A density matrix renormalization group method study of optical properties of porphines and metalloporphines

The symmetrized density matrix renormalization group method is used to study linear and nonlinear optical properties of free base porphine and metalloporphine. Long-range interacting model, namely, Pariser-Parr-Pople model is employed to capture the quantum many-body effect in these systems. The nonlinear optical coefficients are computed within the correction vector method. The computed singlet and triplet low-lying excited state energies and their charge densities are in excellent agreement with experimental as well as many other theoretical results. The rearrangement of the charge density at carbon and nitrogen sites, on excitation, is discussed. From our bond order calculation, we conclude that porphine is well described by the 18-annulenic structure in the ground state and the molecule expands upon excitation. We have modeled the regular metalloporphine by taking an effective electric field due to the metal ion and computed the excitation spectrum. Metalloporphines have D(4h) symmetry and hence have more degenerate excited states. The ground state of metalloporphines shows 20-annulenic structure, as the charge on the metal ion increases. The linear polarizability seems to increase with the charge initially and then saturates. The same trend is observed in third order polarizability coefficients. (C) 2012 American Institute of Physics. [doi: 10.1063/1.3671946]

Comparative study of different nonconserving time integrators for wave propagation in hyperelastic waveguides

This paper addresses the formulation and numerical efficiency of various numerical models of different nonconserving time integrators for studying wave propagation in nonlinear hyperelastic waveguides. The study includes different nonlinear finite element formulations based on standard Galerkin finite element model, time domain spectral finite element model, Taylor-Galerkin finite element model, generalized Galerkin finite element model and frequency domain spectral finite element model. A comparative study on the computational efficiency of these different models is made using a hyperelastic rod model, and the optimal computational scheme is identified. The identified scheme is then used to study the propagation of transverse and longitudinal waves in a Timoshenko beam with Murnaghan material nonlinearity.

Coherent (photon) vs incoherent (current) detection of multidimensional optical signals from single molecules in open junctions

The nonlinear optical response of a current-carrying single molecule coupled to two metal leads and driven by a sequence of impulsive optical pulses with controllable phases and time delays is calculated. Coherent (stimulated, heterodyne) detection of photons and incoherent detection of the optically induced current are compared. Using a diagrammatic Liouville space superoperator formalism, the signals are recast in terms of molecular correlation functions which are then expanded in the many-body molecular states. Two dimensional signals in benzene-1,4-dithiol molecule show cross peaks involving charged states. The correlation between optical and charge current signal is also observed. (C) 2015 AIP Publishing LLC.

Nonlinear optics in planar silica-on-silicon disk resonators

Optical frequency combs (OFCs) provide direct phase-coherent link between optical and RF frequencies, and enable precision measurement of optical frequencies. In recent years, a new class of frequency combs (microcombs) have emerged based on parametric frequency conversions in dielectric microresonators. Micocombs have large line spacing from 10's to 100's GHz, allowing easy access to individual comb lines for arbitrary waveform synthesis. They also provide broadband parametric gain bandwidth, not limited by specific atomic or molecular transitions in conventional OFCs. The emerging applications of microcombs include low noise microwave generation, astronomical spectrograph calibration, direct comb spectroscopy, and high capacity telecommunications.

In this thesis, research is presented starting with the introduction of a new type of chemically etched, planar silica-on-silicon disk resonator. A record Q factor of 875 million is achieved for on-chip devices. A simple and accurate approach to characterize the FSR and dispersion of microcavities is demonstrated. Microresonator-based frequency combs (microcombs) are demonstrated with microwave repetition rate less than 80 GHz on a chip for the first time. Overall low threshold power (as low as 1 mW) of microcombs across a wide range of resonator FSRs from 2.6 to 220 GHz in surface-loss-limited disk resonators is demonstrated. The rich and complex dynamics of microcomb RF noise are studied. High-coherence, RF phase-locking of microcombs is demonstrated where injection locking of the subcomb offset frequencies are observed by pump-detuning-alignment. Moreover, temporal mode locking, featuring subpicosecond pulses from a parametric 22 GHz microcomb, is observed. We further demonstrated a shot-noise-limited white phase noise of microcomb for the first time. Finally, stabilization of the microcomb repetition rate is realized by phase lock loop control.

For another major nonlinear optical application of disk resonators, highly coherent, simulated Brillouin lasers (SBL) on silicon are also demonstrated, with record low Schawlow-Townes noise less than 0.1 Hz^2/Hz for any chip-based lasers and low technical noise comparable to commercial narrow-linewidth fiber lasers. The SBL devices are efficient, featuring more than 90% quantum efficiency and threshold as low as 60 microwatts. Moreover, novel properties of the SBL are studied, including cascaded operation, threshold tuning, and mode-pulling phenomena. Furthermore, high performance microwave generation using on-chip cascaded Brillouin oscillation is demonstrated. It is also robust enough to enable incorporation as the optical voltage-controlled-oscillator in the first demonstration of a photonic-based, microwave frequency synthesizer. Finally, applications of microresonators as frequency reference cavities and low-phase-noise optomechanical oscillators are presented.

Electro-optic integration of embedded electrodes and waveguides in LiNbO3 using a femtosecond laser

We describe the fabrication of a Mach-Zehnder optical modulator in LiNbO3 by femtosecond laser micormachining, which is composed of optical waveguides inscripted by a femtosecond laser and embedded microelectrodes subsequently using femtosecond laser ablation and selective electroless plating. A half-wave voltage close to 19 V is achieved at a wavelength of 632.8 nm with an interaction length of 2.6 mm. This simple and cost-effective technique opens up new opportunities for fabricating integrated electro-optic devices. (C) 2008 Optical Society of America

Polaron effects on the optical absorptions in asymmetrical semi-parabolic quantum wells

The linear and nonlinear optical absorptions considering the weak-coupling electron-LO-phonon interaction in asymmetrical semiparabolic quantum wells are theoretically investigated. The numerical results for the typical GaAs/AlxGa1-xAs material show that the factors of Al content x, the relaxation time and the photon energy have great influence on the optical absorption coefficients. Moreover, the theoretical values of the optical absorptions are more than a factor of 2-3 higher than the one in the structure without considering the electron-LO-phonon interaction by calculating. (C) 2007 Elsevier B.V. All rights reserved.

Wave interactions in periodic structures and periodic dielectric waveguides

This work is concerned with a general analysis of wave interactions in periodic structures and particularly periodic thin film dielectric waveguides.

The electromagnetic wave propagation in an asymmetric dielectric waveguide with a periodically perturbed surface is analyzed in terms of a Floquet mode solution. First order approximate analytical expressions for the space harmonics are obtained. The solution is used to analyze various applications: (1) phase matched second harmonic generation in periodically perturbed optical waveguides; (2) grating couplers and thin film filters; (3) Bragg reflection devices; (4) the calculation of the traveling wave interaction impedance for solid state and vacuum tube optical traveling wave amplifiers which utilize periodic dielectric waveguides. Some of these applications are of interest in the field of integrated optics.

A special emphasis is put on the analysis of traveling wave interaction between electrons and electromagnetic waves in various operation regimes. Interactions with a finite temperature electron beam at the collision-dominated, collisionless, and quantum regimes are analyzed in detail assuming a one-dimensional model and longitudinal coupling.

The analysis is used to examine the possibility of solid state traveling wave devices (amplifiers, modulators), and some monolithic structures of these devices are suggested, designed to operate at the submillimeter-far infrared frequency regime. The estimates of attainable traveling wave interaction gain are quite low (on the order of a few inverse centimeters). However, the possibility of attaining net gain with different materials, structures and operation condition is not ruled out.

The developed model is used to discuss the possibility and the theoretical limitations of high frequency (optical) operation of vacuum electron beam tube; and the relation to other electron-electromagnetic wave interaction effects (Smith-Purcell and Cerenkov radiation and the free electron laser) are pointed out. Finally, the case where the periodic structure is the natural crystal lattice is briefly discussed. The longitudinal component of optical space harmonics in the crystal is calculated and found to be of the order of magnitude of the macroscopic wave, and some comments are made on the possibility of coherent bremsstrahlung and distributed feedback lasers in single crystals.

Super-resolution with a nonlinear thin film: Beam reshaping via internal multi-interference

In laser applications, the size of the focus spot can be reduced beyond the diffraction limit with a thin film of strong nonlinear optical Kerr effect. We present a concise theoretical simulation of the device. The origin of the super-resolution is found to be mainly from the reshaping effect due to the strongly nonlinear refraction mediated multi-interference inside the thin film. In addition, both diffraction and self-focusing effects have been explored and found negligible for highly refractive and ultrathin films in comparison with the reshaping effect. Finally, the theoretic model has been verified in experiments with single Ge2Sb2Te5 film and SiN/Si/SiN/Ge2Sb2Te2 multilayer structures. (c) 2006 American Institute of Physics.

Structure and properties of amorphous thin film for optical data storage

In this paper the magnetic and magneto-optical properties of amorphous rare earth-transition metal (RE-TM) alloys as well as the magnetic coupling in the multi-layer thin films for high density optical data storage are presented. Using magnetic effect in scanning tunneling microscopy the clusters structure of amorphous RE-TM thin films has been observed and the perpendicular magnetic anisotropy in amorphous RE-TM thin films has been interpreted. Experimental results of quick phase transformation under short pulse laser irradiation of amorphous semiconductor and metallic alloy thin films for phase change optical recording are reported. A step-by-step phase transformation process through metastable states has been observed. The waveform of crystallization propagation in micro-size spot during laser recording in amorphous semiconductor thin films is characterized and quick recording and erasing mechanism for optical data storage with high performance are discussed. The nonlinear optical effects in amorphous alloy thin films have been studied. By photo-thermal effect or third order optical nonlinearity, the optical self-focusing is observed in amorphous mask thin films. The application of amorphous thin films with super-resolution near field structure for high-density optical data storage is performed. (c) 2007 Elsevier B.V. All rights reserved.

Preparation and optical properties of silicate glasses containing Pd nanoparticles

We report the space selective precipitation of Pd nanoparticles in Pd2+ -doped silicate glass by ultrashort laser pulses irradiation and further annealing. Absorption spectra, transmission electron microscopy, refractive index measurement and Z-scan technique demonstrated that metallic Pd nanoparticles were precipitated in the glass sample after irradiation by an 800-nm femtosecond laser and subsequent annealing at 600 degrees C. We discuss a refractive index change and nonlinear absorption that combines the precipitation of Pd nanoparticles. Crown Copyright (c) 2005 Published by Elsevier B.V. All rights reserved.

All-optical switching in a vertical coupler space switch employing photocarrier-induced nonlinearity

A novel compact integrated nonlinear optical switch is demonstrated. Using a high-power picosecond pulse of 5-ps pulsewidth and 250-MHz repetition rate, all-optical switching with a contrast ratio of 23 dB has been achieved using an in-fiber input power < 14 dBm (100 pJ/pulse). The switch speed depends on the carrier sweep-out time, which can be reduced to the 10 ps range by either applying a reverse bias or by introduction of carrier recombination centers in the active layer.

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.

PCB-integrated optical waveguide sensors: An ammonia gas sensor

This paper presents a novel platform for the formation of cost-effective PCB-integrated optical waveguide sensors. The sensor design relies on the use of multimode polymer waveguides that can be formed directly on standard PCBs and commercially-available chemical dyes, enabling the integration of all essential sensor components (electronic, photonic, chemical) on low-cost substrates. Moreover, it enables the detection of multiple analytes from a single device by employing waveguide arrays functionalised with different chemical dyes. The devices can be manufactured with conventional methods of the PCB industry, such as solder-reflow processes and pick-and-place assembly techniques. As a proof of principle, a PCB-integrated ammonia gas sensor is fabricated on a FR4 substrate. The sensor operation relies on the change of the optical transmission characteristics of chemically functionalised optical waveguides in the presence of ammonia molecules. The fabrication and assembly of the sensor unit, as well as fundamental simulation and characterisation studies, are presented. The device achieves a sensitivity of approximately 30 ppm and a linear response up to 600 ppm at room temperature. Finally, the potential to detect multiple analytes from a single device is demonstrated using principal-component analysis. © 1983-2012 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.