Quantum mechanical motion of electrons in atoms and molecules is at the heart of many photophysical and photochemical processes. As the natural timescale of electron dynamics is in the range of femtoseconds or shorter, ultrashort pulses are required to study such phenomena. The ultrashort pulse light-matter interaction at high intensity regime can however dramatically alter the atomic and molecular structures. Our current understanding of such transient electronic modification is far from complete, especially when complicated light-induced couplings are involved. In this dissertation, we investigated how a femtosecond strong-field pulse can control or modify the evolution of atomic or molecular polarization, representing electric dipole excitation in various systems. Extreme ultraviolet (XUV) attosecond pulse trains are used to coherently prepare superposition of excited states in various atomic and molecular systems. A subsequent phase-locked infrared (IR) femtosecond pulse is applied to perturb the dipoles, and transient changes in the transmitted XUV spectra are measured. This scheme is termed as XUV attosecond transient absorption spectroscopy. In the first study, we applied this technique to study the modification of Rydberg states in dilute helium gas. We observed several transient changes to the atomic structure, including the ac Stark shift, laser-induced quantum phase, laser-induced continuum structure, and quantum path interference. When the experiments were extended to the study of a dense helium gas sample, new spectral features in the absorption spectra emerged which cannot be explained by linear optical response models. We found that these absorption features arise from the interplay between the XUV resonant pulse propagation and the IR-imposed phase shift. A unified physical model was also developed to account for various scenarios. Extending our work to argon atoms, we studied how an external infrared field can be used to impulsively control different photo-excitation pathways and the transient absorption lineshape of an otherwise isolated autoionizing state. It is found that by controlling the field polarization of the IR pulse, we can modify the transient absorption line shape from Fano-like to Lorentzian-like profiles. Unlike atoms, in our study of autoionizing states of the oxygen molecule, we observed both positive and negative optical density changes for states with different electronic symmetries. The predictions of two distinct and simplified dipole perturbation models were compared against both the experimental results and a full theoretical calculation in order to understand the origin of the sign of absorption change. We relate this symmetry-dependent sign change to the Fano parameters of static photoabsorption. The same approach was applied to study molecular nitrogen, in which we observed the decay dynamics of IR perturbed doubly-excited Rydberg states with many vibrational progressions. In addition, we also conducted experiments to investigate Rydberg state dynamics of other molecular systems such as carbon dioxide. In summary, we experimentally explored the ephemeral light-induced phenomena associated with excited states of atoms and molecules. These studies provide real-time information on ultrafast electronic processes and provide strategies for direct time-domain control of the light-matter interaction.

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We developed an extreme ultraviolet (EUV) polarimeter, which employs laser-generated high-order harmonics as the light source. This relatively high-flux directional EUV source has available wavelengths between 8 nm and 62 nm and easily rotatable linear polarization. The polarimeter will aid researchers at BYU in characterizing EUV thin films and improving their understanding of materials for use in EUV optics. This first-time workhorse application of laser high harmonics enables polarization-sensitive reflection measurements not previously available in the EUV. We have constructed a versatile positioning system that places harmonics on the microchannel plate detector with an accuracy of 0.3 mm, which allows a spectral resolution of about 180. We have demonstrated that reflectance as low as 0.2% can be measured at EUV wavelengths and that this data is repeatable to within the error of our source stability (~7% fluctuation). We have compared reflectance data with that taken from the same sample at Beamline 6.3.2 at the Advanced Light Source. This data agrees well from 5 degrees to 30 degrees and the angular locations of the interference fringes also agree.

We analyse solar extreme ultraviolet (EUV) irradiance observed by the Solar EUV Experiment (SEE) onboard the Thermosphere Ionosphere Mesosphere Energetics and Dynamics (TIMED) satellite, and solar proxies (the F10.7 index, and Mg-II index), and compare their variability with the one of the global mean Total Electron Content (GTEC). Cross-wavelet analysis confirms the joint 27 days periodicity in GTEC and solar proxies. We focus on a comparison for solar minimum (2007-2009) and maximum (2013-2015) and find significant differences in the correlation during low and high solar activity years. GTEC is delayed by approximately 1-2 days in comparison to solar proxies during both low and high solar activity at the 27 days solar rotation period. To investigate the dynamics of the delay process, Coupled Thermosphere Ionosphere Plasmasphere electrodynamics model simulations have been performed for low and high solar activity conditions. Preliminary results using cross correlation analysis show an ionospheric delay of 1 day in GTEC with respect to the F10.7 index during low and high solar activity. / Wir analysieren vom Solar Extreme Ultraviolet Experiment (SEE) an Bord des Thermosphere-Ionosphere-Mesosphere Energetics and Dynamics (TIMED) Satelliten gemessene solare EUV-Irradianzen, solare Proxies (den F10.7-Index und denMg-II-Index), und vergleichen deren Variabilität mit derjenigen des global gemittelten Gesamtelektronengehalts (GTEC). Kreuzwaveletanalysen bestätigen eine gemeinsame Variabilität im Periodenbereich der solaren Rotation (27 Tage). Wir vergleichen insbesondere den Zusammenhang während des solaren Minimums (2007- 2009) und Maximums (2013-2015), wobei signifikante Unterschiede der Korrelation zwischen solaren und ionosphärischen Parametern auftreten. Es tritt eine Verzögerung der Maxima und Minima von GTEC gegenüber denjenigen der solaren Proxies von einem Tag sowohl im solaren Minimum als auch im solaren Maximum auf.

The ionospheric response to solar extreme ultraviolet (EUV) variability during 2011–2014 is shown by simple proxies based on Solar Dynamics Observatory/Extreme Ultraviolet Variability Experiment solar EUV spectra. The daily proxies are compared with global mean total electron content (TEC) computed from global TEC maps derived from Global Navigation Satellite System dual frequency measurements. They describe about 74% of the intra-seasonal TEC variability. At time scales of the solar rotation up to about 40 days there is a time lag between EUV and TEC variability of about one day, with a tendency to increase for longer time scales.

This work explores remote sensing of planetary atmospheres and their circumstellar surroundings. The terrestrial ionosphere is a highly variable space plasma embedded in the thermosphere. Generated by solar radiation and predominantly composed of oxygen ions at high altitudes, the ionosphere is dynamically and chemically coupled to the neutral atmosphere. Variations in ionospheric plasma density impact radio astronomy and communications. Inverting observations of 83.4 nm photons resonantly scattered by singly ionized oxygen holds promise for remotely sensing the ionospheric plasma density. This hypothesis was tested by comparing 83.4 nm limb profiles recorded by the Remote Atmospheric and Ionospheric Detection System aboard the International Space Station to a forward model driven by coincident plasma densities measured independently via ground-based incoherent scatter radar. A comparison study of two separate radar overflights with different limb profile morphologies found agreement between the forward model and measured limb profiles. A new implementation of Chapman parameter retrieval via Markov chain Monte Carlo techniques quantifies the precision of the plasma densities inferred from 83.4 nm emission profiles. This first study demonstrates the utility of 83.4 nm emission for ionospheric remote sensing. Future visible and ultraviolet spectroscopy will characterize the composition of exoplanet atmospheres; therefore, the second study advances technologies for the direct imaging and spectroscopy of exoplanets. Such spectroscopy requires the development of new technologies to separate relatively dim exoplanet light from parent star light. High-contrast observations at short wavelengths require spaceborne telescopes to circumvent atmospheric aberrations. The Planet Imaging Concept Testbed Using a Rocket Experiment (PICTURE) team designed a suborbital sounding rocket payload to demonstrate visible light high-contrast imaging with a visible nulling coronagraph. Laboratory operations of the PICTURE coronagraph achieved the high-contrast imaging sensitivity necessary to test for the predicted warm circumstellar belt around Epsilon Eridani. Interferometric wavefront measurements of calibration target Beta Orionis recorded during the second test flight in November 2015 demonstrate the first active wavefront sensing with a piezoelectric mirror stage and activation of a micromachine deformable mirror in space. These two studies advance our ``close-to-home'' knowledge of atmospheres and move exoplanetary studies closer to detailed measurements of atmospheres outside our solar system.

We developed an extreme ultraviolet (EUV) polarimeter, which employs laser-generated high-order harmonics as the light source. This relatively high-flux, directional EUV source has available wavelengths between 10 nm and 47 nm with easily rotatable linear polarization. The polarimeter has allowed us to characterize the optical constants of materials that may be useful for EUV optics. The instrument has a versatile positioning system and a spectral resolution of about 180, and we have demonstrated that reflectance as low as 0.1% can be measured repeatably at EUV wavelengths. We investigate the high harmonic source used for polarimetry measurements by documenting the spatial evolution of the generating laser in a semi-infinite helium-filled gas cell under conditions suitable for harmonic generation. The laser is observed to focus, diverge, and refocus, accompanied by a flattop beam profile and extended harmonic phase matching. We numerically simulate the propagation to investigate these experimental results. We find that harmonic energy comes from the forward portion of the laser pulse, whereas the latter portion gives rise to the incidental double laser focusing. Good phase matching for the harmonics arises in large measure from a balance between the linear phase delay of the neutral atoms and the Gouy shift, which is elongated and nearly linearized when an aperture is partially closed on the beam. We compare reflectance data taken with the polarimeter instrument with expected results from well-characterized samples and find that they agree. To improve repeatability and reduce the effects of systematic measurement errors we have measured the ratio of p- to s-polarized reflectance and shown that optical constants can be extracted from this data as efficiently as from absolute reflectance measurements. These ratio measurements allow more accurate recovery of optical constants than our absolute reflectance measurements for our well-characterized samples. We use the polarimeter instrument and the ratio reflectance technique to determine the optical constants of copper, uranium, and their natural oxides from 10-47 nm. For copper, this measurement resolves previously conflicting data sets, where disagreement on optical-constant values arises from failure to keep samples from oxidizing before measurement. Uranium has been proposed as a high-reflectance material in the EUV for several years, however difficulties with oxidation have prevented its careful characterization previous to this work. We find that measured optical constants for uranium do not agree well with previously accepted theoretical calculations.

The generation of high-order harmonics opened an era of attosecond science wherein coherent light bursts are used to probe dynamic processes in matter with a time resolution short enough to resolve the motions of electrons. It enabled the development of extreme ultraviolet (XUV) and X-ray table-top sources with both temporal and spatial coherence, which provides the ability to shape the temporal and spatial structure of the XUV pulses. Scientists developed techniques to control and measure the temporal structure high harmonic emissions. These techniques exploited control of the driving laser pulse in the time domain and facilitated development of more advanced high-harmonic based XUV sources that have greatly impacted ultrafast measurements. In this thesis, I apply techniques to control and measure the spatial structure of high harmonic emissions, and discuss the underlying physics and potential applications of the interaction between spatially structured laser beams and materials. This study exploits the spatial degree of freedom in strong field interaction, which has not been given as much attention as the temporal degree of freedom. I use liquid crystal devices to shape the wave front of a fundamental laser beam to a vortex structure, then imprint this structured wave front onto XUV beams through high harmonic generation. This method provides an alternative to special XUV optics, which can manipulate the wave front of XUV radiation by all optical means. This result also reveals the conservation of orbital angular momentum in this extreme nonlinear wave mixing process. In addition to shaping the wave front, shaping the polarization of the driving beam also allows generation of circularly polarized the XUV radiation using a high harmonic source. This thesis also highlights the interplay between shaping the wave front and polarization in the high harmonic generation process. The topology of the structured beam can be maintained through this extreme nonlinear interaction due to the spin selection rules and spin-orbit conservation. Moreover, this thesis demonstrates an approach to integrate a vector beam into a broadband ultrafast light source and overcome the bandwidth limitation of mode converters. We use this approach to generate a few-cycle structured beam. In the future, this beam will be used to generate a strong ultrafast magnetic impulse in gas and solid targets by driving currents in a loop, which is a valuable tool for the future of magnetic metrology. The novel properties of structured laser beams discussed in this thesis expanded the capabilities of high harmonic based XUV sources and have opened a new field to explore this additional degree of freedom in strong field interactions.

Grazing incidence pumping (GRIP) is a scheme to produce x-ray lasers and extreme ultraviolet lithography is a means of lithographic production which requires soft x-rays with a bandwidth of 2% centred at 13,5 nm. In this work firstly a grazing incidence pumping of Ni-like Mo and Ne-like Ti x-ray laser media were simulated by using EHYBRID and a post-processor code coupled to it. The required atomic data were obtained from the Cowan code. Besides, the timing issue needed for amplification purpose in a Ti:Sapphire laser system has been described theoretically. Afterwards, in order to produce soft x-ray lasers for extreme ultraviolet lithographic applications, emission of soft x-rays in the 2% bandwidth centred at 13.5 nm emitted from Sn XII and Sn XIII ions were simulated by using the EHYBRID code for a laser operating at 1064 nm with 1 J of pulse energy and 6 ns of pulse duration. The intensity range that has been investigated is between 1-5 x 1012 W/cm2. Ion fractions of tin ions and line intensities corresponding to different electron temperatures were calculated by using the collisional radiative code NeF.

Molecules are traditionally treated quantum mechanically using the Born-Oppenheimer formalism. In this formalism, different electronic states of the molecule are treated independently. However, most photo-initiated phenomena occurring in nature are driven by the couplings between different electronic states in both isolated molecules and molecular aggregates, and therefore occur beyond the Born-Oppenheimer formalism. These couplings are relevant in reactions relating to the perception of vision in the human eye, the oxidative damage and repair of DNA, the harvesting of light in photosynthesis, and the transfer of charge across large chains of molecules. While these reaction dynamics have traditionally been studied with visible and ultraviolet spectroscopy, attosecond XUV pulses formed through the process of high harmonic generation form a perfect tool for probing coupled electronic dynamics in molecules. In this thesis, I will present our work in using ultrafast, XUV spectroscopy to study these dynamics in molecules of increasing complexity. We begin by probing the relaxation dynamics of superexcited states in diatomic O₂. These states can relax via two types of electronic couplings, either through autoionization or neutral dissociation. We find that our pump-probe scheme can disentangle the two relaxation mechanisms and independently measure their contributing lifetimes. Next, we present our work in observing a coherent electron hole wavepacket initiated by the ionization of polyatomic CO₂ near a conical intersection. The electron-nuclear couplings near the conical intersection drive the electron hole between different orbital configurations. We find that we can not only measure the lifetime of quantum coherence in the electron hole wavepacket, but also control its evolution with a strong, infrared probing field. Finally, we propose an experiment to observe the migration of an electron hole across iodobenzene on the few-femtosecond timescale. We present experimental modifications made to the high harmonic generation set-up in order to probe this ultrafast and elusive charge migration. These results demonstrate the potential of ultrafast, XUV spectroscopy in probing the inner-workings of electronic couplings occurring in nature.