臺灣博碩士論文加值系統

本論文利用超快瞬態吸收光譜研究了二維(2D)和準二維(quais-2D)錫鈣鈦礦的激子和自由載流子結合動力學。我們利用線性丁基銨（BA）陽離子為阻擋層(barriers)來製造二維((BA)2FAn-1SnnI3n+1)鈣鈦礦，其中n = 1、2、5以及10。使用低角度X射線衍射圖(low angle XRD)，GWIAX，SEM，吸收，光致發光（PL）測量來確認鈣鈦礦薄膜中二維結構的形成。 從n = 1和n =2的薄膜吸收光譜和PL光譜，由於量子侷限效應而顯示出尖銳的激子峰。然而，n = 5和n = 10樣品的吸收光譜和PL光譜未顯示任何量子侷限效應。此外，通過擬合所有樣品的吸收帶邊緣，發現隨著量子阱厚度從n ＝ 1增加到n ＝ 10，能帶(band gap)和激子結合能(exction binding energy)都變小。從PL衰減測量結果顯示，隨著量子阱厚度的增加，樣品的生命期變得更長。降低的結合能和增加的樣品生命期結果證明了，隨著量子阱厚度的增加，量子阱的自由載流子性質增強。我們也利用超快瞬態吸收光譜測量來這些樣品，以進一步了解樣品的性質以及激子和自由載流子在其光學性質中的作用。 n = 1和n = 2樣品的TA光譜類似於具有激子性質的量子阱的TA光譜，而n = 5和n = 10的TA光譜類似於3D FASnI3。因此，本文進一步討論了激子(exctions)和自由載體(free carriers)的作用以及他們的重組途徑的機制。

In this thesis, excitonic and free carrier recombination dynamics of two dimensional and quais two dimensional tin perovskites are investigated using ultrafast transient absorption spectroscopy. Linear butylammonium (BA) cations were used as barrier layers during the fabrication of two dimensional and quasi two dimensional formamidinium tin iodide (2D-FASnI3) perovsite structures of the type (BA)2FAn-1SnnI3n+1 where n=1, 2, 5, and 10. The formation of two dimensional structures in the fabricated perovskite thin films were confirmed using low-angle X-ray diffractograms, grazing incidence wide angle X-ray scattering, SEM, absorption, photoluminescence (PL) measurements. The absorption and PL spectra of n=1, and 2 thin film samples show sharp excitonic peaks due to quantum confinement effects. The absorption and PL spectra of n=5 and n=10 samples do not show any quantum confinements effects. Further, by fitting the absorption band edges of all the samples it is found that as the quantum well thickness increases from n=1 to n=10 both the bandgap and exciton binding enegries become smaller. The PL decay measurements show that the lifetime of the emissive species becomes longer as the thickness of quantum well increases. The decreased binding energy and increased lifetime of sample indicate that free carrier nature of the quantum wells enhances as the quantum well thickness increases. Ultrfast transient absorption spectroscopic measurments were carried out on these quantum wells samples to further understand the nature of the samples and roles of exciton and free carriers in their optical properties. The TA spectra of n=1 and 2 samples resemble that of quantum wells with excitonic nature whereas n=5 and n=10 resemble that of a 3D FASnI3. Thus this thesis further discusses the roles of excitons and free carriers and the mechanisms of recombination pathways of these quantum well samples.

摘要 i
Abstract iii
致謝 v
Table of Content vi
List of Figures ix
List of Tables xiii
Chapter 1 Introduction 1
Chapter 2 Literature Survey 3
2-1 Perovskite Solar Cell 3
2-1-1 Development of Perovskite Solar Cell 4
2-1-2 The Two-Dimensional Perovskite 12
2-1-3 The Advantage and Disadvantage of Perovskites 15
2-2 Motivation 17
Chapter 3 Experimental Method and Principle 19
3-2 Time-Resolved Femtosecond Transient Absorption Spectroscopy 22
3-2-1 Pump-Probe Method 22
3-2-2 Experimental system 25
3-2-2-1 Femtosecond Laser System 25
3-2-2-2 Optical Parameter Amplifier 27
3-2-3 The Transient Absorption System Set up 29
3-3 Time-resolved Fluorescence Spectroscopy 30
3-3-1 Time-correlated Single Photon Counting [1] 31
3-3-1-1 Principle 31
3-3-1-2 Instrument 33
Chapter 4 Transient Absorption study of Tin Perovskite Quantum Well 40
4-1 Introduction 40
4-2 Experimental Process 41
4-2-1 Sample Preparation 41
4-2-1-1 UV-visible Absorption Spectra 42
4-2-1-2 Fluorescence Spectra 42
4-2-1-3 The Measurement of Time-resolved Fluorescence Spectroscopy 43
4-2-1-4 The Morphology Measurement 43
4-3 Results and Dicussion 44
4-3-1 The Morphology Characterization 44
4-3-2-1 State-Steady Measurement 47
4-3-2-3 Time-resolved Spectroscopy 50
4-3-2-3 Transient Absorption Spectroscopy 52
4-4 Conclusion 58
 

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