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The warm dense matter regime (WDM), defined by temperatures of a few electron volts and densities comparable with solids, is a complex state of matter where multi-body particle correlations and quantum effects play an important role in determining the overall structure and equation of state. The study of WDM states represents the laboratory analogue of the astrophysical environments found in the cores of planets and in the crusts of old stars, but also has practical applications for controlled thermonuclear fusion. Time resolved X-ray diffraction is used to study the temporal evolution of a sample from solid state towards WDM, either after irradiation with an intense proton/electron beam, in carbon samples, or direct laser illumination, in thin gold nanofoils. The electron-ion equilibration time is extracted through the use of the two-temperature model and in highly excited carbon shown to be longer than previously thought, this is attributed to strong ion-ion coupling screening the interaction (coupled mode theory). Calculation of the dynamic ion-ion structure factor is performed using orbital-free density functional theory (OF-DFT) and shown to compare well with Kohn-Sham DFT in both the static and dynamic cases. Experimental verification of these results is vital and measurement of the microscopic dynamics of warm dense aluminium have been successfully demonstrated through inelastic X-ray scattering. Using the self-seeded beam at the linear coherent light source (LCLS) scattering at a small momentum exchange allowed the first direct measurement of ion acoustic waves in WDM. This data provides the basis for a direct experimental test of many dense plasma theories through direct comparison with the ion-ion dynamic structure factor.

In intense laser – cluster interaction, the experimental results show a strong energetic coupling between radiation and matter. We have measured absolute x – ray yields and charge state distributions under well control conditions as a function of physical parameters governing the interaction; namely laser intensity, pulse duration, wavelength or polarization state of the laser light, the size and the species of the clusters (Ar, Kr, Xe). We have highlighted, for the first time, an intensity threshold in the x – ray production very low (~ 2.1014 W/cm2 for a pulse duration of 300 fs) which can results from an effect of the dynamical polarisation of clusters in an intense electric field. A weak dependence with the wavelength (400 nm / 800 nm) on the absolute x – ray yields has been found. Moreover, we have observed a saturation of the x – ray emission probability below a critical cluster size.

Doctor of Philosophy / Department of Physics / Igor V. Litvinyuk / The goal of this dissertation project was to study the dynamics of nuclear motion in diatomic (H[subscript]2, N[subscript]2, O[subscript]2, CO) and triatomic (CO[subscript]2) molecules initiated by the ionization and/or excitation of these molecules with near-IR few-cycle laser pulses. This dynamics includes vibrational and rotational motion on the electronic potential surfaces of the molecules and their molecular ions. The experimental techniques used included the pump-probe approach, laser Coulomb explosion imaging and the COLTRIMS technique. The results are presented in four chapters. A study of rotational and vibrational nuclear dynamics in H[subscript]2 and D[subscript]2 molecules and ions initiated by 8 fs near-IR pulses is presented in Chapter 4. Transient alignment of the neutral molecules was observed and simulated; rotational frequency components contributing to the rotational wavepacket dynamics were recovered. Chapter 5 is dedicated to revealing the contribution of excited dissociative states of D[subscript]2[superscript]+ ions to the process of fragmentation by electron recollision. It was shown that it is possible to isolate the process of resonant excitation and estimate the individual contributions of the [superscript]2sigma[subscript]u[superscript]+ and [superscript]2pi[subscript]u states. In Chapter 6 the subject of investigation is the nuclear dynamics of N[subscript]2, O[subscript]2 and CO molecules initiated by ionization of a neutral molecule by a short intense laser pulse. It was shown that the kinetic energy release of the Coulomb explosion fragments, measured as a function of the delay time between pump and probe pulses, reveals the behavior of nuclear wave packet evolution on electronic states of the molecular ions. It was shown that information on the dissociation and excitation pathways can be extracted from the experimental spectra and the relative contributions of particular electronic states can be estimated. Chapter 7 is focused on studying the fragmentation of CO[subscript]2 following the interaction of this molecule with the laser field. The most important result of this study was that it presented direct experimental evidence of charge-resonant enhanced ionization (CREI), a phenomenon well-studied for diatomic molecules and predicted theoretically for triatomic molecules. The critical internuclear distance, the relevant ionic charge state and a pair of charge-resonant states responsible for the CREI were also found.

Doctor of Philosophy / Department of Physics / Zenghu Chang / The observation and control of dynamics in atomic and molecular targets requires the use of laser pulses with duration less than the characteristic timescale of the process which is to be manipulated. For electron dynamics, this time scale is on the order of attoseconds where 1 attosecond = 10[superscript]-18 seconds. In order to generate pulses on this time scale, different gating methods have been proposed. The idea is to extract or “gate” a single pulse from an attosecond pulse train and switch off all the other pulses. While previous methods have had some success, they are very difficult to implement and so far very few labs have access to these unique light sources. The purpose of this work is to introduce a new method, called double optical gating (DOG), and to demonstrate its effectiveness at generating high contrast single isolated attosecond pulses from multi-cycle lasers. First, the method is described in detail and is investigated in the spectral domain. The resulting attosecond pulses produced are then temporally characterized through attosecond streaking. A second method of gating, called generalized double optical gating (GDOG), is also introduced. This method allows attosecond pulse generation directly from a carrier-envelope phase un-stabilized laser system for the first time. Next the methods of DOG and GDOG are implemented in attosecond applications like high flux pulses and extreme broadband spectrum generation. Finally, the attosecond pulses themselves are used in experiments. First, an attosecond/femtosecond cross correlation is used for characterization of spatial and temporal properties of femtosecond pulses. Then, an attosecond pump, femtosecond probe experiment is conducted to observe and control electron dynamics in helium for the first time.

This thesis is concerned with the development of an intermediate magnetic field "clock-qubit" in ⁴³Ca⁺ at 146G and techniques to manipulate this qubit using microwaves and lasers. While ⁴³Ca⁺ has previously been used as a qubit, its relatively complicated level structure - with a nuclear spin of 7/2 and low-lying D-states -- makes cooling it in the intermediate field an intimidating prospect. As a result, previous experiments have used small magnetic fields of a few gauss where coherence times are limited and off-resonant excitation is a significant source of experimental error. We demonstrate a simple scheme that allows ⁴³Ca⁺ to be cooled in the intermediate field without any additional experimental complexity compared with low fields. Using the clock-qubit, we achieve a coherence time of T^*<sub style='position:relative;left:-.5em;'>2</sub> = 50 (10)s - the longest demonstrated in any single qubit. We also demonstrate a combined state preparation and measurement error of 6.8(6)x 10^-4 - the lowest achieved for a hyperfine trapped ion qubit [NVG⁺13] - and single-qubit logic gates with average errors of 1.0(3) x 10^-6 - more than an order of magnitude better than the previous record [BWC⁺11]. These results represent the state-of-the-art in the field of single-qubit control. Moreover, we achieve them all in a single scalable room-temperature ion trap using experimentally robust techniques and without relying on the use of narrow-linewidth lasers, magnetic field screening or dynamical decoupling techniques. We also present work on a recent scheme [OWC⁺11] to drive two-qubit gates using microwaves. We have constructed an ion trap with integrated microwave circuitry to perform these gates. Using this trap, we have driven motional sideband transitions, demonstrating the spin-motion coupling that underlies the two-qubit gate. We present an analysis of likely sources of experimental error during a future two-qubit gate and the design and preliminary characterisation of apparatus to minimise the main error contributions. Using this apparatus, we hope to perform a two-qubit gate in the near future.

This thesis examines multiple different molecular networks adsorbed on several different substrates, namely, highly oriented pyrolytic graphite (HOPG), Au(111) and graphene. STM investigations into hydrogen-bonded structures formed by closely related tetracarboxylic acid molecules were performed. The molecule pterphenyl-3,5,3,5-tetracarboxylic acid (TPTC), which is known to form random tiling networks, was observed on a graphene on copper substrate. The network formed from deposition of TPTC from nonanoic acid was examined statistically. Aqueous solutions of TPTC were also examined on HOPG where a new structure, distinct from the random tiling, was observed. Aqueous solutions of related molecules biphenyl-3,3',5,5'-tetracarboxylic acid (BPTC) and quaterphenyl-3,3',5,5'-tetracarboxylic acid (QPTC), were also studied on HOPG. QPTC formed a similar structure to the aqueous solutions of TPTC, but BPTC formed two different phases, one of which was a kagome network. Addition of nonanoic acid to a dried network of TPTC deposited from aqueous solution resulted in solvent induced recrystallisation into a random tiling network comparable to that observed on graphene on copper, which was statistically analysed. Studies investigating the potential for covalent bonded molecular networks identified two distinct phases of the molecule 1,3,5-Tri(4-bromophenyl-benzene (TBPB)) adsorbed on Au(111). Concentration variation indicates an island based growth mechanism for these domains from solution. Dimerisation of TBPB was achieved by deposition onto heated substrates and a discussion of possible reasons for the reaction termination at dimers is provided. Attempts to repeat the TBPB experiments on graphene on copper failed due to excessive corrosion. Variations using larger molecules failed due to lack of solubility. Preliminary experiments on 10,10'-dibromo-9,9'-bianthryl (DBrBA) showed promise but were irreproducible, however micron scale dendritic structures were observed suggesting poor compatibility with the solvent. Finally, a discussion of the development of a nickel catalysis based graphene fabrication method is given and the limits of what is achievable with this method are discussed. The results from this thesis highlight the importance of solvent selection for the future understanding of molecular network fabrication. We also demonstrated the feasibility of covalently bonded networks prepared in ambient conditions.

Les sources X-UV sont l'objet d'un développement important depuis une dizaine d'années. Dans cette gamme spectrale, nous sommes maintenant capables de produire des sources cohérentes, collimatées et de forte brillance. De telles sources ont des applications dans l'imagerie médicale, la photolithographie, ou encore le diagnostic de plasmas denses... Cette thèse a été consacrée à la modélisation du laser X-UV "OFI", source X-UV étudiée au LOA (ENSTA, Palaiseau). Ce type de laser X-UV est généré suite à l'ionisation d'un gaz (Kr, Xe) par un laser infrarouge de forte puissance. Le plasma créé par cette interaction constitue la source X-UV. Le travail produit au cours de la thèse a porté sur l'amplification d'un signal X-UV injecté dans ce plasma. L'objectif était d'obtenir une analyse plus détaillée du profil spatio-temporel du signal. Un nouveau code numérique 3D a alors été élaboré. Il utilise un modèle de transfert radiatif décrit par les équations de Maxwell-Bloch. Les résultats du code ont d'une part montré que le profil temporel du signal X-UV changeait considérablement au cours de l'amplification. Notamment il peut, à forte saturation, révéler des pics d'intensité de très courte durée (<100fs). La forte saturation ne pouvant être obtenue qu'avec un plasma de plusieurs centimètres de long, ceci nous amène à considérer avec intérêt les expériences utilisant le guidage du laser infrarouge, permettant la création de tels plasmas. D'autre part, l'analyse de la structure du profil transverse du signal X-UV en sortie calculé à partir de ce même code, nous a permis de mettre en évidence que le plasma amplifi cateur agissait comme un filtre spatial sur l'impulsion X-UV injectée.

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La diffusion Thomson linéaire – qui correspond à la diffusion d'une onde - électromagnétique de faible intensité par des électrons – est un processus radiatif qui émet du rayonnement à la même fréquence que celle du rayonnement incident. Cependant, lorsque l'intensité de l'onde électromagnétique incidente devient très importante (intensité laser supérieure à 1018 W/cm2), les électrons oscillant dans l'impulsion laser atteignent des vitesses relativistes et ont un mouvement fortement non linéaire. L'onde électromagnétique qu'ils diffusent est alors constituée d'harmoniques pouvant atteindre le domaine spectral des rayons X et la distribution spatiale du rayonnement est anisotrope. La diffusion Thomson est alors dite nonlinéaire et a été proposée à plusieurs reprises comme une source de rayonnement X femtoseconde. Ce n'est qu'aujourd'hui, grâce au développement des lasers intenses, que ce processus radiatif peut être étudié dans le domaine spectral X. Le travail présenté dans cette thèse est consacré à la démonstration expérimentale et à l'étude numérique du rayonnement de diffusion Thomson nonlinéaire X-UV produit lors de l'interaction Laser-Plasma.