Whispering gallery modes (WGM) microcavity have played an ubiquitous role due to their high quality factor Q and small effective mode volume $V_{eff}$. They are suitable for a broad range of applications and scientific research including cavity quantum electrodynamics (c-QED), sensing, parametric oscillation, frequency comb and so forth. The major nonlinear effect in silica is the Kerr nonlinearity that arises from the dependence of refractive index on the signal intensity. In this thesis, we focus on the theoretical analysis of Kerr and Raman nonlinear effects in a silica spherical microcavity. We derive several analytical models for various nonlinear effects, including self phase modulation (SPM), cross phase modulation (XPM) and stimulated Raman scattering (SRS). The first part of this thesis develops a theoretical framework to describe the impact of Kerr nonlinearity, especially SPM on WGM. First a mathematical formulation to express $\chi^{(3)}$ in spherical co-ordinates is developed. We define the effective mode volume $V_{eff}$ for the the first time to analyze SPM effects by taking $\chi^{(3)}$ tensor in spherical co-ordinates and it is found that the effective mode volume is always smaller than the physical volume of the microsphere. Simulation results show that whispering gallery mode undergoes a negative frequency shift proportional to the injected energy due to SPM. Later, we extended the analysis to describe the nonlinear interaction between two WGMs. An analytical model is developed to describe the XPM effect in microsphere. Expressions for effective mode volumes and effective nonlinear coefficients to describe XPM are derived analytically. It is found that, when the effective mode volume increases, effective nonlinear coefficient becomes smaller and hence, we achieve a lower frequency shift. An analytical expression for the coupling of whispering gallery mode is derived. The resonant frequency of a weak probe mode can be shifted by a strong pump mode due to XPM and the frequency shift of the probe is proportional to the pump energy. Also, An analytical expression for describing the Raman effect in a spherical microcavity is developed by including the delayed Raman response. The results show that the signal power is amplified due to the SRS effect. / Thesis / Master of Applied Science (MASc)

Le contrôle des polluants environnementaux présents à faible concentration a conduit à la création de détecteurs miniaturisés, à bas coûts et ultra-sensibles, capables d’identifier spécifiquement certaines substances. Dans cette thèse, la méthode de détection explorée repose sur la sensibilité de micro-lasers polymères à une variation d’indice de réfraction. Cette approche a été mise en application pour détecter des métaux lourds (mercure – Hg2+, cadmium – Cd2+ et plomb – Pb2+) dans l’eau potable. En effet les fréquences de résonance de ces micro-cavités sont particulièrement sensibles à l’indice de réfraction du milieu extérieur et se déplacent lorsque celui-ci est modifié. Ce système permet ainsi une détection sans marqueur (« label ») en recouvrant la cavité d’une couche de reconnaissance spécifique de l’espèce recherchée. L’originalité de ce travail repose sur l’utilisation de micro-cavités actives, ou micro-lasers, fabriquées avec des polymères dopés par des colorants lasers. En effet les micro-lasers permettent d’augmenter le rapport signal/bruit et de profiter de pics de résonance étroits, même pour des facteurs de qualité de l’ordre de quelques milliers seulement. Le choix de matériaux organiques comme milieu à gain a été dicté par les nombreux avantages qu’ils offrent. Contrairement aux semi-conducteurs inorganiques, les polymères peuvent être fonctionnalisés de manière relativement aisée et l’utilisation de matériaux poreux devrait augmenter la sensibilité en faisant circuler le fluide à tester à l’intérieur même du résonateur. De plus le protocole de fabrication des micro-lasers organiques reste d’un coût modéré et permet une intégration aisée en micro-fluidique. Deux voies différentes ont été explorées dans cette thèse : détection d’une variation d’indice de réfraction avec des cavités non-fonctionnalisées et détection d’ions lourds avec des cavités fonctionnalisées. Dans le premier cas, la sensibilité obtenue est comparable à ce qui est publié pour des micro-résonateurs passifs. Dans le second cas, nous avons réussi à mettre en évidence la présence d’ions mercure jusqu’à 10-6 M. Quelques approches ont été envisagées pour diminuer encore le seuil de détection dont certaines ont été vérifiées expérimentalement. Ainsi, cette étude propose un prototype de composant sur puce pour la détection d’espèces chimiques ou biologiques. / Monitoring of environmental pollutants present at low concentrations requires creation of miniature, low-cost, and highly sensitive detectors that are capable to specifically identify target substances. In this thesis, a detection approach based on refractive index sensing with polymer micro-lasers is proposed and its application to the detection of heavy metal pollutants in water (mercury – Hg2+, cadmium – Cd2+ and lead – Pb2+) is studied. The resonance frequencies of the microcavity are highly sensitive to the refractive indices of the resonator surrounding: the resonances shift by a small amount when the surface refractive index changes, resulting from the interaction of the mode evanescent field with the surrounding medium. This permits label-free detection by coating the resonator with a suitable recognition species. The originality of this work lies in the utilization of active microcavities, or microlasers, created of the dye-doped polymers. Active microcavities offer an enhanced signal/noise ratio as compared to the passive ones and very narrow resonance peaks even at moderate quality factors (Q &#8805- 6000). The choice of polymers as an active medium is connected with a number of advantages they offer: as opposite to semiconductors, polymers can be easily functionalized, integrated in microfluidic circuits and are cheaper in processing. Moreover, the use of porous polymer matrices may allow accumulation of analyte ions inside the microcavity and thus enhance the sensitivity. Two possible applications of microlasers are investigated in the thesis: refractive index variation sensing with non-functionalized cavities and heavy metal ion detection with functionalized cavities. In the first case, the sensitivity values have been obtained, comparable with the reported in literature for planar passive microresonators. In the second case, the experimental proofs of specific detection of mercury ions in liquid are presented. The ways of sensitivity improvement are discussed and verified and a foundation is layed for the creation of integrated Lab-on-Chip microfluidic biochemical detector.

No description available.

Raman scattering can accurately identify molecules by their intrinsic vibrational frequencies, but its notoriously weak scattering efficiency for gases presents a major obstacle to its practical application in gas sensing and analysis. This work explores the use of high finesse (50 000) Fabry-Pérot microcavities as a means to enhance Raman scattering from gases. A recently demonstrated laser ablation method, which carves out a micromirror template on fused silica--either on a fiber tip or bulk substrates-- was implemented, characterized, and optimized to fabricate concave micromirror templates ~10 µm diameter and radius of curvature. The fabricated templates were coated with a high-reflectivity dielectric coating by ion-beam sputtering and were assembled into microcavities ~10 µm long and with a mode volume ~100 µm3. A novel gas sensing technique that we refer to as Purcell enhanced Raman scattering (PERS) was demonstrated using the assembled microcavities. PERS works by enhancing the pump laser's intensity through resonant recirculation at one longitudinal mode, while simultaneously, at a second mode at the Stokes frequency, the Purcell effect increases the rate of spontaneous Raman scattering by a change to the intra-cavity photon density of states. PERS was shown to enhance the rate of spontaneous Raman scattering by a factor of 107 compared to the same volume of sample gas in free space scattered into the same solid angle subtended by the cavity. PERS was also shown capable of resolving several Raman bands from different isotopes of CO2 gas for application to isotopic analysis. Finally, the use of the microcavity to enhance coherent anti-Stokes Raman scattering (CARS) from CO2 gas was demonstrated.

Monitoring of environmental pollutants present at low concentrations requires creation of miniature, low-cost, and highly sensitive detectors that are capable to specifically identify target substances. In this thesis, a detection approach based on refractive index sensing with polymer micro-lasers is proposed and its application to the detection of heavy metal pollutants in water (mercury - Hg2+, cadmium - Cd2+ and lead - Pb2+) is studied. The resonance frequencies of the microcavity are highly sensitive to the refractive indices of the resonator surrounding: the resonances shift by a small amount when the surface refractive index changes, resulting from the interaction of the mode evanescent field with the surrounding medium. This permits label-free detection by coating the resonator with a suitable recognition species. The originality of this work lies in the utilization of active microcavities, or microlasers, created of the dye-doped polymers. Active microcavities offer an enhanced signal/noise ratio as compared to the passive ones and very narrow resonance peaks even at moderate quality factors (Q &#8805- 6000). The choice of polymers as an active medium is connected with a number of advantages they offer: as opposite to semiconductors, polymers can be easily functionalized, integrated in microfluidic circuits and are cheaper in processing. Moreover, the use of porous polymer matrices may allow accumulation of analyte ions inside the microcavity and thus enhance the sensitivity. Two possible applications of microlasers are investigated in the thesis: refractive index variation sensing with non-functionalized cavities and heavy metal ion detection with functionalized cavities. In the first case, the sensitivity values have been obtained, comparable with the reported in literature for planar passive microresonators. In the second case, the experimental proofs of specific detection of mercury ions in liquid are presented. The ways of sensitivity improvement are discussed and verified and a foundation is layed for the creation of integrated Lab-on-Chip microfluidic biochemical detector.

Les pérovskites hybrides organiques-inorganiques ont attiré l'attention en raison de leurs applications potentielles dans des dispositifs optiques et plus récemment dans les dispositifs photovoltaïques. L'arrangement cristallin des pérovskites forme une structure en multi-puits quantiques dans laquelle les états excitoniques présentent une grande force d'oscillateur et une énergie de liaison importante, ce qui rend la réalisation de microcavités dans le régime de couplage fort possible à la température ambiante. Etant un matériau relativement nouveau, les pérovskites ont encore beaucoup de comportements qui ne sont pas bien compris et beaucoup de travail de recherche est nécessaire. Ce manuscrit est divisé en deux parties. Dans la première partie, la dynamique des excitons sur une pérovskite particulière (C6H5-C2H4-NH3)2PbI4 (PEPI) est étudiée à température ambiante par mesure de type pompe-sonde sous faible et fort régime d'excitation. Sous forte densité d'excitation, un processus de recombinaison Auger des excitons est présent. Une relaxation intrabande ultra-rapide a été observée. La deuxième partie du manuscrit est consacrée à l'étude de la microphotoluminescence à temperature ambiante de microcavités à base de PEPI à haut facteur de qualité. Des nouvelles pérovskites avec des propriétés optimisées (propriétés optiques d'émission, rugosité de surface et photostabilité) ont également été synthétisées. / The reason for choosing this thesis comes from the fact that in the near future,I would like to gain more knowledge and experience in scientific research and especially in the study of non linear effects in optical microcavities where new opportunities are opened and high efficient light sources could be exploited.In last ten years, an increasing number of studies are dedicated on hybrid organic-inorganic materials, due to the possibility of combining the properties both of inorganic(high mobility, electrical pumping, band engineering ) and of organic materials (low cost technology, high luminescence quantum yield at room temperature).In this context , organic-inorganic perovskites having a chemical formula (R-NH3)2MX4 where M is a metal, X halogen and R an organic chains presents a natural hybrid system . When deposited by spin coating, the molecules self-organize to form a multiple quantum wells structure. Because of the strong binding energy, optical features can be seen at room temperature. Moreover, such pervoskite presents great flexibility in their optical properties such that the spectral position of the excitonic transitions can be tailored by substituting different halides X, and the photoluminescence efficiency can be tailored by changing the organic part R. This kind of perovskites has been studied both for fundamental studies and for applications in optoelectronics. In order to increase the coupling between light and matter (exciton), perovskite has been inserted in planar microcavity and strong coupling regime has been achieved at room temperature. The strong coupling of light with exciton give rise to polariton quasi-particles, which have new properties not seen in either photons or excitons. In order to go further and have better study in stimulated scattering of polaritons in these microcavities ,a better understanding of the electronic structure as well as the excitonic interactions in these quantum wells are necessary due to the lack of information on the dynamic and on the carrier interaction of these structures. In order to study the hybrid polaritons, it will be first necessary to improve the knowledge about the relaxation in the perovskite layers. So, ultrafast pump-probe experiments will be performed on hybrid microcavities, and also on perovskite layers.

Pillar-array based optical cavities have unique properties, e.g., having a large and connected low dielectric index space (normally air space), exhibiting a large band gap for transverse magnetic modes, having a large percent of electric field energy in air and standing on a substrate. These properties make them well suitable for applications such as optical sensing and terahertz quantum cascade lasers. However there has been rare research in it due to the common belief that pillar arrays have excessive leakage to the substrate. With careful design, we provided several methods to reduce such a leakage and experimentally proved a high quality factor (Q) pillar-array based cavity is practical. We also explored the usage of such a cavity for optical sensing. Numerical methods such as finite-difference time-domain and plane-wave expansion were used in the design of the cavity. Then in microwave spectrum, cavities consisting of dielectric rods were used to test the validity of the theory. Additionally, we observed that a high-Q cavity for modes above light line is feasible and it is very suitable to measure the optical absorption of materials introduce inside the mode volume. Finally in the optical domain, pillar arrays were fabricated in Si/SiO2 material system and measured. Q as high as 27,600 was shown and when applying accurate refractive indices, for every delta n = 0.01, the peak wavelength shifted as large as 3.5 nm, testifying the ultra sensitivity of the cavity to the environmental dielectric change.

Pillar-array based optical cavities have unique properties, e.g., having a large and connected low dielectric index space (normally air space), exhibiting a large band gap for transverse magnetic modes, having a large percent of electric field energy in air and standing on a substrate. These properties make them well suitable for applications such as optical sensing and terahertz quantum cascade lasers. However there has been rare research in it due to the common belief that pillar arrays have excessive leakage to the substrate. With careful design, we provided several methods to reduce such a leakage and experimentally proved a high quality factor (Q) pillar-array based cavity is practical. We also explored the usage of such a cavity for optical sensing. Numerical methods such as finite-difference time-domain and plane-wave expansion were used in the design of the cavity. Then in microwave spectrum, cavities consisting of dielectric rods were used to test the validity of the theory. Additionally, we observed that a high-Q cavity for modes above light line is feasible and it is very suitable to measure the optical absorption of materials introduce inside the mode volume. Finally in the optical domain, pillar arrays were fabricated in Si/SiO2 material system and measured. Q as high as 27,600 was shown and when applying accurate refractive indices, for every delta n = 0.01, the peak wavelength shifted as large as 3.5 nm, testifying the ultra sensitivity of the cavity to the environmental dielectric change.

The cavity quantum electrodynamics has been applied to investigate the strong coupling interaction dynamics process between the microcavity field and the atom. The high quality cavity is a key to the realization of cavity quantum electrodynamics. Photonic crystal nanocavities are with small mode volumes and large quality factors. Lights are confined within the nanocavity. They can be used for cavity QED experiments of Fabry-Perot cavity. We have provided a realization of a quantum entanglement method for quantum information processing. In this paper, we discuss the entanglement swapping in the strong coupling process between two level atoms interacting with the photonic crystal microcavities fields of coherent states. We investigate the atomic level population and the entanglement degree of the system. We have found that the atomic maximal entangled state can be transformed into the photonic crystal microcavity maximal coherent entangled state cavity field, whereas the photonic crystal microcavity maximal coherent entangled state cavity field can be transformed into the atomic maximal entangled state.

xvii, 163 p. ; ill. (some col.) A print copy of this title is available from the UO Libraries, under the call number: SCIENCE QC446.2.C85 2008 / We present experimental and theoretical studies of a hemispherical, high-solid-angle external optical micro-cavity strongly coupled to nanoscale optical centers for cavity-quantum electrodynamics (QED) strong coupling and efficient single-photon sources. Implementations of single-photon sources based on various optical centers have been reported in the last three decades. The need for efficient single-photon sources, however, is still a major challenge in the context of quantum information processing. In order to efficiently produce single photons single optical centers are coupled to a resonant high-finesse optical micro-cavity. A cavity can channel the spontaneously emitted photons into a well-defined spatial mode and in a desired direction to improve the overall efficiency, and can alter the spectral width of the emission. It can also provide an environment where dissipative mechanisms are overcome so that a pure-quantum-state emission takes place. We engineered a hemispherical optical micro-cavity that is comprised of a planar distributed Bragg reflector (DBR) mirror, and a concave dielectric mirror having a radius of curvature 60 μm. Nanoscale semiconductor optical centers (quantum dots) are placed at the cavity mode waist at the planar mirror and are located at an antinode of the cavity field to maximize the coherent interaction rate. The three-dimensional scannable optical cavity allows both spatial and spectral selection to ensure addressing single optical centers. This unique micro-cavity design will potentially enable reaching the cavity-QED strong-coupling regime and realize the deterministic production of single photons. This cavity can also be operated with a standard planar dielectric mirror replacing the semiconductor DBR mirror. Such an all-dielectric cavity may find uses in atomic cavity-QED or cold-atom studies. We formulated a theory of single-photon emission in the cavity-QED strong-coupling regime that includes pure dipole dephasing and radiative decay both through the cavity mirror and into the side directions. This allows, for the first time, full modeling of the emission quantum efficiency, and the spectrum of the single photons emitted into the useful output mode of the, cavity. / Adviser: Michael G. Raymer