Doctor of Philosophy / Department of Physics / Charles L. Cocke / The broad objective of ultrafast strong-field studies is to be able to measure and control atomic and molecular dynamics on a femtosecond timescale. This thesis work has two major themes: (1) Study of high-energy photoelectron distributions from atomic targets. (2) Electron localization control in atomic and molecular reactions using shaped laser pulses. The first section focuses on the study of photoelectron diffraction patterns of simple atomic targets to understand the target structure. We measure the full vector momentum spectra of high energy photoelectrons from atomic targets (Xe, Ar and Kr) generated by intense laser pulses. The target dependence of the angular distribution of the highest energy photoelectrons as predicted by Quantitative Rescattering Theory (QRS) is explored. More recent developments show target structure information can be retrieved from photoelectrons over a range of energies, from 4U$_p$ up to 10U$_p$, independent of the peak intensity at which the photoelectron spectra have been measured. Controlling the fragmentation pathways by manipulating the pulse shape is another major theme of ultrafast science today. In the second section we study the asymmetry of electron (and ion) emission from atoms (and molecules) by interaction with asymmetric pulses formed by the superposition of two colors (800 $\&$ 400 nm). Xe electron momentum spectra obtained as a function of the two-color phase exhibit a pronounced asymmetry. Using QRS theory we can analyze this asymmetric yield of the high energy photoelectrons to determine accurately the laser peak intensity and the absolute phase of the two-color electric field. This can be used as a standard pulse calibration method for all two-color studies. Experiments showing strong left-right asymmetry in D$^+$ ion yield from D$_2$ molecules using two-color pulses is also investigated. The asymmetry effect is found to be very ion-energy dependent.

The construction of an apparatus capable of producing Bose-Einstein condensates marks a significant milestone in every experimental cold atom laboratory. In this thesis I describe the development of a system to create a Bose-Einstein condensate of $^{87}Rb$ in a Time-Orbiting Potential trap. I review the optical and magnetic techniques required to trap and cool an atomic sample under vacuum, motivating our decision to build a double MOT system comprised of a high-pressure ($10^{-9}$ torr) chamber to gather atoms and a low-pressure ($10^{-11}$ torr) chamber to cool atoms to degeneracy. By theoretically modeling the atom number and temperature inside the magnetic trap during evaporative cooling I demonstrate a simple approach to determining a cooling path that reaches the transition temperature. By making use of the condensates produced under these non-optimized conditions I determine the heating rate of the condensate in the TOP trap to be $300$ nK/s. I further use the condensates to make a more precise measurement of the TOP trap bias field. I improve upon the conventional evaporation path used in TOP trap experiments by introducing and optimizing additional bias field compression stages in between RF evaporation ramps. I demonstrate how, by adding these additional stages, the system is capable of reaching the BEC phase transition with a final atom number of $2\times 10^{5}$. In contrast, RF evaporation after only a single bias field ramp has yielded condensates with only $30\times 10^3$ atoms.

The construction of an apparatus capable of producing Bose-Einstein condensates marks a significant milestone in every experimental cold atom laboratory. In this thesis I describe the development of a system to create a Bose-Einstein condensate of $^{87}Rb$ in a Time-Orbiting Potential trap. I review the optical and magnetic techniques required to trap and cool an atomic sample under vacuum, motivating our decision to build a double MOT system comprised of a high-pressure ($10^{-9}$ torr) chamber to gather atoms and a low-pressure ($10^{-11}$ torr) chamber to cool atoms to degeneracy. By theoretically modeling the atom number and temperature inside the magnetic trap during evaporative cooling I demonstrate a simple approach to determining a cooling path that reaches the transition temperature. By making use of the condensates produced under these non-optimized conditions I determine the heating rate of the condensate in the TOP trap to be $300$ nK/s. I further use the condensates to make a more precise measurement of the TOP trap bias field. I improve upon the conventional evaporation path used in TOP trap experiments by introducing and optimizing additional bias field compression stages in between RF evaporation ramps. I demonstrate how, by adding these additional stages, the system is capable of reaching the BEC phase transition with a final atom number of $2\times 10^{5}$. In contrast, RF evaporation after only a single bias field ramp has yielded condensates with only $30\times 10^3$ atoms.

Doctor of Philosophy / Department of Physics / Brett D. DePaola / In recent years, advance in ultra fast lasers and related optical technology has enhanced the ability to control the interaction between light and matter. In this dissertation, we try to improve our understanding of the interaction of atomic and molecular ladder systems with short optical pulses. A train of pulses produced by shaping the spectral phase of a single pulse from an ultra fast laser allows us to control the step-wise excitation in rubidium (Rb) atoms. As a diagnostic method, we use magneto-optical trap recoil ion momentum spectroscopy (MOTRIMS) to prepare cold target atoms and to observe atomic ions as a result of the interaction. We have explored the interactions of a finite number of optical short pulses in a train with a three-level Rb atom ladder system. Each pulse in the train is separated by a constant time interval with a fixed pulse-to-pulse phase change. In these experiments, two dimensional (2D) landscape maps show the interaction by measuring population in the uppermost state of the ladder system as a function of pulse-to-pulse time interval and phase shift. The observed structures in the 2D landscape are due to constructive or destructive interference in the interaction. Furthermore, different numbers of pulses in the train are applied to the atomic Rb three level ladder system in order to measure the effect on the interaction. The sharpness of the interference structure is enhanced by increasing the number of pulses. This phenomenon is analogous to increasing the sharpness in an optical multi-slit experiment by increasing the number of slits.

Master of Science / Department of Physics / Brett D. DePaola / A recent powerful spectroscopic technique that has been implemented using femtosecond lasers excites atoms or molecules through quantum interference effects. The results are oscillations in excited state populations that represent the optical frequencies used in the excitation pathway, these frequencies can be found by Fourier analysis. The technique uses a Mach-Zender interferometer wherein one femtosecond pulse is split into two pulses that are phase coherent. These pulses are the pump and probe pulses which are delayed with respect to one another by a variable time. During the delay between pulses the state excited by the first (pump) pulse evolves in time before the probe pulse is used to excite the atom into its final state. The observed final state population exhibits interference between the several possible pathways to the final state. The information gained from this method will allow for advances in other processes such as the dynamics of photo-association.

Master of Science / Department of Physics / Uwe Thumm / In this work we studied the dynamics of deuterium molecules in intense laser fields both experimentally and theoretically. For studying the dynamics of the molecule on a time scale that is less than the period of the laser field (2.7 fs for 800 nm), an advanced experimental technique: COLTRIMS (cold target recoil ion momentum spectroscopy) was used. COLTRIMS allows studying the nuclear dynamics without using attosecond laser pulses. This thesis consists of two main parts. In the first part we deduced the angular dependence of the ionization probability of the molecule without aligning the molecules, by measuring the relative angle between a deuteron resulting from field dissociation and an emitted electron using electron-ion coincidence measurements with circularly polarized light in COLTRIMS. We found out that for 50 fs pulses (1850 nm wavelength and 2 x10[superscript]14 W/cm[superscript]2 intensity), D[subscript]2 molecules are 1.15 times more likely to be ionized when the laser field is parallel to the molecular axis than when the laser field is perpendicular. This result agreed perfectly with the result from our ab initio theoretical model and also with predictions of the molecular Ammosov-Delone-Krainov (mo-ADK) theory. In the second part of this work we calculated the time evolution of an initial nuclear wave packet in D[subscript]2[superscript]+ generated by the rapid ionization of D[subscript]2 by an ultra short laser pulse. We Fourier transformed the nuclear probability density with respect to the delay between the pump and probe pulses and obtained two-dimensional internuclear-distance-dependent power spectra which serve as a tool for visualizing and analyzing the nuclear dynamics in D[subscript]2[superscript]+ in an external laser field. We attempt to model realistic laser pulses, therefore in addition to the main spike of the pulse we include the Gaussian pedestal. The optimal laser parameters for observing field-induced bond softening and bond hardening in D[subscript]2[superscript]+ can be achieved by varying the intensity, wavelength, and duration of the probe-pulse pedestal. Despite the implicit “continuum wave” (infinite pulse length) assumption the validity of the “Floquet picture” is tested for the interpretation of short-pulse laser-molecule interactions.

In this thesis, I report on experiments with cold 85Rb atoms in a far-detuned one-dimensional optical lattice. These experiments are focused on creating efficient coupling between the quantized vibrational states of atoms in the optical lattice, on controlling and maintaining coherence between the vibrational states, and on developing a spectroscopy method to characterize the decay of coherence. First, I present an experimental study of the application of simple and compound pulses consisting of time-dependent spatial translations to coupling vibrational states of ultracold 85Rb atoms in the optical lattice. Experimental results show that a square pulse consisting of lattice displacements and a delay is more efficient than single-step and Gaussian pulses. The square pulse can be seen as an example of coherent control. Numerical calculations are in strong agreement with the experimental results. In addition, it is shown numerically that the vibrational state coupling due to such lattice manipulations is more efficient in shallow lattices than in deep lattices, in which the coupling probability approaches the harmonic oscillator limit. Next, the effectiveness of these pulses in reviving oscillations of atoms in vibrational superposition states using a pulse-echo technique is examined. Experimental results show that the square and Gaussian pulses result in higher echo amplitudes than the single-step pulse. These echo amplitudes are an order of magnitude larger than the echo amplitudes observed previously for the motional states of atoms in optical lattices. With the aim of the optimized square echo pulse, echo amplitude is measured at much longer times, where a surprising coherence freeze (plateau) is observed. To investigate mechanisms responsible for the observed echo decay and the coherence freeze, we developed a new two-dimensional pump-probe spectroscopy technique to monitor the evolution of frequency-frequency correlations in the system, a necessary input for understanding the decay of coherence. Through this 2D technique, we have characterized the temporal decay of frequency memory and through our simulations we find that coherence freeze is related to the shape of this memory loss function. This technique is general in that it can be applied in a variety of quantum information candidate systems to probe the nature of their decoherence.

In this thesis, I report on experiments with cold 85Rb atoms in a far-detuned one-dimensional optical lattice. These experiments are focused on creating efficient coupling between the quantized vibrational states of atoms in the optical lattice, on controlling and maintaining coherence between the vibrational states, and on developing a spectroscopy method to characterize the decay of coherence. First, I present an experimental study of the application of simple and compound pulses consisting of time-dependent spatial translations to coupling vibrational states of ultracold 85Rb atoms in the optical lattice. Experimental results show that a square pulse consisting of lattice displacements and a delay is more efficient than single-step and Gaussian pulses. The square pulse can be seen as an example of coherent control. Numerical calculations are in strong agreement with the experimental results. In addition, it is shown numerically that the vibrational state coupling due to such lattice manipulations is more efficient in shallow lattices than in deep lattices, in which the coupling probability approaches the harmonic oscillator limit. Next, the effectiveness of these pulses in reviving oscillations of atoms in vibrational superposition states using a pulse-echo technique is examined. Experimental results show that the square and Gaussian pulses result in higher echo amplitudes than the single-step pulse. These echo amplitudes are an order of magnitude larger than the echo amplitudes observed previously for the motional states of atoms in optical lattices. With the aim of the optimized square echo pulse, echo amplitude is measured at much longer times, where a surprising coherence freeze (plateau) is observed. To investigate mechanisms responsible for the observed echo decay and the coherence freeze, we developed a new two-dimensional pump-probe spectroscopy technique to monitor the evolution of frequency-frequency correlations in the system, a necessary input for understanding the decay of coherence. Through this 2D technique, we have characterized the temporal decay of frequency memory and through our simulations we find that coherence freeze is related to the shape of this memory loss function. This technique is general in that it can be applied in a variety of quantum information candidate systems to probe the nature of their decoherence.

Doctor of Philosophy / Department of Physics / Itzhak Ben-Itzhak / Lasers are being used widely for the study and manipulation of the dynamics of atomic and molecular targets, and advances in laser technology makes it possible to explore new areas of research — for example attosecond physics. In order to probe the fragmentation dynamics of molecular ions, we have developed a coincidence three-dimensional momentum imaging method that allows the kinematically complete study of all fragments except electrons. Recent upgrades to this method allow the measurement of slow dissociation fragments, down to nearly zero velocity, in intense ultrafast laser fields. Evidences for the low energy breakup are presented using the benchmark molecules diatomic H[subscript]2[superscript]+ and polyatomic H[subscript]3[superscript]+ . The low energy fragments in H[subscript]2[superscript]+ dissociation are due to the intriguing zero-photon dissociation phenomenon. This first experimental evidence for the zero-photon dissociation is further supported by sophisticated theoretical treatment. We have explored the laser pulse length, intensity, wavelength, and chirp dependence of zero-photon dissociation of H[subscript]2[superscript]+, and the results are well described by a two-photon process based on stimulated Raman scattering. Similar studies of the slow dissociation of H[subscript]3[superscript]+ reveal that two-body dissociation is dominant over three-body dissociation. The most likely pathways leading to low-energy breakup into H[superscript]++H[subscript]2, in contradiction to the assessments of the channels in at least one previous study, are explored by varying the laser pulse duration and the wavelength. In addition, we have investigated the dissociation and single ionization of N[subscript]2[superscript]+ , and an interesting high energy feature in addition to the low energy has been observed at higher intensities. Such high energy results from the breakup of molecules in excited states are accessible at higher intensities where their potential energy is changing rapidly with the internuclear distance. We have extended the intense field ionization studies to other molecular ions N[subscript]2[superscript]+ , CO[superscript]+, NO[superscript]+, and O[subscript]2[superscript]+ . The dissociative ionization of these molecules follow a general mechanism, a stairstep ionization mechanism. Utilizing the capability of the upgraded experimental method we have measured the non-dissociative and dissociative ionization of CO[superscript]+ using different pulse lengths. The results suggest that dissociative ionization can be manipulated by suppressing some ionization paths.

Master of Science / Department of Physics / Brian Washburn / This research sought to characterize the length dependent loss of hollow core photonic crystal fibers (HC-PCF) in the mid-infrared. These fibers are used in gas-filled fiber lasers that operate in the mid-infrared range. A black body source which provided a broad mid-infrared spectrum was coupled into a HC-PCF and a fiber cut-back method was implemented to make the length dependent loss measurement. A monochromator was used to observe narrow bands of the broad spectrum provided by the black body source and the loss as a function of wavelength was constructed. The loss for four unique HC-PCF fibers was characterized across the wavelength range [lambda] =1754 nm to [lambda] =3220 nm. The best fibers demonstrated a loss of less than 2 dB/m across this range, with some fibers even exhibiting loss below 1 dB/m.