Investigations of Nonlinear Optical Properties of certain organic photonic materials using Z-Scan and DFWM techniques

Nonlinear optical processes in organic compounds have attracted considerable interest in the field of science and technology because of their compelling technological promises in fields of optical communication,computing,switching and signal processing.As a result of the synthesis of novel organic compounds with varying degree of nonlinear optical strength, many practical devices based on these are getting realised giving new theoretical insights into the nonolinear optical behaviour of materials.Organic compounds like phthalocyanines and porphyrins have evoked great deal of interest in the field of photonic technology.The present thesis describes the results obtained from the investigations carried out on the nonlinear optical properties of certain organo-metallic compounds using Z-Scan and DFWM techniques.

Sensitive detection of nitric oxide using seeded parametric four-wave mixing

A sensitive near-resonant four-wave mixing technique based on two-photon parametric four-wave mixing has been developed. Seeded parametric four-wave mixing requires only a single laser as an additional phase matched seeder field is generated via parametric four-wave mixing of the pump beam in a high gain cell. The seeder field travels collinearly with the pump beam providing efficient nondegenerate four-wave mixing in a second medium. This simple arrangement facilitates the detection of complex molecular spectra by simply scanning the pump laser. Seeded parametric four-wave mixing is demonstrated in both a low pressure cell and an air/acetylene flame with detection of the two-photon C (2) Pi(upsilon'=0)<--X (2) Pi(upsilon =0) spectrum of nitric oxide. From the cell data a detection limit of 10(12) molecules/cm(3) is established. A theoretical model of seeded parametric four-wave mixing is developed from existing parametric four-wave mixing theory. The addition of the seeder field significantly modifies the parametric four-wave mixing behaviour such that in the small signal regime, the signal intensity can readily be made to scale as the cube of the laser pump power while the density dependence follows a more familiar square law dependence, In general, we find excellent agreement between theory and experiment. Limitations to the process result from an ac Stark shift of the two-photon resonance in the high pressure seeder cell caused by the generation of a strong seeder field, as well as a reduction in phase matching efficiency due to the presence of certain buffer species. Various optimizations are suggested which should overcome these limitations, providing even greater detection sensitivity. (C) 1998 American Institute of Physics, [S0021-9606(98)01014-9].

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).

Studies on some nonlinear optical phenomena-optical phase conjugation and continuous wave second harmonic generation

Nonlinear optics has emerged as a new area of physics , following the development of various types of lasers. A number of advancements , both theoretical and experimental . have been made in the past two decades . by scientists al1 over the world. However , onl y few scientists have attempted to study the experimental aspects of nonlinear optical phenomena i n I ndian laboratories. This thesis is the report of an attempt made in this direction. The thesis contains the details of the several investigations which the author has carried out in the past few years, on optical phase conjugation (OPC) and continuous wave CCVD second harmonic generation CSHG). OPC is a new branch of nonlinear optics, developed only in the past decade. The author has done a few experiments on low power OPC in dye molecules held in solid matrices, by making use of a degenerate four wave mixing CDFWND scheme. These samples have been characterised by studies on their absorption-spectra. fluorescence spectra. triplet lifetimes and saturation intensities. Phase conjugation efficiencies with r espect to the various parameters have been i nvesti gated . DFWM scheme was also employed i n achievi ng phase conjugation of a br oadband laser C Nd: G1ass 3 using a dye solution as the nonlinear medium.

Femtosecond Rotational Raman Coherence Spectroscopy of Cyclohexane in a Pulsed Supersonic Jet

We combine the technique of femtosecond degenerate four-wave mixing (fs-DFWM) with a high repetition-rate pulsed supersonic jet source to obtain the rotational coherence spectrum (RCS) of cold cyclohexane (C(6)H(12)) with high signal/noise ratio. In the jet expansion, the near-parallel flow pattern combined with rapid translational cooling effectively eliminate dephasing collisions, giving near-constant RCS signal intensities over time delays up to 5 ns. The vibrational cooling in the jet eliminates the thermally populated vibrations that complicate the RCS coherences of cyclohexane at room temperature [Bragger, G.; et al. J. Phys. Chem. A 2011, 115, 9567]. The rotational cooling reduces the high-J rotational-state population, yielding the most accurate ground-state rotational constant to date, B(0) = 4305.859(9) MHz. Based on this B(0), a reanalysis of previous room-temperature gas-cell RCS measurements of cydohexane gives improved vibration rotation interaction constants for the v(32), v(6), v(16), and v(24) vibrational states. Combining the experimental B(0)(C(6)H(12)) with CCSD(T) calculations yields a very accurate semiexperimental equilibrium structure of the chair isomer of cyclohexane