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請用此 Handle URI 來引用此文件: http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/97763
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dc.contributor.advisor陳永芳zh_TW
dc.contributor.advisorYang-Fang Chenen
dc.contributor.author蔡湋成zh_TW
dc.contributor.authorWEI-CHENG TSAIen
dc.date.accessioned2025-07-16T16:11:20Z-
dc.date.available2025-07-17-
dc.date.copyright2025-07-16-
dc.date.issued2025-
dc.date.submitted2025-07-08-
dc.identifier.citation[1] D. C. Leitao, F. J. F. van Riel, M. Rasly, P. D. R. Araujo, M. Salvador, E. Paz, and B. Koopmans, "Enhanced performance and functionality in spintronic sensors," npj Spintron. 2, 54 (2024).
[2] X. Zhao, Y. Yao, Y. Sun, and C. Liu, "Circle polarization shift keying with direct detection for free-space optical communication," J. Opt. Commun. Netw. 1, 307–312 (2009).
[3] B. Y. Toh, R. Cahill, and V. F. Fusco, "Understanding and measuring circular polarization," IEEE Trans. Educ. 46, 313–318 (2003).
[4] X. Zhang, L. Li, Y. Chen, C. Valenzuela, Y. Liu, Y. Yang, Y. Feng, L. Wang, and W. Feng, "Mechanically tunable circularly polarized luminescence of liquid crystal-templated chiral perovskite quantum dots," Angew. Chem. Int. Ed. 63, e202404202 (2024).
[5] Z. Li, Q. Fan, Z. Ye, C. Wu, Z. Wang, and Y. Yin, "A magnetic assembly approach to chiral superstructures," Science 380, 1384–1390 (2023).
[6] J. Lu, B. Shao, R.-W. Huang, L. Gutiérrez-Arzaluz, S. Chen, Z. Han, J. Yin, H. Zhu, S. Dayneko, M. N. Hedhili, X. Song, P. Yuan, C. Dong, R. Zhou, M. I. Saidaminov, S.-Q. Zang, O. F. Mohammed, and O. M. Bakr, "High-efficiency circularly polarized light-emitting diodes based on chiral metal nanoclusters," J. Am. Chem. Soc. 146, 4144–4152 (2024).
[7] W. B. Sparks, J. Hough, T. A. Germer, W. Martin et al., "Detection of circular polarization in light scattered from photosynthetic microbes," Proc. Natl. Acad. Sci. U.S.A. 106, 7816–7821 (2009).
[8] D. Zhang, T. Huang, and L. Duan, "Emerging self-emissive technologies for flexible displays," Adv. Mater. 32, 1902391 (2020).
[9] X. Shi, Y. Zuo, P. Zhai, J. Shen, Y. Yang, Z. Gao, M. Liao, J. Wu, J. Wang, X. Xu, Q. Tong, B. Zhang, B. Wang, X. Sun, L. Zhang, Q. Pei, D. Jin, P. Chen, and H. Peng, "Large-area display textiles integrated with functional systems," Nature 591, 240–245 (2021).
[10] R. Su, S. H. Park, X. Ouyang, S. I. Ahn, and M. C. McAlpine, "3D-printed flexible organic light-emitting diode displays," Sci. Adv. 8, eabl8798 (2022).
[11] Y. Deng, M. Wang, Y. Zhuang, S. Liu, W. Huang, and Q. Zhao, "Circularly polarized luminescence from organic micro-/nano-structures," Light Sci. Appl. 10, 76 (2021).
[12] J. Li, X. Li, X. Huang, R. Kaissner, F. Neubrech, S. Sun, and N. Liu, "High space-bandwidth-product (SBP) hologram carriers toward photorealistic 3D holography," Laser Photonics Rev. 18, 2301173 (2024).
[13] J. Huang, H. Wang, X. Sun, X. Zhang, and H. Wang, "Multifunctional La₀.₆₇Sr₀.₃₃MnO₃ (LSMO) thin films integrated on mica substrates toward flexible spintronics and electronics," ACS Appl. Mater. Interfaces 10, 42698–42705 (2018).
[14] B. P. Bloom, Y. Paltiel, R. Naaman, and D. H. Waldeck, "Chiral induced spin selectivity," Chem. Rev. 124, 1950–1983 (2024).
[15] L. Guo, S. Hu, X. Gu, R. Zhang, K. Wang, W. Yan, and X. Sun, "Emerging spintronic materials and functionalities," Adv. Mater. 36, 2301854 (2024)
[16] R. Naaman, Y. Paltiel, and D. H. Waldeck, "Chiral molecules and the electron spin," Nat. Rev. Chem. 3, 250–260 (2019).
[17] R. Naaman, Y. Paltiel, and D. H. Waldeck, "Chiral induced spin selectivity gives a new twist on spin-control in chemistry," Acc. Chem. Res. 53, 2659–2667 (2020).
[18] G. Wang, H. Zhang, H. Kuang, C. Xu, and L. Xu, "Chiral inorganic nanomaterials for bioapplications," Matter 6, 1752–1781 (2023).
[19] F. Qi, L. Li, Z. Li, L. Qiu, Z. Meng, and Y. Yin, "Magnetic/plasmonic hybrid nanodisks with dynamically tunable mechano-chiroptical responses," ACS Nano 17, 1427–1436 (2023).
[20] H. Furukawa, K. E. Cordova, M. O’Keeffe, and O. M. Yaghi, "The chemistry and applications of metal-organic frameworks," Science 341, 1230444 (2013).
[21] H.-C. Zhou, J. R. Long, and O. M. Yaghi, "Introduction to metal–organic frameworks," Chem. Rev. 112, 673–674 (2012).
[22] M. Mustaqeem, P.-T. Chou, S. Kamal, N. Ahmad, J.-Y. Lin, Y.-J. Lu, X.-H. Lee, K.-H. Lin, K.-L. Lu, and Y.-F. Chen, "Solution-processed and room-temperature spin light-emitting diode based on quantum dots/chiral metal-organic framework heterostructure," Adv. Funct. Mater. 33, 2213587 (2023).
[23] M. Mustaqeem, S. Kamal, N. Ahmad, P.-T. Chou, K.-H. Lin, Y.-C. Huang, G.-Y. Guo, C. R. P. Inbaraj, W.-K. Li, H.-C. Yao, K.-L. Lu, and Y.-F. Chen, "Chiral metal-organic framework based spin-polarized flexible photodetector with ultrahigh sensitivity," Mater. Today Nano 21, 100303 (2023).
[24] W. Gong, Z. Chen, J. Dong, Y. Liu, and Y. Cui, "Chiral metal–organic frameworks," Chem. Rev. 122, 9078–9144 (2022).
[25] L. A. Hall, D. M. D’Alessandro, and G. Lakhwani, "Chiral metal–organic frameworks for photonics," Chem. Soc. Rev. 52, 3567–3590 (2023).
[26] Y. Zhang, Y. Ma, W. Sun, W. Li, and G. Li, "Structural and electronic chirality in inorganic crystals: From construction to application," Chem. Eur. J. 30, e202400436 (2024).
[27] X.-X. Yang, N. Li, C. Li, Z.-B. Jin, Z.-Z. Ma, Z.-G. Gu, and J. Zhang, "Chiral liquid crystalline metal–organic framework thin films for highly circularly polarized luminescence," J. Am. Chem. Soc. 146, 16213–16220 (2024).
[28] H.-R. Fu, N. Wang, X.-X. Wu, F.-F. Li, Y. Zhao, L.-F. Ma, and M. Du, "Circularly polarized room-temperature phosphorescence and encapsulation engineering for MOF-based fluorescent/phosphorescent white light-emitting devices," Adv. Opt. Mater. 8, 2000330 (2020).
[29] P.-F. Gao, Y.-Y. Jiang, H. Liu, M.-S. Zhou, T. Li, H.-R. Fu, L.-F. Ma, and D.-S. Li, "Pillar-layer chiral MOFs as a crystalline platform for circularly polarized luminescence and single-phase white-light emission," ACS Appl. Mater. Interfaces 14, 16435–16444 (2022).
[30] C. Zhang, Z.-P. Yan, X.-Y. Dong, Z. Han, S. Li, T. Fu, Y.-Y. Zhu, Y.-X. Zheng, Y.-Y. Niu, and S.-Q. Zang, "Enantiomeric MOF crystals using helical channels as palettes with bright white circularly polarized luminescence," Adv. Mater. 32, 2002914 (2020).
[31] J. Chen, Q. Zhao, B. Yu, and U. Lemmer, "A review on quantum dot-based color conversion layers for mini/micro-LED displays: Packaging, light management, and pixelation," Adv. Opt. Mater. 12, 2300873 (2024).
[32] E. Jang and H. Jang, "Quantum dot light-emitting diodes," Chem. Rev. 123, 4663–4692 (2023).
[33] A. I. Lebedev, "A new approach to analyzing the spinor wave functions: Effect of strain on the electronic structure and optical transitions in bulk CdSe," arXiv:2307.15534v2 [cond-mat.mtrl-sci] (2024).
[34] Y.-H. Kim, Y. Zhai, H. Lu, X. Pan, C. Xiao, E. A. Gaulding, S. P. Harvey, J. J. Berry, Z. V. Vardeny, and M. C. Beard, "Chiral-induced spin selectivity enables a room-temperature spin light-emitting diode," Science 371, 1129–1133 (2021).
[35] L. Sui, Z.-B. Jin, G. Niu, J. Jiang, Q.-H. Li, L.-M. Chang, K. Yuan, Z.-G. Gu, J. Zhang, and X. Yang, "Breaking mirror circularly polarized luminescence of chiral metal–organic frameworks by high-pressure stimulation," CCS Chem. 5, 2215–2224 (2023).
[36] M. Mustaqeem, J.-Y. Lin, S. Kamal, A. Thakran, G.-Z. Lu, G. Naikoo, P.-T. Chou, K.-L. Lu, and Y.-F. Chen, "Optically encodable and erasable multilevel nonvolatile flexible memory device based on metal–organic frameworks," ACS Appl. Mater. Interfaces 14, 26895–26904 (2022).
[37] T. Zhao, J. Han, X. Jin, M. Zhou, Y. Liu, P. Duan, and M. Liu, "Dual-mode induction of tunable circularly polarized luminescence from chiral metal-organic frameworks," Research 2020, 6452123 (2020).
[38] J.-Y. Lin, F.-C. Hsu, Y.-C. Chao, G.-Z. Lu, M. Mustaqeem, and Y.-F. Chen, "Self-assembled monolayer for low-power-consumption, long-term-stability, and high-efficiency quantum dot light-emitting diodes," ACS Appl. Mater. Interfaces 15, 25744–25752 (2023).
[39] E. Aktas, N. Phung, H. Köbler, D. A. González, M. Méndez, I. Kafedjiska, S.-H. Turren-Cruz, R. Wenisch, I. Lauermann, A. Abate, and E. Palomares, "Understanding the perovskite/self-assembled selective contact interface for ultra-stable and highly efficient p–i–n perovskite solar cells," Energy Environ. Sci. 14, 3976–3985 (2021).
[40] R. Naaman, Y. Paltiel, and D. H. Waldeck, "Chiral molecules and the electron spin," Nat. Rev. Chem. 3, 250–260 (2019).
[41] R. Naaman, Y. Paltiel, and D. H. Waldeck, "Chiral molecules and the spin selectivity effect," J. Phys. Chem. Lett. 11, 3660–3666 (2020).
[42] Y. Sun, Y. Xu, H. Li, Y. Liu, F. Zhang, H. Cheng, S. Tao, H. Wang, W. Hu, Y. Lu, C. Zhao, T. Nie, W. Zhao, Q. Guo, and L. Wen, "Flexible control of broadband polarization in a spintronic terahertz emitter integrated with liquid crystal and metasurface," ACS Appl. Mater. Interfaces 14, 32646–32656 (2022).
[43] F. Furlan, J. M. Moreno-Naranjo, N. Gasparini, S. Feldmann, J. Wade, and M. J. Fuchter, "Chiral materials and mechanisms for circularly polarized light-emitting diodes," Nat. Photonics 18, 658–668 (2024).
[44] N. Guan, X. Dai, A. V. Babichev, F. H. Julien, and M. Tchernycheva, "Flexible inorganic light emitting diodes based on semiconductor nanowires," Chem. Sci. 8, 7904–7911 (2017).
[45] M. K. Choi, J. Yang, T. Hyeon, and D.-H. Kim, "Flexible quantum dot light-emitting diodes for next-generation displays," npj Flexible Electron. 2, 10 (2018).
[46] Y. Zhang, S. Yu, B. Han, Y. Zhou, X. Zhang, X. Gao, and Z. Tang, "Circularly polarized luminescence in chiral materials," Matter 5, 837–875 (2022).
[47] J. Liu, Z. P. Song, L. Y. Sun, B. X. Li, Y. Q. Lu, and Q. Li, "Circularly polarized luminescence in chiral orientationally ordered soft matter systems," Respons. Mater. 1, 20230005 (2023).
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dc.identifier.urihttp://tdr.lib.ntu.edu.tw/jspui/handle/123456789/97763-
dc.description.abstract本研究提出一種新穎策略,成功以手性金屬有機框架(Chiral Metal-Organic Frameworks, chiral-MOFs)作為自旋選擇性載子注入層,實現無需外加磁場與鐵磁接觸之下的室溫自旋極化圓偏振發光元件。相較於傳統自旋元件仰賴磁性材料進行載子極化的方式,本研究運用 MOF 材料內在的手性結構,透過「手性誘導自旋選擇性(Chiral-Induced Spin Selectivity, CISS)」效應,選擇性的傳輸特定自旋態的電洞,進一步促使量子點層產生顯著的圓偏振電致發光(Circularly Polarized Electroluminescence, CP-EL)。
我們透過水熱法合成對掌結構明確的 D-/L-Eu(Tar)MOFs,並藉由 CD 與 CPL 光譜證實其鏡像手性與優異的圓偏振發光能力(glum ≈ 0.41)。隨後,將其整合於全柔性元件架構中:FITO/SAM (P3HT-COOH)/D- or L-MOF/CdSe QDs/ZnO/Ag,其中自組裝單分子層(SAM)有效提升載子注入效率與介面穩定性,CdSe/ZnS 量子點則提供窄頻寬(FWHM = 27 nm)、高效率的紅光發射。
實驗結果顯示,導入 chiral-MOF 後的元件在 632 nm 發光波長處展現極高的圓偏振度,其圓偏振發光偏極度(PCP-EL)最高可達 ±21.86%,遠優於過去文獻中以有機或無機手性材料構成之 spin-LED 裝置。此外,對照組(未加入 MOF 層)之元件無法產生明顯的圓偏振光,進一步證實 CISS 效應為造成 CPL 發光的關鍵機制。
更進一步地,我們系統性研究了元件在不同彎折曲率下的發光特性變化。隨著曲率半徑由 降低,偏極度由 21.86% 漸降至 13.54%,且該變化為可逆,顯示元件具備優異的力學可調性與穩定性。配合拉曼光譜測量發現,MOF 結構在彎曲時 C–H 鍵振動峰產生藍移,證實其內部結構因機械應力產生局部微調,進一步影響 CISS 效應的強度與發光極化表現。
本研究成功展示以 MOF 為核心的手性自旋選擇材料不僅能實現高效率的自旋注入,亦能在無磁場條件下產生穩定的圓偏振發光。更重要的是,其柔性結構具備機械可調特性,提供一全新自由度以操控發光偏極行為,為可撓式自旋光電子元件、量子資訊傳輸與未來穿戴型光電技術之開發,奠定關鍵基礎。
zh_TW
dc.description.abstractIn this study, we propose a novel strategy to successfully use chiral metal–organic frameworks (chiral-MOFs) as spin-selective carrier injection layers to realize room-temperature spin-polarized circularly polarized light-emitting diode (spin-CP-LED) devices without the need for an applied magnetic field or ferromagnetic contacts. In contrast to conventional spintronic devices that rely on magnetic materials to induce spin polarization, the present study utilizes the intrinsic chirality of MOFs to selectively transport holes in specific spin states through the chiral-induced spin selectivity (CISS) effect, thereby enabling the quantum dot (QD) layer to emit significant circularly polarized electroluminescence (CP-EL).
We synthesized D-/L-Eu(Tar) MOFs with well-defined enantiomeric structures via a hydrothermal method, and confirmed their mirror-image chirality and excellent circularly polarized emission capability (glum ≈ 0.41) using circular dichroism (CD) and circularly polarized luminescence (CPL) spectroscopy. These chiral MOFs were subsequently integrated into a fully flexible device architecture: flexible ITO (FITO)/self-assembled monolayer (SAM, P3HT-COOH)/D- or L-MOF/CdSe QDs/ZnO/Ag, where the SAM layer significantly improves carrier injection efficiency and interfacial stability, while the CdSe/ZnS quantum dots provide narrow emission bandwidth (FWHM = 27 nm) and high-efficiency red emission.
Experimental results show that the chiral-MOF-integrated device exhibits a remarkably high degree of polarization (PCP-EL) at an emission wavelength of 632 nm, reaching ±21.86%, which is significantly higher than the PCP-EL values reported for spin-LEDs based on organic or inorganic chiral materials. In contrast, the control devices without the MOF layer fail to generate measurable circularly polarized light, further confirming that the CISS mechanism is the primary origin of the observed CP-EL.
Furthermore, we systematically investigated the luminescence behavior of the devices under various bending radii. As the curvature radius decreased, the degree of polarization decreased from 21.86% to 13.54%, with the change being fully reversible, indicating excellent mechanical tunability and structural robustness. Raman spectroscopy revealed a blue shift in the C–H vibrational modes of the MOF structure under bending, confirming that localized structural modulation occurs due to mechanical stress, which in turn affects the strength of the CISS effect and the resulting polarization characteristics.
In conclusion, this study successfully demonstrates that MOF-based chiral spin-selective materials not only enable efficient spin injection but also allow for stable circularly polarized light emission under ambient, non-magnetic conditions. More importantly, the mechanical tunability of the flexible architecture provides a new degree of freedom for controlling polarization behavior, establishing a solid foundation for the future development of flexible spintronic devices, quantum information technologies, and next-generation wearable optoelectronics.
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dc.description.tableofcontents口試委員會審定書 i
致謝 ii
中文摘要 iii
Abstract v
CONTENTS viii
LIST OF FIGURES x
LIST OF TABLES xiv
Chapter 1 Introduction 1
Chapter 2 Theoretical Background 4
2.1 Chiral-Induced Spin Selectivity (CISS) [14][15][16][17] 4
2.2 Circularly Polarize Light 9
2.3 Metal Organic Farmwork 11
2.4 Quantum Dot LED 12
Chapter 3 Experiment Details 17
3.1 Powder X-ray Diffraction (PXRD) 17
3.2 UV spectra 19
3.3 Fourier Transform Infrared Spectroscopy (FTIR) 21
3.4 Circular Dichroism (CD) spectroscopy 23
3.5 PL spectra 26
3.6 Circularly Polarized Luminescence (CPL) spectroscopy 28
3.7 Indium Tin Oxide (ITO) 30
3.8 Poly[3-(6-carboxyhexyl)thiophene-2,5-diyl] (P3HT-COOH) 31
3.9 Cadmium Selenide (CdSe) Quantum Dot 32
3.10 Zinc Oxide (ZnO) Nanoparticles 34
Chapter 4 Result and Discussion 41
Chapter 5 Conclusion 57
REFERENCE 59
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dc.language.isoen-
dc.subjectLEDzh_TW
dc.subject自旋電子元件zh_TW
dc.subject量子點zh_TW
dc.subject柔性材料zh_TW
dc.subject金屬有機框架zh_TW
dc.subject圓偏振光zh_TW
dc.subjectLEDen
dc.subjectquantum dotsen
dc.subjectspintronic componentsen
dc.subjectflexible materialsen
dc.subjectmetal-organic frameworken
dc.subjectcircularly polarized lighten
dc.title機械可調自旋金屬有機框架LEDzh_TW
dc.titleMechanically Tunable spin MOF-based Light-Emitting Diodesen
dc.typeThesis-
dc.date.schoolyear113-2-
dc.description.degree碩士-
dc.contributor.coadvisor謝馬利歐zh_TW
dc.contributor.coadvisorMario Hofmannen
dc.contributor.oralexamcommittee邱雅萍;林彥甫zh_TW
dc.contributor.oralexamcommitteeYa-Ping Chiu;Yen-Fu Linen
dc.subject.keywordLED,圓偏振光,金屬有機框架,柔性材料,量子點,自旋電子元件,zh_TW
dc.subject.keywordLED,circularly polarized light,metal-organic framework,flexible materials,quantum dots,spintronic components,en
dc.relation.page66-
dc.identifier.doi10.6342/NTU202501566-
dc.rights.note同意授權(全球公開)-
dc.date.accepted2025-07-10-
dc.contributor.author-college理學院-
dc.contributor.author-dept物理學系-
dc.date.embargo-lift2025-07-17-
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