Organic Lasing: Correlation between Molecular Structure, Optical and Optoelectronic Properties

학위논문 (박사)-- 서울대학교 대학원 : 화학과, 2013. 2. Frédéric Laquai.In this thesis mainly two alternating indenofluorene-phenanthrene copolymers were investigated with a variety of spectroscopic and optoelectronic experiments. The different experimental techniques allowed to retrieve deeper insights into their unique optical as well as optoelectronic properties. The motivation of the research presented in this work was to correlate their photophysical properties with respect to their application in electrically pumped lasing. This thesis begins with the description of optical properties studied by classical absorption and emission spectroscopy and successively describes an overall picture regarding their excited state dynamics occurring after photoexcitation studied by time-resolved spectroscopy. The different spectroscopic methods do not only allow to elucidate the different optical transitions occurring in this class of materials, but also contribute to a better understanding of exciton dynamics and exciton interaction with respect to the molecular structure as well as aggregation and photooxidation of the polymers. Furthermore, the stimulated emission properties were analyzed by amplified spontaneous emission (ASE) experiments. Especially one of the investigated materials, called BLUE-1, showed outstanding optical properties including a high optical gain, a low threshold for ASE and low optical losses. Apart from the optical experiments, the charge carrier mobility was measured with the time-of-flight technique and a comparably high hole mobility on the order of 1 x 10² cm²/(Vs) was determined for BLUE-1 which makes this material promising for organic lasing. The impact of the high charge carrier mobility in this material class was further analyzed in different optoelectronic devices such as organic LEDs (OLEDs) and organic solar cells.1 introduction 1 2 theoretical basics 5 2.1 Absorption and Emission of Light 5 2.2 Electronic configuration of carbon atoms in molecules 7 2.3 Optical Properties of Organic Molecules 8 2.3.1 Optical transitions in organic molecules 8 2.3.2 Absorption of light in organic molecules 10 2.3.3 Spectral lineshapes in organic molecules 13 2.3.4 Photoluminescence quantum efficiency 14 2.3.5 Intermolecular interactions of molecules 15 2.4 The Gaussian Disorder Model 17 2.5 Lasing in Organic Semiconductors 21 2.6 Organic light emitting diodes 22 3 optical spectroscopy 25 3.1 The class of poly(indenofluorenes) 25 3.1.1 Introduction 25 3.2 Experimental 26 3.2.1 Sample preparation 26 3.2.2 Steady-state spectroscopy 27 3.2.3 Time-resolved spectroscopy 27 3.2.4 Amplified spontaneous emission and lasing 30 3.3 Absorption and emission spectroscopy 32 3.3.1 Quasi steady-state excited state absorption 33 3.4 Time-resolved fluorescence spectroscopy on BLUE-1 and BLUE-2 34 3.4.1 Fluorescence spectroscopy 34 3.4.2 Defect emission 39 3.4.3 The origin of non-monoexponential dynamics in BLUE-1 42 3.4.4 Delayed fluorescence of BLUE-1 47 3.5 Amplified spontaneous emission and lasing 51 3.5.1 Introduction 51 3.5.2 Results and discussion on PIF, BLUE-1 and BLUE-2 53 3.5.3 Lasing characteristics 60 3.5.4 ASE from a PIF-triphenylamine copolymer 63 3.6 Transient absorption spectroscopy on BLUE-1 72 3.7 Summary and conclusions of chapter 3 76 4 the influence of high mobilities in optoelectronic devices 79 4.1 Introduction 79 4.2 Experimental 80 4.2.1 Time-of-flight technique 80 4.2.2 OLED preparation 80 4.2.3 OLED characterization 81 4.2.4 Organic solar cell preparation and characterization 82 4.3 The time-of-flight technique 82 4.4 OLED characterization of different PIF-based copolymers 86 4.4.1 Introduction 86 4.4.2 OLED characteristics of BLUE-1 87 4.4.3 OLED characteristics of BLUE-2 91 4.4.4 Multilayer OLEDs- the impact of hole injection layers 93 4.5 Consequences of results on BLUE-1 for future lasing diodes 98 4.6 Exciton dissociation in a wide bandgap polymer 100 4.6.1 Introduction 100 4.6.2 Optical properties of BLUE-1 blended with PCBM 101 4.6.3 Solar cell performance of BLUE-1:PCBM blends 105 4.7 Summary and conclusions of chapter 4 107 5 conclusions and outlook 109 a appendix a 113 bibliography 123Docto

Atomistic origins of mechanical amorphization of SiO2 using solid-state 29Si NMR and local electronic structures for SiO2 high pressure phases using ab initio calculation

학위논문 (석사)-- 서울대학교 대학원 : 지구환경과학부, 2017. 2. 이성근.Silica (SiO2), the most abundant material on the earth, is a major component of the crust and mantle. Therefore the structure of silica affects the dynamic process of crust or the structural properties of the earth interior. The structure of silica changes not only by pressure-temperature change but also mechanical energy like friction without melting. To understand the properties of interior of rocky planets and the geological process, the detailed understanding of the structure of silica with various conditions is needed. In this study, we performed two major subject related to structure of silica. The first study is about atomistic origin of the mechanical amorphization of silica with an experimental methodology. There have been reported the reduction of fault strength during fault slip, and one of the causes is reported as the formation of the amorphous silica and the silica gel layer on the fault plane. The formation of amorphous silica is due to the frictional energy between the fault surfaces, and the formation of silica gel layer is due to reaction with the water present in the layer or air. In previous, studies on frictional experiments using quartzite rocks, reported the formation of silica and silica gel and also the decrease of friction coefficient, and the observation of the silica gel layer in natural faults has been reported. However, due to the complex structure of amorphous silica and the analytical method limitations, the atomic structure of the amorphized silica and the detailed origin of the mechanical amorphization process have not been clearly identified. In this study, silica was amorphized with mechanical energy by ball mill method, and the resulting amorphous structure was analyzed by high resolution nuclear magnetic resonance (NMR) spectroscopy. The morphology of the amorphized silica and the phases formed by other elements were analyzed using XRD, HR-TEM, and EDS-mapping method. Solid-state nuclear magnetic resonance spectroscopy (NMR) is suitable for the analysis of complex amorphous structures because it yields atomic environments in short range order around specific atoms and provides quantitative information on atomic unit bonding. The 29Si MAS NMR spectra of amorphous silica milled at different rates present that the spectra of samples milled above 600 rpm show a broad amorphous peak over -80 to -120 ppm. These amorphous peaks indicate the presence of Q2 and Q3 structures in the mechanically amorphized silica. The results indicate that the mechanical amorphization of silica occurs only above a certain energy level, and that the amorphization process results in a change in the short range atomic structure and imply the presence of reaction with other elements. This results help to understand the atomic structure of the mechanically amorphized silica and the mechanical amorphization process that occurs without melting in the fault plane. The second study is an electronic structure and detailed origin of spectral feature of O K-edge XRS for crystalline silica using computational computation. Crystalline silica undergoes various phase transition according to pressure-temperature change. Therefore, many studies on the structure of high-pressure phase silica have been reported to understand the internal structure of rocky planets in high temperature and high pressure environment. The most powerful method of in situ high-pressure study for electronic structure is O K-edge x-ray Raman spectroscopy (XRS) using diamond anvil cell and as experimental limitation above ~70 GPa, the computational methods is used to understand the XRS spectrum. However, the detailed relation between spectral feature of O K-edge XRS and structure is still in debate. In this study, we calculated electronic structures and O K-edge XRS spectra for various crystalline silica using ab initio calculation, and proved the origin of O K-edge XRS spectrum. Previous studies have suggested that the origin of the O K-edge XRS spectrum is attributed to the number of Si atoms or the number of O atoms. However, in this study, we have found that the O K-edge XRS spectra of hp-cristobalite with 4-coordination Si, of penta-SiO2 with 5-coordination Si and of stishovite with 6-coordination Si are similar, and O site resolved K-edge XRS spectra the penta-SiO2 revealed that the coordination of atoms does not directly affect the O K-edge XRS spectral feature. These results not only provide an understanding of the electronic structure of high-pressure phase silica, but also provide clear criteria for O K-edge XRS spectral analysis.1. INTRODUCTION 1 2. THEORETICAL BACGROUNDS 3 2.1 NMR TECHNIQUES 3 2.2 BALL MILL METHOD 4 2.3 AB INITIO CALCULATIONS 5 3. ATOMISTIC ORIGINS OF MECHANICAL AMORPHIZATION BY BALL MILL EXPERIMENTS: INSIGHTS FROM SI-29 NUCLEAR MAGNETIC RESONANCE 7 3.1. INTRODUCTION 7 3.2. EXPERIMENTS 9 3.2.1 Sample Preparation and Analysis 9 3.2.2 Planetary Ball Mill 9 3.2.3 NMR Spectroscopy 10 3.2.4 X-ray Diffraction 10 3.3. RESULTS AND DISCUSSION 11 3.3.1. TEM EDS 11 3.3.2. X-ray Diffraction Patterns 11 3.3.3. Si-29 MAS NMR 12 3.4. CONCLUSION 13 REFERENCE 14 4. AB INITIO CALCULATIONS OF LOCAL ELECTRONIC STRUCTURES AND X-RAY RAMAN SCATTERING SPECTRA FOR SIO2 HIGH PRESSURE PHASE 16 4.1 INTRODUCTION 16 4.2 AB INITIO CALCULATIONS 16 4.2.1 Crystal structures 16 4.2.2 Calculation conditions 19 4.2.3 PDOS and O K-edge XRS calculations 20 4.3 RESULTS AND DISCUSSION 21 4.3.1 O K-edge x-ray Raman scattering 21 4.3.2 Correlation between spectrum and crystal structure 22 4.4 CONCLUSION 23 REFERENCE 25 TABLES 29 FIGURE 30 APPENDIX SECTION 42 ABSTRACT IN KOREAN 44Maste

REINTERPRETATION ON DURKEIM'S THEORY OF MORAL EDUCATION

사회적 존재(social being)로서의 인간 파악으로부터 뒤르껭은 도덕성의 근원을 '사회'에서 찾는다. 인간은 사회적 사실과 사회적 정신(집합의식)으로 가득찬 '공동체'내에 태어나게 되며, 이로부터 사회에 의해 권위가 부여된 도덕적 규범과 가치에 감정적으로 그리고 이성적으로 결합하게 된다. 학교교육을 통한 도덕교육의 역활은 바로 이러한 도덕성을 학생 개개인에 내면화시켜 의무의식과 연대의식을 그 사회내에 정착시키는 것이다. 그러나 뒤르껭의 도덕교육론은 그것이 기초로 하고 있는 '사회' 중심적인 논지로 인해 많은 비판을 받아왔다. 인간의 자율성에 대한 제한이나, 규범과 가치에 대한 교화문제 등이 주로 거론되었고, 개인의 자율적 선택을 중시하는 현대 도덕교육론가들은 이러한 뒤르껭의 도덕교육론을 시대에 뒤떨어진 이론이라고 무시하기에 이르렀다. 본 논문은 뒤르껭의 이론에 대한 이와 같은 비판을 수용, 검토한 후, 뒤르껭의 도덕교육론을 그것이 지닌 현대적 시사에 촛점맞추어 재해석하는데 목적을 두었다. 이러한 목적을 위해 뒤르껭의 저서를 통한 문헌연구의 방법을 취하였다. 그 결과 현대의 도덕교육이론에서 거부되었거나 소홀히 되어 왔던 학교규범과 규율을 통한 도덕적 사회화는 '강요'나 '강제'의 부정적 측면만을 지니는 것이 아니라, 그것을 통하여서만이 보다 자율적이고 합리적인 도덕성에로 나갈 수 있는 기반으로서 중요한 도덕적 가치를 지닌다는 점이 부각되었다. 또한 Kant이래로 '도덕성'에서 애타적 감정을 포함한 모든 감정과 성향을 무시한 도덕이론들이 우세하였으나, 뒤르껭은 이와 달리 도덕성의 중심적인 준거로 '사랑' 혹은 '애타심'이라는 도덕적 감정을 드러내어 도덕생활에서 이러한 감정과 성향의 역할을 강조하고 있음이 부각되었다. 뿐만 아니라 뒤르껭이 제시한 도덕적 감정과 성향은 '사리적 차원'과 맞닿아 사회의 구조적 모순이나 부조리에 대한 '도덕적 의식화'에까지 뻗어나감을 알 수 있다. 뒤르껭 도덕교육론에 대한 재해석은 인지주의적 편견에 의해 도덕성을 합리성에 국한시키면서 합리적 이성에 의해 고육가능하다고 보는 현대 도덕교육론의 편협한 인식을 극복, 보완하는데 새로운 시사를 준다.;(이전원문누락) norms and values. And modern moralists who lay stress on the autonomy have gone to disregarding this theory of Durkheim's moral education as an old-fashioned theory. In the present study, an attempt was made to reinterpret the theory of Durkheim's moral education on the focus of its possible modern suggestion, after those critics were admitted and restudied. The method of literature study was taken for the purpose. As the result, it was embossed that moral socialization, through school norms and rules, which mordern moralists have disagreed and neglected, has not the only negative aspects of compelling and forcing, but has important moral value as the possible base of accomplishing autonomous and rations morality. The theories of moral education which ignored every kinds of emotions and characters, including altruistic, have maintained a superior position. On the other hand, Durkheim puts central standards of morality upon 'love' or 'altruism', and underlines this emotion in moral life. These sentiment of 'love' and 'altruism' are connected to social level, and can go to moral conscientization against structural contraction and improperness. Reinterpretation of the theory of Durkheim's moral education gives a new suggestion that Hay overcome and supplement the narrow-minded view of modern moralists who have cognitivistic bias and prefer education by rational reason with limiting morality within rationality.목차 = ⅲ 논문개요 = ⅳ Ⅰ. 서론 = 1 A. 연구의 목적 = 1 B. 연구의 문제 및 제한점 = 3 Ⅱ. 뒤르껭의 도덕교육론 = 6 A. 개인과 사회 = 6 B. 사회적 사실로서의 도덕 = 10 C. 도덕성의 3요소 = 15 D. 도덕교육 = 20 Ⅲ. 뒤르껭의 도덕교육론에 대한 비판 = 26 A. 도덕적 자율성에 관한 비판 = 26 B. 도덕적 사회화에 관한 비판 = 30 C. 환원주의의 오류 = 35 D. 뒤르껭에 대한 반동으로서의 현대 도덕교육이론 = 39 Ⅳ. 뒤르껭의 도덕교육론에 대한 재해석 = 46 A. 필요선으로서의 규범화 = 46 B. 도덕성에서의 도덕적 감정 = 53 Ⅴ. 결론 및 논의 = 65 A. 요약 및 결론 = 65 B. 논의 = 68 참고문헌 = 71 ABSTRACT = 7

Intermediate and long term results for extracardiac donduit repair between right ventricle and pulmonary artery in congenital cardiac defects.

의학과/석사[한글] 선천성 심장 질환 교정 수술에서 우심실과 폐동맥을 도관(conduit)으로 연결해주는 Rastelli 술식은 술후 임상증상을 현저히 호전시킬 수 있지만, 환아의 성장이나 도관의 협착 으로 재수술이 불가피하다는 약점을 안고 있다. 저자 등은 1978년 부터 1993년 10월까지 연세대학교 의과대학 세브란스 병원 흉부외과에 입원한 선천성 심장질환자 중 우심실과 폐동맥 사이에 도관을 연결해 주는 Rastelli 술식을 이용하여 교정수술한 총 47례에 대해 평균 76.1 ± 51.3 개월간 추적 관찰하여 Rastelli 수술후 장기적인 성적에 미치는 인자를 알아보고자 본 연구를 하여 다음과 같은 결과를 얻었다. 1) 수술시 사용한 도관은 판막이 있는 도관을 사용한 경우가 30례(63.8%), 판막이 없는 도관을 사용한 경우가 17례(36.2%)였다. 수술후 47례중 8례가 수술사망(17%) 하였는데 수술사망을 도관 종류별로 보면 판막이 있는 도관을 사용한 경우가 5례(16.7%), 판막이 없는 도관을 사용한 경우가 3례(17.6%)로 양군간에 통계학적으로 유의한 차이는 없었다. 수술시 사용한 판막의 크기는 체표 면적과 통계적으로 유의한 상관 관계가 있었다. (Y=3.86X + 14.6, R=0.55, p<0.01) 2) 추적기간 동안 10례(30.3%)에서 도관 재치환 수술을 받았다. 도관 재치환술을 시행한 경우를 도관 종류별로 보면 lonescu-Shiley 판막도관이 3례중 1례(33%), Carpentier-Edwards 판막도관이 13례중 4례(30.8%), Hancock 판막도관이 5례중 4례(80%), 판막없는 도관을 사용한 환자 11례중 1례(9.1%)가 재수술하였다. Kaplan-Meier의 누적한계 생존 분석에 의한 수술후 median 재수술 회피 기간은 판막 있는 도관이 110개월, 판막없는 도관이 79개월 이었으나 통계적으로 유의한 차이는 없었다. 판막도관의 종류별 median 재수술 회피 기간은 lonescu-Shiley 판막도관이 110개월, Csrpentier-Edwards 판막도관이 112개월, Hancock 판막도관이 102개월로 이들간에도 통계적으로 유의한 차이가 없었다. 3) 재수술을 하지 않은 23례 모든 환자들은 현지 운동능력 제한 없이 건강하게 지내고 있으며 (New York Heart Association functional classification: class I), 이들 환자 23례중 10명에 대해 심장 Doppler 초음파 검사 결과 우심실과 폐동맥간의 압력차는 20 ± 11 mmHg(0mmHg - 40 mmHg) 였으나, 재수술한 환자의 재수술전 우심실과 폐동맥간의 압력차는 92 ± 9 mmHg(80mmHg - 110mmHg)로 매우 높았다. 4) 인조혈관 및 판막 협착으로 인해 재수술한 10례중 Gore-tex 18mm 인조 혈관으로 재치환술을 시행한 경우가 3례, Vascutec 20mm 가 3례, 기존의 인조판막 혈관에 판막을 제거하고 첨포확장을 해 준 경우가 2례, 첨포 확장시 monocusp 판막으로 폐동맥 판막을 만들어준 경우가 1례, 자신의 폐동맥이 발달하여 자신의 폐동맥에 첨포 확장술을 시행한 경우가 1례였다. 이중 재수술전 심내막염이 있었던 2례가 패혈증으로 사망하였다. 그외 8례에서는 재수술 후 2개월에서 89개월(평균 32.7 ± 33.9)이 지난 현재 운동 능력 제한없이 건강하게 지내고 있다. 5) 전체 퇴원 환자의 5년(n=23), 7년(n=19), 10년(n=4) 재수술 회피율은 각각 96%, 91%, 29%였으며 5년(n=23), 7년(n=20), 10턴(n=5) 생존율은 각각 82%, 82%, 71%였다. 이상의 결과로, 선천성 심기형 환자에서 Rastelli 수술을 이용하여 교정한 결과 비교적 좋은 성적을 보여 주고 있으며, 향후 판막 도관 및 도관의 선택에 대한 장기적인 추적 관찰을 하는것이 필요할 것으로 생각된다. Intermediate and long term results for extracardiac conduit repair between right ventricle and pulmonary artery in congenital cardiac defects Hoon Kim Department of Medical Science The Graduate School, Yonsei University (Directed by Professor Bum Koo Cho) Rastelli operation which connects right ventricle to pulmonary artery with artificial graft in correction of congenital heart disease, can improve clinical manifestations, but it needs inevitable reoperation due to stenosis of artificial graft with the develoment of patients. The purpose of this study was to evaluate factors which could influence the long term results after Rastelli operation. We have the fellowing results from 47 patients with Rastelli operation who had been performed for Rastelli operation between 1978 are october. 1993. The patients had been followed up for 76.1 ± 51.3 months. 1) The number of artificial grafts with valve used in operation are 30 cases (63.8%), and those without valve are 17 cases(36.2%). There were 8 surgical deaths. Among them, valved conduit was used in 5 patients and nonvalved conduit was used in 3 patients. However there is no statiscally significant difference. There were good linear correlations between the body surface area(X) and the size of used conduit(Y)(Y3=86X + 14.6, R=0.55, P<0.01). 2) Ten patients underwent re-replacement of artificial graft: lonescu-Shiley valved conduit: one case(33%), Carpentier-Edward valved conduit: 4 cases. Haycock valved conduit: 4 cases(80%). and artificial graft without valve: one case(9.1%). Median duration of reoperation-free interval is 110 months in the patients with valved conduit and is 79 months in patients with non-valved conduit. However, there is no statistically significant difference between the two groups. Median duration of the reoperation since primary operation is 110 months for Ionescu-Shiley, 112 months for Carpentier-Edward, 102 months for Hancock valved oconduit. There were no statistically difference between them. 3) Patients who did not have reoperation are well without difficulty of physical activity. (New York Heart Association functional classification. class Ⅰ). Ten randomly selected patients underwent a doppler echocardiography and the pressure gradient between the right ventricle and pulmonary artery is 20 ± 11 mmHg, and 92 ± 9 mmHg respectively for the patlents who had have operation. 4) Among 10 cases which had operations due to stenosis of artificial vessel and valve. 3 cases had replacement operation with patch enlargement fo previous valved conduit after removal of the valved one case with monocusp valve with the patch enlargement, and 1 case with patch enlargement. Eight cases are doing well without physical problems during 2 months to 89 months(mean 32.7 ± 33.9 mouth) after reoperation and the remaining 2 cases died of sepsis by endocarditis which occurred before the reoperation. 5) The percentage of reoperation-free among the patients at 5 years, 7 years. ard 10 years is 96%, 91%, 29% respectively, and the survival rata shows 82%, 82% 71% respectively. In conclusion. the above findings show good results for congenital heart dlsease patients who had been corrected with Rastelli operation. However, it is suggested that long term follow up for selection of conduit is necessary. [영문] Rastelli operation which connects right ventricle to pulmonary artery with artificial graft in correction of congenital heart disease, can improve clinical manifestations, but it needs inevitable reoperation due to stenosis of artificial graft with the develoment of patients. The purpose of this study was to evaluate factors which could influence the long term results after Rastelli operation. We have the fellowing results from 47 patients with Rastelli operation who had been performed for Rastelli operation between 1978 are october. 1993. The patients had been followed up for 76.1 ± 51.3 months. 1) The number of artificial grafts with valve used in operation are 30 cases (63.8%), and those without valve are 17 cases(36.2%). There were 8 surgical deaths. Among them, valved conduit was used in 5 patients and nonvalved conduit was used in 3 patients. However there is no statiscally significant difference. There were good linear correlations between the body surface area(X) and the size of used conduit(Y)(Y3=86X + 14.6, R=0.55, P<0.01). 2) Ten patients underwent re-replacement of artificial graft: lonescu-Shiley valved conduit: one case(33%), Carpentier-Edward valved conduit: 4 cases. Haycock valved conduit: 4 cases(80%). and artificial graft without valve: one case(9.1%). Median duration of reoperation-free interval is 110 months in the patients with valved conduit and is 79 months in patients with non-valved conduit. However, there is no statistically significant difference between the two groups. Median duration of the reoperation since primary operation is 110 months for Ionescu-Shiley, 112 months for Carpentier-Edward, 102 months for Hancock valved oconduit. There were no statistically difference between them. 3) Patients who did not have reoperation are well without difficulty of physical activity. (New York Heart Association functional classification. class Ⅰ). Ten randomly selected patients underwent a doppler echocardiography and the pressure gradient between the right ventricle and pulmonary artery is 20 ± 11 mmHg, and 92 ± 9 mmHg respectively for the patlents who had have operation. 4) Among 10 cases which had operations due to stenosis of artificial vessel and valve. 3 cases had replacement operation with patch enlargement fo previous valved conduit after removal of the valved one case with monocusp valve with the patch enlargement, and 1 case with patch enlargement. Eight cases are doing well without physical problems during 2 months to 89 months(mean 32.7 ± 33.9 mouth) after reoperation and the remaining 2 cases died of sepsis by endocarditis which occurred before the reoperation. 5) The percentage of reoperation-free among the patients at 5 years, 7 years. ard 10 years is 96%, 91%, 29% respectively, and the survival rata shows 82%, 82% 71% respectively. In conclusion. the above findings show good results for congenital heart dlsease patients who had been corrected with Rastelli operation. However, it is suggested that long term follow up for selection of conduit is necessary.restrictio

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