Die Erzeugung immer kürzerer und energiereicherer Laserimpulse ist eine der wichtigsten Aufgaben der Laserphysik, um physikalische Phänomene in bisher unerreichten elektrischen Feldstärkebereichen zugängig zu machen und Beobachtungen auf kleinster Zeitskala zu ermöglichen. Mit Hilfe der Nachkompression verstärkter, in edelgasgefüllten Hohlfasern selbstphasenmodulierter Ti:Saphir-Laserimpulse werden die momentan kürzesten Impulse des sichtbaren Spektralbereiches erzeugt, die nur noch wenige Schwingungszyklen des elektrischen Feldes umfassen. Ebenso notwendig wie ein solcher Schritt der Impulskompression ist der verlässliche Nachweis seines Ergebnisses. Allerdings wächst auch die physikalische und technische Herausforderung einer präzisen und vollständigen Messung des ultrakurzen Laserimpulses mit zunehmender Komplexität und Breite des Impulsspektrums. Die vorliegende Arbeit stellt sowohl auf dem Gebiet der Kompression von Sub-10-fs Impulsen als auch auf dem der vollständigen Charakterisierung solcher Impulse optimierte aber auch neue Verfahrenstechniken vor. In Experimenten an einem zweistufigen Hohlfaserkompressor wird die Erzeugung der momentan kürzesten, nicht adaptiv komprimierten Impulse mit einer Dauer von lediglich 3,8 fs demonstriert. Eine elegante Alternative zu bisherigen Kompressionsmethoden zeigt der Nachweis effektiver Selbstkompression von mJ-Impulsen auf unter 8 fs in einem selbstführenden Edelgasfilament auf. Zur Kontrolle erfolgreicher Impulskompression und für eine phasenempfindliche Untersuchung des Prozesses der Dispersionskompensation über spektrale Bandbreiten von bis zu einer Oktave mussten etablierte Impulsmesstechniken wie das SPIDER- (Spectral Phase Interferometry for Direct Electric-field Reconstruction) und das FROG- (Frequency-Resolved Optical Gating) Verfahren weiterentwickelt werden. So wird mit der Realisierung und vollständigen Analyse interferometrischer FROG-Messungen ein neues phasenempfindliches Impulsmessverfahren vorgestellt. / One challenge of today’s laser physics is the stable compression of more and more intense laser pulses to the shortest possible pulse duration to enable new high-field laser experiments and to investigate fast atomic or molecular dynamics. At present, the shortest laser pulses of the visible spectral region envelop only a few cycles of the electric field. The state of the art method to generate such short pulses behind a Ti:sapphire amplifier laser system is by means of successive steps of spectral broadening inside a gas-filled hollow fibre and dispersion compensation. However, a reliable pulse characterization is as important as the pulse compression. The more spectral bandwidth the pulse covers the more technically challenging is the measurement of the pulse’s electric field structure. In this work, new concepts of compression and characterization of pulses down to durations below 10 fs are demonstrated as well as further optimization of established techniques. Due to modern, chirped-mirror based dispersion compensation pulses as short as 3.8 fs were generated with a two-stage hollow fibre compressor. At present, these are the shortest pulses of the visible spectral region, compressed without adaptive means for dispersion compensation. For the first time the effect of self-compression of mJ-pulses to below 8 fs in a self-guiding noble gas filament is demonstrated experimentally and determined by numerical simulations. Advanced pulse characterization schemes were needed for a phase-sensitive investigation of dispersion compensation and pulse compression of white light pulses. An optimized design of the SPIDER (Spectral Phase Interferometry for Direct Electric-field Reconstruction) technique is demonstrated that facilitates the measurement of the pulse’s spectral phase in case of broadband structured spectra. With the implementation of an interferometric FROG (Frequency-Resolved Optical Gating) a new phase-sensitive pulse characterization method is introduced.

In the field of second harmonic (SH) generation most studies have been concerned with maximizing conversion efficiencies, generally achievable at the phase matching (PM) condition. Outside of the PM the conversion efficiency drastically decreases. This has caused that the possible working conditions out of PM to remain largely unexplored. In this thesis work we initiated a systematic study of the SH behavior in under conditions of large phase mismatch. When a pump pulse crosses an interface between a linear and a nonlinear medium there are always two generated SH components. These components may be understood on the basis of the mathematical solution of the inhomogeneous wave equations at the SH frequency. The homogeneous (HOM) solution is a component with wave-vector k(2¿) as expected from the dispersion relation and exchanges energy with the pump until the inevitable walk-off. The inhomogeneous (INH) solution is a component with a wave-vector 2k(¿), twice the pump wave-vector, and travels locked to the pump pulse. We divide our work in two parts, one for each generated component. Inhomogeneous component. We start a systematic study of the behavior of the generated INH component, phase locked to the pump. The consequences of phase locking (PL) can guide us towards new scenarios by allowing working conditions hitherto assumed inaccessible for absorbing materials. We show that while the HOM component travels with the group velocity given by material dispersion, the IHN component is captured by the pump pulse and experiences the same effective dispersion of the pump. It does not follow the PM condition. It naturally follows that the suppression of absorption at the SH wavelengths will occur if the pump is tuned to a region of transparency. We extended the same theory for the generated third harmonic (TH). We then studied the surprising behavior of SH and TH INH components with frequencies above the absorption edge when the material is placed inside a cavity resonant only at the fundamental frequency. We have shown that the PL mechanism not only inhibits absorption but also fosters the enhancement of harmonic generation by several orders of magnitude compared to the no-cavity case. Finally, we tested the INH SH and TH behaviors in metallic frequency regime of material. Homogeneous component. The techniques used to PM the nonlinear interaction enable efficient nonlinear interactions but drastically limit the spectral bandwidth of the nonlinear optical process, making the designed frequency converter only suitable for a fixed input wavelength and single interaction only. It has been shown that the use of disordered nonlinear media relaxes the PM condition thus allowing one to achieve relatively efficient broad bandwidth regime of the frequency conversion. An example of a quadratic nonlinear medium with a disordered domain structure is an un-poled Strontium Barium Niobate (SBN) crystal. It is composed of a system of random size anti parallel ferroelectric domains that allow to phase-match any second-order parametric process over a broad range of wavelengths without any poling. We have initiated an experimental and theoretical investigation of the properties of the SH waves generated in SBN crystals, with an extension to the generated TH. This study covers the coherence and polarization properties of the generated signal, as well as its spatial distribution. In addition, we have made an experimental study of the noncollinear interaction of short optical pulses in a SBN crystal by using two fundamental waves intersecting inside the crystal. We have shown that this effect may be employed as a simple tool for monitoring both the pulse duration and initial chirp. This method offers a simple and economic alternative to the existing methods for pulse characterization.

Die Methode „interferometric frequency-resolved optical gating“ (iFROG) zur Charakterisierung ultrakurzer Laserimpulse wurde erweitert. Als optische Nichtlinearität werden sowohl die Erzeugung der 2. als auch der 3. Harmonischen (THG) separat verwendet. Eine iFROG-Messung stellt ein inverses Problem dar, bei dem die Amplitude und Phase des elektrischen Feldes des Laserimpulses nur durch einen iterativen Algorithmus rekonstruiert werden kann. In dieser Arbeit wird ein mathematischer Formalismus entwickelt und mit einem evolutionären Optimierungsalgorithmus kombiniert, um einen neuartigen Impuls-Rekonstruktions-Algorithmus für iFROG zu erschaffen. Während iFROG ursprünglich ausschließlich zur Charakterisierung von Laserimpulsen konzipiert wurde, kann die Technik gleichermaßen für spektroskopische Zwecke eingesetzt werden. Wird das nichtlineare Medium in iFROG durch ein Untersuchungsobjekt ersetzt und ein bekannter Laserimpuls erneut charakterisiert, so kann die Antwortfunktion des Untersuchungsobjekts mit einer sub-Femtosekunden-Auflösung entschlüsselt werden. Da für die THG-Variante bisher keine Lösung bekannt ist, ermöglicht der vorgestellte Rekonstruktion-Algorithmus die erstmalige Nutzung von iFROG zur Untersuchung ultraschneller nichtlinearer Effekte dritter Ordnung. Die spektroskopische Fähigkeit von iFROG wird durch das Studium von drei unterschiedlichen physikalischen Systemen (Nanostrukturen) geprüft. In ZnO-Nanostäben wird die Leistungsabhängigkeit der durch Multiphotonenabsorption induzierten Lumineszenz gemessen, wobei nachgewiesen werden konnte, dass diese mit einer Lokalisierung des optischen Nahfelds verknüpft ist. Eine Dreiphotonenresonanz in einem dünnen Titandioxid Film und eine Oberflächenplasmonenresonanz in Au-Nanoantennen führen beide zu einer endlichen Lebensdauer der induzierten Materialpolarisation. Die iFROG-Methode wird verwendet, um die ultraschnelle zeitliche Dynamik dieser Systeme auf der Nanometer- und wenige Femtosekunden-Skala zu messen. / The ultrashort laser pulse characterization method “interferometric frequency-resolved optical gating” (iFROG) is extended. Both second- and third harmonic generation (SHG and THG) are separately employed as the optical nonlinearity. An iFROG measurement represents an inverse problem, where the electric field amplitude and phase of the underlying laser pulse can only be reconstructed by an iterative algorithm. In this work, a mathematical formalism for both the SHG and THG variants of iFROG is developed and combined with an evolutionary optimization algorithm to create a novel pulse retrieval algorithm for iFROG. While iFROG was originally conceived solely for pulse characterization, the technique can equally well be applied for spectroscopic purposes. By replacing the nonlinear medium in iFROG with an object of study, say a nanostructure, and characterizing a known pulse again such that the sample affects the harmonic generation process, the response of the object can be deciphered with sub-femtosecond precision. As no previous solution for the THG variant exists, the presented retrieval algorithm allows iFROG to be exploited in the study of ultrafast third-order nonlinear effects for the first time. The spectroscopic capability of iFROG is put to test by studying three differing physical systems, each consisting of nanostructures resting on dielectric substrates. Subjecting these specimen to few-cycle near-infrared pulses, a rich variety of nonlinear optical phenomena is observed. In ZnO nanorods, the power dependence of multiphoton-absorption induced luminescence is measured and found to be connected to a localization of the optical near-field. A three-photon resonance in a thin film of titania and a localized surface plasmon resonance in Au nanoantennas both lead to a finite lifetime of the induced material polarization. The THG-iFROG method is harnessed to measure the ultrafast temporal dynamics of these systems at the nanometer and few-femtosecond scales.

Se describe la aplicación de pulsos láser ultracortos (≤10fs) en espectroscopía y microscopía de dos fotones llevada a cabo en nuestro grupo de investigación, subrayando las ventajas y requerimientos de este enfoque. Además se presenta una breve descripción de la manipulación de pulsos, de las distorsiones de fase experimentadas por los pulsos láser de femtosegundo y de cómo corregir tales distorsiones utilizando manipuladores de pulsos. / Femtosecond laser pulses in two-photon spectroscopy and microscopy: The application of shaped ultrashort laser pulses (≤10fs) in two-photon spectroscopy and microscopy carried out in our group is  described, highlighting the advantages and requirements of this approach. In addition, a brief description of pulse shaping, phase distortions experienced by femtosecond laser  pulses and how to correct these distortions using a pulse shaper is also presented.

Abstract Although gain-switching is a simple, well-established technique for obtaining ultrashort optical pulses generated with laser diodes, the optical energy in a pulse achievable from commercial structures using this technique is no more than moderate and the ‘spiking’ behaviour seen at turn-on is likely to evolve into trailing oscillations. This thesis investigates, develops and improves laser diodes in order to offer experimentally verified solutions for maximizing the optical energy so as to achieve a peak power of several watts in a single optical pulse of picosecond-range duration in the gain-switching operation regime, and for suppressing the energy located in any trailing pulses to a negligible level relative to the total optical pulse energy. This was addressed by means of either (i) an ultrashort pump current pulse with an amplitude range ~(1–10) A or (ii) custom laser diode structures, both options being capable of operating uncooled at room temperature (23±3°C). For the first solution a unique superfast gallium arsenide (GaAs) avalanche transistor was utilized as a switch in order to achieve an injection current pulse with a duration of < 1 ns, which is short enough to generate only a first optical ‘spike’ when pumping a commercial laser diode. The most promising structure with regard to the second solution was an edge-emitting semiconductor laser having a strongly asymmetric broadened double heterostructure with a relatively thick active layer. Laser pulses with full width at half maximum (FWHM) of ~100 ps and an optical energy of >3 nJ but with some trailing oscillations were achieved in experiments employing injection current pulses in the nanosecond range with an amplitude of ≤17 A, generated using inexpensive silicon (Si) electronics. The performance was improved by introducing a saturable absorber (SA) into the laser cavity, which suppressed the formation of trailing oscillations, resulting in a single optical pulse. / Tiivistelmä ”Gain switching” (vahvistuskytkentä) on tunnettu tekniikka lyhyiden (<100 ps) optisten pulssien generoimiseen laserdiodeilla. Kaupallisia laserdiodirakenteita käyttäen optinen energia rajoittuu kuitenkin 10…100 pJ:n tasolle. Tällöinkin, erityisesti suurilla energiatasoilla, optisessa pulssissa ilmenee voimakkaita jälkioskillaatioita. Tässä väitöskirjassa tutkittiin ja kehitettiin kokeellisesti varmennettuja laserdiodilähetinrakenteita tavoitteena saavuttaa >1 nJ:n optisen pulssin energia ja ~100 ps:n pulssinpituus gain-switching -toimintamoodissa. Tavoitteena oli myös minimoida jälkipulssien energia. Tutkimuksen pääsisältönä on kaksi toimintaperiaatetta: Toisessa tekniikassa päähuomio kohdistuu laseridiodin virta-ajuriin, johon kehitettiin elektroniikka, joka kykenee tuottamaan nopeita virtapulsseja laajalla pulssivirta-alueella. Virtapulssin nopeuden kasvattamisen (<1 ns) osoitettiin edistävän gain switching -ilmiötä. Toisena tekniikkana tutkittiin räätälöityä laserdiodirakennetta, joka sisäisen toimintansa perusteella tuottaa dynaamisessa ohjaustilanteessa tehokkaan ja nopean laserpulssin. Kummankin periaatteen osoitettiin toimivan huonelämpötilassa (23±3°C) ilman erillistä jäähdytystä. Ensimmäisessä ratkaisussa käytettiin nopeaa gallium-arsenidi (GaAs) -avalanchetransistoria virtakytkimenä, jolla saavutettiin <1 ns FWHM injektiovirtapulssi 10 A:n virtatasolla. Tällainen virtapulssi on riittävän lyhyt virittämään ”gain switching” -ilmiön nJ-energiatasolla. Lupaavin rakenne toiseksi ratkaisuksi oli reunaemittoiva puolijohdelaseri, jossa epäsymmetrinen aaltoputki ja aktiivinen alue ovat sijoitettu normaalista laserdiodirakenteesta poiketen rinnakkain. Tällä rakenteella voitiin tuottaa ~100 ps levyisiä (FWHM) ja >3 nJ optisen kokonaisenergian omavia laserpulsseja edullisella pii-pohjaisella (Si) elektroniikalla luoduilla 1.5–2 ns:n (FWHM) ≤17 A injektiovirtapulsseilla. Suorituskykyä saatiin edelleen parannettua istuttamalla saturoiva absorbaattori (SA) laserin optiseen onteloon. Tämän osoitettiin vähentävän jälkioskillaatioiden muodostumista.

Ces travaux de thèse rapportent l’étude des instabilités non-linéaires et des évènements extrêmesse développant lors de la propagation guidée d’un champ électromagnétique au sein de fibresoptiques. Après un succinct rappel des divers processus linéaires et non-linéaires menant à lagénération de super continuum optique, nous montrons que le spectre de celui-ci peut présenterde larges fluctuations, incluant la formation d’événements extrêmes, dont les propriétés statistiqueset l’analogie avec les vagues scélérates hydrodynamiques sont abordées en détail. Nous présentonsune preuve de principe de l’application de ces fluctuations spectrales à la génération de nombres etde marches aléatoires et identifions le phénomène d’instabilité de modulation, ayant lieu lors de laphase initiale d’expansion spectrale du super continuum, comme principale contribution à la formationd’événements extrêmes. Ce mécanisme est étudié numériquement et analytiquement, en considérantune catégorie de solutions exactes de l’équation de Schrödinger non-linéaire présentant descaractéristiques de localisations singulières. Les résultats obtenus sont vérifiés expérimentalement,notamment grâce à un système de caractérisation spectrale en temps réel et à l’utilisation conjointede métriques statistiques innovantes (ex : cartographie de corrélations spectrales). L’excellent accordentre simulations et expériences a permis de valider les prédictions théoriques et d’accéder àune meilleure compréhension des dynamiques complexes inhérentes à la propagation non-linéaired’impulsions optiques. / This thesis reports the study of nonlinear instabilities and extreme events occurring during the guidedpropagation of an electromagnetic field into optical fibers. After a short overview of the various linearand nonlinear processes leading to optical supercontinuum generation, we show that its spectrumcan exhibit large fluctuations, including the formation of extreme events, whose statistical propertiesas well as hydrodynamic rogue waves analogy are studied in detail. We provide a proof of principle ofusing these spectral fluctuations for random number and random walk generation and identify modulationinstability, associated with the onset phase of supercontinuum spectral broadening, as themain phenomenon leading to extreme event formation. This mechanism is studied both numericallyand analytically, considering a class of exact solutions of nonlinear Schrödinger equation which exhibitsingular localization characteristics. The results are experimentally verified, especially througha real-time spectral characterization system along with the use of innovative statistical metrics (e.g.spectral correlation maps). The excellent agreement between simulations and experiments allowedus to validate the theoretical predictions and get further insight into the complex dynamics associatedto nonlinear optical pulse propagation.