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首页> 外文学位 >Chemistry within the thermally activated boundary layer during APCVD of silicon dioxide from TEOS and ozone using in-situ infrared spectroscopy: Effects of phosphorus and boron on the gas phase chemistry.
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Chemistry within the thermally activated boundary layer during APCVD of silicon dioxide from TEOS and ozone using in-situ infrared spectroscopy: Effects of phosphorus and boron on the gas phase chemistry.

机译：使用原位红外光谱法从TEOS和臭氧进行二氧化硅的APCVD过程中热活化边界层内的化学：磷和硼对气相化学的影响。

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摘要

The deposition of phosphorus and boron doped silicon dioxide films at 450°C was studied in quasi real-time by probing the thermally activated boundary layer region near the growing surface during atmospheric pressure chemical vapor deposition. Quantitative methods are developed for FT-IR (Fourier transform infrared) spectroscopy during ozonation of TEOS (tetraethylorthosilicate), TMPi (trimethylphosphite), TEPi (triethylphosphite), and TMB (trimethylborate). The novel measurement of gaseous alcohols of boron and silicon alkoxides by FT-IR demonstrates the application of a new in-situ methodology which probes the high temperature region within the CVD environment. Upon addition of phosphite dopant sources a two fold reduction is noted in both the isolated ethoxysilanol (3737 cm−1) and isolated methoxyboranol (3705 cm−1) concentrations and leads to an understanding of the radical chain kinetics involving oxidation of phosphites, borates and silicates. Chemical boundary layer difference spectra (CBL-DS) formed by taking the 1:1 difference between FT-IR spectra before and after phosphite dopant addition provides vibrational spectra of ethoxysilanols ((EtO)xSiOH) (3737, 960, 810 cm −1), siloxane (Si-O-Si) (1000–1250 cm−1), and phosphorus oxide (P-O) (1293 cm−1) film growth intermediates. Calculation of the standard deviation spectra from a series of CBL-DS shows that ethoxysilanol groups formed during ozonation are nearly independent of the amount of added phosphorus for gas phase phosphorus concentrations up to 10 mol %. Peroxy radical and phosphite radical reactions that produce phosphoranyl radical intermediates (R′OOP·(OR) 3) during phosphite ozonation largely affect silanol and boranol product formation routes without significantly affecting the organic by-product concentrations. Partial least squares (PLS) Beer's law absorption models are used in the determination of TEOS, ozone and ethoxysilanol levels and yield the reaction stoichiometry between TEOS and ozone at 2:1, as well as the fractional reaction order in TEOS at 1.65(+/−.02). Similarly, the relative change in ethoxysilanol formed versus the amount of residual ozone during reaction was measured at ca. 1:3. A radical chain oxidative process involving direct reaction of ozone and TEOS is implicated in the mechanism of formation of active silanol groups and acetic acid. Subsequent dehydration reactions of silanol functionalities then lead to hydroxylated silica both in the gas phase and on the growing surface.
机译：通过在大气压化学气相沉积过程中探查生长表面附近的热活化边界层区域，实时地研究了磷和硼掺杂的二氧化硅薄膜在450°C的沉积情况。开发了在TEOS（原硅酸四乙酯），TMPi（亚磷酸三甲酯），TEPi（亚磷酸三乙酯）和TMB（硼酸三甲酯）臭氧化过程中进行FT-IR（傅立叶变换红外）光谱的定量方法。 FT-IR对硼和烷氧基硅的气态醇进行的新颖测量证明了一种新的就地方法的应用，该方法可探测CVD环境中的高温区域。添加亚磷酸盐掺杂剂源后，分离的乙氧基硅烷醇（3737 cm -1 ）和分离的甲氧基硼醇（3705 cm）均降低了两倍。 -1 ）的浓度，导致对涉及亚磷酸盐，硼酸盐和硅酸盐氧化的自由基链动力学的理解。通过在添加亚磷酸盐掺杂剂之前和之后的FT-IR光谱之间以1：1的差形成的化学边界层差光谱（CBL-DS）提供了乙氧基硅烷醇（（EtO）xsubSiOH）的振动光谱（3737 ，960、810 cm -1 ），硅氧烷（Si-O-Si）（1000–1250 cm -1 ）和氧化磷（PO）（1293 cm < super> -1 ）薄膜生长中间体。由一系列CBL-DS计算的标准偏差光谱显示，在臭氧化过程中形成的乙氧基硅烷醇基<斜体>几乎与气相磷浓度最高为10 mol％时所添加的磷量无关。在亚磷酸酯臭氧化过程中产生磷烷基自由基中间体（R ' OOP·（OR） 3 ）的过氧自由基和亚磷酸酯自由基反应在很大程度上不会影响硅烷醇和硼醇的形成途径。有机副产物浓度。使用偏最小二乘（PLS）的比尔定律吸收模型确定TEOS，臭氧和乙氧基硅烷醇的水平，并得出TEOS和臭氧之间的化学计量比为2：1，以及TEOS中的分数反应阶数为1.65（+ / -.02）。同样，在反应过程中，测得形成的乙氧基硅烷醇相对于反应中残留臭氧量的相对变化。 1：3涉及臭氧和TEOS直接反应的自由基链氧化过程与活性硅烷醇基和乙酸的形成机理有关。硅烷醇官能团的随后脱水反应随后导致气相和生长表面上的羟基化二氧化硅。

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