Surface plasmon-polaritons are optical surface waves formed through the interaction of photons with free electrons at the surface of metals. They offer interesting applications in a broad range of scientific fields such as physics, chemistry, biology, and material science. However, many of such applications face limitations imposed by the high propagation losses of these waves at visible and near-infrared wavelengths, which result mainly from power dissipation in the metal. In principle, the propagation losses of surface plasmon-polaritons can be compensated through optical amplification. The objective of this thesis is to provide deeper insights on the physics of surface plasmon-polariton amplification and spontaneous emission in surface plasmon-polariton amplifiers through theoretical and experimental vehicles applied (but not necessarily restricted) to a particular plasmonic mode termed long-range surface plasmon-polariton. On the theoretical side, the objective is approached by developing a realistic theoretical model to describe the small-signal amplification of surface plasmon-polaritons in planar structures incorporating dipolar gain media such as organic dye molecules, rare-earth ions, and quantum dots. This model takes into account the inhomogeneous gain distribution formed near the metal surface due to a non-uniform excitation of dipoles and due to a position-dependent excited-state dipole lifetime that results from near-field interactions between the excited dipoles and the metal. Also, a theoretical model to describe the amplified spontaneous emission of surface plasmon-polaritons supported by planar metallic structures is developed. This model takes into account the different energy decay channels into which an exited dipole located in the vicinity of the metal can relax. The validity of this model is confirmed through experimentation. On the experimental side, the objective is approached by providing a direct experimental demonstration of complete loss compensation in a plasmonic waveguide. The experiments are conducted using the long-range surface plasmon-polariton supported by a symmetric thin gold waveguide incorporating optically pumped organic dye molecules in solution as the gain medium. Also, an experimental study of spontaneous emission in a long-range surface plasmon-polariton amplifier is presented. It is shown that this amplifier benefits from a low spontaneous emission into the amplified mode, which leads to an optical amplifier with low noise characteristics. The experimental setup and techniques are explained in detail.

Two-photon absorption (2PA) has been used for a number of scientific and technological applications, exploiting the fact that the 2PA probability is directly proportional to the square of the incident light intensity (while one-photon absorption bears a linear relation to the incident light intensity). This intrinsic property of 2PA leads to 3D spatial localization, important in fields such as optical data storage, fluorescence microscopy, and 3D microfabrication. The spatial confinement that 2PA enables has been used to induce photochemical and photophysical events in increasingly smaller volumes and allowed nonlinear, 2PA-based, technologies to reach sub-diffraction limit resolutions. The primary focus of this dissertation is the development of novel, efficient 2PA, fluorene-based molecules to be used either as photoacid generators (PAGs) or fluorophores. A second aim is to develop more effective methods of synthesizing these compounds. As a third and final objective, the new molecules were used to develop a write-once-read many (WORM) optical data storage system, and stimulated emission depletion probes for bioimaging. In Chapter I, the microwave-assisted synthesis of triarylsulfonium salt photoacid generators (PAGs) from their diphenyliodonium counterparts is reported. The microwave-assisted synthesis of these novel sulfonium salts afforded reaction times 90 to 420 times faster than conventional thermal conditions, with photoacid quantum yields of new sulfonium PAGs ranging from 0.01 to 0.4. These PAGs were used to develop a fluorescence readout-based, nonlinear three-dimensional (3D) optical data storage system (Chapter II). In this system, writing was achieved by acid generation upon two-photon absorption (2PA) of a PAG (at 710 or 730 nm). Readout was then performed by interrogating two-photon absorbing dyes, after protonation, at 860 nm. Two-photon recording and readout of voxels was demonstrated in five and eight consecutive, crosstalk-free layers within a polymer matrix, generating a data storage capacity of up to 1.8 x 1013 bits/cm3. The possibility of using these PAGs in microfabrication is described in Chapter III, where two-photon induced cationic ring-opening polymerization (CROP) crosslinking of an SU8 resin is employed to produce free-standing microstructures. Chapter IV describes the investigation of one- and two-photon stimulated emission transitions by the fluorescence quenching of a sulfonyl-containing fluorene compound in solution at room temperate using a picosecond pump-probe technique. The nature of stimulated transitions under various fluorescence excitation and quenching conditions were analyzed theoretically, and good agreement with experimental data was demonstrated. Two-photon stimulated transitions S1 to S0 were shown at 1064 nm. The two-photon stimulated emission cross section of the sulfonyl fluorophore was estimated as aproximately 240 - 280 GM, making this compound a good candidate for use in two-photon stimulated emission depletion (STED) microscopy.

No description available.

No description available.

Il y a des indications que les nanocristaux de silicium (nc-Si) présentent un gain optique qui est potentiellement assez grand pour permettre l'amplification optique dans la gamme de longueurs d'ondes où une photoluminescence (PL) intense est mesurée (600- 1000 nm). Afin de fabriquer des cavités optiques, nous avons implantés des morceaux de silice fondue avec des ions de Si pour former une couche de nc-Si d'une épaisseur d'environ 1 μm. Le Si a été implanté à quatre énergies comprises entre 1 MeV et 1,9 MeV de manière à obtenir une concentration atomique de Si en excès variant entre 25% et 30%. Les pièces ont été flanquées de miroirs diélectriques composés de filtres interférentiels multicouches. Sur une plage de longueurs d'ondes d'environ 200 nm de large, un filtre réfléchit près de 100%, alors que l'autre a une réflexion moyenne d'environ 90%. Nous avons mesuré et comparé les spectres de PL de trois échantillons: le premier sans miroir, le second avec des filtres réfléchissant autour de 765 nm (entre 700 nm et 830 nm), et la troisième avec des filtres agissant autour de 875 nm (entre 810 nm et 940 nm). Lorsque les échantillons sont excités avec un laser pulsé à 390 nm, des mesures de photoluminescence résolue dans le temps (PLT) révèlent des taux de décroissance plus rapides en présence de miroirs dans le domaine de longueurs d'onde où ceux-ci agissent comparé aux échantillons sans miroirs. Aussi, l'intensité PL en fonction de la fluence d'excitation montre une augmentation plus rapide de la présence de miroirs, même si celle-ci reste sous-linéaire. Nous concluons que de l'émission stimulée pourrait être présente dans la cavité optique, mais sans dominer les autres mécanismes d'émission et de pertes. / There are indications that silicon nanocrystals (nc-Si) exhibit an optical gain that is potentially large enough to enable optical amplification in the wavelength range where intense photoluminescence (PL) is measured (600-1000 nm). We fabricated optical cavities on fused silica pieces ion-implanted with Si in order to form a nc-Si layer with a thickness of about 1 μm. Si was implanted at four energies between 1 MeV and 1.9 MeV to obtain an excess atomic concentration varying between 25% and 30%. The pieces were sandwiched between dielectric mirrors consisting of multilayer interference filters. Over a wavelength range of about 200 nm wide, one filter reflects nearly 100%, while the other one shows an average reflection of 90%. We measured and compared the PL spectra of three samples: the first one with no mirrors, the second one with filters reflecting around 765 nm (between 700 nm and 830 nm), and the third one with filters acting around 875 nm (between 810 nm and 940 nm). When exciting the samples with a pulsed laser, timeresolved PL measurements exhibited faster decay rates in the wavelength domain where the reflection of the mirrors is maximal compared to samples without mirrors. Also, PL intensity as a function of excitation flux showed a faster increase in the presence of mirrors, although the increase remained sub-linear. From this, we conclude that stimulated emission could be present in the optical cavity, but does not dominate the other emission and loss processes.

Il y a des indications que les nanocristaux de silicium (nc-Si) présentent un gain optique qui est potentiellement assez grand pour permettre l'amplification optique dans la gamme de longueurs d'ondes où une photoluminescence (PL) intense est mesurée (600- 1000 nm). Afin de fabriquer des cavités optiques, nous avons implantés des morceaux de silice fondue avec des ions de Si pour former une couche de nc-Si d'une épaisseur d'environ 1 μm. Le Si a été implanté à quatre énergies comprises entre 1 MeV et 1,9 MeV de manière à obtenir une concentration atomique de Si en excès variant entre 25% et 30%. Les pièces ont été flanquées de miroirs diélectriques composés de filtres interférentiels multicouches. Sur une plage de longueurs d'ondes d'environ 200 nm de large, un filtre réfléchit près de 100%, alors que l'autre a une réflexion moyenne d'environ 90%. Nous avons mesuré et comparé les spectres de PL de trois échantillons: le premier sans miroir, le second avec des filtres réfléchissant autour de 765 nm (entre 700 nm et 830 nm), et la troisième avec des filtres agissant autour de 875 nm (entre 810 nm et 940 nm). Lorsque les échantillons sont excités avec un laser pulsé à 390 nm, des mesures de photoluminescence résolue dans le temps (PLT) révèlent des taux de décroissance plus rapides en présence de miroirs dans le domaine de longueurs d'onde où ceux-ci agissent comparé aux échantillons sans miroirs. Aussi, l'intensité PL en fonction de la fluence d'excitation montre une augmentation plus rapide de la présence de miroirs, même si celle-ci reste sous-linéaire. Nous concluons que de l'émission stimulée pourrait être présente dans la cavité optique, mais sans dominer les autres mécanismes d'émission et de pertes. / There are indications that silicon nanocrystals (nc-Si) exhibit an optical gain that is potentially large enough to enable optical amplification in the wavelength range where intense photoluminescence (PL) is measured (600-1000 nm). We fabricated optical cavities on fused silica pieces ion-implanted with Si in order to form a nc-Si layer with a thickness of about 1 μm. Si was implanted at four energies between 1 MeV and 1.9 MeV to obtain an excess atomic concentration varying between 25% and 30%. The pieces were sandwiched between dielectric mirrors consisting of multilayer interference filters. Over a wavelength range of about 200 nm wide, one filter reflects nearly 100%, while the other one shows an average reflection of 90%. We measured and compared the PL spectra of three samples: the first one with no mirrors, the second one with filters reflecting around 765 nm (between 700 nm and 830 nm), and the third one with filters acting around 875 nm (between 810 nm and 940 nm). When exciting the samples with a pulsed laser, timeresolved PL measurements exhibited faster decay rates in the wavelength domain where the reflection of the mirrors is maximal compared to samples without mirrors. Also, PL intensity as a function of excitation flux showed a faster increase in the presence of mirrors, although the increase remained sub-linear. From this, we conclude that stimulated emission could be present in the optical cavity, but does not dominate the other emission and loss processes.

No description available.

We use spectroscopy to study infrared optoelectronic inter and intraband semiconductor carrier dynamics. The overall aim of this thesis was to study both III-V and Pb chalcogenide material systems in order to show their future potential use in infrared emitters. The effects of bandstructure engineering have been studied in the output characteristics of mid-IR III-V laser diodes to show which processes (defects, radiative, Auger and phonon) dominate and whether non-radiative processes can be suppressed. A new three-beam pump probe experiment was used to investigate interband recombination directly in passive materials. Experiments on PbSe and theory for non-parabolic near-mirror bands and non-degenerate statistics were in good agreement. Comparisons with HgCdTe showed a reduction in the Auger coefficient of 1-2 orders of magnitude in the PbSe. Using Landau confinement to model spatial confinement in quantum dots (QDs) "phonon bottlenecking" was studied. The results obtained from pump probe and cyclotron resonance saturation measurements showed a clear suppression in the cooling of carriers when Landau level separation was not resonant with LO phonon energy. When a bulk laser diode was placed in a magnetic field to produce a quasi quantum wire device the resulting enhanced differential gain and reduced Auger recombination lowered Ith by 30%. This result showed many peaks in the light output which occurred when the LO phonon energy was a multiple of the Landau level separation. This showed for the first time evidence of the phonon bottleneck in a working laser device. A new technique called time resolved optically detected cyclotron resonance, was used as a precursor to finding the earner dynamics within a spatially confined quantum dot. By moving to the case of a spatial QD using an optically detected intraband resonance it was possible to measure the energy separation interband levels and conduction and valence sublevels within the dot simultaneously. Furthermore this technique has been shown that the inhomogeneous broadening of the photoluminescence spectrum is not purely affected by just size and composition. We suggest that other processes such as state occupancy, In roughing, and exciton binding energies may account for the extra energy.

No description available.

Organinė elektronika pastaruoju metu yra viena sparčiausiai besiplėtojančių puslaidininkių prietaisų krypčių. Ši kryptis labai sparčiai vystoma dėl nuolat kuriamų naujų organinių junginių ir tobulėjančių inžinerijos galimybių. Šiuo metu organinės medžiagos naudojamos organiniuose šviestukuose (OLED), plonasluoksniuose tranzistoriuose, saulės celėse, jutikliuose ir kt. Organinės medžiagos įgalina gaminti didelio ploto bei lanksčius elektronikos prietaisus, gamybai pasitelkiant pigias gaminimo technologijas. Modernios organinės elektronikos medžiagos yra daugiafunkcinės – tai leidžia ne tik pagerinti medžiagos savybes, bet ir supaprastinti technologiją, kur viename sluoksnyje daugiafunkcinė molekulė atlieka keletą funkcijų. Tačiau molekulinės struktūros sudėtingėjimas iškelia naujas problemas susijusias su naujais sudėtingais reiškiniais daugiafunkciniame molekuliniame darinyje, tokiais kaip agregatų formavimas, vidujemolekulinė krūvio pernaša, vidujemolekulinė sąsūka ir kt. Todėl naujų daugiafunkcinių molekulinių darinių savybių optimizavimas yra aktuali nūdienos organinės elektronikos problema. Šiame darbe didžiausias dėmesys skiriamas daugiafunkcinių organinių spinduolių fotofizikinių savybių valdymui. Čia nagrinėjami daugiafunkcinių molekulinių spinduolių agregacijos nulemti reiškiniai ir jų valdymo galimybės, optimizuojant sluoksnio funkcines savybes tokias kaip plėvėdaros savybės, krūvio pernaša, emisijos našumas, sustiprintos savaiminės spinduliuotės slenkstis ir kt. / Currently, organic electronics is one of the most expanding technology of semiconductor devices. This direction is rapidly developing due to the constant synthesis of new organic compounds and sophisticated advances in device engineering. Currently, organic materials are used in organic light-emitting diodes (OLEDs), organic thin-film transistors, solar cells and sensors. Low-cost manufacturing techniques such as wet casting or inkjet printing enable organic materials use in large-area and flexible electronic devices. Modern organic electronic materials are multifunctional – this enables not only to improve the material properties, but also to simplify the device architecture. However, the complexity of the molecular structure brings new problems associated with complex phenomena of the new multifunctional molecules -such as the formation of aggregates, intramolecular charge transfer, intramolecular torsion and others. Therefore, the control of the features of new multifunctional molecules is the main problem of organic electronics today. This work focuses on the control of photophysical characteristics of multifunctional organic emitters. Here we study aggregation induced emission and quenching of multifunctional molecular emitters and the possibilities to control these phenomena by optimizing functional properties of the film such as film forming properties, charge transfer, the emission efficiency, amplified spontaneous emission threshold and others.