Ce travail analyse la formation d'états liés par interaction coulombienne d'excitons dans un ensemble de nanotubes de carbone de chiralité (6,5) en solution. Sous l'action d'une impulsion laser de forte intensité, une grande densité d'excitons est formée dans le nanotube et conduit à la formation d'état de trion et de biexciton. Les mécanismes physiques responsables de la photogénération de ces états ont été analysés dans le cadre de cette thèse. Ces travaux sont effectués à l'aide d'une expérience pompe-sonde dans laquelle le faisceau sonde est un continuum de lumière blanche permettant ainsi l'observation simultanée des états d'exciton, de trion et de biexciton. Cela conduit à l'obtention des énergies de liaison des différentes contributions excitoniques. En outre la dynamique de ces états excitoniques a aussi pu être obtenue avec une résolution temporelle de l'ordre de la centaine de femtosecondes. / In this thesis, we have studied the excitonic bound states formation in an ensemble of chirality (6,5) carbon nanotubes in solution. Under intense laser excitation, a large density of excitons is reached in the nanotube. This leads to the formation of bound states such as trion and biexciton. The physical mecanisms responsible for the photogeneration of these states have been analysed in this thesis. We performed a pump-probe experiment using a white light continuum as the probe beam. This allows the simultaneous observation of the excitonic, trion and biexciton states which gives information about the binding energies of the bound states. Finally, we also studied the dynamics of these excitonic bound states that have been obtained with a temporal resolution close to hundred of femtoseconds.

Kvantsammanflätning har varit ett populärt ämne bland fysiker i snart 100 år då det tydligt belyser hur annorlunda kvantmekanikens värld är jämfört med den klassiska verklighet vi lever i. Med tiden har kvantsammanflätning blivit mer och mer välförstått och teknologier ämnade att utnyttja det har de senaste årtionden kommit allt närmare till industriell använding. Kvantdatorer är fortfarande i forskningsstadiet men idag excisterar det en kvantdator som kan lösa vissa problem betydligt mycket snabbare än en klassisk dator. På grund av algorithmer som Shors faktoriseringsalgoritm och Grovers sökalgoritm så riskerar dagens krypteringsprotokoll för kommunikation att bli otillräckliga. Som svar på detta har en fysikalisk icke-hackbar krypterings metodik tagits fram i form av QKD. Det baseras på att generara krypteringsnycklar från slumptal och att dessa distribueras tack vare kvantsammanflätning. För att lyckas med detta så krävs generering av sammanflätade kvanttillstånd, kvantbitar, samt singel-fotonsdetektorer. I den här masteruppsatsen har en kvantprick karaktäriserats och används för att generera sammanflätade kvantbitar i QNP-gruppens lab på KTH samt för att skicka enstaka fotoner via Stockholms fibernät till Ericsson i Kista där de detekteras av singel foton detectorer. Multifoton sannolikheten har uppmäts till 0.049 för exciton fotoner samt 0.169 för biexciton fotoner i labbet medan ett värde på 0.176 har uppmäts för exciton fotoner detekterade hos Ericsson, vilket är betydligt lägre än singel emission gränsen 0.5 (dvs foton källan sänder ut singel fotoner). Synkronisering av data är avgörande för att få QKD att fungera varpå en post process-tidssynkroniserings metod baserad på biexciton-exciton kaskad-sönderfall har implementerats i lab. / Quantum entanglement has been a popular topic amongst physicists for almost 100 years as it clearly illuminates the extreme difference between the quantum mechanical world and our classical reality. Over time, the quantum physical property of entanglement became more and more well understood and technologies utilizing entanglement are coming closer to reach industry. Quantum computers are still in the research stage but there already exists a quantum computer capable of solving tailored problems significantly faster than a classical computer. Due to algorithms like Shor’s factorization algorithm and Grover’s search algorithm the current cryptography schemes used to ensure secure communication risk rendering obsolete. A response to this was the invention of the theoretically un­hackable Quantum key Distribution (QKD) scheme, based on generating and distributing random cryptography keys by using quantum entanglement. To achieve this, the generation of entangled photons, or qubits, as well as detection of single photons is required. In this thesis a Quantum Dot (QD) is characterized and used to generate quantum entangled states in the Quantum Nano Photonics (QNP)­group lab at KTH as well as sending single photons via the metropolitan fiber network in Stockholm to Ericsson in Kista, where they are detected using single photon detectors. A multi­photon emission probability of 0.049 was measured for the exciton emission and 0.169 for the biexciton emission in the KTH lab as well as a probability of 0.176 was measured for the exciton photons sent to Kista which is significantly lower than the single emitter limit of 0.5 (i.e. the source is emitting pure single photons). Synchronization of data is of high importance in order to implement a working QKD scheme, therefore a post process temporal synchronization method based on the biexciton­exciton cascaded decay is implemented in the lab.

Cette thèse porte d'une part sur l'étude de la stabilité du biexciton dans le nanotube de carbone et, d'autre part, sur le contrôle de l'émission du nanotube par le couplage des nanotubes de carbone à des antennes plasmoniques. La technique de spectroscopie optique non-linéaire de saturation d'absorption, appliquée aux nanotubes de carbone, nous a permis d'effectuer la première observation du biexciton dans cette nanostructure. Plus précisément, deux raies d'absorptions induites sont observées et attribuées au trion et à l'exciton par des études en températures et en puissance du laser de pompe. La mise en oeuvre d'une configuration à trois faisceaux basée sur un schéma en double-pompe permet de confirmer la photo-génération du biexciton en tant qu'excitation élémentaire du nanotube de carbone. Le biexciton est observé avec une énergie de liaison de 107 ± 1 meV pour la chiralité (9,7) et présente un profil asymétrique de Fano. Une première estimation de la dynamique de recombinaisondu biexciton est donnée par description quantitative du processus de Fano. Le modèle est basé sur le formalisme de la susceptibilité non-linéaire du troisième ordre χ(3) incluant le couplage coulombien entre le biexciton et le continuum des paires électron-trou de la première singularité de Van Hove. Le facteur de Fano est évaluée à q = 5 et conduit à l'estimation du taux de recombinaison Auger du biexciton B ∈ [0.1; 1] μm·ps−1 . Le rendement radiatif du biexciton est ainsi estimé à 10−6 .Dans le but d'étudier les nanotubes en cavité plasmonique, une expérience de micro-photoluminescence et une expérience de spectroscopie en champ sombre, sont développés dans le domaine spectrale des télécommunications (1.3 μm et 1.55 μm). La caractérisation de divers types échantillons de nanotube et des antennes plasmoniques sont présentés. Des résultats préliminaires sur un échantillon de nanotubes associés dans une configuration patch à des antennes plasmoniques montrent une corrélation entre la position des antennes et les zones luminescentes, ainsi qu'un changement de l'allure des spectres de photoluminescence. Ces premiers résultats constituent une transition dans la démarche de notre projet. L'étape de calibration des expériences est en phase de finition et l'étude des propriétés physique des nanotubes en cavité plasmonique représente désormais une activité opérationnelle au sein de notre équipe. / This thesis focus on both the biexciton's stability in carbon nanotubes, and the control of the nanotube emission through its coupling to plasmonic antenna.We report the first observation of biexciton in carbon nanotubes by means of spectral holeburning nonlinear optical spectroscopy. More precisely, two induced absorption lines are detected and assigned to trion and biexciton after investigation of their temperature and pump power dependences. An additional proof of the detection of the biexciton, as an elementary excitation of carbonnanotubes, is given in a three-beam configuration based on a two-pump scheme. The biexciton of the (9,7) chirality is observed with a binding energy of 107 ± 1 meV and shows an asymetric Fano lineshape. A first estimation of the biexciton's recombinaison dynamics is given by the quantitative analysis of the nonlinear signal. Our analytic model is formulated in the framework of the chi(3) nonlinear response, including coulomb interaction between biexcitons and free electron-hole pairs lying in the first Van Hove singularity. A Fano factor of about q = 5 is determined, which drives us to the estimation of biexciton's Auger recombinaison rate B ∈ [0.1; 1] μm · ps−1 . The Biexciton's radiative yield is then estimated of the order of 10−6 .In order to study nanotubes in plasmonic cavities, we developed micro-photoluminescence and dark-field spectroscopy experiments in the optical fiber telecommunication wavelengths (1.3 μm and 1.55 μm). Caracterisation of nanotube samples and plasmonic antenna are presented. Preliminary results on nanotubes inserted in a patch antenna have shown correlation between antenna's position and the spatial distribution of luminescence. Moreover, a change in the carbon nanotube's photoluminescence profile is observed. These results appear to be a turning point in our work. The calibration of our experiment is at its end and studies of optical properties of carbon nanotubes coupled to plasmonic antenna are now on stream in our team.

<p>GaN quantum dots grown by molecular beam epitaxy are examined by micro-photoluminescence. The exciton and biexciton emission are identified successfully by power-dependence measurement. With two different samples, it can be deduced that the linewidth of the peaks is narrower in the thicker deposited layer of GaN. The size of the GaN quantum dots is responsible for the binding energy of biexciton (E^b_XX); E^b_XXdecreases with increasing size of GaN quantum dots. Under polarization studies, polar plot shows that emission is strongly linear polarized. In particular, the orientation of polarization vector is not related to any specific crystallography orientation. The polarization splitting of fine-structure is not able to resolve due to limited resolution of the system. The emission peaks can be detected up to 80 K. The curves of transition energy with respect to temperature are S-shaped. Strain effect and screening of electric field account for  blueshift of transition energy, whereas Varshni equation stands for redshifting. Both blueshifting and redshifting are compensated at temperature ranging from 4 K to 40 K.</p>

GaN quantum dots grown by molecular beam epitaxy are examined by micro-photoluminescence. The exciton and biexciton emission are identified successfully by power-dependence measurement. With two different samples, it can be deduced that the linewidth of the peaks is narrower in the thicker deposited layer of GaN. The size of the GaN quantum dots is responsible for the binding energy of biexciton (EbXX); EbXX decreases with increasing size of GaN quantum dots. Under polarization studies, polar plot shows that emission is strongly linear polarized. In particular, the orientation of polarization vector is not related to any specific crystallography orientation. The polarization splitting of fine-structure is not able to resolve due to limited resolution of the system. The emission peaks can be detected up to 80 K. The curves of transition energy with respect to temperature are S-shaped. Strain effect and screening of electric field account for  blueshift of transition energy, whereas Varshni equation stands for redshifting. Both blueshifting and redshifting are compensated at temperature ranging from 4 K to 40 K.

The construction of a high-resolution optical microscope system for micro-photoluminescence (µ-PL) spectroscopy is described, and a range of time-integrated and time-resolved experimental work on single InGaN quantum dots (QDs) is presented. Time-integrated measurements demonstrate the existence of InGaN QDs in three different samples via the presence of sharp exciton recombination lines in the µ-PL spectra. The narrowest peaks display a linewidth Γ of ~230 µeV, implying a decoherence time T2 ≥5.7 ps. Time-resolved measurements on exciton recombination lines from single self-assembled InGaN QDs reveal typical lifetimes of ~2.0 ns (which decrease with increasing temperature), while typical lifetimes for excitons in single selectively-grown micropyramidal InGaN QDs are found to be ~0.4 ns. The shorter exciton recombination lifetime in selectively-grown QDs is believed to be due to a stronger coupling of these QDs to the underlying quantum well. Temporal fluctuations (on a timescale of seconds) in the energy, intensity and FWHM of µ-PL peaks arising from the recombination of excitons in single self-assembled InGaN QDs are observed. These are attributed to transient Stark shifts induced by a fluctuating local charge distribution as carriers become trapped in defect states in the vicinity of the QDs. Time-integrated power-dependent measurements are used to demonstrate the presence of biexciton states in single self-assembled InGaN QDs. The exciton–biexciton energy splitting is found to be ~41 meV, in agreement with values predicted by theoretical calculations. Time-resolved studies of the biexciton and exciton decay curves reveal a coupling as the exciton population is refilled by biexciton decays. The biexciton lifetime is found to be ~1.4 ns, compared to an exciton lifetime of ~1.0 ns. Lateral electric fields are applied to a single self-assembled InGaN QD using aluminium electrodes lithographically defined on the sample surface. Application of fields of the order of ~0.17 MVcm-1 is found to cause both a red-shift and a reduction in the intensity of the exciton recombination peak in the µ-PL spectrum.

Beginning with the discovery of graphene, two-dimensional materials have amassed a strong interest. Like graphene, transition metal dichalcogenides (TMDs) can be coaxed into atomically thin sheets which have some impressive properties. Unlike graphene, TMDs also has a change in their electronic band structure causing an indirect band gap to a direct gap transition in its monolayer form. Additionally, these materials lose their inversion symmetry as a monolayer. These unique properties make TMDs a strong candidate for being used in optoelectronic and valleytronic devices. In order for these devices to be successful, the optical properties of TMDs must be thoroughly understood. Due to this class of material's strong Coulomb interaction, the optical properties are dominated by excitons, a quasiparticle made up of an electron-hole pair. Therefore, the success of these devices relies, in part, on understanding and manipulating excitons. One key parameter of excitons is their dephasing rate which characterizes the lifetime of the coherent superposition of two states (i.e. how the coherence decays which is caused by excitons interacting with their environment). In this work, two optical properties are investigated: (1) How the linear absorption of the TMDs A-exciton peak varies as the material increases in thickness. By looking at how the absorption varies by sample thickness, the interaction between emitters can be understood. Experimental results for the diamagnetic shift are presented which are used to determine the lateral excitonic size. Through theoretical calculations, based on the semiconductor Maxwell-Bloch equations, additional insight into the radiative coupling of the systems are obtained. (2) How the coherence prole of the exciton changes in the presence of an external magnetic eld and specic valley excitation. By varying the polarization scheme in the four wave mixing measurement, specic valley excitation can be selected, allowing for insight into the dephasing mechanisms. By applying an external magnetic eld, the energy levels of the electron and hole can be discretized and the corresponding eects on the system's coherence seen. In conjunction with time-dependent density function theory calculations and the experimental results, a deeper understanding of exciton dynamics and multi-exciton complexes was obtained. Finally, a new system is proposed in which complex spectroscopic techniques can be performed on micron sized samples as well as devices in the presence of an external magnetic eld at cryogen temperatures. This system will allow for the investigation of the optical properties of stacked monolayers (heterostructures) as well as devices.

No description available.

Cette thèse a porté principalement sur la caractérisation de nanocristaux dont la structure permet de réduire de façon drastique leur scintillement. La caractéristique essentielle de ces nanocristaux de CdSe est qu'ils sont entourés d'une coquille épitaxiée très épaisse de CdS qui les préserve d'interactions trop importantes avec l'extérieur. La réalisation d'une coquille très épaisse permet de supprimer les longues périodes d'extinction. De plus, on a pu vérifier que si le trou reste localisé dans le coeur du nanocristal, l'électron est délocalisé dans l'ensemble de la structure. Cet effet de délocalisation provoque une réduction de l'efficacité des processus Auger. À bas taux de pompage, cette propriété implique que les nanocristaux ne présentent plus d'états réellement éteints. Ce résultat, associé aux mesures des durées de vie correspondant aux périodes d'extinction et d'émission, nous a permis de calculer les taux de recombinaisons des différents processus en jeu dans un nanocristal faiblement excité, qu'il soit neutre ou ionisé. A plus fort taux de pompage, nous montrons la possibilité d'observer des cascades radiatives consécutives à des recombinaisons d'états multiexcitoniques. La dernière partie a été consacrée à des premiers résultats concernant le contrôle de l'émission de nanocristaux par leur insertion dans des cavités photoniques à miroirs de Bragg. Nous observons l'émission de photons uniques et nous démontrons l'effet de la cavité sur la durée de vie radiative des nanocristaux.

This thesis presents an exploration of the photophysics of colloidal semiconductor nanocrystals using both linear and non-linear optical measurement techniques. These optical methodologies are used to follow population dynamics in both singly and multiply excited nanocrystal systems as well as determine material properties of the ensemble. Topics covered in the thesis include, the identification and characterization of bulk-like nanocrystals, study of the fine structure states of the lowest energy exciton, single and multiexciton population dynamics, acoustic phonon modes, elasticity and surface stress properties of a colloidal ensemble in solution.Through linear spectroscopy, the properties of both quantum confined and bulk-like colloidal semiconductor nanocrystals are compared. The identification of a model system of bulk-like nanocrystals with a non-standard absorption profile serves to resolve an ambiguity in literature concerning their characterization. The remainder of the thesis is focused on the size-dependent properties of quantum confined CdSe colloidal nanocrystals. The population dynamics and material properties of these systems are studied using a nonlinear optical technique called transient grating. A third order transient grating measurement with a cross-polarized configuration, which follows the relaxation within the fine structure levels of the lowest energy exciton state, is demonstrated and used to compare systems with different crystal field splittings. Transient grating experiments performed with specific polarization sequences allow for selective observation of the dynamics amongst nearly degenerate levels at room temperature. Cross-polarized transient grating is also used to observe a quantized acoustic phonon mode in a series of nanocrystal samples. The observation of this mode allows experimental determination of the elasticity and surface stress of the nanocrystal ensemble in solution. The anisotropic origin of the acoustic phonon is discussed using a combination of theoretical analysis, modelling and experimental data. In addition, third- and fifth-order transient grating experiments are used to study exciton and multiexciton population relaxation dynamics. The work presented here spans the optical and material properties of quantum confined and `bulk' nanocrystals. This thesis attempts to illustrate the broad scope of the observed behaviour of colloidal nanocrystal systems and to contribute to a greater understanding of their physical properties.