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系統識別號 U0002-0608201416121500
中文論文名稱 有機高分子Ph-LPPP在高壓下的光學與電子特性
英文論文名稱 The Optical and Electronic Properties of Conjugated Polymer(ladder-type poly para-phenylene) Ph-LPPP under Hydrostatic Pressures
校院名稱 淡江大學
系所名稱(中) 物理學系博士班
系所名稱(英) Department of Physics
學年度 102
學期 2
出版年 103
研究生中文姓名 許喆閎
研究生英文姓名 Che-Hung Hsu
電子信箱 694180158@s94.tku.edu.tw
學號 897210026
學位類別 博士
語文別 英文
口試日期 2014-07-17
論文頁數 87頁
口試委員 指導教授-楊淑君
委員-唐建堯
委員-鄭振益
委員-張淑美
委員-高柏青
中文關鍵字 螢光光譜  吸收光譜  光調制光譜  拉曼光譜  靜水壓  共軛高分子 
英文關鍵字 PL  absorption  photo-modulaion spectrum  Raman scattering  hydrostatic pressure  conjugated polymer 
學科別分類
中文摘要 本論文主要是測量掺雜金屬的階梯型有機共軛高分子(ladder type poly para-phenylene)Ph-LPPP粉末態與薄膜態的樣品在不同壓力下的吸收光譜、螢光光譜、光調制光譜和拉曼光譜等光學特性。在壓力增加的情況下,我們可以看到所有光譜譜線有紅位移和變寬的現象。共軛高分子的pi-pi*電子特性使得分子鍵間距因壓力增加而縮短,導致能隙變小,因而使光譜有紅位移。除此之外,分子的聚集作用造成電子雲層相互干擾,使得分子鏈間的交互作用增強,因此所有的譜線變寬。三重態激子和光漂白的生命期也被描述。由所有的光譜特性可發現壓力會造成分子的平面化,此效應可增加分子間的交互作用,因此增長其有效共軛長度,使得三重態未定域化。透過這份研究,我們可以了解Ph-LPPP的單重態、三重態、震動特性和其有效共軛長度之間的關係。
英文摘要 The optical properties, such as absorption, photoluminescence, photo-modulation and Raman scattering spectra, of blue light-emitting organic conjugated polymer, ladder-type poly(para-phenylene) (Ph-LPPP) with trace-concentration of metallic impurities, both in the powder form and in film form under various pressures were measured. Red-shift and broadening effects were found in all spectra with increasing pressure. Due to the pi-pi* character of conjugated polymers, the distance between bonds decreasing under pressure made the energy gap smaller resulting in the red shifts of spectra. Besides, the aggregates would affect the interfering between electronic clouds, such that the inter-chain coupling was stronger and resulted in the broadening of all spectra of polymer. The lifetimes of the triplet excitions and the photo-bleaching were also reported. The planarization of Ph-LPPP under pressure was discovered through all spectral features, which increases the intermolecular interaction, therefore, the effective conjugated length of the polymer, and causes the delocalization of triplet state. Through this work, we could understand the relationship between the singlet and triplet transitions, as well as the vibronic properties, of Ph-LPPP and its effective conjugated length.
論文目次 CONTENTS
ACKNOWLEDGEMENTS i
ABSTRACT iii
LIST OF TABLES viii
LIST OF FIGURES ix

1 INTRODUCTION 1
1-1 Prologue 1
1-2 Introduction to Conjugated Polymer Development 2
1-3 Introduction to Polymer 4
1-3.1 The Fundamental Principles of Conjugated Polymers 5

2 FUNDAMENTAL OF THEORY 9
2-1 Motivation for Using Optical Spectroscopy 9
2-2 Absorption Spectra 10
2-2.1 Optical Absorption in Semiconductor 10
2-2.2 Absorptance 11
2-2.3 Wavelength Dependence of α 13
2-3 Photoluminescence Spectra 13
2-3.1 The Theory of Photoluminescenc 13
2-3.2 Organic semiconductors light-emitting and electronic energy band 14
2-3.3 The Optical Properties of Polymer 16
2-4 Photo-Modulation Spectra 18
2-5 Raman Scattering Spectra 19
2-5.1 The Theory of Raman Scattering 22

3 EXPERIMENTS AND INSTRUMENTATION 27
3-1 The Diamond Anvil Cell 27
3-1.1 The Calibration of Faces of Diamond 29
3-1.2 Gasket Production 31
3-1.3 Pressure Calibration 32
3-2 The Setup of Experiments 35
3-2.1 The Experimental Setup for Absorption Spectrum 35
3-2.2 The Experimental Setup for Photo-Modulation Spectrum 35
3-2.3 The Experimental Setup for Raman Scattering 37

4 INTRODUCTION TO SAMPLE 38
4-1 Properties of PPP 38
4-2 Properties and Structure of LPPP 40
4-3 Synthesis and Properties of Ph-LPPP 42
4-4 Loading Polymer Films 44

5 RESULTS AND DISCUSSION 46
5-1 Early Work in Ph-LPPP 46
5-2 Absorption and Photoluminescence 52
5-3 Photo-Modulation spectroscopy 56
5-4 Raman Spectroscopy 66
5-4.1 Raman Spectrum of Ph-LPPP at Atmospheric Pressure .67
5-4.2 Raman Spectra of Ph-LPPP Under High Pressure 71

6 CONCLUSION 75
REFERENCES 77










LIST OF TABLES
Table5.1: The shift rates of PL and absorption peaks under pressure 50
Table5.2: The triplet-triplet absorption maxima energies for conjugated polymers 58
Table5.3: The shift rates of TT and PB under pressure 62
Table5.4: The peak positions of three vibration peaks in backbone of Ph-LPPP and Me-LPPP 70
Table5.5: The shift rates of the peaks at 1600、1564 cm-1 and 1311 cm-1 with pressures 72

LIST OF FIGURES
Figure 1-1: Structure of ladder-type poly(para-phenylene) with a phenyl side chain at R2 1
Figure 1-2: The light-emitting layer of Alq3 nano-film 3
Figure 1-3: Schematic diagram of LED structure 4
Figure 1-4: Chemical structure of common conjugated polymer 4
Figure 1-5:The shape of the σ-bonds 6
Figure 1-6:The diagrams of molecular orbitals and energy level for side-by-side combination between neighboring π orbitals. 7
Figure 2-1: The process of optical absorption in a semiconductor 11
Figure 2-2: The status of shinning light on a sample 12
Figure 2-3: The theory of electroluminescence 15
Figure 2-4: The theory of photoluminescence 15
Figure 2-5: Scheme of electronic states in conjugated molecules 17
Figure 2-6: The quantum energy transitions for Rayleigh and Raman Scattering 21
Figure 2-7: The spectrum of Rayleigh and Raman Scattering 21
Figure 3-1: Sectional view of the Piston Cylinder type DAC 27
Figure 3-2: Schematics diagram of the core of a diamond anvil cell 28
Figure 3-3: The graphic of AgI of concentric circles in 1bar and 100kbar 30
Figure 3-4: The graphic of AgI of non-parallel diamond faces 30
Figure 3-5: Schematic diagram of the prepressing notch of gasket 31
Figure 3-6: Schematic diagram of the Electric Discharge Machine (EDM) 32
Figure 3-7: Schematic diagram of the energy level and the fluorescence of ruby 34
Figure 3-8: The fluorescence spectra of ruby in various pressure 34
Figure 3-9: The experimental setup for absorption measurements 35
Figure 3-10: The schematic experimental setup for photo-modulation spectrum 36
Figure 3-11: The experimental setup for Raman scattering measurements 37
Figure 4-1: Synthesis of soluble PPP (R=alkyl) 39
Figure 4-2: The chemical structure of LPPP 41
Figure 4-3: The synthetic scheme for the formation of ladder-type poly (para-phenylene) Ph-LPPP 42
Figure 5-1: PL spectra of Ph-LPPP powder and film at various pressures at 300K 47
Figure 5-2: The PL spectra of Ph-LPPP film with different thickness 48
Figure 5-3: Pressure dependence of the PL peak position in Ph-LPPP powder and Ph-LPPP film at 300K 50
Figure 5-4: FWHM of the PL peaks of Ph-LPPP powder and film 51
Figure 5-5: PL and Absorbance of Ph-LPPP film at 1bar at room temperature 53
Figure 5-6: The Absorption of the Ph-LPPP film at various pressures at 300K 54
Figure 5-7: Pressure dependence of absorption peaks position in Ph-LPPP film at 300K 55
Figure 5-8: The PL spectra of Ph-LPPP film at different temperature at 1bar 56
Figure 5-9: The photo-modulation spectrum of a Ph-LPPP film in vacuum at 13K. Inset figure provides the PL of Ph-LPPP film in vacuum at 13K. 57
Figure 5-10: The triplet-triplet absorption of a Ph-LPPP film in vacuum at 13K in the pressure range 1.1kbar to 51kbar 59
Figure 5-11: The photobleaching of the fundamental absorption of a Ph-LPPP film in vacuum at 13K in the pressure range 1.1kbar to 51kbar 60
Figure 5-12: The peak positions of TT of Ph-LPPP film as functions of pressure 61
Figure 5-13: The peak positions of PB of Ph-LPPP film as functions of pressure 62
Figure 5-14: The PB and TT at various chopper-wheel frequencies 65
Figure 5-15: The lifetimes of the PB and TT at various chopper-wheel frequencies 65
Figure 5-16: Raman spectrum of Ph-LPPP at atmospheric pressure and 300K 67
Figure 5-17: Molecular Structure and bonding relative Raman spectrum of Ph-LPPP 69
Figure 5-18: Raman spectra of Ph-LPPP at various pressures at 300K 71
Figure 5-19: The rate of I1169/I1311 of Ph-LPPP with pressure up to 20 kbar 74
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