Photoelectron angular distributions of molecules in bichromatic laser fields of circular polarization

Photoelectron angular distributions (PADs) from above-threshold ionization of O-2 and N-2 molecules irradiated by a bichromatic laser field of circular polarization are Studied. The bichromatic laser field is specially modulated such that it can be used to mimic a sequence of one-cycle laser pulses. The PADs are greatly affected by the molecular alignment, the symmetry of the initial electronic distribution, and the carrier-envelope phase of the laser pulses. Generally, the PADs do not show any symmetry, and become symmetric about an axis only when the symmetric axis of laser field coincides with the symmetric axis of molecules. This study shows that the few-cycle laser pulses call be used to steer the photoelectrons and perform the selective ionization of molecules. (C) 2008 Elsevier B.V. All rights reserved.

Fluorescent Ag nanoclusters in glass induced by an infrared femtosecond laser

We report a method for the selective introduction of fluorescent Ag nanoclusters in glass. Extinction and photoluminescence spectra show that a fraction of the Ag atoms are generated through femtosecond laser induced multiphoton reduction and then aggregate to form Ag nanoclusters after heat treatment. Red luminescence from the irradiated region is observed under blue or green laser excitation. The fluorescence can be attributed to interband transitions within Ag nanoclusters. This method provides a novel route to fabricate fluorescent nanomaterials in 3D transparent materials. (c) 2007 Elsevier B.V. All rights reserved.

Methods for melting temperature calculation

Melting temperature calculation has important applications in the theoretical study of phase diagrams and computational materials screenings. In this thesis, we present two new methods, i.e., the improved Widom's particle insertion method and the small-cell coexistence method, which we developed in order to capture melting temperatures both accurately and quickly.

We propose a scheme that drastically improves the efficiency of Widom's particle insertion method by efficiently sampling cavities while calculating the integrals providing the chemical potentials of a physical system. This idea enables us to calculate chemical potentials of liquids directly from first-principles without the help of any reference system, which is necessary in the commonly used thermodynamic integration method. As an example, we apply our scheme, combined with the density functional formalism, to the calculation of the chemical potential of liquid copper. The calculated chemical potential is further used to locate the melting temperature. The calculated results closely agree with experiments.

We propose the small-cell coexistence method based on the statistical analysis of small-size coexistence MD simulations. It eliminates the risk of a metastable superheated solid in the fast-heating method, while also significantly reducing the computer cost relative to the traditional large-scale coexistence method. Using empirical potentials, we validate the method and systematically study the finite-size effect on the calculated melting points. The method converges to the exact result in the limit of a large system size. An accuracy within 100 K in melting temperature is usually achieved when the simulation contains more than 100 atoms. DFT examples of Tantalum, high-pressure Sodium, and ionic material NaCl are shown to demonstrate the accuracy and flexibility of the method in its practical applications. The method serves as a promising approach for large-scale automated material screening in which the melting temperature is a design criterion.

We present in detail two examples of refractory materials. First, we demonstrate how key material properties that provide guidance in the design of refractory materials can be accurately determined via ab initio thermodynamic calculations in conjunction with experimental techniques based on synchrotron X-ray diffraction and thermal analysis under laser-heated aerodynamic levitation. The properties considered include melting point, heat of fusion, heat capacity, thermal expansion coefficients, thermal stability, and sublattice disordering, as illustrated in a motivating example of lanthanum zirconate (La₂Zr₂O₇). The close agreement with experiment in the known but structurally complex compound La₂Zr₂O₇ provides good indication that the computation methods described can be used within a computational screening framework to identify novel refractory materials. Second, we report an extensive investigation into the melting temperatures of the Hf-C and Hf-Ta-C systems using ab initio calculations. With melting points above 4000 K, hafnium carbide (HfC) and tantalum carbide (TaC) are among the most refractory binary compounds known to date. Their mixture, with a general formula Ta_xHf_1-xC_y, is known to have a melting point of 4215 K at the composition Ta₄HfC₅, which has long been considered as the highest melting temperature for any solid. Very few measurements of melting point in tantalum and hafnium carbides have been documented, because of the obvious experimental difficulties at extreme temperatures. The investigation lets us identify three major chemical factors that contribute to the high melting temperatures. Based on these three factors, we propose and explore a new class of materials, which, according to our ab initio calculations, may possess even higher melting temperatures than Ta-Hf-C. This example also demonstrates the feasibility of materials screening and discovery via ab initio calculations for the optimization of "higher-level" properties whose determination requires extensive sampling of atomic configuration space.

Part I. Electric birefringence studies of deoxyribonucleic acids. Part II. Selective dissociation of nucleohistone complexes

Part I

The electric birefringence of dilute DNA solutions has been studied in considerable detail and on a large number of samples, but no new and reliable information was discovered concerning the tertiary structure of DNA. The large number of variables which effect the birefringence results is discussed and suggestions are made for further work on the subject.

The DNA molecules have been aligned in a rapidly alternating (10 to 20 kc/sec) square wave field confirming that the orientation mechanism is that of counterion polarization. A simple empirical relation between the steady state birefringence, Δn_st, and the square of the electric field, E, has been found: Δn_st = E²/(a E² + b), where a = 1/Δn_s and b = (E²/Δn_st)_E→o. Δn_s is the birefringence extrapolated to infinite field strength.

The molecules show a distribution of relaxation times from 10^-4 to 0.2 sec, which is consistent with expectations for flexible coil molecules. The birefringence and the relaxation times decrease with increasing salt concentrations. They also depend on the field strength and pulse duration in a rather non-reproducible manner, which may be due in part to changes in the composition of the solution or in the molecular structure of the DNA (other than denaturation). Further progress depends on the development of some control over these effects.

Part II

The specificity of the dissociation of reconstituted and native deoxyribonucleohistones (DNH) by monovalent salt solutions has been investigated. A novel zone ultracentrifugation method is used in which the DNH is sedimented as a zone through a preformed salt gradient, superimposed on a stabilizing D₂O (sucrose) density gradient. The results, obtained by scanning the quartz sedimentation tubes in a spectrophotometer, were verified by the conventional, preparative sedimentation technique. Procedures are discussed for the detection of microgram quantities of histones, since low concentrations must be used to prevent excessive aggregation of the DNH.

The data show that major histone fractions are selectively dissociated from DNH by increasing salt concentrations: Lysine rich histone (H I) dissociates gradually between 0.1 and 0.3 F, slightly lysine rich histone (H II) dissociates as a narrow band between 0.35 and 0.5 F, and arginine rich histone (H III, H IV) dissociates gradually above 0.5 F NaClO₄.

The activity of the partially dissociated, native DNH in sustaining RNA synthesis, their mobility and their unusual heat denaturation and renaturation behavior are described. The two-step melting behavior of the material indicates that the histones are non-randomly distributed along the DNA, but the implications are that the uncovered regions are not of gene-size length.

Radially polarized and pulsed output from passively Q-switched Nd:YAG ceramic microchip laser

For the first time, to the best of our knowledge, a radially polarized laser pulse was produced from a passively Q-switched Nd:YAG ceramic microchip laser with a piece of Cr4+:YAG crystal as the saturable absorber and multilayer concentric subwavelength grating as the polarization-selective output coupler. The averaged laser power reached 450 mW with a slope efficiency of 30.2%. The laser pulse had a maximum peak power of 759 W, a minimum pulse duration of 86 ns, and a 6.7 kHz repetition rate at 3.7 W absorbed pump power. The polarization degree of the radially polarized pulse was measured to be as high as 97.4%. Such a radially polarized laser pulse with a high peak power and a short width is important to numerous applications such as metal cutting. (C) 2008 Optical Society of America

Numerical and experimental analysis on green laser crystallization of amorphous silicon thin films

The effect of laser fluence on the crystallization of amorphous silicon irradiated by a frequency-doubled Nd:YAG laser is studied both theoretically and experimentally. An effective numerical model is set up to predict the melting threshold and the optimized laser fluence for the crystallization of 200-nm-thick amorphous silicon. The variation of the temperature distribution with time and the melt depth is analyzed. Besides the model, the Raman spectra of thin films treated with different fluences are measured to confirm the phase transition and to determine the optimized fluence. The calculating results accord well with those obtained from the experimental data in this research. (C) 2008 Elsevier Ltd. All rights reserved.

Valence state change and refractive index change induced by femtosecond laser irradiation in Sm3+ doped fluoroaluminate glass

We report femtosecond laser induced valence state and refractive index change in transparent Sin(3+)-doped fluoroaluminate glass. The effect of annealing on the induced changes was studied and the thermal stability of these changes was discussed. The results show that the femtosecond laser induced valence state change is more stable than the induced refractive index change. The observed phenomenon could be applied to design the thermally erasable or stable storage medium. (c) 2007 Elsevier B.V. All rights reserved.

Direct writing computer-generated holograms on metal film by an infrared femtosecond laser

Writing computer-generated holograms has been achieved by using near infrared femtosecond laser selective ablation of metal film deposited on glass substrate. The diffraction features with data reconstruction of fabricated computer-generated holograms were evaluated. Both transmission and reflection holograms can be fabricated in a single process. The process required no mask, no pre- or post-treatment of the substrate. (C) 2005 Optical Society of America.

Space-selective precipitation of Au nanoparticles inside silica gel

Au colloids were prepared by irradiation with a Nd:YAG laser. Au nanoparticles were characterized by absorption spectra, transmission electron microscopy (TEM) and X-ray diffraction (XRD) analysis. It is found that the wavelength of the laser has no effect on the size but the number of the Au nanoparticles. By irradiating a transparent silica gel doped with gold ions with the focused laser in the gel and subsequent exposing in air, a space-selective pattern of letter "P" consisting of Au nanoparticles was observed inside the silica gel.

Three-dimensional micro- and nano-fabrication in transparent materials by femtosecond laser

Femtosecond pulsed lasers have been widely used for materials microprocessing. Due to their ultrashort pulse width and ultrahigh light intensity, the process is generally characterized by the nonthermal diffusion process. We observed various induced microstructures such as refractive-index-changed structures, color center defects, microvoids and microcracks in transparent materials (e.g., glasses after the femtosecond laser irradiation), and discussed the possible applications of the microstructures in the fabrication of various micro optical devices [e.g., optical waveguides, microgratings, microlenses, fiber attenuators, and three-dimensional (3D) optical memory]. In this paper, we review our recent research developments on single femtosecond-laser-induced nanostructures. We introduce the space-selective valence state manipulation of active ions, precipitation and control of metal nanoparticles and light polarization-dependent permanent nanostructures, and discuss the mechanisms and possible applications of the observed phenomena.

Study of thermal behaviors in CO2 laser irradiated glass

To understand mechanisms underlying laser-induced damage of BK7 and fused silica, we calculate the temperature field of the substrates with CO2 laser irradiating at a given laser power and beam radius. We find that the two glasses show different thermal behaviors. A model is developed for estimating the time t to heat the surface of the substrates up to a particular temperature T with cw CO2 laser irradiation. We calculate theoretically the duration t that the samples are irradiated, from the beginning to visual catastrophic damage, with the assumption of damage threshold determined by the critical temperature. The duration t that the samples are irradiated, from the beginning to visual catastrophic damage, is investigated experimentally as well. Here we take the melting point or softening point as the critical temperature, given the thermomechanical coupling properties, which is enough to cause damage for BK7. Damage features are characterized by the sound of visual cracks. Finally, we calculate stresses induced by laser heating. The analysis of stress indicates that the damage of BK7 is due to the stresses induced by laser heating. (c) 2005 Society of Photo-Optical Instrumentation Engineers.

Study of thermal behaviors in CO2 laser irradiated glass

To understand mechanisms underlying laser-induced damage of BK7 and fused silica, we calculate the temperature field of the substrates with CO2 laser irradiating at a given laser power and beam radius. We find that the two glasses show different thermal behaviors. A model is developed for estimating the time t to heat the surface of the substrates up to a particular temperature T with cw CO2 laser irradiation. We calculate theoretically the duration t that the samples are irradiated, from the beginning to visual catastrophic damage, with the assumption of damage threshold determined by the critical temperature. The duration t that the samples are irradiated, from the beginning to visual catastrophic damage, is investigated experimentally as well. Here we take the melting point or softening point as the critical temperature, given the thermomechanical coupling properties, which is enough to cause damage for BK7. Damage features are characterized by the sound of visual cracks. Finally, we calculate stresses induced by laser heating. The analysis of stress indicates that the damage of BK7 is due to the stresses induced by laser heating. (c) 2005 Society of Photo-Optical Instrumentation Engineers.

Laser slotting: a new laser machining technique

This work describes a new technique for the selective removal of steel using a conventional CO2 laser beam and a novel arrangement of inert and reactive gas jets to produce the gas equivalent of a rotary cutter.

Selective epitaxial growth in silicon on insulator: Planarity and mass flow

Seeded zone-melt recrystallization using a dual electron beam system has been performed on silicon-on-insulator material, which was prepared with single-crystal silicon filling of the seed windows by selective epitaxial growth. The crystal quality has been assessed by a variety of microscopic techniques, and it is shown that single-crystal films 0.5-1.0 μm thick over 1.0 μm of isolating oxide may be prepared by this method. These films have considerably less lateral variation in thickness than standard material, in which the windows are not so filled. The filling method is suitable for both single- and multiple-layer silicon-on-insulator, and gives the advantages of excellent layer uniformity after recrystallization and improved planarity of the whole chip structure. Experiments using various amounts of seed window filling have shown that the lateral variations of silicon film thickness seen in unplanarized material are due to stress relief in the cap oxide when the silicon film is molten, rather than the effect previously postulated in which they were assumed to be due to the contraction of silicon on melting.

Highly flexible all-optical wavelength conversion at 2.488 Gbits/s using a multi-output-wavelength laser

An integrated multiwavelength grating cavity (MGC) laser fabricated by selective area regrowth is demonstrated. In addition to allowing wavelength conversion, the device can perform various important network functions such as space switching and multiplexing. The use of the device for these functions offers several advantages from a wavelength division multiplexing (WDM) network, such as flexibility, reduced component count, size, and the associated cost reduction.