Photoionization of H atoms in few-cycle laser pulses

Photoionization of hydrogen atoms in few-cycle laser pulses is studied numerically. The total ionization probability, the. instantaneous ionization probability; and the partial ionization probabilities in a pair of opposite directions are obtained. The partial ionization probabilities are not always equal to each other which is termed as inversion asymmetry. The variation of asymmetry degree with the CE phase, the pulse duration and the pulse intensity is studied. It is found that the pulse intensity affects the asymmetry degree in many aspects. Firstly, the asymmetry is more distinct at higher intensities than that at lower intensities when the pulse duration exceeds 4 cycles; secondly, the maximal asymmetry in lower intensities varies with the CE phase visibly while at higher intensities riot; thirdly, the partial ionization probabilities equal to each other for some special CE phases. For lower pulse intensities, the corresponding value of CE phase is always 0.5 pi and 1.5 pi, while for higher pulse intensities, the corresponding value varies with the pulse intensity. Similar phenomena were observed in a recent experiment using few-cycle radio-frequency (RF) pulses.

Propagation of an arbitrary elliptically polarized few-cycle ultrashort laser pulse in resonant two-level quantum systems

We investigate the propagation of an arbitrary elliptically polarized few-cycle ultrashort laser pulse in resonant two-level quantum systems using an iterative predictor-corrector finite-difference time-domain method. It is shown that when the initial effective area is equal to 2 pi, the effective area will remain invariant during the course of propagation, and a complete Rabi oscillation can be achieved. However, for an elliptically polarized few-cycle ultrashort laser pulse, polarization conversion can occur. Eventually, the laser pulse will evolve into two separate circularly polarized laser pulses with opposite helicities.

Duration-dependent asymmetry in photoionization of H atoms in few-cycle laser pulses

The photoionization of H atoms irradiated by few-cycle laser pulses is studied numerically. The variations of the total ionization, the partial ionizations in opposite directions, and the corresponding asymmetry with the carrier-envelope phase in several pulse durations are obtained. We find that besides a stronger modulation on the partial ionizations, the change of pulse duration leads to a shift along carrier-envelope (CE) phase in the calculated signals. The phase shift arises from the nonlinear property of ionization and relates closely to the Coulomb attraction of the parent ion to the ionized electron. Our calculations show good agreement with the experimental observation under similar conditions.

Propagation of a few-cycle laser pulse in a V-type three-level system

Propagation of a few-cycle laser pulse in a V-type three-level system (fine structure levels of rubidium) is investigated numerically. The full three-level Maxwell-Bloch equations without the rotating wave approximation and the standing slowly varying envelope approximation are solved by using a finite-difference time-domain method. It is shown that, when the usual unequal oscillator strengths are considered, self-induced transparency cannot be recovered and higher spectral components can be produced even for small-area pulses. (c) 2005 Pleiades Publishing, Inc.

Optimization of high-order harmonic by genetic algorithm for the chirp and phase of few-cycle pulses

The brightness of a particular harmonic order is optimized for the chirp and initial phase of the laser pulse by genetic algorithm. The influences of the chirp and initial phase of the excitation pulse on the harmonic spectra are discussed in terms of the semi-classical model including the propagation effects. The results indicate that the harmonic intensity and cutoff have strong dependence on the chirp of the laser pulse, but slightly on its initial phase. The high-order harmonics can be enhanced by the optimal laser pulse and its cutoff can be tuned by optimization of the chirp and initial phase of the laser pulse.

Accurate determination of the absolute phase and temporal-pulse phase of few-cycle laser pulses

A Fourier analysis method is used to accurately determine not only the absolute phase but also the temporal-pulse phase of an isolated few-cycle (chirped) laser pulse. This method is independent of the pulse shape and can fully characterize the light wave even though only a few samples per optical cycle are available. It paves the way for investigating the absolute phase-dependent extreme nonlinear optics, and the evolutions of the absolute phase and the temporal-pulse phase of few-cycle laser pulses.

A scaling law of photoionization in few-cycle regime

In this paper, a scaling law of photoionization of atoms irradiated by intense, few- cycle laser pulses is established. The scaling law sets a relation to the phase- dependent ionization with the kinetic energy of photoelectrons, the duration and peak intensity of short pulses, and the ionization potential of the target atoms. We find that it will be advantageous to manifest the phase- dependent photoionization by choosing the target atoms with larger ionization potential, using laser with smaller carrier- frequency, and increasing the pulse intensity. (c) 2007 Optical Society of America.

Iridium and rhodium analogues of the Shilov cycle catalyst; and the investigation and applications of the Reduction-Coupled Oxo Activation (ROA) mechanistic motif towards alkane upgrading

This dissertation will cover several disparate topics, with the overarching theme centering on the investigation of organometallic C-H activation and hydrocarbon transformation and upgrading. Chapters 2 and 3 discuss iridium and rhodium analogues of the Shilov cycle catalyst for methane to methanol oxidation, and Chapter 4 on the recently discovered ROA mechanistic motif in catalysts for various alkane partial oxidation reactions. In addition, Chapter 5 discusses the mechanism of nickel pyridine bisoxazoline Negishi catalysts for asymmetric and stereoconvergent C-C coupling, and the appendices discuss smaller projects on rhodium H/D exchange catalysts and DFT method benchmarking.

Polarization evolution of a few-cycle ultrashort laser pulse propagating in a degenerate three-level medium

The propagation of an arbitrary polarized few-cycle ultrashort laser pulse in a degenerate three-level medium is investigated by using an iterative predictor-corrector finite-difference time-domain method. It is found that the polarization evolution of the ultrashort laser pulse is dependent not only on the initial atomic coherence of the medium but also on the polarization condition of the incident laser pulse. When the initial effective area is equal to 2 pi, complete linear-to-circular and circular-to-linear polarization conversion of few-cycle ultrashort laser pulses can be achieved due to the quantum interference effects between the two different transition paths.

Quantum path control in few-optical-cycle regime

We theoretically show that selection of a single quantum path in high-order harmonics generation can be realized in a few-optical-cycle regime with two-color schemes. We also demonstrate, in theory as well, the generation of spectrally smooth and ultrabroad extreme ultraviolet supercontinuum in argon gas which can produce single similar to 79 as pulses with currently available ultrafast laser sources. Our finding can be beneficial for generating isolated sub-100 as extreme ultraviolet pulses.

Magnetic alignment of high-aspect ratio microwires into vertical arrays

Fundamental studies of magnetic alignment of highly anisotropic mesostructures can enable the clean-room-free fabrication of flexible, array-based solar and electronic devices, in which preferential orientation of nano- or microwire-type objects is desired. In this study, ensembles of 100 micron long Si microwires with ferromagnetic Ni and Co coatings are oriented vertically in the presence of magnetic fields. The degree of vertical alignment and threshold field strength depend on geometric factors, such as microwire length and ferromagnetic coating thickness, as well as interfacial interactions, which are modulated by varying solvent and substrate surface chemistry. Microwire ensembles with vertical alignment over 97% within 10 degrees of normal, as measured by X-ray diffraction, are achieved over square cm scale areas and set into flexible polymer films. A force balance model has been developed as a predictive tool for magnetic alignment, incorporating magnetic torque and empirically derived surface adhesion parameters. As supported by these calculations, microwires are shown to detach from the surface and align vertically in the presence of magnetic fields on the order of 100 gauss. Microwires aligned in this manner are set into a polydimethylsiloxane film where they retain their vertical alignment after the field has been removed and can subsequently be used as a flexible solar absorber layer. Finally, these microwires arrays can be protected for use in electrochemical cells by the conformal deposition of a graphene layer.

Generation of strong quasistatic magnetic fields in interactions of ultraintense and short laser pulses with overdense plasma targets

An analytical fluid model is proposed for the generation of strong quasistatic magnetic fields during normal incidence of a short ultraintense Gaussian laser pulse with a finite spot size on an overdense plasma. The steepening of the electron density profile in the originally homogeneous overdense plasma and the formation of electron cavitation as the electrons are pushed inward by the laser are included self-consistently. It is shown that the appearance of the cavitation plays an important role in the generation of quasistatic magnetic fields: the strong plasma inhomogeneities caused by the formation of the electron cavitation lead to the generation of a strong axial quasistatic magnetic field B-z. In the overdense regime, the generated quasistatic magnetic field increases with increasing laser intensity, while it decreases with increasing plasma density. It is also found that, in a moderately overdense plasma, highly intense laser pulses can generate magnetic fields similar to 100 MG and greater due to the transverse linear mode conversion process.

Carrier-envelope phase dependence of few-cycle ultrashort laser pulse propagation in a polar molecule medium

We theoretically investigate carrier-envelope phase dependence of few-cycle ultrashort laser pulse propagation in a polar molecule medium. Our results show that a soliton pulse can be generated during the two-photon resonant propagation of few-cycle pulse in the polar molecule medium. Moreover, the main features of the soliton pulse, such as pulse duration and intensity, depend crucially on the carrier-envelope phase of the incident pulse, which could be utilized to determine the carrier-envelope phase of a few-cycle ultrashort laser pulse from a mode-locked oscillator.