工程驅動的光偵測器在各種科學和工業應用中發揮著重要作用，包括通信、生物成像、遙測和環境監測。在光偵測器中，光生電荷載流子在外部電壓的作用下從光活性通道向相反的電極移動，或者在異質界面處被內建電勢驅動以產生光電流。理想的光偵測器必須具有高光譜選擇性、超靈敏性和高信噪比。傳統上，Si、Ge、ZnO-CdS 及其異質結構已被用於可見光偵測器。此外，InGaAs、InSb、GaSb、HgCdTe等窄帶隙III-V族半導體材料被用於包括從近紅外到長波紅外區域的探測範圍。然而，由於其複雜且漫長的製造過程，它們的成本很高。因此，正在研究許多材料以簡化結構並製造具有成本效益的光偵測器。其中，幾種二維材料（例如，石墨烯、黑磷 (BP)、MoS2、鈣鈦礦量子點 (PQD) 和銅基硫族化物 Cu2NiSnS4 (CNTS)）表現出優異的光學特性，包括具厚度和元素成分相關性的可調帶隙、環境溫度下的高載流子遷移率和 CMOS 兼容性，使它們成為中紅外 (MIR) 和可見光偵測應用的有力候選者。
儘管上述光敏材料具有優異的光學特性，但由於光與物質的相互作用較弱，它們的光偵測器仍然存在較差的光電性能。電漿子和超材料可能是增強光與物質相互作用的潛在工具。在電漿子中，主要是金屬銀 (Ag)、金 (Au) 和銅 (Cu) 納米結構被用於可見到紅外頻率區域。這些電漿子納米結構將附近的入射電磁場局域化，並通過局域表面電漿子共振 (LSPR) 實現強烈的光-物質相互作用。同時，超材料的光學特性取決於其設計和結構參數。因此，將電漿子納米結構和超材料整合到不同的光活性材料中已經被研究以提高光電性能。牢記這一事實，在這篇論文中我們探索了使用電漿子納米結構和電漿子超表面與上述光活性半導體材料混合，並設計了光偵測器以進一步增強其光電性能。
對於第一篇研究，我們展示了一種電漿子超表面整合的基於黑磷 (BP) 的中紅外 (MIR) 光偵測器，具有高響應度和速度。由於結構和光學各向異性特性，BP 表現出 0.3-2.0 eV 的層數相關之可調直接帶隙、環境溫度下的高載流子遷移率 (5×103 cm2 V−1S−1) ，這使其成為MIR光偵測器應用的強力候選者。儘管已經提出了幾種基於 BP 的 MIR 光偵測器，但由於環境溫度下的小光吸收截面，它們的性能仍然受到限制。在此，我們設計了一個在 3.7 µm 處具有局域表面電漿子共振 (LSPR) 的電漿子超表面，如 FTIR 測量結果所示，它與 BP 薄片的能帶邊緣完美匹配。在設計的電漿子超表面的共振波長下，使用有限差分模擬結果觀察了 Au 盤邊緣周圍的場限制。此外，我們將 BP 薄片與電漿子超表面整合在一起，並觀察到顯著的光致發光猝滅（≈ 12 倍），這是由於激子和電漿子激元之間的偶極-偶極耦合引起的 Förster 共振能量轉移效應。此外，我們製造了一個電漿子超表面整合石墨烯/BP/石墨烯基夾層垂直結構光偵測器，並探測了中紅外波長的光電響應。我們展示了在 3.7 µm 波長下以 8.55 µW 的入射功率實現 495.85 mAW−1 的高響應度和超高運行速度 (>10MHz)。展出的電漿子整合基於 BP 的混合光偵測器為中紅外光譜中的光電應用創造了新的選擇。
對於可見電漿子光偵測器裝置的第二項研究，我們研究了電漿子增強量子點/石墨烯光偵測。由於其出色的載流子遷移率、高吸收係數、出色的量子效率和低成本的溶液可加工性，鈣鈦礦量子點 (PQD) 是光偵測有前途的候選者。然而，基於 PQD 的光偵測器通常表現出較差的光電性能，主要受限於它們弱的光-物質相互作用。在這項工作中，我們將 MAPbBr3 PQD 與石墨烯和形態控制的電漿子金納米晶體 (AuNC) 混合，以通過協同效應在 432 nm 處展示出卓越的光偵測器。我們的實驗結果表明，三種形狀的 AuNC（即球形、八面體 (OD) 和菱形十二面體 (RD)）都有助於更好的光電探測行為，這是由於表面陷阱態鈍化和增強的電荷載流子密度，與原始 AuNC 相比具有更長的壽命PQD。特別是，PQDs/RD-AuNCs/Gr 系統表現出創紀錄的 2.7×105 AW−1 響應率、4.9×1013 瓊斯探測率和 1.6 µWcm−2 下 7.9×107% 的外量子效率 (EQE) 在432 nm 波長的 1.6 µWcm−2 照明功率密度下以最低施加電壓為 1.0 V，對於基於無閘極的 PQD/AuNCs/Gr光偵測器。此外，據我們所知，我們的設備在基於 PQD/AuNC/Gr 的靜電無閘極橫向配置光偵測器中顯示出最高的響應度。
對於電漿子器件的第三項研究，我們展示了將電漿子金屬納米結構以核-殼結構的形式結合到半導體化合物中，為顯著提高光偵測器的性能提供了一條新途徑。在此，我們首次報告了 Cu2NiSnS4 (CNTS) 納米晶體 (NCs) 和 Au/CNTS 核-殼 NCs 的開發，作為使用膠體熱注入法的概念驗證實驗，因為它對尺寸、形狀和元素組成的出色控制。此外，我們將 Au/CNTS 核-殼 NC 與 Gr 薄膜混合，以在可見光範圍內呈現超高光電響應。這些光活性 Au/CNTS 核-殼 NC 表現出增強的光吸收、載流子提取效率和改進的光敏性能。增強的光電性能主要歸功於Au核的電漿子誘導共振能量轉移（PIRET）效應； Au 核和 CNTS 殼之間的載流子密度顯著增加。因此，測得的響應率、比探測率和外量子效率 (EQE) 分別達到 1.2×103 AW─1、6.2×1011 瓊斯和 3.8×105 %（在 318.5 µWcm─2 的照明功率密度下），優於受控的原始 CNTS/石墨烯基光偵測器。此外，使用 Au/CNTS 的器件具有 2.58秒/11.14 秒的快速響應時間/恢復時間和出色的運行可靠性。這些結果開啟了用於成像應用的基於電漿子核殼納米結構的可見光傳感設備的製造和開發的新時代。
對於電漿子裝置的最後研究，我們展示了一個基於 Au 納米盤陣列/MoS2 的超靈敏光偵測器。由於其原子級薄的厚度、依賴於層的可調帶隙、柔韌性和 CMOS 兼容性，MoS2 是光電探測的有前途的候選者。然而，基於單層 MoS2 的光偵測器通常表現出較差的光電性能，主要受限於它們低的光吸收。在這項工作中，我們將 CVD 生長的單層 MoS2 與金納米盤 (AuND) 陣列結合，以通過協同效應展示出卓越的可見光偵測器。從我們的實驗結果可以明顯看出，AuND 和單層 MoS2 之間存在強烈的光物質相互作用，與原始 MoS2 相比，由於表面陷阱態鈍化和更短的電荷載流子壽命，這導致更好的光偵測。特別是，AuND/MoS2 系統在 632 nm 波長的 31.84 µWcm−2 照明功率密度和施加電壓為4.0 V基於 AuND/MoS2 的光偵測器為，表現出創紀錄的 8.7× 104AW−1 響應率、6.9× 1013 瓊斯探測率和1.7× 105 的增益。據我們所知，這些光電響應比文獻中基於 CVD MoS2 的光偵測器的報告結果高一個數量級。
進一步地，這些展示的混合器件顯示出出色的操作可靠性、低成本的可加工性，以及在中紅外和可見光區域用作低光成像光電傳感器器件的潛力。

Engineering-driven photodetectors play an essential role in various scientific and industrial applications, including communications, bioimaging, remote sensing, and environmental monitoring. It is necessary to be highly spectral selective, ultrasensitive, and have a high signal-to-noise ratio for an ideal photodetector. Traditionally, Si, Ge, ZnO-CdS, and their heterostructures have been used for visible photodetectors. Moreover, narrow bandgaps III-V semiconductor materials such as InGaAs, InSb, GaSb, and HgCdTe are used to cover the detection range from near-infrared to long-wave infrared region. However, they are costly because of their complicated and prolonged fabrication process. Therefore, many materials are being investigated to simplify the structures and fabricate cost-effective photodetectors. Among them, several 2D materials (e.g., Graphene (Gr), Black Phosphorus (BP), MoS2), Perovskite Quantum Dots (PQDs), and copper-based chalcogenides Cu2NiSnS4 (CNTS)) exhibits superior optical properties, including a thickness and elemental constituents-dependent tunable band gap, high carrier mobility at ambient temperature, and CMOS compatibility, making them a strong candidate for mid-infrared (MIR) and visible photodetector applications.
Although the aforementioned photoactive materials possess superior optical characteristics, their photodetectors still suffer from poor optoelectronic performance due to weak light-matter interaction. Plasmonic and metamaterials could be potential tools to enhance light-matter interaction. In plasmonic, mostly metallic silver (Ag), gold (Au), and copper (Cu) nanostructures are being used for visible to infrared frequency regions. These plasmonic nanostructures localized incident electromagnetic field in the vicinity and enabled strong light-matter interaction via localized surface plasmon resonance (LSPR). At the same time, the optical properties of the metamaterials depend on their designs and structure parameters. Therefore, the integration of plasmonic nanostructures and metamaterials in different photoactive materials has been studied to boost optoelectronic performance. Keeping this fact in mind, in this dissertation, we explored using plasmonic nanostructures and plasmonic metasurface to hybridize with those above photoactive semiconducting materials and designed photodetectors to enhance further their optoelectronic performance.
For the first study, we demonstrated a plasmonic metasurface integrated Black Phosphorus (BP)-based mid-infrared (MIR) photodetector with high responsivity and speed. Owing to the structural and optical anisotropic properties, BP exhibits a layer-dependent tunable direct band gap from 0.3-2.0 eV, and a high carrier mobility (5×103 cm2 V−1S−1) at ambient temperature is a strong candidate for MIR photodetector applications. Although several BP-based MIR photodetectors have been proposed, their performance is still constrained due to the small optical absorption cross-section at ambient temperature. Herein, we designed a plasmonic metasurface with localized surface plasmon resonance (LSPR) at 3.7 µm, which demonstrates an excellent match with the band edge of a BP flake as shown by FTIR measurement results. The field confinement around the edge of the Au-disk was observed using finite difference simulation results at the resonance wavelength of the designed plasmonic metasurface. Furthermore, we integrated a BP flake with the plasmonic metasurface and observed a significant photoluminescence quenching (≈ 12-fold) owing to the Förster resonance energy transfer effect induced by dipole-dipole coupling between excitons and plasmons. Moreover, we fabricated a plasmonic metasurface integrated graphene/BP/graphene-based sandwich vertical structured photodetector and probed the optoelectronic responses in MIR wavelength. We demonstrated to achieve a high responsivity of 495.85 mAW−1 and ultrahigh operation speed (>10MHz) at the incident power of 8.55 µW at the wavelength of 3.7 µm. The exhibited plasmonic integrated BP-based hybrid photodetector creates a new option for optoelectronic applications in the MIR spectrum.
For the second study of the visible plasmonic photodetector device, we studied the plasmons-enhanced QDs/Graphene photodetection. Owing to their excellent carrier mobility, high absorption coefficient, exceptional quantum efficiency, and low-cost solution processability, perovskite quantum dots (PQDs) are a promising candidate for photodetection. However, PQDs-based photodetectors typically show poor optoelectronic performances, mainly limited by their weak light-matter interaction. In this work, we hybridize MAPbBr3 PQDs with the graphene and morphologically controlled plasmonic gold nanocrystals (AuNCs) to demonstrate a superior photodetector at 432 nm through a synergetic effect. Our experimental results indicate that three shaped AuNCs (i.e., sphere, the octahedron (OD), and rhombic dodecahedron (RD) all contribute to better photodetection behaviors due to surface trap state passivation and enhanced charge carrier densities with longer lifetime compared to that of pristine PQDs. In particular, the PQDs/RD-AuNCs/Gr system demonstrated a record-high responsivity of 2.7×105 AW−1, a detectivity of 4.9×1013 Jones, and external quantum efficiency (EQE) of 7.9×107 % at 1.6 µWcm−2 illumination power density of 432 nm wavelength with a lowest applied voltage of 1.0 V for a gate-free PQDs/AuNCs/Gr-based photodetector. Furthermore, to our knowledge, our device shows the highest responsivity among the PQDs/AuNCs/Gr-based electrostatic gate-free lateral configuration photodetectors.
For the third study of the plasmonic devices, we demonstrated the incorporation of plasmonic metal nanostructures into the semiconductor compounds in the form of core-shell structures, offering a new route to significantly improve the performance of photodetectors. Herein, we report the development of Cu2NiSnS4 (CNTS) nanocrystals (NCs) and Au/CNTS core-shell NCs for the first time as a proof-of-concept experiment using the colloidal hot-injection method owing to its excellent control over size, shape, and elemental composition. Furthermore, we hybridize Au/CNTS core-shell NCs with a Gr film to present an ultrahigh optoelectronic response in a visible regime. These photoactive Au/CNTS core-shell NCs exhibit enhanced optical absorption, carrier extraction efficiency, and improved photo-sensing performance. The enhanced optoelectronic performance is mainly due to the plasmonic-induced resonance energy transfer (PIRET) effect of the Au core; carrier density is significantly increased between the Au core and CNTS shell. As a consequence, the measured responsivity, specific detectivity, and external quantum efficiency (EQE) reach 1.2 103 AW─1, 6.2×1011 Jones, and 3.8×105 %, respectively (at an illumination power density of 318.5 µWcm─2), outperforming the controlled a pristine CNTS/graphene-based photodetector. Further, the device using Au/CNTS exhibits a fast response/recovery time of 2.58/11.14 sec and excellent operational reliability. These results enlighten a new era in the fabrication and development of plasmonic core-shell nanostructures-based visible photo-sensing devices for imaging applications.
For the last study of the plasmonic device, we demonstrated an Au nanodisk array/MoS2-based ultrasensitive photodetector. Owing to its atomically thin thickness, layer-dependent tunable band gap, flexibility, and CMOS compatibility, MoS2 is a promising candidate for photodetection. However, mono-layer MoS2-based photodetectors typically show poor optoelectronic performances, mainly limited by their low optical absorption. In this work, we hybridized CVD-grown monolayer MoS2 with a gold nanodisk (AuND) array to demonstrate a superior visible photodetector through a synergetic effect. It is evident from our experimental results that there is a strong light-matter interaction between AuNDs and monolayer MoS2, which results in better photodetection due to a surface trap state passivation with a shorter charge carrier lifetime compared to pristine MoS2. In particular, the AuND/MoS2 system demonstrated a record-high responsivity of 8.7× 104 AW─1, detectivity of 6.9× 1013Jones, and gain 1.7× 105 at 31.84 µWcm−2 illumination power density of 632 nm wavelength with an applied voltage of 4.0 V for AuND/MoS2-based photodetector. To our knowledge, these optoelectronic responses are one order higher than reported results for CVD MoS2-based photodetector in the literature.
Further, these demonstrated hybrid devices show excellent operational reliability, low-cost processability, and potential to be used as low-light imaging photosensor devices in MIR and visible regions.

Table of Contents
Chapter 1 1
Introduction 1
1.1 Photodetectors 1
1.2 Photoactive Materials 3
1.3 Plasmonic and Metamaterials 10
1.4 Dissertation Structure 14
Chapter 2 15
Literature Review 15
2.1 Black Phosphorus-Based Photodetectors 15
2.2 Perovskite Quantum Dots-Based Photodetectors 16
2.3 Cu2NiSnS4 (CNTS)-Based Photodetectors 18
2.4 MoS2-Based Photodetectors 18
Chapter 3 21
Plasmonic Metasurface Integrated Black Phosphorus-Based Photodetector 21
3.1 Introduction and Motivation 21
3.2 Numerical Methods and Optimization of Plasmonic Metasurface 23
3.3 Plasmonic Metasurface and Photodetector Fabrication Process 25
3.4 Optical Characterization 27
3.5 Optoelectronic Characterization 32
3.6 Conclusions 43
Chapter 4 44
Perovskite QDs/Graphene Hybrid Gate -Free Photodetector 44
4.1 Introduction and Motivation 44
4.2 Design of Photodetector 46
4.3 Synthesis of PQDs, Structural and Optical Characterization 47
4.4 Synthesis, Structural and Optical Characterization of AuNCs 50
4.5 Synthesis of Graphene and Characterizations 54
4.6 Optical Properties of Hybrid Structure 55
4.7 Surface Electronic Properties of Hybrid Structure 59
4.8 Energy Band Diagram of Hybrid Structure 60
4.9 Device Fabrication Process 62
4.10 Optoelectronic Characterization 63
4.11 Conclusions 72
Chapter 5 73
Core-Shell Au/Cu2NiSnS4/Graphene-Based Gate-Free Photodetector 73
5.1 Introduction and Motivation 73
5.2 Design of the Photodetector 74
5.3 Synthesis and Structural Characterization of CNTS and Au/CNTS 75
5.4 Optical Characterization 80
5.5 Energy Band Diagram 83
5.6 Device Fabrication Process 85
5.7 Optoelectronic Characterization 86
5.8 Conclusions 94
Chapter 6 95
Plasmonically Enhanced AuNDs/MoS2-Based Phototransistor 95
6.1 Introduction and Motivation 95
6.2 Design of Phototransistor 97
6.3 Gold Nanodisk Parameter Optimization 97
6.4 Synthesis of MoS2 and Transfer Process 99
6.5 Device Fabrication Process 100
6.6 Optical Characterization 101
6.7 Transfer Characteristics 104
6.8 Energy Band Diagram 105
6.9 Optoelectronic Characteristics 106
6.10 Conclusions 113
Chapter 7 114
Summary 114
Chapter 8 116
Future Prospect 116
Bibliography 117
Appendix 138

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