rayleigh scattering (HRS) measurements at fundamental wavelength of 1500 nm and the calculated static beta(0) values are found to fall in the range 65-212 x 10(-30) esu. Compound presenting beta(0) = 212 x 10(-30) esu has revealed to be 1.2 times more efficient than urea standard in the second harmonic generation (SHG) property, measured in the solid state by Kurtz powder technique, using a Nd:YAG laser (1064 nm). (C) 2013 Elsevier B.V. All rights reserved.

Mono(Eta(5)-cyclopentadienyl)metal(II) complexes with thienyl acetylide chromophores: synthesis, electrochemical studies, and first hyperpolarizabilities

A series of mono(eta(5)-cyclopentadienyl)metal-(II) complexes with nitro-substituted thienyl acetylide ligands of general formula [M(eta(5)-C5H5)(L)(C C{C4H2S}(n)NO2)] (M = Fe, L = kappa(2)-DPPE, n = 1,2; M = Ru, L = kappa(2)-DPPE, 2 PPh3, n = 1, 2; M = Ni, L = PPh3, n = 1, 2) has been synthesized and fully characterized by NMR, FT-IR, and UV-Vis spectroscopy. The electrochemical behavior of the complexes was explored by cyclic voltammetry. Quadratic hyperpolarizabilities (beta) of the complexes have been determined by hyper-Rayleigh scattering (HRS) measurements at 1500 nm. The effect of donor abilities of different organometallic fragments on the quadratic hyperpolarizabilities was studied and correlated with spectroscopic and electrochemical data. Density functional theory (DFT) and time-dependent DFT (TDDFT) calculations were employed to get a better understanding of the second-order nonlinear optical properties in these complexes. In this series, the complexity of the push pull systems is revealed; even so, several trends in the second-order hyperpolarizability can still be recognized. In particular, the overall data seem to indicate that the existence of other electronic transitions in addition to the main MLCT clearly controls the effectiveness of the organometallic donor ability on the second-order NLO properties of these push pull systems.

Vibration and two-photon absorption

The rigorous and transparent treatment of the effects of nuclear vibrational motion in two-photon absorption (TPA) was discussed. Perturbation formula for diatomic molecules were developed and applied to the X¹Σ+–A¹Π transition in CO. The analysis showed that the vibrations played an important role in TPA, just as their role in the calculation of conventional nonlinear optical (NLO) hyperpolarizabilities

Simple finite field method for calculation of static and dynamic vibrational hyperpolarizabilities: curvature contributions

In the static field limit, the vibrational hyperpolarizability consists of two contributions due to: (1) the shift in the equilibrium geometry (known as nuclear relaxation), and (2) the change in the shape of the potential energy surface (known as curvature). Simple finite field methods have previously been developed for evaluating these static field contributions and also for determining the effect of nuclear relaxation on dynamic vibrational hyperpolarizabilities in the infinite frequency approximation. In this paper the finite field approach is extended to include, within the infinite frequency approximation, the effect of curvature on the major dynamic nonlinear optical processes

Silicon nanocrystals as an enabling material for silicon Ppotonics

Silicon nanocrystals (Si-nc) is an enabling material for silicon photonics, which is no longer an emerging field of research but an available technology with the first commercial products available on the market. In this paper, properties and applications of Si-nc in silicon photonics are reviewed. After a brief history of silicon photonics, the limitations of silicon as a light emitter are discussed and the strategies to overcome them are briefly treated, with particular attention to the recent achievements. Emphasis is given to the visible optical gain properties of Si-nc and to its sensitization effect on Er ions to achieve infrared light amplification. The state of the art of Si-nc applied in a few photonic components is reviewed and discussed. The possibility to exploit Si-nc for solar cells is also presented. in addition, nonlinear optical effects, which enable fast all-optical switches, are described.

Design, Fabrication and Characterization of Passive and Active Polymer Photonic Devices

The rapid developments in fields such as fibre optic communication engineering and integrated optical electronics have expanded the interest and have increased the expectations about guided wave optics, in which optical waveguides and optical fibres play a central role. The technology of guided wave photonics now plays a role in generating information (guided-wave sensors) and processing information (spectral analysis, analog-to-digital conversion and other optical communication schemes) in addition to its original application of transmitting information (fibre optic communication). Passive and active polymer devices have generated much research interest recently because of the versatility of the fabrication techniques and the potential applications in two important areas – short distant communication network and special functionality optical devices such as amplifiers, switches and sensors. Polymer optical waveguides and fibres are often designed to have large cores with 10-1000 micrometer diameter to facilitate easy connection and splicing. Large diameter polymer optical fibres being less fragile and vastly easier to work with than glass fibres, are attractive in sensing applications. Sensors using commercial plastic optical fibres are based on ideas already used in silica glass sensors, but exploiting the flexible and cost effective nature of the plastic optical fibre for harsh environments and throw-away sensors. In the field of Photonics, considerable attention is centering on the use of polymer waveguides and fibres, as they have a great potential to create all-optical devices. By attaching organic dyes to the polymer system we can incorporate a variety of optical functions. Organic dye doped polymer waveguides and fibres are potential candidates for solid state gain media. High power and high gain optical amplification in organic dye-doped polymer waveguide amplifier is possible due to extremely large emission cross sections of dyes. Also, an extensive choice of organic dye dopants is possible resulting in amplification covering a wide range in the visible region.

Synthesis and Laser induced Studies of nanosized ZnO for Photonic Applications

Over the past few years, a little word with big potential has been rapidly entering into the world's consciousness-'nano'. Nanoscience and technology is a multidisciplinary field, involving the fabrication and understanding of matter at the finest level of a few nanomters.This thesis is about the synthesis and laser induced studies of nanosized ZnO,a versatile material with a wide range of applications.After synthesizing colloids and films of nano ZnO,the samples are studied using different optical methods.Interactions of intense laser beams with nanosized particles are found to open up many interesting scenarios with possible applications in the field of photonics.

Studies on Two-Photon Absorption of Aniline Using Thermal Lens Effect

Two-photon absorption spectrum of aniline is recorded using thermal lens effect with optical parametric oscillator as the pump source. Studies show that the two-photon absorption spectrum observed corresponds to I Al -. I B2 transition of aniline.

Two and Three Photon Absorption in Rhodamine 6G Methanol Solutions Using Pulsed Thermal Lens Technique

Dual beam transient thermal lens studies were carried out in rhodamine 6G methanol solutions using 532 nm pulses from a frequency doubled Nd:YAG laser. Analysis of thermal lens signal shows the existence of different nonlinear processes like two photon absorption and three photon absorption phenomena along with one photon absorption. Concentration of the dye in the solution has been found to influence the occurrence of the different processes in a significant way.

Cadmium Selenide Based Core-Shell Quantum Dots for Biosensing and Imaging Applications

The overall focus of the thesis involves the synthesis and characterization of CdSe QDs overcoated with shell materials for various biological and chemical sensing applications. Second chapter deals with the synthesis and characterization of CdSe and CdSe/ZnS core shell QDs. The primary attention of this work is to develop a simple method based on photoinduced charge transfer to optimize the shell thickness. Synthesis of water soluble CdSe QDs, their cytotoxicity analysis and investigation of nonlinear optical properties form the subject of third chapter. Final chapter deals with development of QD based sensor systems for the selective detection of biologically and environmentally important analytes from aqueous media.