碳化硅中氦离子辐照缺陷演化及SiCOI薄膜合成的研究

碳化硅是一种宽带隙半导体材料,具有禁带宽度大、击穿电压高、热导率高、电子饱和漂移速度大、介电常数小、抗辐射能力强、化学稳定性好等优良特性,使其在越来越多的领域如航空航天、太空探测、人造卫星、地热勘探、核能仪器、雷达通讯等, 所需要高温、高速、高频、大功率的微电子器件方面倍受青睐,并和氮化镓、金刚石一起被誉为发展前景十分广阔的第三代半导体材料。本论文采用He+离子注入,在SiC衬底一定深度引入纳米气泡/空腔的方法,来增强对氧原子的俘获以增加O原子在RP处局域浓度,使得更利于O与Si的反应,从而促进氧化埋层的形成,以达到降低注入O的剂量而形成优良的氧化物电绝缘层的目的。由于高剂量的O注入会引起表层SiC材料的损伤，该方法有望缓解目前SIMOX技术中O离子高剂量注入引起表层材料的损伤问题，以期获得低成本、低缺陷密度的SiCOI材料。论文主要开展了如下研究：（1）对He+离子高温（600 K）注入6H-SiC中产生的辐照缺陷,以及缺陷在阶梯温度退火的演化行为的特征进行了分析。实验采用100 keV的He+,辐照剂量范围为3.0×1015～3.0×1016 He+/cm2。利用拉曼光谱、室温光致发光谱、红外吸收光谱、沟道卢瑟福背散射谱的特征进行了分析。实验结果表明,离子注入所产生晶格损伤的程度与He+离子注入剂量有关；高温退火使得损伤得到恢复,不同注入剂量造成的晶格损伤需要不同的退火温度才可恢复。高剂量注入的样品在阶梯温度退火条件下呈现出了点缺陷的复合、氦-空位团的产生、氦泡的形核、长大等特性。与室温注入相比,高温注入引入的自退火作用使大部分简单缺陷发生复合,限制了损伤的积累,从而在材料中产生相对较小的损伤。在一定剂量范围内是避免注入层非晶化的一个重要方法,为后续利用氦离子注入空腔掩埋层吸杂或者制备低成本、低缺陷密度的绝缘层上碳化硅(SiCOI)材料提供了可能。 （2）对He的预注入引入的辐照缺陷与随后注入的氧原子的相互作用机理进行了初步分析。实验采用先He后O注入的方法，采用的离子能量为30 keV (He+)，100 keV (O+)；剂量分别为3.0×1016 (He+)、1.0×1017 (O+) ions/cm2。拉曼散射谱结果表明,空腔对氧的吸收主要是通过捕获简单缺陷释放出来的间隙氧原子实现的,进而促进了对氧的吸附,形成硅氧化合物,有利于氧化埋层的形成。紫外-可见吸收谱中的干涉带表明在材料表面下大概198 nm处是损伤层与晶体层的分界面，接近于SRIM2006估算得到的30 keV He+和100 keV O+辐照损伤的深度（He+辐照损伤的深度为195 nm；O+辐照损伤的深度为165 nm）。沟道卢瑟福背散射谱表明，在特定深度（约150 nm）处,样品中形成了接近非晶的埋层。He离子预注入的碳化硅基体由于含有较多的空位,注入的氧在退火过程中从简单缺陷中释放,向空腔层扩散并捕获在空腔层内,使得He离子预先注入形成的空腔层限制了随后O离子注入造成的损伤层的厚度

非全裸氟离子与氦原子和氖原子碰撞中的多电子过程研究

本工作采用反冲离子飞行时间技术和散射离子位置灵敏探测技术测量了F~(2+)、F~(3+)离子与He原子和Ne原子碰撞中转移电离截面与单电子俘获截面比和入射离子损失一个电子情况下靶原子多重电离与单重电离的截面比。研究了这些截面比随作用强度κ的变化规律，并对不同的碰撞体系进行了比较，总结了强相互作用区(1.4 < κ < 4.4) F~(2+)、F~(3+)离子与He和Ne原子碰撞中的转移电离过程和入射离子电子损失过程的规律。实验发现：（1）对本工作中所有的碰撞体系，转移电离截面与单电子俘获截面比随作用强度κ的增大而减小；（2）对He原子靶，入射离子损失一个电子时He原子二重电离与单重电离的截面比随作用强度κ的增大而减小；（3）对于Ne原子靶，入射离子损失一个电子时Ne原子四重电离、三重电离、二重电离截面与单重电离截面比随作用强度κ有不同的变化规律。本工作对于上述实验现象进行了定性分析和讨论。在本实验能区，转移电离现象可视作一个电子被俘获、另一个电子被电离的两步过程；当入射离子损失一个电子时，He原子二重电离的主要机制为Two-Step机制，而Ne原子的多重电离则为Two-Step机制和随后的电子重组过程的共同作用的结果。深入研究强相互作用区离子一原子碰撞过程，还需要积更多的实验数据和发展有效的理论模型。

多电荷态硫离子与氦原子和氢分子碰撞中的多电子转移过程研究

本工作采用反冲离子飞行时间技术和散射离子位置灵敏探测技术，实验研究了Sq+离子与He、H2碰撞中的多电子转移过程和分子离子的碎裂现象。研究了转移电离截面与单电子俘获截面比值和入射离子损失一个电子和两个电子的情况下，靶原子双重电离与单重电离的截面比值随入射离子能量和入射离子电荷态的变化规律，并对不同的碰撞体系的结果进行了比较。研究发现：在本工作研究的入射离子能区，对于HZ分子靶，双电子俘获自电离反应道：S2+H2→S(q-l)+2H++e-。是转移电离过程的主要贡献，而直接转移电离的贡献可以忽略；随着入射离子电荷态的增加，双电子俘获自电离的贡献增加，直接转移电离的贡献逐渐减小，但双电子俘获自电离的贡献的增加比理论预言的要慢。建立了蒙特卡罗程序模拟离子与分子碰撞中产生的具有不同的初始动能的离子碎片的飞行时间谱，深入分析和研究了Sq＋与H2分子碰撞中产生的H2+的解离过程和库仑爆炸过程，以及H＋碎片的能量分布。模拟结果与实验测量到的TOF谱的分析比较说明：在Sq＋与H2分子碰撞实验中，库仑爆炸是产生H+的主要反应道，而氢分子离子H2+发生解离产生H+的反应道相对很弱。

A 2-kW COIL with a square pipe-array JSOG and nitrogen buffer gas

A 2-kW-class chemical oxygen-iodine laser (COIL) using nitrogen buffer gas has been developed and tested since industrial applications of COIL devices will require the use of nitrogen as the buffer gas. The laser, with a gain length of 11.7 cm, is energized by a square pipe-array jet-type singlet oxygen generator (SPJSOG) and employs a nozzle bank with a designed Mach number of 2.5. The SPJSOG has advantages over the traditional plate-type JSOG in that it has less requirements on basic hydrogen peroxide (BHP) pump, and more important, it has much better operational stability. The SPJSOG without a cold trap and a gas-liquid separator could provide reliable operations for a total gas flow rate up to 450 mmol/s and with a low liquid driving pressure of around 0.7 atm or even lower. The nozzle bank was specially designed for a COIL using nitrogen as the buffer gas. The cavity was designed for a Mach number of 2.5, in order to provide a gas speed and static temperature in the cavity similar to that for a traditional COIL with helium buffer gas and a Mach 2 nozzle. An output power of 2.6 kW was obtained for a chlorine flow rate of 140 mmol/s, corresponding to a chemical efficiency of 20.4%. When the chlorine flow rate was reduced to 115 mmol/s, a higher chemical efficiency of 22.7% was attained. Measurements showed that the SPJSOG during normal operation could provide a singlet oxygen yield Y greater than or equal to 55%, a chlorine utilization U greater than or equal to 85%, and a relative water vapor concentration w = [H2O]/([O-2] + [Cl-2]) less than or equal to 0.1.

Gas permeability of a novel cellulose membrane

A novel cellulose membrane was prepared by using amine oxides as the solvent and its mechanical performance was measured. Steady-state permeation rates of carbon dioxide, hydrogen, methane, nitrogen, oxygen, argon and helium in the homogeneous dense cellulose membrane were measured in the temperature range of 298-353 K and under gas pressures up to 1 MPa. The effect of swelling on hydrophilic membrane permeability was studied in some detail on the cellulose membrane. The difference in gas permeability between the "dry" cellulose membrane and the "water-swollen" cellulose membrane was investigated, and the gas permeability between the cellulose membrane and the Cellophane was compared. In this paper, the separation performance Of CO2 over H-2 in a "water-swollen" cellulose membrane is reported for the first time and the separation factor Of CO2/H-2 can be up to 15. (C) 2002 Elsevier Science B.V. All rights reserved.

Tide-influenced acidic hydrothermal system offshore NE Taiwan

Elemental sulfur and hydrogen sulfide emitted offshore of northeastern Taiwan known to local fishermen for generations, but never studied until recently, are found to have originated from a cluster of shallow (< 30 m depth) hydrothermal vents. Among the mounds is a massive 6 m high chimney with a diameter of 4 m at the base composed of almost pure sulfur and discharging hydrothermal fluid containing sulfur particles. The sulfur in the chimney has a delta(34)S= 1.1 parts per thousand that is isotopically lighter than seawater. A yellow smoker at shallow depths with such characteristics has never been reported on anywhere else in the world. Gas discharges from these vents are dominated by CO2 (> 92%) with small amounts of H2S. Helium isotopic ratios 7.5 times that of air indicate that these gases originate from the mantle. High temperature hydrothermal fluids have measured temperatures of 78-116 degrees C and pH (25 degrees C) values as low as 1.52, likely the lowest to be found in world records. Low temperature vents (30-65 degrees C) have higher pH values. Continuous temperature records from one vent show a close correlation with diumal tides, suggesting rapid circulation of the hydrothermal fluids. (c) 2005 Elsevier B.V. All rights reserved.

He, Ne and Ar isotope compositions of fluid inclusions in hydrothermal sulfides from the TAG hydrothermal field, Mid-Atlantic Ridge

Helium, rieon and argon isotope compositions of fluid inclusions have been measured in hydrothermal sulfide samples from the TAG hydrothermal field at the Mid-Atlantic Ridge. Fluid-inclusion He-3/He-4 ratios are 2.2-13.3 times the air value (Ra), and with a mean of 7.2 Ra. Comparison with the local vent fluids (He-3/He-4=7.5-8.2 Ra) and mid-ocean ridge basalt values (He-3/He-4=6-11 Ra) shows that the variation range of He-3/He-4 ratios from sulfide-hosted fluid inclusions is significantly large. Values for Ne-20/Ne-22 are from 10.2 to 11.4, which are significantly higher than the atmospheric ratio (9.8). And fluid-inclusion Ar-40/Ar-36 ratios range from 287 to 359, which are close to the atmospheric values (295.5). These results indicate that the noble gases of fluid inclusions in hydrothermal sulfides are a mixture of mantle- and seawater-derived noble gases; the partial mantle-derived components of trapped hydrothermal fluids may be from the lower mantle; the helium of fluid inclusions is mainly from upper mantle; and the Ne and Ar components are mainly from seawater.

新疆萨吾尔金矿带构造-流体地球化学及成矿作用

The Sawuer gold belt is located in the transition belt between Siberian plate and Kazakhstan-Junggar plate. Based on the geological and geochemical studies on the Kuoerzhenkuola and Buerkesidai gold deposits, in Sawuer gold mineralization belt, the time-space structure of mineralization and mineralizing factor are studied, the metallogenic regularity is concluded in thistheses. The ore bodies have the regularity that orebody are of the extensive and compressive in the sallow and depth of volcanic apparatue, respectively, and the vertical extension of orebody is more intensive than the horizontal extension. The gold deposits were controlled by the fractures of volcanic apparatus and regional faults, and featured by the hydrothermal alteration and metasomatism type disseminated mineralization and filling type vein mineralization. By virtue of the geological and geochemical studies on the two deposits that the formation of the two deposits are significantly related to the volcanic activity, we propose new ideas about their origin: (1) the two deposits are located in the same strata, and share the same genesis. (2) both of two deposits are volcanogenic late-stage hydrothermal gold deposits. Based on mapping of volcanic lithofacies and structure for the first time, it is discovered that a volcanic apparatus existed in the study area. Volcanic-intrusive activity can be divided into three cycles and nine lithofacies. where the two deposits are hosted in the same volcanic cycle, in this case, the wall-rock should belong to the same strata. The 40Ar-39Ar age method is employed in this work to analyze the fluid inclusions of quartz in the ore bodies from Kuoerzhenkuola and Buerkesidai gold deposits. The results show that the main mineralization occurred in 332.05 + 2.02-332.59 + 0.5IMa and 335.53 + 0.32Ma~336.78 + 0.50Ma for Kuoerzhenkuola and Buerkesidai gold deposits respectively, indicating that the two deposits are formed almost at the same time, and the metallogenic epoch of the tow deposits are close to those of the hosting rocks formed by volcanic activity of Sawuer gold belt. This geochronological study supplies new evidence for determining the timing of gold mineralization, the geneses of gold deposits? and identifies that in Hercynian period, the Altai developed tectonic-magmatic-hydrothermal mineralization of Early Carboniferous period, except known two metallogenic mineralization periods including tectonic-magmatic-hydrothermal mineralization of Devonian period and Late Carboniferous-Permian period respectively. The study of fluid inclusions indicates that the ore-forming fluid is a type of NaCl-HbO fluid with medium-low temperature and low salinity, Au is transported by the type of auric-sulfur complex (Au (HS)2-), the ore is formed in reduction condition. Hydrogen and oxygen isotopes of fluid inclusions in the major mineralizating stage show that the solutions mainly originated from magmatic water and meteoric water. The fluid mixing and water-rock reaction cause the deposition of Au. The helium and argon isotope compositions of fluid inclusions hosted in pyrite have been measured from Kuoerzhenkuola and Buerkesidai gold deposits in Sawuer gold belt. The results show that the ore-forming fluids of two deposits possessed the same source and is a mixture of mantle- and partial meteoric water-derived fluid, and the reliability of He and Ar isotopic compositions in Hercynian period is discussed. Isotopic studies including H, O, He, C, S, Pb and Sr reveal the same result that the ore-forming fluids of two deposits possessed the same source: the water derived mainly from magmatic water, partially from meteoric water; the mineralizers and ore materials derived mainly from mantle beneath the island arc, and partially from crust. The ore-forming fluids of two deposits are a mixture of mantle-derived fluids being incorporated by crust-derived fluid, and shallow partial meteoric water. Based on these results, it is proposed that the geneses of the two gold deposits are the same, being volcanogenic late-stage hydrothermal gold deposits that the ore-forming fluids filled in fractures of volcanic apparatus and metasomatized the host rocks in the volcanic apparatus. It is the first time we carried out the geophysical exploration, that is, the EH-4 continuous electrical conductivity image system measurement, the results show that relative large-size mineralizing anomalies in underground have been discovered.lt can confirm the law and genesis of the deposits mentioned above, and change the two abandoned mines to current large-size potenial exploration target.

Perovskite-type B-site Bi-doped ceramic membranes for oxygen separation

Novel mixed conducting oxides, B-site Bi-doped perovskites were exploited and synthesized. Cubic perovskite structures were formed for BaBi0.2COyFe0.8-yO3-delta (y less than or equal to 0.4) and BaBixCo0.2Fe0.8-xP3-delta (x=0.1-0.5) The materials exhibited considerable high oxygen permeability at high temperature. The oxygen permeation flux of BaBi0.2Co0.35Fe0.45O3-delta membrane reached about 0.77 x 10(-6) mol/cm(2) s under an air/helium oxygen partial pressure gradient at 900 degrees C, which was much higher than that of other bismuth-contained mixed conducting membranes. The permeation fluxes of the materials increased with the increase of cobalt content, but no apparent simple relationship was found with the bismuth content. The materials also demonstrated excellent reversibility of oxygen adsorption and desorption. Stable time-related oxygen permeation fluxes were found for BaBi0.2CO0.35Fe0.45O3-delta and BaBi0.3Co0.2Fe0.5O3-delta a membranes at 875 degrees C.

Performance of a mixed-conducting ceramic membrane reactor with high oxygen permeability for methane conversion

A mixed-conducting perovskite-type Ba0.5Sr0.5Co0.8Fe0.2O3-delta (BSCFO) ceramic membrane reactor with high oxygen permeability was applied for the activation of methane. The membrane reactor has intrinsic catalytic activities for methane conversion to ethane and ethylene. C-2 selectivity up to 40-70% was achieved, albeit that conversion rate were low, typically 0.5-3.5% at 800-900 degreesC with a 50% helium diluted methane inlet stream at a flow rate of 34 ml/min. Large amount of unreacted molecular oxygen was detected in the eluted gas and the oxygen permeation flux improved only slightly compared with that under non-reactive air/He experiments. The partial oxidation of methane to syngas in a BSCFO membrane reactor was also performed by packing LiLaNiO/gamma -Al2O3 with 10% Ni loading as the catalyst. At the initial stage, oxygen permeation flux, methane conversion and CO selectivity were closely related with the state of the catalyst. Less than 21 h was needed for the oxygen permeation flux to reach its steady state. 98.5% CH4 conversion, 93.0% CO selectivity and 10.45 ml/cm(2) min oxygen permeation flux were achieved under steady state at 850 degreesC. Methane conversion and oxygen permeation flux increased with increasing temperature, No fracture of the membrane reactor was observed during syngas production. However, H-2-TPR investigation demonstrated that the BSCFO was unstable under reducing atmosphere, yet the material was found to have excellent phase reversibility. A membrane reactor made from BSCFO was successfully operated for the POM reaction at 875 degreesC for more than 500h without failure, with a stable oxygen permeation flux of about 11.5 ml/cm(2) min. (C) 2001 Elsevier Science B.V. All rights reserved.

Cluster-assistant generation of multiply charged atomic ions in nanosecond laser ionization of seeded methyl iodide beam

The photoionization of methyl iodide beam seeded in argon and helium is studied by time-of-flight mass spectrometry using a 25 ns, 532 nm Nd-YAG laser with intensities in the range of 2 x 10(10)-2 x 10(11) W/cm(2). Multiply charged ions Of Iq+ (q = 2-3) and C2+ with tens of eV kinetic energies have been observed when laser interacts with the middle part of the pulsed molecular beam, whose peak profiles are independent on the laser polarization directions. Strong evidences show that these ions are coming from the Coulomb explosion of multiply charged CH3I clusters, and laser induced inverse bremsstrahlung absorption of caged electrons plays a key role in the formation of multiply charged ions. (C) 2004 Elsevier B.V. All rights reserved.