臺灣博碩士論文加值系統

此篇論文敘述利用紅外線吸收光譜(IR absorption)及表面拉曼散射(surface Raman scattering)技術來研究半導體氫化表面的表面振動動力學。經由分析光譜中的 XH/D (X=C, Si, 及 Ge) 在不同溫度下伸展振動(stretching)譜帶形狀的變化關係，研究其振動能階的能量鬆弛(energy relaxation)及去相位(dephasing)的動力學。所測定得的鑽石表面CD振動能緩解時間約為 ~3x10^-13 秒，此為所有半導體和絕緣體表面之吸附分子系統中最短者。此超快能量鬆弛速率，源自於強烈的聲子-聲子間耦合機制及其在鑽石表面的能量鬆弛過程為雙聲子(two-phonon)釋放程序。拉曼光譜技術被應用於單晶矽及鍺氫化表面的測量, 以研究其振動去相位動力學。我們利用單式去相位模型(single-mode dephasing model)分析振動光譜的頻率移動及其線寬變化，獲得交換頻率(exchange-mode frequencies)及其耦合強度(coupling strength)。我們經由比較在矽 (100) 氫化表面的頻率及時間域上的實驗結果，而推論出多式去相位模型(multi-mode dephasing model)可以解釋兩者間之歧異。並且我們發現在 X(100) 面的XH伸展振動頻率的交換頻率與彎曲振動(bending)頻率相吻合。另一方面，X(111) 氫化表面的交換頻率則位於晶體聲子投射於表面之頻譜(projected bulk phonon spectrum)中。此種去相位交換頻率與表面結構之相依性發現與晶格表面結構鬆弛(structure relaxation)及其對應之對稱性變化有關聯。此結果也由半導體氘化表面實驗結果進一步確認。根據吸附分子表面的對稱性，我們得以分析出其在表面聲子光譜中的交換頻率。並且利用高靈敏的拉曼光譜技術, 我們得以分析由濺射(sputtering)及退火(annealing)所製備的良序(well-ordered) Ge(111) 氫化表面的特性。

The vibrational dynamics at hydrogenated semiconductor surfaces is investigated by infrared absorption spectroscopy and surface Raman scattering. The temperature dependence of the spectral profiles has been analyzed to reveal vibrational energy relaxation and dephasing dynamics of XH/D (X = C, Si, and Ge) stretchings on diamond, silicon and germanium surfaces. The energy relaxation time of CD stretching on diamond surface was determined to be ~3x10^-13 second. This is the shortest among all of the semiconductor and insulator surfaces. This ultrafast decay rate is originated from the two-phonon emission process during the relaxation as well as the strong phonon-phonon coupling mechanism in diamond. Raman scattering has been performed on single crystal hydrogenated silicon and germanium surfaces to investigate their vibrational dephasing dynamics. Based on the single-mode dephasing model, the frequency shift and line broadening were analyzed to extract exchange mode frequencies and coupling strengths. The comparison between the frequency- and time-domain results on hydrogenated Si(100) surfaces led us to propose a multi-mode dephasing model to rationalize its inconsistency. Furthermore, the exchange mode of the XH stretching on X(100) surfaces was found to match with its bending frequency. The corresponding ones for X(111) surfaces, on the other hand, are located within the projected bulk phonon spectrum. This surface dependence of the exchange mode in surface vibrational dephasing dynamics was found to correlate with the structural relaxation and its associated symmetry variation at surfaces. Its has been further confirmed by the experiments performed on deuterated semiconductor surfaces. We have identified the exchange modes in the surface phonon spectra according to their symmetry properties. With high-sensitivity Raman spectroscopy, we also characterized a well-ordered hydrogenated Ge(111) surface prepared by sputtering and annealing.

COVER
Abstract
Acknowledgment
Table of contents
List of Figures
List of Tables
Chapter I Introduction
References
Chapter 2 Surfaces of semiconductors
2.1 Atomic structure of surfaces
2.1.1 Bare and hydrogenated semiconductor surfaces
2.1.1.1 Diamond
2.1.1.2 Silicon
2.1.1.3 Germanium
2.1.2 Reciprocal lattice and surface Brillouin zone
2.2 Vibrations at surfaces
2.2.1 Surface phonons
2.2.2 Vibrations of adsorbed surfaces
2.2.2.1 Si(lll)-(lxl):HandC(lll)-(lxl):H
2.2.2.2 Si(100)-(2xl):H and C(100)-(2xl):H
2.3 Hydrogenation of semiconductor surfaces with atomic hydrogen
2.3.1 Diamond
2.3.2 Silicon
2.3.3 Germanium
References
Chapter 3 Experimental methodologies
3.1 Infrared absorption spectoscopy
3.2 Raman spectroscopy
3.3 Electromagnetic fields at surfces
3.4 Deconvolution
3.5 Comparison between IR and Raman spectroscopy
References
Chapter 4 Theory of surface vibrational dynamics
4.1 Vibrational dephasing
4.2 Vibrational energy reaxation
4.3 Quantum vibron-phonon coupling and symmetry considerations
References
Chapter 5 Experiment
5.1 Infrared measurements
5.2 Raman measurements
References
Chapter 6 Hydrogenated diamond surfaces
6.1 Sample preparation and spectrum assignment
6.2 Vibrational dephasing and energy relaxation
References
Chapter 7 Hydrogenated silicon and germanium surfaces
7.1 Vibrational dephasing dynamics
7.1.1 Multi-mode dephasing model
7.1.2 Structural dependence of vibrational dephasing dynamics
7.1.3 Dependence on surface symmetry
7.1.4 Comparison with CO/metal systems
7.1.5 The effect of thermal expansion to frequency shift
7.1.6 Symmetry rules applied to vibrational relaxation dynamics
7.2 Characterization ofGe(l I l)-(lxl):H
7.2.1 LEED studies
7.2.2 Vibrational spectroscopic measurements
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