Time-resolved investigation of low-density plasma channels produced by a kilohertz femtosecond laser in air

By employing pump-probe back longitudinal diffractometry, the electron density and decay dynamics of a weak plasma channel created by a 1-KHz fs laser in air has been investigated. With ultrashort laser pulses of 50 fs and low energy of 0.6 mJ, we observe weak plasma channels with a length similar to 2 cm in air. An analytical reconstruction method of electron density has been analyzed, which is sensitive to the phase shift and channel size. The electron density in the weak plasma channel is extracted to be about 4x10(16) cm(-3). The diameters of the plasma channel and the filament are about 50 and 150 mu m, respectively, and the measurable electron density can be extended to less than 10(15) cm(-3). Moreover, a different time-frequency technique called linearly chirped longitudinal diffractometry is proposed to time-resolved investigate ultrafast ionization dynamics of laser-irradiated gas, laser interaction with cluster beam, etc.

Proton transfers at the air-water interface

Proton transfer reactions at the interface of water with hydrophobic media, such as air or lipids, are ubiquitous on our planet. These reactions orchestrate a host of vital phenomena in the environment including, for example, acidification of clouds, enzymatic catalysis, chemistries of aerosol and atmospheric gases, and bioenergetic transduction. Despite their importance, however, quantitative details underlying these interactions have remained unclear. Deeper insight into these interfacial reactions is also required in addressing challenges in green chemistry, improved water quality, self-assembly of materials, the next generation of micro-nanofluidics, adhesives, coatings, catalysts, and electrodes. This thesis describes experimental and theoretical investigation of proton transfer reactions at the air-water interface as a function of hydration gradients, electrochemical potential, and electrostatics. Since emerging insights hold at the lipid-water interface as well, this work is also expected to aid understanding of complex biological phenomena associated with proton migration across membranes.

Based on our current understanding, it is known that the physicochemical properties of the gas-phase water are drastically different from those of bulk water. For example, the gas-phase hydronium ion, H₃O⁺(g), can protonate most (non-alkane) organic species, whereas H₃O⁺(aq) can neutralize only relatively strong bases. Thus, to be able to understand and engineer water-hydrophobe interfaces, it is imperative to investigate this fluctuating region of molecular thickness wherein the ‘function’ of chemical species transitions from one phase to another via steep gradients in hydration, dielectric constant, and density. Aqueous interfaces are difficult to approach by current experimental techniques because designing experiments to specifically sample interfacial layers (< 1 nm thick) is an arduous task. While recent advances in surface-specific spectroscopies have provided valuable information regarding the structure of aqueous interfaces, but structure alone is inadequate to decipher the function. By similar analogy, theoretical predictions based on classical molecular dynamics have remained limited in their scope.

Recently, we have adapted an analytical electrospray ionization mass spectrometer (ESIMS) for probing reactions at the gas-liquid interface in real time. This technique is direct, surface-specific,and provides unambiguous mass-to-charge ratios of interfacial species. With this innovation, we have been able to investigate the following:

1. How do anions mediate proton transfers at the air-water interface?

2. What is the basis for the negative surface potential at the air-water interface?

3. What is the mechanism for catalysis ‘on-water’?

In addition to our experiments with the ESIMS, we applied quantum mechanics and molecular dynamics to simulate our experiments toward gaining insight at the molecular scale. Our results unambiguously demonstrated the role of electrostatic-reorganization of interfacial water during proton transfer events. With our experimental and theoretical results on the ‘superacidity’ of the surface of mildly acidic water, we also explored implications on atmospheric chemistry and green chemistry. Our most recent results explained the basis for the negative charge of the air-water interface and showed that the water-hydrophobe interface could serve as a site for enhanced autodissociation of water compared to the condensed phase.

Few-cycle spatiotemporal soliton wave excited by filamentation of a femtosecond laser pulse in materials with anomalous dispersion

The nonlinear dynamics of 1.6-mu m fs laser pulses propagating in fused silica is investigated by employing a full-order dispersion model. Different from the x-wave generation in normally dispersive media, a few-cycle spatiotemporally compressed soliton wave is generated with the contrary contributions of anomalous group velocity dispersion (GVD) and self-phase-modulation. However, at the tailing edge of the pulse forms a shock wave which generates separate and strong supercontinuum peaked at 670 nm. It is also the origin of conical emission formed both in time and frequency domain with the contribution of normal GVD at visible light.

Nonlinear propagation of fs laser pulses in liquids and evolution of supercontinuum generation

Nonlinear propagation of fs laser pulses in liquids and the dynamic processes of filamentation such as self-focusing, intensity clamping, and evolution of white light production have been analyzed by using one- and two-photon fluorescence. The energy losses of laser pulses caused by multiphoton absorption and conical emission have been measured respectively by z-scan technique. Numerical simulations of fs laser propagation in water have been made to explain the evolution of white light production as well as the small-scale filaments in liquids we have observed by a nonlinear fluorescence technique. (c) 2005 Optical Society of America.

Enhancement of four-wave mixing induced by interacting dark resonances

We analyse a four-wave mixing (FWM) scheme in a five-level atomic system in which double-dark resonances are present. It is found that the enhancement of FWM in both electromagnetically induced transparency (EIT) windows can be obtained even without the condition of multiphoton resonance. Moreover, the conversion efficiency of FWM in one EIT window can be much larger than that in the other due to the presence of interacting dark resonances.

A scaling law of photoionization in ultrashort pulses

By means of the numerical solution of time-dependant Schrodinger equation, we verify a scaling law of photoionization in ultrashort pulses. We find that for a given carrier-envelope phase and duration of the pulse, identical photoionizations are obtained provided that when the central frequency of the pulse is enlarged by k times, the atomic binding potential is enlarged by k times, and the laser intensity is enlarged by k(3) times. The scaling law allows us to reach a significant control over direction of photoemission and offers exciting prospects of reaching similar physical processes in different interacting systems which constitutes a novel kind of coherent control.

Asymmetry of the photoionization rate of H atoms by a sequence of one-cycle laser pulses

Using an unperturbed scattering theory, the characteristics of H atom photoionization are studied respectively by a linearly- and by a circularly- polarized one-cycle laser pulse sequence. The asymmetry for photoelectrons in two directions opposite to each other is investigated. It is found that the asymmetry degree varies with the carrier-envelope (CE) phase, laser intensity, as well as the kinetic energy of photoelectrons. For the linear polarization, the maximal ionization rate varies with the CE phase, and the asymmetry degree varies with the CE phase in a sine-like pattern. For the circular polarization, the maximal ionization rate keeps constant for various CE phases, but the variation of asymmetry degree is still in a sine-like pattern.

A scaling law of photoelectron angular distributions in one-cycle laser pulses

The photoelectron angular distributions (PADs) from above-threshold ionization of atoms irradiated by one-cycle laser pulses satisfy a scaling law. The scaling law denotes that the main features of the PADs are determined by four dimensionless parameters: (1) the ponderomotive number u(p) = U-p/hw, the ponderomotive energy U-p in units of laser photon energy; (2) the binding number E-b = E-b/h(w), the atomic binding energy E-b in units of laser photon energy; (3) the number of absorbed photons q; (4) the carrier-envelope phase phi(0), the phase of the carrier wave with respect to the envelope. We verify the scaling law by theoretical analysis and numerical calculation, compared to that in long-pulse case. A possible experimental test to verify the scaling law is suggested.

Creation of arbitrary coherent superposition states in four-level systems

Using the technique of stimulated Raman adiabatic passage, we propose schemes for creating arbi- trary coherent superposition states of atoms in four-level systems: a A-type system with twofold final states and a four-level ladder system. With the use of a control field, arbitrary coherent superposition states are created without the condition of multiphoton resonance. Suitable manipulation of detunings and the control field can create either a single state or any superposition states desired. (c) 2005 Pleiades Publishing, Inc.

周期量级超短激光脉冲作用下导带电子的光吸收与碰撞电离

激光照射下光学材料的损伤过程中，导带电子的加热和碰撞电离是非常重要的过程，影响着导带电子的产生、晶格能量的沉积和破坏．分析了Drude模型的局限性，从经典力学出发求解了周期量级激光场中导带电子的运动方程，计算了导带电子的光吸收和碰撞电离，分析了激光强度、载波相位等对碰撞电离的影响．

飞秒强激光场中大尺寸氩团簇爆炸机理的实验研究

By using time-of-flight spectroscopy, the ionization and explosion of large argon clusters ( (n) over bar = 3 x 10(3) - 3 x 10(6)) in the intense femtosecond pulsed laser field (60 fs,2 x 10(16) W/cm(2)) has been studied, and the dependence of average energy of ions emitted from argon clusters on the gas backing pressure has been measured. By comparing the average ion energies obtained with two different supersonic conical nozzles and considering the Hagena's scaling law of clusters, we have found that the average ion energy is determined by the cluster size when the laser parameters are kept unchanged. The experimental results indicated that when the cluster size is less than 3 x 10(5) atoms per cluster, the Coulomb repulsion force is the dominating factor in the expansion mechanism. Beyond this size, for 3 x 10(5) < (n) over barn < 3 x 10(6), the expansion is the result of the combined effect of both the Coulomb repulsion force and the hydrodynamic force, and the latter will play the dominating role for increasing cluster size.

Fracture of materials undergoing solid-solid phase transformation

A large number of technologically important materials undergo solid-solid phase transformations. Examples range from ferroelectrics (transducers and memory devices), zirconia (Thermal Barrier Coatings) to nickel superalloys and (lithium) iron phosphate (Li-ion batteries). These transformations involve a change in the crystal structure either through diffusion of species or local rearrangement of atoms. This change of crystal structure leads to a macroscopic change of shape or volume or both and results in internal stresses during the transformation. In certain situations this stress field gives rise to cracks (tin, iron phosphate etc.) which continue to propagate as the transformation front traverses the material. In other materials the transformation modifies the stress field around cracks and effects crack growth behavior (zirconia, ferroelectrics). These observations serve as our motivation to study cracks in solids undergoing phase transformations. Understanding these effects will help in improving the mechanical reliability of the devices employing these materials.

In this thesis we present work on two problems concerning the interplay between cracks and phase transformations. First, we consider the directional growth of a set of parallel edge cracks due to a solid-solid transformation. We conclude from our analysis that phase transformations can lead to formation of parallel edge cracks when the transformation strain satisfies certain conditions and the resulting cracks grow all the way till their tips cross over the phase boundary. Moreover the cracks continue to grow as the phase boundary traverses into the interior of the body at a uniform spacing without any instabilities. There exists an optimal value for the spacing between the cracks. We ascertain these conclusion by performing numerical simulations using finite elements.

Second, we model the effect of the semiconducting nature and dopants on cracks in ferroelectric perovskite materials, particularly barium titanate. Traditional approaches to model fracture in these materials have treated them as insulators. In reality, they are wide bandgap semiconductors with oxygen vacancies and trace impurities acting as dopants. We incorporate the space charge arising due the semiconducting effect and dopant ionization in a phase field model for the ferroelectric. We derive the governing equations by invoking the dissipation inequality over a ferroelectric domain containing a crack. This approach also yields the driving force acting on the crack. Our phase field simulations of polarization domain evolution around a crack show the accumulation of electronic charge on the crack surface making it more permeable than was previously believed so, as seen in recent experiments. We also discuss the effect the space charge has on domain formation and the crack driving force.

飞秒强激光经氩气和氩团簇的传播

通过数值求解三维电场传播方程，理论模拟了飞秒强激光脉冲（50fs，10^16w／cm^2）在氩气和中等尺寸氩团簇中的传播效应．结果表明，飞秒强激光脉冲经氩气传播将发生频谱蓝移展宽和光束发散；而经中等尺寸氩团簇传播，则存在一定程度的自聚焦效应．

μ^-子催化核聚变中强脉冲激光对介原子μ^3He的电离

数值求解了一维含时的Schroedinger方程，研究了μ子催化核聚变反应中激光强度和波长对介原子μ^3He电离的影响．发现当激光强度为10^19-10^23W/cm^2量级时，介原子μ^3He有2．7％左右的电离率；当激光强度达到6．0×10^24W/cm^2时，对介原子μ^3He有显著的电离，并且电离率随着激光的强度、波长而递增，进而会有效提高μ子的催化效率．

双色激光场中激光强度和脉宽对线性多原子分子离子电离的影响

利用强激光场电离和离解分子来研究分子激发态的波包结构是强场物理的重要研究方向。利用短时指数传播子对称分割法和快速傅里叶变换技术。数值求解了一维含时Schr（oe）dinger方程，探讨了双色激光场中激光的基波和谐波强度之间的不同配比以及脉宽对线性多原子分子离子电离的影响。理论计算结果表明：基波和谐波的相对相位为π时，尽管随着激光的基波和谐波强度之间配比的变化，电离几率随原子间距变化的趋势基本保持不变，但在一定的激光基波强度下(1．2×10^13～1．2×10^15W／cm^2)，激光基波强度的变化可以明显