We look at the theory of ionization of atoms and molecules in the presence of a strong laser field. The history of ionization of atoms is reviewed and the methods used to calculate the ionization rates are examined in detail. In particular the quasi-classical methods used to solve for atomic rates are examined in detail. Early work on the ionization of molecules is also examined. A new method of calculating ionization rates is developed which allows for clear, analytic descriptions of atoms and molecules in intense light fields. The results and implications of this new theory are also examined in both atoms and molecules. The results are compared against known analytic results in the case of atoms and against numerical computation for molecules. Finally, applications of the study of atoms and molecules in intense fields are examined. We show how processes such as high harmonic generation and laser induced electron diffraction occur in strong fields and give an overview of the current state of the art and likely goals for the future. The process of laser induced electron diffraction is given close examination and ways of optimizing the diffraction patterns are discussed. The use of two-color orthogonal fields is shown to greatly increase contrast and efficiency when the carrier phases are tuned correctly.

The main contributions of this thesis to the field of ultrashort pulse measurement are a new set of experimental tools to measure the spatio-temporal fields of femtosecond pulses, and a new simplified formalism to describe such fields in the presence of distortions. More specifically, we developed an experimental technique based on scanning-wavelength digital holography and frequency-resolved optical gating that allows the complete measurement of the electric field E(x,y,t) of trains of identical femtosecond pulses. A related method, wavelength-multiplexed digital holography, is also introduced. It achieves a single-shot measurement of the three-dimensional field E(x,y,t) but at a reduced resolution using a simple experimental apparatus. Both methods can be used to measure various spatio-temporal distortions that often plague femtosecond laser systems, in particular amplified ones. Finally, to unambiguously and intuitively quantify such distortions, we introduce normalized correlation coefficients so that a common language can be used to describe the severity of these effects.

Nonlinear optical microscopy (NLOM) offers many advantages when imaging intact biological samples. By using ultrafast lasers in the near infrared and two photon excitation (TPE), signal production is limited to the focal volume and provides an excellent means for rendering thin, microscopic images from within the sample. Exogenous fluorophores/lumiphores may be used as efficient contrast agents to tag specific targets and provide enhanced signal. The efficiency of the TPE process in these contrast agents is broadly assumed to vary inversely with the laser pulsewidth, τ. In this work, we investigate the TPE efficiency of transform limited broadband (~133nm, ~10fs) and narrowband (~11nm, ~170fs) pulses in the generation of twophoton luminescence from semiconductor nanocrystals or quantum dots (QD’s) both theoretically and experimentally. Compared to standard organic dyes, QD’s possess a relatively broad, uniform spectral response that enables better use of the full bandwidth from the broadband laser. Theoretical calculations including both degenerate and non-degenerate TPE indicate a rolloff from the 1/τ behavior as the pulses’ spectral bandwidth becomes broader than the absorption spectra of the QD’s. Experimentally measured enhancement in luminescence intensity while using a broadband pulse is compared with the simulated enhancement in two-photon luminescence. A combination of increased understanding of the excitation processes in NLOM and proper selection of contrast agents will help in advancing the role of broadband ultrafast lasers in NLOM.

I studied a family of closely connected topics related to the production and application of ultrashort laser pulses. I achieved broadband cascade Raman generation in crystals, producing mutually coherent frequency sidebands which can possibly be used to synthesize optical pulses as short as a fraction of a femtosecond (fs). Unlike generation using gases, there is no need for a cumbersome vacuum system when working with room temperature crystals. Our method, therefore, shows promise for a compact system. One problem for sideband generation in solids is phase matching, because the dispersion is significant. I solved this problem by using non-collinear geometry. I observed what to our knowledge is a record-large number of spectral sidebands generated in a popular Raman crystal PbWO4 covering infrared, visible, and ultraviolet spectral regions, when I applied two 50 fs laser pulses tuned close to the Raman resonance. Similar generation in diamond was also observed, which shows that the method is universal. When a third probe pulse is applied, a very interesting 2-D color array is generated in both crystals. As many as 40 anti-Stokes and 5 Stokes sidebands are generated when a pair of time-delayed linear chirped pulses are applied to the PbWO4 crystal. This shows that pulses with picosecond duration, which is on the order of the coherence decay time, is more effective for sidebands generation than Fourier transform limited fs pulses. I also studied the technique of fs coherent Raman anti-Stokes scattering (CARS) which is used as a tool for detecting dipicolinic acid, the marker molecule for bacterial spores. I observed that there is a maximum when the concentration dependence of the near-resonant CARS signal is measured. I presented a model to describe this behavior, and found an analytical solution that agrees with our experimental data. Theoretically, I explored a possible application for single-cycle pulses: laser induced nuclear fusion. I performed both classical and quantum mechanical calculations for a system of two nuclei moving under a superintense ultrashort field. From our calculation I noted that the nuclear collisions occur on a sub-attosecond time scale, and are predicted to result in an emission of zeptosecond bursts of light.

Nonlinear optical microscopy (NLOM) offers many advantages when imaging intact biological samples. By using ultrafast lasers in the near infrared and two photon excitation (TPE), signal production is limited to the focal volume and provides an excellent means for rendering thin, microscopic images from within the sample. Exogenous fluorophores/lumiphores may be used as efficient contrast agents to tag specific targets and provide enhanced signal. The efficiency of the TPE process in these contrast agents is broadly assumed to vary inversely with the laser pulsewidth, τ. In this work, we investigate the TPE efficiency of transform limited broadband (~133nm, ~10fs) and narrowband (~11nm, ~170fs) pulses in the generation of twophoton luminescence from semiconductor nanocrystals or quantum dots (QD's) both theoretically and experimentally. Compared to standard organic dyes, QD's possess a relatively broad, uniform spectral response that enables better use of the full bandwidth from the broadband laser. Theoretical calculations including both degenerate and non-degenerate TPE indicate a rolloff from the 1/τ behavior as the pulses' spectral bandwidth becomes broader than the absorption spectra of the QD's. Experimentally measured enhancement in luminescence intensity while using a broadband pulse is compared with the simulated enhancement in two-photon luminescence. A combination of increased understanding of the excitation processes in NLOM and proper selection of contrast agents will help in advancing the role of broadband ultrafast lasers in NLOM.

Electron dynamics in atoms and molecules occurs on a time-scale of attoseconds (10⁻¹⁸s). With the availability of strong field (∼ 10¹²- 10¹³ W cm⁻²) femtosecond (10⁻¹⁵s) laser pulses with electric fields that can reach and exceed the Coulomb field strength experienced by an electron in the ground state of an atom, it is now possible to generate even shorter pulses with durations on the order of attoseconds by the process of high-harmonic generation (HHG). In this dissertation, experiments to study electron dynamics on attosecond time-scales in a helium atom using attosecond pulses generated by HHG will be described. We use extreme-ultraviolet (XUV) attosecond pulse trains and strong femtosecond near-infrared (IR) laser pulses to excite and ionize helium atoms. We first discuss an experimental technique that allows us to quantify and reduce the detrimental effects of Gouy phase slip on attosecond XUV-IR experiments. We then discuss our experiments to study the dynamic behavior of electronic states in a strong field modified helium atom where we use attosecond pulses to explore the strong-field modified atomic landscape. Using the Floquet theory to interpret our experimental observations we measure the variation in quantum phase of interferences between different fourier components of Floquet states as the IR intensity is varied and as different ionization channels dominate, in real-time. Next, we briefly discuss quantum interferences between photo-electrons ionized from XUV excited states in helium using an IR field which is polarized orthogonal to the XUV polarization. We observe variation in angular distribution of photo-electrons as a function of XUV-IR time-delay. We then discuss a new technique to measure the time-of-birth of attosecond pulses using XUV+IR photo-ionization in helium as a measurement probe. Finally, experiments to study the evolution of XUV excited wave-packets in helium on a time-scale of 100's of femtoseconds with attosecond resolution will be described.

The debate over the origin of the ultrafast demagnetization has been intensively active for the past 16 years. Several microscopic mechanisms have been proposed but none has managed so far to provide direct and incontrovertible evidences of their validity. In this context I have proposed an approach based on spin dependent electron superdiffusion as the driver of the ultrafast demagnetization. Excited electrons and holes in the ferromagnetic metal start diffusing after the absorption of the laser photons. Being the material ferromagnetic, the majority and minority spin channels occupy very different bands. It is then not surprising that transport properties are strongly spin dependent. In most of the ferromagnetic metals, majority spin excited electrons have better transport properties than minority ones. The effect is that majority carriers are more efficient in leaving the area irradiated by the laser, triggering a net spin transport. Recent experimental findings are revolutionising the field by being incompatible with previously proposed models and showing uncontrovertibly the sign of spin superdiffusion. We have shown that spin diffusing away from a layer undergoing ultrafast demagnetization can be used to create an ultrafast increase of magnetization in a neighboring magnetic layer. We have also shown that optical excitation is not a prerequisite for the ultrafast demagnetization and that excited electrons superdiffusing from a non-magnetic substrate can trigger the demagnetization. Finally we have shown that it is possible to control the time shape of the spin currents created and developed a technique to detect directly spin currents in a contact-less way.  The impact of these new discoveries goes beyond the solution of the mystery of ultrafast demagnetization. It shows how spin information can be, not only manipulated, as shown 16 years ago, but most importantly transferred at unprecedented speeds. This new discovery lays the basis for a full femtosecond spintronics.

Femtosecond time scale allows us to follow and control atomic and molecular motion. The atomic vibrations happen in the range of femtosecond scale. Thus, femtosecond technology effectively measures the atomic vibration. However, to determine electron motion, one needs to reach sub-femtosecond time scale that is in attosecond time scale. High Harmonic Generation (HHG) is a non-linear process that converts infrared light to shortest wavelength, such as in the XUV regime. HHG allows to explore electronic motion and to control electron dynamics. HHG easily reaches to XUV region and is enabling attosecond pulse generation. In this thesis we focused to generate attosecond pulses by using noble gases and their mixtures. We used only argon gas, only hydrogen molecule and their mixture with neon gas. We wanted to improve the conversion efficiency (10^-6) of the fundamental light into high harmonics. We use Ne and H2 gas mixture to look enhancement of the HHs.

We look at the theory of ionization of atoms and molecules in the presence of a strong laser field. The history of ionization of atoms is reviewed and the methods used to calculate the ionization rates are examined in detail. In particular the quasi-classical methods used to solve for atomic rates are examined in detail. Early work on the ionization of molecules is also examined. A new method of calculating ionization rates is developed which allows for clear, analytic descriptions of atoms and molecules in intense light fields. The results and implications of this new theory are also examined in both atoms and molecules. The results are compared against known analytic results in the case of atoms and against numerical computation for molecules. Finally, applications of the study of atoms and molecules in intense fields are examined. We show how processes such as high harmonic generation and laser induced electron diffraction occur in strong fields and give an overview of the current state of the art and likely goals for the future. The process of laser induced electron diffraction is given close examination and ways of optimizing the diffraction patterns are discussed. The use of two-color orthogonal fields is shown to greatly increase contrast and efficiency when the carrier phases are tuned correctly.

Thesis (PH. D.)--Michigan State University. Chemistry, 2008. / Title from PDF t.p. (viewed on Sept. 8, 2009) Includes bibliographical references (p. 134-148). Also issued in print.