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Attosecond pulse generation is a powerful tool to study electron dynamics in atoms and molecules. However, application of attosecond pulses is limited by the low photon flux of attosecond sources. Theoretical models predict that the harmonic efficiency scales as [lambda][superscript]-6 in the plateau region of the HHG spectrum, where [lambda] is the wavelength of the driving laser. This indicates the possibility of generating more intense attosecond pulses using short wavelength driving lasers. The purpose of this work is to find a method to generate intense single attosecond pulses using a 400 nm driving laser. In our experiments, 400 nm femtosecond laser pulses are used to generate high harmonics. First, the dependence of the high harmonic generation yield on the ellipticity of 400 nm driving laser pulse is studied experimentally, and it is compared with that of 800 nm driving lasers. A semi-classical theory is developed to explain the ellipticity dependence where the theoretical calculations match experiment results very well. Next, 400 nm short pulses (sub-10 fs) are produced with a hollow core fiber and chirped mirrors. Finally, we propose a scheme to extract single attosecond pulses with the Generalized Double Optical Gating (GDOG) method.
Generation of reproducible attosecond (10−18s) pulses is an exciting goal: in the same way as femtosecond pulses were used to make "movies" of the atomic motion in molecules, attosecond pulses could "uncover" the motion of electrons around nuclei. In this dissertation, we have suggested new ideas that will allow improving one scheme for obtaining such ultra-short pulses: The molecular modulation technique. In a theoretical proposal called Raman Additive technique, we have suggested a method that will allow (with a proper phase stabilization of generated sidebands) to obtain reproducible waveforms of arbitrary shape. An exciting range of possibilities could open up - not only for absolute phase control or sub-cycle shape control, but also for investigation of multiphoton ionization rates as a function of the sub-cycle shape. We have elaborated on the latter subject in another theoretical project, where we have exploited the unique feature of such ultrashort laser pulses, which is synchronization with molecular motion (rotational or vibrational), in order to investigate photoionization of molecules. From experimental point of view, a different construction of driving lasers than previously employed led to establishment of larger molecular coherences at higher operating pressure than in previous experiments. This resulted in simultaneous generation of rotational and vibrational sidebands with only two fields applied. In another experimental proposal using rotational transition in deuterium we have shown that employing a hollow waveguide instead of normal Raman cell improves the efficiency of the generation process. By optimizing gas pressure and waveguide geometry to compensate the dispersion, the method can be extended to efficiently generate Raman sidebands at a much lower energy of driving fields than previously employed. At the end, a very exciting possibility for controlling the molecular motion in a Raman driven system will be shown. Based on the interference effects (EIT like) that take place inside of a molecule, selectivity of different degrees of freedom can be achieved (for example switching from rotational-vibrational motion to pure rotational).
The few-cycle femtosecond laser pulse has proved itself to be a powerful tool for controlling the electron dynamics inside atoms and molecules. By applying such few-cycle pulses as a driving field, single isolated attosecond pulses can be produced through the high-order harmonic generation process, which provide a novel tool for capturing the real time electron motion. The first part of the thesis is devoted to the state of the art few-cycle near infrared (NIR) laser pulse development, which includes absolute phase control (carrier-envelope phase stabilization), amplitude control (power stabilization), and relative phase control (pulse compression and shaping). Then the double optical gating (DOG) method for generating single attosecond pulses and the attosecond streaking experiment for characterizing such pulses are presented. Various experimental limitations in the attosecond streaking measurement are illustrated through simulation. Finally by using the single attosecond pulses generated by DOG, an attosecond transient absorption experiment is performed to study the autoionization process of argon. When the delay between a few-cycle NIR pulse and a single attosecond XUV pulse is scanned, the Fano resonance shapes of the argon autoionizing states are modified by the NIR pulse, which shows the direct observation and control of electron-electron correlation in the temporal domain.
The PUILS series delivers up-to-date reviews of progress in Ultrafast Intense Laser Science, a newly emerging interdisciplinary research field spanning atomic and molecular physics, molecular science, and optical science, which has been stimulated by the recent developments in ultrafast laser technologies. Each volume compiles peer-reviewed articles authored by researchers at the forefront of each their own subfields of UILS. Every chapter opens with an overview of the topics to be discussed, so that researchers unfamiliar to the subfield, as well as graduate students, can grasp the importance and attractions of the research topic at hand; these are followed by reports of cutting-edge discoveries. This tenth volume covers a broad range of topics from this interdisciplinary research field, focusing on electron scattering by atoms in intense laser fields, atoms and molecules in ultrashort pulsed EUV and X-ray light fields, filamentation induced by intense laser fields, and physics in super-intense laser fields.
At present, the energy of a single isolated attosecond pulse is limited to nanojoule levels. As a result, an intense femtosecond pulse has always been used in combination with a weak attosecond pulse in time-resolved experiments. To reach the goal of conducting true attosecond pump-attosecond probe experiments, a high flux laser source has been developed that can potentially deliver microjoule level isolated attosecond pulses in the 50 eV range, and a unique experimental end station has been fabricated and implemented that can provide precision control of the attosecond-attosecond pump-probe pulses. In order to scale up the attosecond flux, a unique Ti:-Sapphire laser system with a three-stage amplifier that delivers pulses with a 2 J energy at a 10 Hz repetition rate was designed and built. The broadband pulse spectrum covering from 700 nm to 900 nm was generated, supporting a pulse duration of 12 fs. The high flux high-order harmonics were generated in a gas tube filled with argon by a loosely focused geometry under a phase-matching condition. The wavefront distortions for the driving laser were corrected by a deformable mirror with a Shack-Hartmann sensor to significantly improve the extreme ultraviolet radiation conversion efficiency due to the excellent beam profile at focus. A high-damage-threshold beam splitter is demonstrated to eliminate energetic driving laser pulses from high-order harmonics. The extreme ultraviolet pulse energy is measured to be 0.3 microjoule at the exit of the argon gas target. The experimental facilities developed will lead to the generation of microjoule level isolated attosecond pulses and the demonstration of true atto pump-atto probe experiments in near future. Finally, in experiment, we show the first demonstration of carrier-envelope phase controlled filamentation in air using millijoule-level few-cycle mid-infrared laser pulses.
Extremely broad bandwidth attosecond pulses (which can support 16as pulses) have been demonstrated in our lab based on spectral measurements, however, compensation of intrinsic chirp and their characterization has been a major bottleneck. In this work, we developed an attosecond streak camera using a multi-layer Mo/Si mirror (bandwidth can support ~100as pulses) and position sensitive time-of-flight detector, and the shortest measured pulse was 107.5as using DOG, which is close to the mirror bandwidth. We also developed a PCGPA based FROG-CRAB algorithm to characterize such short pulses, however, it uses the central momentum approximation and cannot be used for ultra-broad bandwidth pulses. To facilitate the characterization of such pulses, we developed PROOF using Fourier filtering and an evolutionary algorithm. We have demonstrated the characterization of pulses with a bandwidth corresponding to ~20as using synthetic data. We also for the first time demonstrated single attosecond pulses (SAP) generated using GDOG with a narrow gate width from a multi-cycle driving laser without CE-phase lock, which opens the possibility of scaling attosecond photon flux by extending the technique to peta-watt class lasers. Further, we generated intense attosecond pulse trains (APT) from laser ablated carbon plasmas and demonstrated ~9.5 times more intense pulses as compared to those from argon gas and for the first time demonstrated a broad continuum from a carbon plasma using DOG. Additionally, we demonstrated ~100 times enhancement in APT from gases by switching to 400 nm (blue) driving pulses instead of 800 nm (red) pulses. We measured the ellipticity dependence of high harmonics from blue pulses in argon, neon and helium, and developed a simple theoretical model to numerically calculate the ellipticity dependence with good agreement with experiments. Based on the ellipticity dependence, we proposed a new scheme of blue GDOG which we predict can be employed to extract intense SAP from an APT driven by blue laser pulses. We also demonstrated compression of long blue pulses into>240 [mu]J broad-bandwidth pulses using neon filled hollow core fiber, which is the highest reported pulse energy of short blue pulses. However, compression of phase using chirp mirrors is still a technical challenge.
Abstract: We present an efficient and realizable scheme for the generation of an ultrashort single attosecond (as) pulse from H atom with a 800-nm fundamental laser field combined with a terahertz (THz) field. The high-order harmonic generation (HHG) can be obtained by solving the time-dependent Schrödinger equation accurately and efficiently with time-dependent generalized pseudo-spectral (TDGPS) method. The result shows that the plateau of high-order harmonics is extended and the broadband spectra can be produced by the combined laser pulse, which can be explained by the corresponding ionization probability. The time–frequency analysis and semi-classical three-step model are also presented to further investigate this mechanism. Besides, by the superposition of the harmonics near the cutoff region, an isolated 133-as pulse can be obtained.