New generations of ultrashort and intense laser pulses as well ashigh power synchrotron radiation sources and x-ray free electronlasers have promoted fast developments in nonlinear optics andx-ray spectroscopy.The new experimental achievements and the appearance of varieties of novelnonlinear phenomena call for further development of theories. The objective of this thesis is to develop and apply thetheories to explain existing experimental data and to suggest new experiments. The first part of the thesis is devoted to nonlinear propagation of optical pulses. It is shown that the vibrational levels can be selectively populated by varying the duration, shape and intensity of the pump pulse. We obtained a strict analytical solution for the resonant two-photon interaction in a multilevel system beyond rotating wave approximation. Simulations show that the polarization anisotropy of the two-photon excitation affects strongly the anisotropy of photobleaching.The two-photon area theorem is reformulated with taking into account the dynamical Stark shift and the contribution from the permanent dipole moments. In general the dynamical Stark shift does not allow complete population of the excited state, but it can be compensated by detunings in atoms. A dynamical theory of the sequential two-photon absorption of  microsecond pulses  is developed to explore the role of transverse inhomogeneity of the light beam on optical limiting properties.  The propagation of ultrashort laser pulses in nondipolar and dipolar media is investigated with special attention to the generation of superfluorescence and supercontinuum and the formation of attosecond pulses. The second part of the thesis addresses the interaction of molecules with x-ray radiation.  We explore here the role of nuclear dynamics in resonant Auger scattering. Multimode simulations of the Auger spectra of ethylene molecule explain the main spectral features of the experimental spectra and show that the spectral profiles are formed mainly due to six vibrational modes. We predict the Doppler splitting of the atomic peak in resonant Auger scattering from SF6 molecule for circularly polarized x-rays. This effect is confirmed by the recent experiment. A new scheme of x-ray pump-probe spectroscopy, namely, resonant inelastic x-ray scattering accompanied by core-hole hopping induced by strong laser fields is suggested. The laser-induced promotion of core holes opens the symmetry forbidden scattering channels and gives rise to new spectral lines in the x-ray scattering spectrum. The strength of the symmetry forbidden lines becomes strong when  the time of Rabi flopping is shorter than the lifetime of the core-excited state. We study the role of propagation of femtosecond x-ray free-electron pulses on the Auger process. Simulations show  that there exists a strong competition between Auger decay and stimulated emission. The Auger yield and Auger branching ratio are strongly suppressed in the course of pulse propagation. / QC 20100729

This thesis explores the use of engineered nonlinear crystals from the KTiOPO4 (KTP) family as the gain material in optical parametric amplifiers (OPAs), with the aim to achieve more knowledge about the benefits and limitations of these devices. The work aims further at extending the possible applications of OPAs by constructing and investigating several efficient and well performing amplifiers. An OPA consists of a strong pump source, which transfers its energy to a weak seed beam while propagating through a nonlinear crystal. The crystals employed in this work are members of the KTP family, which are attractive due to their large nonlinear coefficients, high resistance to damage and wide transparency range. The flexibility of OPAs with respect to different wavelength regions and pulse regimes was examined by employing various dissimilar seed and pump sources. The possibility to adapt an OPA to a specific pump and seed wavelength and achieve efficient energy conversion between the beams, originates from quasi-phasematching, which is achieved in periodically poled (PP) nonlinear crystals. Quasi-phasematched samples can be obtained by changing the position of certain atoms in a ferroelectric crystal and thereby reversing the spontaneous polarisation. In this thesis several material properties of PP crystals from the KTP family were examined. The wavelength and temperature dispersion of the refractive index were determined for PP RbTiOPO4, which is essential for future use of this material. Another experiment helped to increase the insight into the volumes close to domain walls in PP crystals Further, several OPAs were built and their ability to efficiently amplify the seed beam without changing its spectral or spatial properties was studied. Small signal gains of up to 55 dB and conversion efficiencies of more than 35 % were achieved for single pass arrangements employing 8 mm long PPKTP crystals. Apart from constructing three setups, which generated powerful nanosecond, picosecond and femtosecond pulses, the possibility to amplify broadband signals was investigated. An increase of the OPA bandwidth by a factor of approximately three was achieved in a noncollinear configuration. / QC 20101013

This thesis describes research on near degenerate quasi phase-matched opticalparametric oscillators (OPO) where volume Bragg gratings (VBG) are used toproduce narrow oscillation bandwidth. These OPOs are then used to pump a secondOPO to generate mid-infrared radiation. The atmospheric transmission windows in the 3.5 to 5 μm wavelength region areused for seekers on infrared homing missiles. These missiles are available to guerrillaand terrorist groups and have been used in a number of attacks on military and civilianaircraft. Laser sources at the same wavelengths are an important component incountermeasure systems for aircraft self-protection. Similar laser sources also haveapplications in laser surgery. At wavelengths longer than 4 μm crystal materials for multi-Watt level averagepower nonlinear devices is a problem. The best solution so far is to use ZnGeP2(ZGP). ZGP and the available alternatives all have a problem of near-infraredabsorption, and a mid-infrared OPO thus has to use a pump wavelength near 2 μm.This pump source can be a neodymium laser at 1.06 μm with a near degenerate OPO. Nonlinear devices for low to medium pulse energies are dominated by quasi phasematchedmaterials because of their higher effective nonlinearities and lack of walkoff.In addition they allow type I interaction where signal and idler from the OPOhave the same polarization, which has the advantage that both waves can be used topump the ZGP OPO. The drawback of this is that the near-degenerate interaction hasvery wide gain bandwidth. Efficient pumping of the second OPO demands narrowbandwidth output from the first OPO.Volume Bragg gratings that are glass materials with a periodic refractive indexmodulation have emerged as high quality narrow bandwidth reflectors. By using aVBG as one cavity mirror in an OPO the feedback bandwidth and hence the OPOoscillation bandwidth can be kept very narrow. Signal and idler bandwidths of 10 and20 GHz (FWHM) at 2122 and 2135 nm, respectively, have been demonstrated. Thisshould be compared to the several hundred nanometre bandwidth from an OPO usingdielectric mirrors. Very narrow bandwidth operation has been achieved so close todegeneracy that the signal and idler are not resolvable. The total output energy generated in the PPKTP OPO (signal and idler together)has been used to pump a ZGP OPO that produced mid-IR radiation. Tuning of thesignal from a ZGP OPO from 2.9 μm to degeneracy at 4.3 μm has been shown, with acorresponding idler wavelength tuneable up to 8 μm. The highest conversionefficiency that has been reached from 1.06 μm to the mid-IR was 12 %. This setupused a PPKTP OPO with 30 % conversion efficiency and 13 nm separation of signaland idler (2122 and 2135 nm). The pulse repetition frequency was 20 kHz and thegenerated output power in the mid-IR was 3.2 W. / QC 20100517

No description available.

Silicon Nanowires (SiNWs) with ability to confine carriers and photons in two directions while allowing propagation in third dimension offer interesting modified optical properties such as increased material absorption and optical non-linearities with regard to that of bulk silicon. Enhanced optical properties in SiNWs open a window not only to improve the performance of existing devices but also to realize novel structures. As such, I chose to investigate SiNWs for their applications in photonics, especially for sensing and non-linear devices. My goal was to conduct fundamental research on the optical properties of these SiNWs, and then develop an integration platform to realize practical devices. The platform should be compatible with IC manufacturing. Electron Beam Lithography (EBL) using a Poly Methyl Methacrylate (PMMA) resist followed by Inductively Coupled Plasma Reactive Ion Etching (ICP-RIE) is used for SiNWs fabrication. Now we are able to fabricate nanowires as small as 15 nm in diameter with the smallest separation of 50 nm. In addition, the interface between SiNWs and Si substrate is optically smooth enabling us to fundamentally understand optical properties of these structures. During the course of this project, I have contributed new fundamental knowledge about SiNWs. For example, Second Harmonic Generation (SHG) is demonstrated in SiNWs, which is absent in bulk silicon. This is achieved by self-straining the nanowires and is the first demonstration of this kind. Second-order non-linearities are more efficient for optical signal processing than third-order ones (which have been used for silicon photonics devices so far). Therefore, these results open a new area of research in silicon. In addition to second order nonlinearity, high enhancement of Raman scattering is achieved in SiNWs fabricated on Silicon on Insulator (SOI) substrate. This can find promising applications in sensing and nonlinear based devices such as optical switches and logic gates. Further, polarization resolved reflections from these nanowire arrays were measured and significant differences were observed for the reflection characteristics for the sand p-polarized beams. In order to understand these reflections, an effective index model is proposed based on calculations using Finite Difference Time Domain (FDTD) method. Results of this analysis provide useful information for designing of many optical devices using SiNWs such as solar cells and photodetectors. As another part of this thesis, vivid colors in mutually coupled SiNWs is demonstrated where nanowire diameters range from 105 nm to 345 nm. A simple sensor is demonstrated by observing the change in the reflected color with changing refractive index of the surrounding medium. A refractive index resolution of 5×10−5 is achieved using a simple charge coupled device (CCD) camera. Although, there were some paradigm shifting results during my fundamental studies, it became very apparent that SiNWs suffer from a major issue inhibiting their use in photonics devices. Below the diameter of 100 nm where these enhanced material properties were observed, SiNW is a poor optical waveguide with less than 1 % of light confined. The low confinement factor means that though the intrinsic properties of SiNWs increase, the overall device performance is not significantly enhanced. To overcome this issue, a new platform technology is invented, called Silicon Nanowire Optical Waveguide (SNOW). It combines the material advantages of nanostructures with the optical properties of conventional waveguides, and consists of arrays of nanowires in close proximity. It is shown that such a structure can guide an optical mode using the FDTD method. This waveguide structure can be used as a versatile platform to manufacture various devices such as sensors, switches, modulators, grating, and delay lines. For instance, a novel bio-sensor is proposed and designed whose sensitivity is enhanced by a factor of 20, compared to conventional silicon-wire waveguides.

The lateral spatial separation between the circular polarization components of a linearly polarized light beam impinging at off-normal incidence on an air-semiconductor interface is investigated experimentally and theoretically. This fundamental optical phenomenon is referred to as the Spin Hall effect of light (SHEL). An optical pump-probe technique is demonstrated to resolve in situ the nanometer size SHEL displacement of a beam transmitted inside an absorptive material. Three different types of optical interactions in silicon and GaAs demonstrate the technique’s general applicability. First, resonant ∼150 fs pump and probe pulses at λ = 820 nm resolve the SHEL displacement via free-carrier absorption in a 10 μm thick silicon sample. The measured SHEL displacements for a p-polarized probe beam are obtained between −10 to 150 nm as a function of the angle of incidence on the sample. Different angles of incidence are achieved by keeping a fixed angular separation between the pump and the probe beams while rotating the sample about the axis perpendicular to the plane of incidence. In another experiment, an optically thin (500 nm thick) GaAs sample allows one to use Pauli-blocking as an optical interaction to investigate the polarization and angular dependence of the SHEL in the probe beam. For such a polarization-dependent imaging technique, the SHEL displacement in the pump beam also contributes to the measured signal and is evaluated experimentally. A probe beam at normal incidence is used to measure a SHEL displacement of ∼180 nm in a transmitted p-polarized pump beam impinging on the sample with an angle of incidence of 55 degrees. Finally, two-photon absorption is used to resolve the SHEL in a (001) oriented 500 μm thick GaAs wafer using an optical source generating sub-bandgap radiation (λ = 1550 nm) with a pulse duration of 120 fs. Linearly p- and s- co-polarized pump and probe beams are also used to investigate the polarization dependence of the SHEL. All the experimental results obtained using these different optical interactions agree with the theory within the experimental error. Finally, analytical expressions of the shifts experienced by the circular components of a beam impinging at an interface between two optical media are also derived for an incident beam with an arbitrary spatial distribution.

The lateral spatial separation between the circular polarization components of a linearly polarized light beam impinging at off-normal incidence on an air-semiconductor interface is investigated experimentally and theoretically. This fundamental optical phenomenon is referred to as the Spin Hall effect of light (SHEL). An optical pump-probe technique is demonstrated to resolve in situ the nanometer size SHEL displacement of a beam transmitted inside an absorptive material. Three different types of optical interactions in silicon and GaAs demonstrate the technique’s general applicability. First, resonant ∼150 fs pump and probe pulses at λ = 820 nm resolve the SHEL displacement via free-carrier absorption in a 10 μm thick silicon sample. The measured SHEL displacements for a p-polarized probe beam are obtained between −10 to 150 nm as a function of the angle of incidence on the sample. Different angles of incidence are achieved by keeping a fixed angular separation between the pump and the probe beams while rotating the sample about the axis perpendicular to the plane of incidence. In another experiment, an optically thin (500 nm thick) GaAs sample allows one to use Pauli-blocking as an optical interaction to investigate the polarization and angular dependence of the SHEL in the probe beam. For such a polarization-dependent imaging technique, the SHEL displacement in the pump beam also contributes to the measured signal and is evaluated experimentally. A probe beam at normal incidence is used to measure a SHEL displacement of ∼180 nm in a transmitted p-polarized pump beam impinging on the sample with an angle of incidence of 55 degrees. Finally, two-photon absorption is used to resolve the SHEL in a (001) oriented 500 μm thick GaAs wafer using an optical source generating sub-bandgap radiation (λ = 1550 nm) with a pulse duration of 120 fs. Linearly p- and s- co-polarized pump and probe beams are also used to investigate the polarization dependence of the SHEL. All the experimental results obtained using these different optical interactions agree with the theory within the experimental error. Finally, analytical expressions of the shifts experienced by the circular components of a beam impinging at an interface between two optical media are also derived for an incident beam with an arbitrary spatial distribution.

Two colour pumping was used to investigate the short-pulse technique of Multifrequency Raman Generation (MRG) in the transient regime of Raman scattering. In the course of this study we have demonstrated the ability to generate over thirty Raman orders spanning from the infrared to the ultraviolet, investigated the dependence of this generation on the pump intensities and the dispersion characteristics of the hollow-fibre system in which the experiment was conducted, and developed a simple computer model to help understand the exhibited behaviours. These dependence studies have revealed some characteristics that have been previously mentioned in the literature, such as the competition between MRG and self-phase modulation, but have also demonstrated behaviours that are dramatically different than anything reported on the subject. Furthermore, through a simple modification of the experimental apparatus we have demonstrated the ability to scatter a probe pulse into many Raman orders, generating bandwidth comparable to the best pump-probe experiments of MRG. By using a numeric fast Fourier transform, we predict that our spectra can generate pulses as short as 3. 3fs, with energies an order of magnitude larger than pulses of comparable duration that are made using current techniques.

Two colour pumping was used to investigate the short-pulse technique of Multifrequency Raman Generation (MRG) in the transient regime of Raman scattering. In the course of this study we have demonstrated the ability to generate over thirty Raman orders spanning from the infrared to the ultraviolet, investigated the dependence of this generation on the pump intensities and the dispersion characteristics of the hollow-fibre system in which the experiment was conducted, and developed a simple computer model to help understand the exhibited behaviours. These dependence studies have revealed some characteristics that have been previously mentioned in the literature, such as the competition between MRG and self-phase modulation, but have also demonstrated behaviours that are dramatically different than anything reported on the subject. Furthermore, through a simple modification of the experimental apparatus we have demonstrated the ability to scatter a probe pulse into many Raman orders, generating bandwidth comparable to the best pump-probe experiments of MRG. By using a numeric fast Fourier transform, we predict that our spectra can generate pulses as short as 3. 3fs, with energies an order of magnitude larger than pulses of comparable duration that are made using current techniques.

<p>Collective behavior in many-body systems, where the dynamics of an individual element depend on the state of the entire ensemble, play an important role in both basic science research and applied technologies. Over the last twenty years, studies of such effects in cold atomic vapors have lead to breakthroughs in areas such as quantum information science and atomic and condensed matter physics. Nevertheless, in order to generate photon-mediated atom-atom coupling strengths that are large enough to produce collective behavior, these studies employ techniques that intrinsically limit their applicability. In this thesis, I describe a novel nonlinear optical process that enables me to overcome these limitations and realize a new regime of collective light-matter interaction.</p><p>My experiment involves an anisotropic cloud of cold rubidium atoms illuminated by a pair of counterpropagating optical (pump) fields propagating at an angle to the trap's long axis. When the pump beam intensities exceed a threshold value, a collective instability occurs in which new beams of light are generated spontaneously and counterpropagate along the trap's long axis. In order to understand the physical mechanism responsible for this behavior, I study first the system's nonlinear optical response when driven below the instability threshold. I find that the incident optical fields produce an optical lattice that causes the atoms to become spatially organized on the sub-wavelength length scale. This organization corresponds to the formation of an atomic density grating, which effectively couples the involved fields to one another and enables the transfer of energy between them. The loading of atoms into this grating is enhanced by my choice of field polarizations, which simultaneously results in cooling of the atoms from T~30 &mu;K to T~3 &mu;K via the Sisyphus effect. As a result, I observe a fifth-order nonlinear susceptibility &chi;^{(5)}=1.9x10^-12 (m/V)^4 that is 7 orders of magnitude larger than previously observed. In addition, because of the unique scaling of the resulting nonlinear response with material parameters, the magnitude of the nonlinearity can be large for small pump intensities (\ie, below the resonant electronic saturation intensity 1.6 mW/cm^2) while simultaneously suffering little linear absorption. I confirm my interpretation of the nonlinearity by developing a theoretical model that agrees quantitatively with my experimental observations with no free parameters.</p><p>The collective instability therefore corresponds to the situation where the cold vapor transitions spontaneously from a spatially-homogeneous state to an ordered one. This emergent organization leads to the simultaneous emission of new optical fields in a process that one can interpret either in terms of mirrorless parametric self-oscillation or superradiance. By mapping out the phase diagram for this transition, I find that the instability can occur for pump intensities as low as 1 mW/cm^2, which is approximately 50 times smaller than previous observations of similar phenomena. The intensity of the emitted light can be up to 20% of the pump beam intensity and depends superlinearly on the number of atoms, which is a clear signature of collective behavior. In addition, the generated light demonstrates temporal correlations between the counterpropagating modes of up to 0.987 and is nearly coherent over several hundred &mu;s. The most significant attributes of the light, though, are that it consists of multiple transverse spatial modes and persists in steady-state. This result represents the first observation of such dynamics, which have been shown theoretically to lead to a rich array of new phenomena and possible applications.</p> / Dissertation