Quantum cascade lasers (QCLs) operate due to population inversion on intersubband in unipolar mutiple-quantum-well (MQW) heterostructure. QCLs are considered one of the most flexible and powerful light semiconductor sources in the mid- and far-infrared (IR) wavelength range, covering most of the critical spectral regions relevant to IR applications. InGaAs/InAlAs/InP QCLs are the only semiconductor lasers capable of continuous wave (CW) operation at room temperature (RT) in the spectral range 3.4-12 micron. This dissertation details the development of RT QCLs based on passive nonlinear coupled-quantum-well structures monolithically integrated into mid-IR QCLs to provide a giant nonlinear response for the pumping frequency. The primary focus of short-wavelength approach in this dissertation is to develop of RT InGaAs/InAlAs/InP QCLs for lamda=2.5-3.7 micron region, based on quasi-phase-matched intracavity second harmonic generation (SHG) associated with intersubband transition. Intersubband optical transition can be engineered by the choice of quantum well and barrier thicknesses to provide the appropriate energy levels, optical dipole matrix elements, and electron scattering rates amongst other parameters. Thus, aside from their linear optical properties, resonant intersubband transitions in coupled QW's can also be designed to produce nonlinear optical medium with giant nonlinear optical susceptibilities. In long-wavelength region, at high temperature, the population inversion is reduced between the upper and lower laser levels due to the longitudinal optical (LO) phonon scattering of thermal carriers in the upper laser state and the thermal backfilling of carriers into the lower laser level from the injector state. This dissertation aims to improve an alternative approach for THz QCL sources based on intra-cavity difference frequency generation (DFG) in dual-wavelength mid-IR QCLs with a passive nonlinear structure, designed for giant optical nonlinearity. Further studies describe that Cerenkov DFG scheme allows for extraction of THz radiation along the whole length of the laser waveguide and provides directional THz emission in 1.2-4.5 THz range. An important requirement for many applications, like chemical sensing and molecular spectroscopy, is single-mode emission. We demonstrate single-mode RT DFG THz QCLs operation in 1-5 THz region by employing devices as integrated dual-period DFB lasers, where efficient solid state RT sources do not exist. / text

This thesis describes a number of studies on organic semiconductors focused around using them as gain media for lasers. The photophysical properties of organic semiconductors are studied using a wide range of experimental techniques, allowing the evaluation of new materials and novel excitation schemes for use in organic semiconductor lasers. Polyfluorene is a well-established conjugated polymer laser gain medium and in this thesis its excellent lasing properties are combined with its two photon absorption properties to demonstrate a tunable two-photon pumped solid-state laser based on a commercially available organic semiconductor. A family of bisfluorene dendrimers was studied using a number of photophysical techniques to evaluate their potential as laser materials. Distributed feedback lasers based on one of the dendrimers are demonstrated with lasing thresholds comparable to polyfluorene. The same materials were found to have enhanced two-photon absorption properties in comparison to polyfluorene, leading to the fabrication of tunable two-photon pumped dendrimer lasers. A member of a novel family of star-shaped oligofluorene truxenes was evaluated as a laser gain material and the distributed feedback lasers made from them show some of the lowest lasing thresholds reported for organic semiconductors, partly as a consequence of exceptionally low waveguide losses in comparison to other single-material thin films. Finally, an organic laser dye is blended with a conjugated polymer, where the dye molecules harvest the excitation light of a GaN laser diode and transfer its energy to the polymer molecules. This is the first time such a scheme is used in an organic laser and in combination with a novel surface-emitting distributed Bragg reflector resonator allows the demonstration of a diode-pumped organic laser, a significant step towards simplifying organic lasers.

This dissertation investigates two long standing issues in nonlinear optics: complete characterization of the ultrafast dynamics of simple molecules, and the potential of a two-photon laser using a bulk semiconductor gain medium. Within the Born-Oppenheimer approximation, nonlinear refraction in molecular liquids and gases can arise from both bound-electronic and nuclear origins. Knowledge of the magnitudes, temporal dynamics, polarization and spectral dependences of each of these mechanisms is important for many applications including filamentation, white-light continuum generation, all-optical switching, and nonlinear spectroscopy. In this work the nonlinear dynamics of molecules are investigated in both liquid and gas phase with the recently developed beam deflection technique which measures nonlinear refraction directly in the time domain. Thanks to the utility of the beam deflection technique we are able to completely determine the third-order response function of one of the most important molecular liquids in nonlinear optics, carbon disulfide. This allows the prediction of essentially any nonlinear refraction or two-photon absorption experiment on CS2. Measurements conducted on air (N2 and O2) and gaseous CS2 reveal coherent rotational revivals in the degree of alignment of the ensemble at a period that depends on its moment of inertia. This allows measurement of the rotational and centrifugal distortion constants of the isolated molecules. Additionally, the rotational contribution to the beam deflection measurement can be eliminated thanks to the particular polarization dependence of the mechanism. At a specific polarization, the dominant remaining contribution is due to the bound-electrons. Thus both the bound-electronic nonlinear refractive index of air, and second hyperpolarizability of isolated CS2 molecules, are measured directly. The later agrees well with liquid CS2 measurements, where local field effects are significant. The second major portion of this dissertation addresses the possibility of using bulk semiconductors as a two-photon gain medium. A two-photon laser has been a goal of nonlinear optics since shortly after the original laser*s development. In this case, two-photons are emitted from a single electronic transition rather than only one. This processes is known as two-photon gain (2PG). Semiconductors have large two-photon absorption coefficients, which are enhanced by ~2 orders of magnitude when using photons of very different energies, e.g., ћωa≈10ћωb. This enhancement should translate into large 2PG coefficients as well, given the inverse relationship between absorption and gain. Here, we experimentally demonstrate both degenerate and nondegenerate 2PG in optically excited bulk GaAs via pump-probe experiments. This constitutes, to my knowledge, the first report of nondegenerate two-photon gain. Competition between 2PG and competing processes, namely intervalence band and nondegenerate three-photon absorption (ND-3PA), in both cases are theoretically analyzed. Experimental measurements of ND-3PA agree with this analysis and show that it is enhanced much more than ND-2PG. It is found for both degenerate and nondegenerate photon pairs that the losses dominate the two-photon gain, preventing the possibility of a two-photon semiconductor laser.