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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 鄭原忠(Yuan-Chung Cheng) | |
dc.contributor.author | Petra Shih | en |
dc.contributor.author | 施欣妤 | zh_TW |
dc.date.accessioned | 2021-05-12T09:36:44Z | - |
dc.date.available | 2018-08-21 | |
dc.date.available | 2021-05-12T09:36:44Z | - |
dc.date.copyright | 2018-08-21 | |
dc.date.issued | 2018 | |
dc.date.submitted | 2018-08-17 | |
dc.identifier.citation | [1] R. E. Blankenship. Molecular Mechanisms of Photosynthesis. Wiley, New York, 2014.
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dc.identifier.uri | http://tdr.lib.ntu.edu.tw/handle/123456789/1340 | - |
dc.description.abstract | 分子激發態的非絕熱躍遷在許多光物理和光化學過程中起著重要作用。特別是,葉綠素(chlorophyll)中Qx→Qy的超快內轉換(internal conversion)對於光合作用中光捕獲(light harvesting)的高效率至關重要,但其機制尚未明確闡明。在本工作中,我們通過評估振動耦合(vibronic coupling)來建構研究非絕熱內轉換的有效哈密頓算符(effective Hamiltonian),從理論上探索了葉綠素a和細菌葉綠素a之Qx→Qy動力學。通過結合含時密度泛函理論(time-dependent density functional theory)和透熱化(diabatization)方法,最大化兩個低激發態的組態(configuration)均勻性,實現了無輻射弛豫(non-radiative relaxation)的第一原理研究。使用費米黃金律(Fermi’s Golden rule)計算的弛豫速率表明,快於100飛秒Qx→Qy過程可以用具有弱振動耦合的透熱模型充分描述。此外,我們還確定了一些支配Qx→Qy弛豫的關鍵振動模式(vibrational normal mode),高度溶劑和取代基相關的弛豫速率可歸因於Qy/Qx能階間隙(energy gap)的變化。預計所開發的方法能廣泛應用於分子系統中能量弛豫的詳細動力學研究,並且還使我們能夠深入了解自然界光合作用中最重要的發色團的設計。 | zh_TW |
dc.description.abstract | Non-adiabatic transitions in molecular excited states play significant roles in many photophysical and photochemical processes. In particular, the ultrafast internal conversion of Qx→Qy in chlorophylls is crucial to the high efficiency of light harvesting in photosynthesis, yet the mechanism has not been clearly elucidated. In this work, we explored the internal conversion processes of chlorophyll a and bacteriochlorophyll a theoretically by evaluating the vibronic couplings and electronic couplings to construct effective Hamiltonians for the non-adiabatic Qx→Q¬y dynamics. The first principle study of the radiationless relaxation was achieved by combining time dependent density functional theory (TD-DFT) and diabatization method through enforcement of configuration uniformity for the two low lying excited states. The relaxation rates calculated using Fermi’s Golden rule suggest that the sub-100 fs Qx→Qy process can be fully described by a diabatic model with weak vibronic couplings. In addition, we also identified a few key vibrational modes that dominate the Qx→Qy relaxation, and the highly solvent and substituent dependent relaxation rates can be attribute to variations in Qy/Qx energy gaps. The methodology developed is expected to enable detailed dynamical study of energy relaxation in general molecular systems, and it also allows us to gain insights into the natural design of the most important chromophores in photosynthesis. | en |
dc.description.provenance | Made available in DSpace on 2021-05-12T09:36:44Z (GMT). No. of bitstreams: 1 ntu-107-R05223118-1.pdf: 8458323 bytes, checksum: 0b976d17c2350d2fdfcc1ac704ed36e3 (MD5) Previous issue date: 2018 | en |
dc.description.tableofcontents | 中文摘要 . . . . . . . .i
Abstract . . . . . . . .iii List of Figures . . . . . . . . ix List of Tables . . . . . . . .xiii 1 Introduction . . . . . . . .1 1.1 Light Harvesting in Photosynthesis . . . . . . . . . . . . . . . . . . . . . 1 1.2 Pigments in Light-Harvesting Complex . . . . . . . . . . . . . . . . . . 3 1.2.1 Chlorophylls and Bacteriochlorophylls . . . . . . . . . . . . . . 3 1.2.2 Studies of Chlorophyll Excited States . . . . . . . . . . . . . . . 5 1.2.3 Internal Conversion in Chlorophylls . . . . . . . . . . . . . . . . 7 1.3 Non-Adiabatic Transition . . . . . . . . . . . . . . . . . . . . . . . . . . 9 1.3.1 Recent Developments . . . . . . . . . . . . . . . . . . . . . . . 10 1.3.2 Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11 2 Theoretical Background . . . . . . . .13 2.1 Molecular Hamiltonian . . . . . . . . . . . . . . . . . . . . . . . . . . . 14 2.1.1 Separation of the Electronic and Nuclear Motions . . . . . . . . . 14 2.1.2 Born-Oppenheimer Approximation . . . . . . . . . . . . . . . . 15 2.1.3 Non-Adiabatic Coupling . . . . . . . . . . . . . . . . . . . . . . 17 2.2 Theoretical Treatments of Non-Adiabatic Dynamics . . . . . . . . . . . . 18 2.2.1 Multi-Configuration Time-Dependent Hartree . . . . . . . . . . . 19 2.2.2 Fewest Switch Surface Hopping . . . . . . . . . . . . . . . . . . 19 2.2.3 Ehrenfest Mean Field . . . . . . . . . . . . . . . . . . . . . . . . 20 2.2.4 Path Integral for Non-Adiabatic Dynamics . . . . . . . . . . . . 21 2.3 Diabatic Representation . . . . . . . . . . . . . . . . . . . . . . . . . . . 21 2.3.1 Definition of Diabatic Basis . . . . . . . . . . . . . . . . . . . . 23 2.3.2 Nonexistence of Strictly Diabatic Basis for General Molecules . . 23 2.3.3 Quasi-diabatization Methods Overview . . . . . . . . . . . . . . 24 2.4 Enforcement of Configuration Uniformity . . . . . . . . . . . . . . . . . 26 2.4.1 Configurational Expansions of Adiabatic and Diabatic States . . . 26 2.4.2 Deformation of Configurations and Molecular Orbitals . . . . . . 28 2.4.3 Uniformity of Electronic Structures . . . . . . . . . . . . . . . . 29 2.4.4 Diabatization Criterion . . . . . . . . . . . . . . . . . . . . . . . 30 3 Electronic Excitations of Chlorophylls . . . . . . . .33 3.1 Methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 33 3.1.1 Computational Details . . . . . . . . . . . . . . . . . . . . . . . 33 3.1.2 Transition Density and Transition Dipole Moment . . . . . . . . 34 3.2 Excited States Properties . . . . . . . . . . . . . . . . . . . . . . . . . . 36 3.2.1 Energy Levels . . . . . . . . . . . . . . . . . . . . . . . . . . . . 36 3.2.2 Configurations . . . . . . . . . . . . . . . . . . . . . . . . . . . 39 3.2.3 Transition Density and Transition Dipole Moment . . . . . . . . 43 3.3 Solvent and Coordination Dependences . . . . . . . . . . . . . . . . . . 46 3.3.1 Structures . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 46 3.3.2 Energy Levels . . . . . . . . . . . . . . . . . . . . . . . . . . . . 48 3.4 Diabatization . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 49 3.4.1 Molecular Orbitals Deformations . . . . . . . . . . . . . . . . . 49 3.4.2 Transformation Matrix . . . . . . . . . . . . . . . . . . . . . . . 52 3.4.3 Dominant CI Coefficients in Adiabatic and Diabatic Basis . . . . 53 3.5 Analysis of Potential Energy Surfaces . . . . . . . . . . . . . . . . . . . 55 3.6 Transition Density of the Diabatic States . . . . . . . . . . . . . . . . . . 56 3.7 Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 57 4 Vibronic Couplings of Chlorophylls . . . . . . . . 59 4.1 Theory . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 59 4.1.1 Coupling of Electronic and Nuclear Motion . . . . . . . . . . . . 59 4.2 Vibronic Coupling in Adiabatic Basis . . . . . . . . . . . . . . . . . . . 64 4.2.1 Four-Point Method . . . . . . . . . . . . . . . . . . . . . . . . . 64 4.2.2 Huang-Rhys Factor Method . . . . . . . . . . . . . . . . . . . . 67 4.2.3 Spectra Simulations . . . . . . . . . . . . . . . . . . . . . . . . 76 4.3 Vibronic Coupling in Diabatic Basis . . . . . . . . . . . . . . . . . . . . 84 4.3.1 Evaluate Coupling Constant from Potential Energy Surfaces . . . 84 4.3.2 Analysis of Off-Diagonal Strong-Coupled Modes . . . . . . . . . 85 4.4 Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 86 5 Internal Conversion Dynamics . . . . . . . .91 5.1 Theory . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 92 5.1.1 Spin-Boson Hamiltonian . . . . . . . . . . . . . . . . . . . . . . 92 5.1.2 Fermi’s Golden Rule for Vibronic Transitions . . . . . . . . . . . 93 5.1.3 Studying Internal Conversion using Fermi’s Golden Rule . . . . . 95 5.2 Results and Discussion . . . . . . . . . . . . . . . . . . . . . . . . . . . 98 5.2.1 Characteristic Frequencies . . . . . . . . . . . . . . . . . . . . . 98 5.2.2 Energy Gap Dependence . . . . . . . . . . . . . . . . . . . . . . 102 5.2.3 Mode-Specific Contributions to Rate . . . . . . . . . . . . . . . . 105 5.3 Reduced Vibrational Models . . . . . . . . . . . . . . . . . . . . . . . . 107 5.3.1 Selected Vibrational modes . . . . . . . . . . . . . . . . . . . . . 108 5.3.2 Effective Underdamped Harmonic Oscillators . . . . . . . . . . . 110 5.4 Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 113 6 Concluding Remarks . . . . . . . .115 Appendix A. Molecular Structures . . . . . . . .119 Appendix B. Basis Set Benchmark . . . . . . . .127 Appendix C. Vibronic Coupling in Diabatic Basis . . . . . . . .129 Bibliography . . . . . . . .139 | |
dc.language.iso | en | |
dc.title | 葉綠素內轉換之理論研究 | zh_TW |
dc.title | A Theoretical Study on the Internal Conversion Dynamics of Chlorophylls | en |
dc.type | Thesis | |
dc.date.schoolyear | 106-2 | |
dc.description.degree | 碩士 | |
dc.contributor.oralexamcommittee | 金必耀,林倫年,許昭萍 | |
dc.subject.keyword | 內轉換,葉綠素,非絕熱動力學,透熱化,震動耦合, | zh_TW |
dc.subject.keyword | diabatization,internal conversion,chlorophyll,non-adiabatic dynamics,vibronic coupling, | en |
dc.relation.page | 152 | |
dc.identifier.doi | 10.6342/NTU201803678 | |
dc.rights.note | 同意授權(全球公開) | |
dc.date.accepted | 2018-08-17 | |
dc.contributor.author-college | 理學院 | zh_TW |
dc.contributor.author-dept | 化學研究所 | zh_TW |
顯示於系所單位: | 化學系 |
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