Density functional theory embedding for correlated wavefunctions

Methods that exploit the intrinsic locality of molecular interactions show significant promise in making tractable the electronic structure calculation of large-scale systems. In particular, embedded density functional theory (e-DFT) offers a formally exact approach to electronic structure calculations in which the interactions between subsystems are evaluated in terms of their electronic density. In the following dissertation, methodological advances of embedded density functional theory are described, numerically tested, and applied to real chemical systems.

First, we describe an e-DFT protocol in which the non-additive kinetic energy component of the embedding potential is treated exactly. Then, we present a general implementation of the exact calculation of the non-additive kinetic potential (NAKP) and apply it to molecular systems. We demonstrate that the implementation using the exact NAKP is in excellent agreement with reference Kohn-Sham calculations, whereas the approximate functionals lead to qualitative failures in the calculated energies and equilibrium structures.

Next, we introduce density-embedding techniques to enable the accurate and stable calculation of correlated wavefunction (CW) in complex environments. Embedding potentials calculated using e-DFT introduce the effect of the environment on a subsystem for CW calculations (WFT-in-DFT). We demonstrate that WFT-in-DFT calculations are in good agreement with CW calculations performed on the full complex.

We significantly improve the numerics of the algorithm by enforcing orthogonality between subsystems by introduction of a projection operator. Utilizing the projection-based embedding scheme, we rigorously analyze the sources of error in quantum embedding calculations in which an active subsystem is treated using CWs, and the remainder using density functional theory. We show that the embedding potential felt by the electrons in the active subsystem makes only a small contribution to the error of the method, whereas the error in the nonadditive exchange-correlation energy dominates. We develop an algorithm which corrects this term and demonstrate the accuracy of this corrected embedding scheme.

Numerical modeling of optical levitation and trapping of the "stuck" particles with a pulsed optical tweezers

We present the theoretical analysis and the numerical modeling of optical levitation and trapping of the stuck particles with a pulsed optical tweezers. In our model, a pulsed laser was used to generate a large gradient force within a short duration that overcame the adhesive interaction between the stuck particles and the surface; and then a low power continuous - wave (cw) laser was used to capture the levitated particle. We describe the gradient force generated by the pulsed optical tweezers and model the binding interaction between the stuck beads and glass surface by the dominative van der Waals force with a randomly distributed binding strength. We numerically calculate the single pulse levitation efficiency for polystyrene beads as the function of the pulse energy, the axial displacement from the surface to the pulsed laser focus and the pulse duration. The result of our numerical modeling is qualitatively consistent with the experimental result. (C) 2005 Optical Society of America.

Experimental study of the Talbot effect under femtosecond laser illumination

Experimental results of the Talbot effect of an amplitude grating under femtosecond laser illumination are reported. Compared with Talbot image under continuous wave (CW) illumination, Talbot images under femtosecond laser illumination are different due to the wide spectral bandwidth and the Talbot images are more distorted at longer Talbot distances. The spectrums and the pulsewidths of femtosecond laser pulses are measured with the frequency-resolved optical gating (FROG) apparatus. Experimental results are in good agreement with the theoretical analysis. (c) 2005 Elsevier B.V. All rights reserved.

I. A study of the dynamics of triplet excitons in molecular crystals. II. An investigation of delayed light emission from Chlorella pyrenoidosa

I. PREAMBLE AND SCOPE

Brief introductory remarks, together with a definition of the scope of the material discussed in the thesis, are given.

II. A STUDY OF THE DYNAMICS OF TRIPLET EXCITONS IN MOLECULAR CRYSTALS

Phosphorescence spectra of pure crystalline naphthalene at room temperature and at 77˚ K are presented. The lifetime of the lowest triplet ³B_1u state of the crystal is determined from measurements of the time-dependence of the phosphorescence decay after termination of the excitation light. The fact that this lifetime is considerably shorter in the pure crystal at room temperature than in isotopic mixed crystals at 4.2˚ K is discussed, with special importance being attached to the mobility of triplet excitons in the pure crystal.

Excitation spectra of the delayed fluorescence and phosphorescence from crystalline naphthalene and anthracene are also presented. The equation governing the time- and spatial-dependence of the triplet exciton concentration in the crystal is discussed, along with several approximate equations obtained from the general equation under certain simplifying assumptions. The influence of triplet exciton diffusion on the observed excitation spectra and the possibility of using the latter to investigate the former is also considered. Calculations of the delayed fluorescence and phosphorescence excitation spectra of crystalline naphthalene are described.

A search for absorption of additional light quanta by triplet excitons in naphthalene and anthracene crystals failed to produce any evidence for the phenomenon. This apparent absence of triplet-triplet absorption in pure crystals is attributed to a low steady-state triplet concentration, due to processes like triplet-triplet annihilation, resulting in an absorption too weak to be detected with the apparatus used in the experiments. A comparison of triplet-triplet absorption by naphthalene in a glass at 77˚ K with that by naphthalene-h₈ in naphthalene-d₈ at 4.2˚ K is given. A broad absorption in the isotopic mixed crystal triplet-triplet spectrum has been tentatively interpreted in terms of coupling between the guest ³B_1u state and the conduction band and charge-transfer states of the host crystal.

III. AN INVESTIGATION OF DELAYED LIGHT EMISSION FROM Chlorella Pyrenoidosa

An apparatus capable of measuring emission lifetimes in the range 5 X 10^-9 sec to 6 X 10^-3 sec is described in detail. A cw argon ion laser beam, interrupted periodically by means of an electro-optic shutter, serves as the excitation source. Rapid sampling techniques coupled with signal averaging and digital data acquisition comprise the sensitive detection and readout portion of the apparatus. The capabilities of the equipment are adequately demonstrated by the results of a determination of the fluorescence lifetime of 5, 6, 11, 12-tetraphenyl-naphthacene in benzene solution at room temperature. Details of numerical methods used in the final data reduction are also described.

The results of preliminary measurements of delayed light emission from Chlorella Pyrenoidosa in the range 10^-3 sec to 1 sec are presented. Effects on the emission of an inhibitor and of variations in the excitation light intensity have been investigated. Kinetic analysis of the emission decay curves obtained under these various experimental conditions indicate that in the millisecond-to-second time interval the decay is adequately described by the sum of two first-order decay processes. The values of the time constants of these processes appear to be sensitive both to added inhibitor and to excitation light intensity.

Laser ranging based on electro-optic switch

Based on electro-optic switch effect in crystal, a novel laser ranging method is proposed. CW-laser emitted by laser transmitter propagates forward to the measured target, after being reflected by the target, and then goes back to the transmitter. Close to the transmitter, a special mono-block LiNbO3 crystal is added into the round-trip light beams. High-voltage pulses with the sharp enough changes in rising edges are loaded on the crystal. Based on electro-optic effect, double refraction and internal double reflection effect in crystal, the crystal cuts off the round-trip light beams, and reflects a light pulse cut out by the crystal to a detector aside from the original beam path. The pulse width T is the period that laser propagates forward and back between the crystal and the target. The feasibility of the new idea is proved by our experiments and a brand-new way for the laser ranging is provided. (c) 2005 Elsevier GmbH. All rights reserved.

单纵模相移DFB掺Yb3+光纤激光器运行特性的研究

对我们所制作的λ/4相移DFB掺Yb3+光纤激光器的运行特性进行了研究。研究表明：光纤端面菲涅尔反射会破坏激光器的单纵模运行,因此为获得稳定的羊纵模运行须使用隔离器或甘油清除光纤端面菲涅尔反射；机械扰动则会使沿光纤传输的单偏振激光的偏振面发生变化；温度的涨落则会引起激光输出功率的不稳定涨落。所研制à/4相移DFB单纵模、单偏振激光器具有如下特性：阈值为38mW,当泵浦功率为140 mW时,获得了25mW的1053 nm单 纵模、羊偏振激光.偏振消光比约30 dB,单纵模激光功率涨落小于2%,边模抑制比约6

Yb:YAG/YAG复合陶瓷薄片连续和调Q输出特性

采用面泵浦的CAMIL结构，我们研究了970 nm泵浦的Yb:YAG/YAG复合陶瓷薄片激光器，获得了连续和调Q的激光输出。在连续运转情况下，获得了最高1.05 W的激光输出，中心波长为1031 nm，后腔输出镜透射率为2％。我们同时获得了声光调Q的脉冲输出，重复频率从1 kHz到30 kHz，脉宽分别从166 ns到700 ns。

Cr^4＋：YAG被动调QNd：YAG陶瓷激光器的研究

介绍了近几年迅速发展的一种新型激光介质——透明Nd：YAG多晶陶瓷的发展状况，对比分析了多晶陶瓷与单晶的光谱特性、激光特性和连续实验研究情况。并对钛宝石激光器调谐至808nm，端面抽运Nd：YAG陶瓷被动调Q全固态激光器的脉冲运转进行了较为详细的理论分析和实验研究。采用初始透射率为90％的Cr^4＋：YAG可饱和吸收晶体，被动调Q的阈值功率为119mW，当端面抽运功率为465mW时，获得波长为1064nm，脉宽为16ns，重复频率为18．18kHz，单脉冲能量为3．4μJ，平均输出功率为61mW的稳定调Q

高重复频率、窄脉宽全固态光纤放大器种子源

高重复频率、窄脉宽的全固态激光器种子源级联光纤放大器是获得高功率脉冲激光输出的有效手段.短上能态寿命的Nd∶YVO4晶体在连续抽运、高重复频率Q开关工作时容易得到接近连续性能的平均输出功率.理论分析了声光(AO)调Q器件中影响输出能量和脉宽大小的主要因素,优化配置了腔型参数.利用激光二极管(LD)光纤耦合模块端面抽运Nd∶YVO4晶体,实现了声-光调Q重复频率100 kHz以上,脉宽20 ns以下,波长1064 nm的激光输出.在抽运功率5.7 W时,得到了脉宽15.3 ns,重复频率150 kHz的种子光输出,在级联单级光纤放大器后,得到了20 W的输出.

Experimental study of Ti : sapphire laser end-pumped Nd : YAG ceramic laser Q-switched by Cr4+: YAG saturable absorber

By employing a continuous-wave (CW) Ti:sapphire tunable laser as a pumping source and a Cr4+:YAG single crystal as the saturable absorber (SA), a passively Q-switched Nd:YAG ceramic laser has been demonstrated at room temperature. With an absorbed pumping power of 541 mW at 808 nm, an average output power of 61 mW at 1064 nm has been obtained with 3.5 mu J pulse energy, 15 ns pulse width and 18.18 kHz repetition rate, and the corresponding slope-efficiency is 15%. The relationships between the pulse width, repetition rate, average output power, pulse energy, and peak power on the absorbed pumping power for different initial transmission of the Cr4+:YAG SA are discussed separately. The Nd:YAG ceramic is one of the most promising laser materials for compact, efficient, all-solid-state pulsed lasers.

High optical-optical efficiency of 52.5% obtained in high power Nd : YAG ceramic laser

Using a quite uniformly side-around arranged compact pumping system, a high power Nd:YAG ceramic quasi-CW laser has been demonstrated with high optical-to-optical conversion efficiency over 50% for the first time. With 450 W quasi-CW stacked laser diode bars pumping at 808 run. 236 W Output at 1064 run was obtained and no saturation phenomena were observed.

Nd-glass belt lasers with improved beam quality

Nd-doped phosphate glass belt lasers pumped by laser diodes are demonstrated. The Nd-glass belt with a large cross-section and a small Fresnel number is air-cooled to provide around 18-W continuous wave (CW) output power with a beam quality factor of My2

Nd : YAG ceramic laser obtained high slope-efficiency of 62% in high power applications

By using quite uniformly nine-stacks side-around arranged compact pumping system, a high power Nd:YAG ceramic quasi-CW laser with high slope efficiency of 62% has been demonstrated. With 450 W quasi-CW stacked laser diode bars pumping at 808 nm, performance of the Nd: YAG ceramic laser with different output coupling mirrors has been investigated. Optimum output power of 236 W at 1064 nm was obtained and corresponding optical-to-optical conversion efficiency was as high as 52.5%. The laser system operated quite stably and no saturation phenomena have been observed, which means higher output laser power could be obtained if injecting higher pumping power. The still-evolving Nd: YAG ceramics are potential super excellent media for high power practical laser applications. (c) 2005 Optical Society of America.