3D Finite Volume Scheme for Czochralski Single Crystal Growth

Czochralski (Cz) technique, which is used for growing single crystals, has dominated the production of single crystals for electronic applications. The Cz growth process involves multiple phases, moving interface and three-dimensional behavior. Much has been done to study these phenomena by means of numerical methods as well as experimental observations. A three-dimensional curvilinear finite volume based algorithm has been developed to model the Cz process. A body-fitted transformation based approach is adopted in conjunction with a multizone adaptive grid generation (MAGG) technique to accurately handle the three-dimensional problems of phase-change in irregular geometries with free and moving surfaces. The multizone adaptive model is used to perform a three-dimensional simulation of the Cz growth of silicon single crystals.Since the phase change interface are irregular in shape and they move in response to the solution, accurate treatment of these interfaces is important from numerical accuracy point of view. The multizone adaptive grid generation (MAGG) is the appropriate scheme for this purpose. Another challenge encountered is the moving and periodic boundary conditions, which is essential to the numerical solution of the governing equations. Special treatments are implemented to impose the periodic boundary condition in a particular direction and to determine the internal boundary position and shape varying with the combination of ambient physicochemical transport process and interfacial dynamics. As indicated above that the applications and processes characterized by multi-phase, moving interfaces and irregular shape render the associated physical phenomena three-dimensional and unsteady. Therefore a generalized 3D model rather than a 2D simulation, in which the governing equations are solved in a general non-orthogonal coordinate system, is constructed to describe and capture the features of the growth process. All this has been implemented and validated by using it to model the low pressure Cz growth of silicon. Accuracy of this scheme is demonstrated by agreement of simulation data with available experimental data. Using the quasi-steady state approximation, it is shown that the flow and temperature fields in the melt under certain operating conditions become asymmetric and unsteady even in the absence of extrinsic sources of asymmetry. Asymmetry in the flow and temperature fields, caused by high shear initiated phenomena, affects the interface shape in the azimuthal direction thus results in the thermal stress distribution in the vicinity, which has serious implications from crystal quality point of view.

Study On Buoyancy Convection Phenomenon In The Crystal Growth Process

Real-time phase shift Mach-Zehnder interference technique, imaging technique, and computer image processing technique were combined to perform a real-time diagnosis of NaClO3 crystal, which described both the dissolution process and the crystallization process of the NaClO3 crystal in real-time condition. The dissolution fringes and the growth fringes in the process were obtained. Moreover, a distribution of concentration field in this process was obtained by inversion calculation. Finally, the buoyancy convection phenomenon caused by gravity in the crystal growth process was analyzed. The results showed that this convection phenomenon directly influences the growth rate of each crystal face in the crystal.

Influence Of Gravity On Structure Of Colloidal Crystal Using Simulated Microgravity

Liquid mixtures of water and deuterium oxide as the liquid phase, were used to match the density of charged colloidal particles. Kossel diffraction method was used to detect the crystal structures. The experiments under the density-matched (g=0) and unmatched (g=1) conditions are compared to examine the influence of gravity on the crystal structures formed by self-assembly of 110 nm (in diameter) polystyrene microspheres. The result shows that die gravity tends to make the lattice constants of colloidal crystals smaller at lower positions, which indicates that the effect of gravity should be taken into account in the study of the colloidal crystals.

Broadband high-gain optical parametric chirped-pulse amplification near 780 nm with LBO-I near-degenerate near-collinear phase match

Near-degenerative near-collinear phase-match geometry for broadband optical parametric chirped-pulse amplification (OPCPA) at approximate to 780 nm is calculated in comparison with nondegenerate noncollinear phase-match geometry. In an experiment on LBO-I near-degenerate near-collinear OPCPA, high gain with broad gain bandwidth (approximate to 71 nm, FWHM) at approximate to 780 nm is achieved by using an approximate to 390-nm pumping pulse. The stretched broadband chirped signal pulse near 780 nm is amplified to approximate to 412 mu J with a pumping energy of approximate to 15 mJ, and the total gain is > 3.7 X 10(6), which agrees well with the calculation. For a broadband (covering approximate to 100 nm) chirped signal pulse, the theoretical gain bandwidth has been attained experimentally for the first time. (c) 2005 Society of Photo-Optical Instrumentation Engineers.

Broadband high-gain optical parametric chirped-pulse amplification near 780 nm with LBO-I near-degenerate near-collinear phase match

Near-degenerative near-collinear phase-match geometry for broadband optical parametric chirped-pulse amplification (OPCPA) at approximate to 780 nm is calculated in comparison with nondegenerate noncollinear phase-match geometry. In an experiment on LBO-I near-degenerate near-collinear OPCPA, high gain with broad gain bandwidth (approximate to 71 nm, FWHM) at approximate to 780 nm is achieved by using an approximate to 390-nm pumping pulse. The stretched broadband chirped signal pulse near 780 nm is amplified to approximate to 412 mu J with a pumping energy of approximate to 15 mJ, and the total gain is > 3.7 X 10(6), which agrees well with the calculation. For a broadband (covering approximate to 100 nm) chirped signal pulse, the theoretical gain bandwidth has been attained experimentally for the first time. (c) 2005 Society of Photo-Optical Instrumentation Engineers.

Nonlinear copropagation of two optical pulses of different frequencies in photonic crystal fibers

A theoretical investigation of the nonlinear copropagation of two optical pulses of different frequencies in a photonic crystal fiber is presented. Different phenomena are observed depending on whether the wavelength of the signal pulse is located in the normal or the anomalous dispersion region. In particular, it is found that the phenomenon of pulse trapping occurs when the signal wavelength is located in the normal dispersion region while the pump wavelength is located in the anomalous dispersion region. The signal pulse suffers cross-phase modulation by the Raman shifted soliton pulse and it is trapped and copropagates with the Raman soliton pulse along the fiber. As the input peak power of the pump pulse is increased, the red-shift of the Raman soliton is considerably enhanced with the simultaneous further blue-shift of the trapped pulse to satisfy the condition of group velocity matching.

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.

Fermionic quantum systems. Part I: Phase transitions in quantum dots. Part II: Nuclear matter on a lattice

In the first part I perform Hartree-Fock calculations to show that quantum dots (i.e., two-dimensional systems of up to twenty interacting electrons in an external parabolic potential) undergo a gradual transition to a spin-polarized Wigner crystal with increasing magnetic field strength. The phase diagram and ground state energies have been determined. I tried to improve the ground state of the Wigner crystal by introducing a Jastrow ansatz for the wave function and performing a variational Monte Carlo calculation. The existence of so called magic numbers was also investigated. Finally, I also calculated the heat capacity associated with the rotational degree of freedom of deformed many-body states and suggest an experimental method to detect Wigner crystals.

The second part of the thesis investigates infinite nuclear matter on a cubic lattice. The exact thermal formalism describes nucleons with a Hamiltonian that accommodates on-site and next-neighbor parts of the central, spin-exchange and isospin-exchange interaction. Using auxiliary field Monte Carlo methods, I show that energy and basic saturation properties of nuclear matter can be reproduced. A first order phase transition from an uncorrelated Fermi gas to a clustered system is observed by computing mechanical and thermodynamical quantities such as compressibility, heat capacity, entropy and grand potential. The structure of the clusters is investigated with the help two-body correlations. I compare symmetry energy and first sound velocities with literature and find reasonable agreement. I also calculate the energy of pure neutron matter and search for a similar phase transition, but the survey is restricted by the infamous Monte Carlo sign problem. Also, a regularization scheme to extract potential parameters from scattering lengths and effective ranges is investigated.

Study of noncollinear quasi-phase matching optical parametric amplification with group-velocity matching based on periodically poled crystals

The properties of noncollinear optical parametric amplification (NOPA) based on quasi-phase matching of periodically poled crystals are investigated, under the condition that the group velocity matching (GVM) of the signal and idler pulses is satisfied. Our study focuses on the dependence of the gain spectrum upon the noncollinear angle, crystal temperature, and crystal angle with periodically poled KTiOPO4 (PPKTP), periodically poled LiNbO3 (PPLN), and periodically poled LiTaO3 (PPLT), and the NOPA gain properties of the three crystals are compared. Broad gain bandwidth exists above 85 nm at a signal wavelength of 800 nm with a 532 nm pump pulse, with proper noncollinear angle and grating period at a fixed temperature for GVM. Deviation from the group-velocity-matched noncollinear angle can be compensated by accurately tuning the crystal angle or temperature with a fixed grating period for phase matching. Moreover, there is a large capability of crystal angle tuning.

Broad-bandwidth semi-noncollinear optical parametric amplification in periodically poled LiNbO3 based on tilted quasi-phase-matched gratings

On the basis of noncollinear optical parametric amplification in periodically poled lithium niobate (PPLN) which is realized by quasi-phase matching (QPM) technology, we consider the possibility of semi-noncollinear phase matching between collinear and noncollinear geometries by tilting a PPLN-crystal's parallel grating at a sure angle. Numerical simulation with proper parameters shows that we can achieve a broader optical parametric amplification (OPA) bandwidth than that of noncollinear geometry. About 121 nm at a signal wavelength of 800 and 70 nm at a signal wavelength of 1064 nm under optimal conditions are obtained when the crystal length is 9 mm.

Coherent enhancement of broadband frequency up-conversion in BBO crystal by shaping femtosecond laser pulses

An optimal feedback control of broadband frequency up-conversion in BBO crystal is experimentally demonstrated by shaping femto-second laser pulses based on genetic algorithm, and the frequency up-conversion efficiency can be enhanced by similar to 16%. SPIDER results show that the optimal laser pulses have shorter pulse-width with the little negative chirp than the original pulse with the little positive chirp. By modulating the fundamental spectral phase with periodic square distribution on SLM-256, the frequency up-conversion can be effectively controlled by the factor of about 17%. The experimental results indicate that the broadband frequency up-conversion efficiency is related to both of second harmonic generation (SHG) and sum frequency generation (SFG), where the former depends on the fundamental pulse intensity, and the latter depends on not only the fundamental pulse intensity but also the fundamental pulse spectral phase. (c) 2006 Elsevier B.V. All rights reserved.

On Ultrafast Time-Domain TeraHertz Spectroscopy in the Condensed Phase: Linear Spectroscopic Measurements of Hydrogen-Bond Dynamics of Astrochemical Ice Analogs and Nonlinear TeraHertz Kerr Effect Measurements of Vibrational Quantum Beats

Much of the chemistry that affects life on planet Earth occurs in the condensed phase. The TeraHertz (THz) or far-infrared (far-IR) region of the electromagnetic spectrum (from 0.1 THz to 10 THz, 3 cm^-1 to 300 cm^-1, or 3000 μm to 30 μm) has been shown to provide unique possibilities in the study of condensed-phase processes. The goal of this work is to expand the possibilities available in the THz region and undertake new investigations of fundamental interest to chemistry. Since we are fundamentally interested in condensed-phase processes, this thesis focuses on two areas where THz spectroscopy can provide new understanding: astrochemistry and solvation science. To advance these fields, we had to develop new instrumentation that would enable the experiments necessary to answer new questions in either astrochemistry or solvation science. We first developed a new experimental setup capable of studying astrochemical ice analogs in both the TeraHertz (THz), or far-Infrared (far-IR), region (0.3 - 7.5 THz; 10 - 250 cm^-1) and the mid-IR (400 - 4000 cm^-1). The importance of astrochemical ices lies in their key role in the formation of complex organic molecules, such as amino acids and sugars in space. Thus, the instruments are capable of performing variety of spectroscopic studies that can provide especially relevant laboratory data to support astronomical observations from telescopes such as the Herschel Space Telescope, the Stratospheric Observatory for Infrared Astronomy (SOFIA), and the Atacama Large Millimeter Array (ALMA). The experimental apparatus uses a THz time-domain spectrometer, with a 1750/875 nm plasma source and a GaP detector crystal, to cover the bandwidth mentioned above with ~10 GHz (~0.3 cm^-1) resolution.

Using the above instrumentation, experimental spectra of astrochemical ice analogs of water and carbon dioxide in pure, mixed, and layered ices were collected at different temperatures under high vacuum conditions with the goal of investigating the structure of the ice. We tentatively observe a new feature in both amorphous solid water and crystalline water at 33 cm^-1 (1 THz). In addition, our studies of mixed and layered ices show how it is possible to identify the location of carbon dioxide as it segregates within the ice by observing its effect on the THz spectrum of water ice. The THz spectra of mixed and layered ices are further analyzed by fitting their spectra features to those of pure amorphous solid water and crystalline water ice to quantify the effects of temperature changes on structure. From the results of this work, it appears that THz spectroscopy is potentially well suited to study thermal transformations within the ice.

To advance the study of liquids with THz spectroscopy, we developed a new ultrafast nonlinear THz spectroscopic technique: heterodyne-detected, ultrafast THz Kerr effect (TKE) spectroscopy. We implemented a heterodyne-detection scheme into a TKE spectrometer that uses a stilbazoiumbased THz emitter, 4-N,N-dimethylamino-4-N-methyl-stilbazolium 2,4,6-trimethylbenzenesulfonate (DSTMS), and high numerical aperture optics which generates THz electric field in excess of 300 kV/cm, in the sample. This allows us to report the first measurement of quantum beats at terahertz (THz) frequencies that result from vibrational coherences initiated by the nonlinear, dipolar interaction of a broadband, high-energy, (sub)picosecond THz pulse with the sample. Our instrument improves on both the frequency coverage, and sensitivity previously reported; it also ensures a backgroundless measurement of the THz Kerr effect in pure liquids. For liquid diiodomethane, we observe a quantum beat at 3.66 THz (122 cm^-1), in exact agreement with the fundamental transition frequency of the υ4 vibration of the molecule. This result provides new insight into dipolar vs. Raman selection rules at terahertz frequencies.

To conclude we discuss future directions for the nonlinear THz spectroscopy in the Blake lab. We report the first results from an experiment using a plasma-based THz source for nonlinear spectroscopy that has the potential to enable nonlinear THz spectra with a sub-100 fs temporal resolution, and how the optics involved in the plasma mechanism can enable THz pulse shaping. Finally, we discuss how a single-shot THz detection scheme could improve the acquisition of THz data and how such a scheme could be implemented in the Blake lab. The instruments developed herein will hopefully remain a part of the groups core competencies and serve as building blocks for the next generation of THz instrumentation that pushes the frontiers of both chemistry and the scientific enterprise as a whole.

Quantitative measurement of domain inversion in RuO2 : LiNbO3 crystal by digital holographic interferometry

We quantitatively study the domain inversion in a RuO2:LiNbO3 crystal wafer by the digital holographic interferometry. The crystal wafer is placed into one arm of a Mach-Zehnder-type interferometer to record a series of holograms. Making use of the angular spectrum backward propagation algorithm, we reconstruct the optical wave field in the crystal plane. The extracted phase difference from the reconstructed optical wave field is a well linear function of the applied external voltage. We deduce that the linear electro-optic coefficient of the detected RuO2:LiNbO3 crystal sample is 9.1x10(-12) m/V. An unexpected phase contrast at the antiparallel domain wall is observed and the influence of the applied external voltage on it is studied in detail. Also the built-in internal field is quantitatively measured as 0.72 kV/mm. (c) 2006 American Institute of Physics.

Digital holographic interferometry and the angular spectrum method applied to measuring the domain inversion in ferroelectric crystal

The application of digital holographic interferometry on the quantitative measurement of the domain inversion in a RuO2: LiNbO3 crystal wafer is presented. The recorded holograms are reconstructed by the angular spectrum method. From the reconstructed phase distribution we can clearly observe the boundary between the inverted and un-inverted domain regions. Comparisons with the results reconstructed by use of the Fresnel transform method are given. Factors that influence the measurement include the spectrum filter size and the spectrum movement are discussed. The spectrum filter size has an effect on the measurement of the details. Although the spectrum movement affects every single reconstructed image, it has no influence on the final measurement.