傑納斯過渡金屬二硫化物（TMDs）是一種新型的二維（2D）材料，由於其非對稱結構具有新穎的特性。在傑納斯 TMDs中，鏡像對稱性的破壞導致了一些有趣的現象，如拉許巴分裂（Rashba splitting）、垂直壓電效應和二次諧波產生（SHG）性能等。本研究中我們對傑納斯 TMDs進行了理論和實驗分析。首先，我們探討基於Pt的傑納斯單層（ML）PtXY（X，Y = S，Se，Te）上的各向異性拉許巴分裂，並發現有所有三種基於Pt的傑納斯 TMD單層在聲子色散圖上都是熱力學穩定的。此外，所有基於Pt的傑納斯 TMD單層都保留了1T相作為穩定結構，如同其對應TMD（例如PtS2，PtSe2和PtTe2）。在電子性質方面，PtSSe、PtSTe和PtSeTe是具有間接帶隙的絕緣材料，分別為2.108、1.335和1.221電子伏特。Pt系列之傑納斯 TMD，由於其單層中心對稱性破壞，可以觀察到自旋軌道耦合（SOC）引起的各向異性拉許巴分裂。在傑納斯 PtXY單層中，PtSSe在M到Γ (α_R^(M-Γ))和M到K(α_R^(M-K))分別具有最大的拉許巴強度(1.654和1.333 eV•Å-1)。同時，對PtSTe和PtSeTe，其Γ (α_R^(M-Γ))許巴強度分別為1.103和1.244 eV•Å-1，而(α_R^(M-K))值則分別為0.435和0.746 eV•Å-1。此外，根據自旋紋理結果，德雷塞爾豪斯效應(Dresselhaus effect)對各向異向性自旋分裂做出了貢獻。此外，拉許巴分裂和帶隙可以通過應用雙軸應變來調控。接下來，我們討論了透過電漿輔助硒化（PASP）成功合成ML 傑納斯 TMDs。通過控制溫度、電漿功率和硒化時間等動力學參數，可以將頂部硫（S）原子置換為Se，從而合成傑納斯 TMDs。根據拉曼結果，PASP可應用於大面積成長，因為135個單獨的MoS2薄片都成功轉換為傑納斯 MoSSe。此外，透過PASP可以成功合成傑納斯 MoSSe和WSSe單層，揭示了合成傑納斯 TMDs的過程的普遍性。我們可以藉由改變硒化溫度控制其相變，在200°C時，可以獲得2H相的傑納斯 MoSSe，而將溫度提高到400°C或600°C則可以得到MoSSe的1T/1T’相。最後，我們透過PASP從2英寸連續MoS2薄膜合成晶圓尺寸的傑納斯 MoSSe。我們的研究結果對於傑納斯 TMDs應用於未來新型電子和光電子器件提供了重要貢獻。

Janus transition metal dichalcogenides (TMDs) are new kinds of two-dimensional (2D) materials that possess novel properties due to their asymmetric structure. The breaking of the out-of-plane mirror symmetry in Janus TMDs results to interesting phenomena such as Rashba splitting, vertical piezoelectric effect, and a second harmonic generation (SHG) performance, among others. In this work, we performed theoretical and experimental investigations of Janus TMDs. First, we explored the anisotropic Rashba splitting on Pt-based Janus monolayers (ML) PtXY (X,Y = S, Se, Te). We found that all three Pt-based Janus TMD monolayers are thermodynamically stable based on the Phonon dispersion plot. Furthermore, all the Pt-based Janus TMD monolayers retained the 1T-phase as the stable structure, like their classical counterpart (e.g., PtS2, PtSe2, and PtTe2). In terms of electronic properties, PtSSe, PtSTe, and PtSeTe are insulating materials with an indirect bandgap of 2.108, 1.335, and 1.221 eV, respectively. Due to centrosymmetry breaking in the Pt-based Janus TMD monolayers, spin-orbit coupling (SOC)-induced anisotropic Rashba splitting can be observed. Among the Janus PtXY monolayers, PtSSe has the greatest Rashba strength at 1.654 and 1.333 eV•Å-1 from M to Γ (α_R^(M-Γ)) and M to K (α_R^(M-K)), respectively. Meanwhile, for PtSTe and PtSeTe, the Rashba strengths for α_R^(M-Γ)are 1.103 and 1.244 eV•Å-1, while the values for α_R^(M-K) are 0.435 and 0.746 eV•Å-1, respectively. Also, based on the spin texture results, Dresselhaus effect contributed to the anisotropic spin-splitting. Furthermore, the Rashba splitting and bandgap can be manipulated by applying biaxial strain. Next, we discuss our successful synthesis of ML Janus TMDs through plasma-assisted selenization process (PASP). By carefully controlling the kinetic parameters such as temperature, plasma power, and selenization time, the top sulfur (S) atom can be replaced with Se, creating the Janus TMDs. Based on the Raman results, PASP is suitable for high-yield production as 135 individual MoS2 flakes were all converted to Janus MoSSe. Furthermore, Janus MoSSe and WSSe monolayers can be created through PASP, indicating the universality of the process for synthesizing Janus TMDs. By changing the selenization temperature, phase-transition can be observed. At 200 °C, Janus MoSSe at 2H can be obtained while increasing the temperature to 400 °C or 600 °C can lead to 1T/1T’ phase of MoSSe. Finally, wafer-scale Janus MoSSe was synthesized by PASP from 2-inch continuous MoS2. Our findings provide significant contributions towards full exploration of Janus TMDs for future novel electronics and optoelectronics devices application.

Table of Contents
Dissertation Validation Letter i
Dissertation Publication Form ii
Abstract (Chinese)iii
Abstract (English)iv
Table of Contentsv
List of Figuresvii
List of Tablesix
List of Publicationsx
Chapter 1 Introduction1
1.1 The rise of two-dimensional (2D) materials1
1.2 Janus 2D materials2
1.2.1 Janus Graphene3
1.2.2 Janus Silicene4
1.2.3 Janus Germanene4
1.3 Janus Transition metal dichalcogenides (TMDs)5
Chapter 2 Motivation8
Chapter 3 Anisotropic rashba splitting in Pt-based janus monolayers PtXY (X,Y= S, Se, or Te)9
3.1 Introduction9
3.2 Methodology11
3.3 Results and Discussion12
3.4 Conclusion22
Chapter 4 Controllable structure-engineered janus and alloy polymorphic monolayer transition metal dichalcogenides by plasma assisted selenization process toward high-yield and wafer-scale production24
4.1 Introduction24
4.2 Methodology27
4.2.1 Synthesis of monolayer TMDs27
4.2.2 Synthesis of a wafer-scale MoS2 film28
4.2.3 Plasma-assisted selenization process on formation of Janus monolayer TMDs28
4.2.4 Transfer of a Wafer-scale Janus MoSSe film29
4.2.5 Optical measurements29
4.2.6 FET device fabrication and measurements30
4.2.7 Nanogeneration Performance Test30
4.2.8 Density function theory (DFT) calculations30
4.3 Results and Discussion31
4.4 Conclusion43
Chapter 5 Concluding remarks44
Chapter 6 Future Prospective45
Appendix for Chapter 347
Appendix for Chapter 461
Bibliography80

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