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全光信号处理中具有优异非线性光学特性的光子平台对于提升器件的集成度、调制速度以及工作带宽等性能参数至关重要. 成熟的硅、氧化硅以及氮化硅光子平台由于材料本身中心对称, 基于这些平台的集成光子器件可实现的非线性光学功能受限; 二维材料尽管有着优异的非线性光学特性, 但只有原子层厚, 其非线性潜能无法被充分利用. 将二维材料与成熟的光子平台集成, 在充分利用光子平台成熟加工工艺的基础上, 可以显著提高光与二维材料的相互作用, 提升光子平台的非线性光学性能. 基于以上背景, 本文总结了近年来在基于转移方法和直接生长法制备的多种异质集成二维材料光子器件中进行非线性光学特性研究的最新进展; 阐述了相较于传统转移方法, 基于直接生长方法进行集成二维材料非线性光学研究的优势以及未来需要解决的技术难点; 指明了该领域未来的研究发展趋势; 并指出直接在各种成熟的光子平台上生长二维材料进行集成非线性光学特性的研究会对未来光通信、信号处理、光传感以及量子技术等领域的发展产生深远影响.Photonic platforms with excellent nonlinear optical characteristics are very important to improve the devices' performance parameters such as integration, modulation speeds and working bandwidths for all-optical signal processing. The traditional processing technology of photonic platforms based on silicon, silicon nitride and silicon oxide is mature, but the nonlinear function of these optical platforms is limited due to the characteristics of materials; Although two-dimensional (2D) materials possess excellent nonlinear optical properties, their nonlinear potentials cannot be fully utilized because of their atomic layer thickness. Integrating 2D materials with mature photonic platforms can significantly improve the interaction between light and matter, give full play to the potentials of 2D materials in the field of nonlinear optics, and improve the nonlinear optical performances of the integrated platforms on the basis of fully utilizing the mature processing technology of the photonic platforms. Based on the above ideas, starting from the basic principle of nonlinear optics (Section 2), this review combs the research progress of various nonlinear photonic platforms (resonators, metasurfaces, optical fibers, on-chip waveguides, etc.) heterogeneously integrated with 2D materials, realized by traditional transfer methods (Section 3) and emerging direct-growth methods (Section 4) in recent years, and the introduction is divided into second-order and third-order nonlinearity. Comparing with the transfer methods, the advantages of using direct-growth methods to realize the heterogeneous integration of 2D materials and photonic platforms for the study of nonlinear optics are expounded, and the technical difficulties to be overcome in preparing the actual devices are also pointed. In the future, we can try to grow 2D materials directly onto the surfaces of various cavities to study the enhancement of second-order nonlinearity; we can also try to grow 2D materials directly onto the on-chip waveguides or microrings to study the enhancement of third-order nonlinearity. Generally speaking, the research on integrated nonlinearity by directly growing 2D materials onto various photonic structures has aroused great interest of researchers in this field. As time goes on, breakthrough progress will be made in this field, and technical problems such as continuous growth of high-quality 2D materials onto photonic structures and wafer-level large-scale preparation will be broken through, further improving the performance parameters of chips and laying a good foundation for optical communication, signal processing, optical sensing, all-optical computing, quantum technology and so on.
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Keywords:
- silicon/silicon nitride photonic platforms /
- two-dimensional materials /
- photonic integration /
- nonlinearity enhancement /
- growth of material
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图 1 集成二维材料非线性光子平台研究框架
Fig. 1. Research framework of nonlinear photonic platforms integrated with two-dimensional materials.
图 2 非线性光学过程中典型的频率转换过程能量示意图, 其中包括二阶非线性过程中的SHG (a) 和SFG (b) 以及三阶非线性过程中的THG (c) 和FWM (d)
Fig. 2. Typical energy diagrams of frequency conversion process in nonlinear optical processes, including SHG (a) and SFG (b) in second-order nonlinear process and THG (c) and FWM (d) in third-order nonlinear process.
图 3 二维材料中腔增强的SHG过程研究进展 (a) 二维材料中SHG的光机械增强[64]; (b) 二维MoS2中腔增强的SHG[65]; (c) 单层WSe2[66]以及 (d)层状GaSe[68]中Si光子晶体腔增强的SHG; (e) 单层WS2-Ag纳米腔中谐波谐振增强的SHG[69]; (f) 单层WS2置于Si基底上实现SHG的增强[70]
Fig. 3. Research progress on cavity-enhanced SHG process in 2D materials: (a) Optomechanical enhancement of SHG in 2D material[64]; (b) microcavity enhanced SHG in 2D MoS2[65]; silicon photonic crystal cavity enhanced SHG from monolayer WSe2[66] (c) and layered GaSe[68] (d); (e) harmonic resonance enhanced SHG in a monolayer WS2–Ag nanocavity[69]; (f) enhancement of SHG from monolayer WS2 on Si substrate[70].
图 4 二维材料中等离激元增强的SHG过程研究进展 (a) 柔性衬底上单层WS2中等离激元增强的SHG[72]; (b) 单层WS2中等离激元增强的光学非线性[73]; (c) WS2–Au纳米孔洞集成超表面在可见光波段实现非线性超透镜[74]; (d) 单层MoS2置于悬空的金属纳米结构上通过等离激元谐振效应实现SHG的增强[75]
Fig. 4. Research progress on plasmonic-enhanced SHG process in 2D materials: (a) Plasmon-enhanced SHG from monolayer WS2 on flexible substrates[72]; (b) plasmonic enhancement of optical nonlinearity in monolayer WS2[73]; (c) WS2–Au nanohole hybrid metasurface for nonlinear metalenses in the visible region[74]; (d) enhanced SHG in monolayer MoS2 on suspended metallic nanostructures by plasmonic resonances[75].
图 5 二维材料中介质超表面增强的SHG过程研究进展 (a) Si超表面与二维GaSe集成实现SHG和SFG[77]; (b) WS2单层中准BIC谐振增强的SHG[78]; (c) 借助Si3N4亚波长光栅结构实现单层MoS2中SHG的增强[79]; (d) 混合介电超表面上MoS2单层中SHG的增强[80]
Fig. 5. Research progress on SHG process enhanced by dielectric metasurface in 2D materials: (a) SHG and SFG from a Si metasurface integrated with 2D GaSe[77]; (b) quasi-BIC resonant enhancement of SHG in WS2 Monolayers[78]; (c) enhancement of SHG in monolayer MoS2 by a Si3N4 subwavelength grating[79]; (d) hybrid dielectric metasurfaces for enhancing SHG in MoS2 monolayers[80].
图 6 (a) 基于转移方法制备的单层WS2-光纤纳米线混合结构实现SHG的增强[81]. (b)—(e) 基于溶液法制备的二维材料-光纤集成结构实现二阶非线性过程增强的研究进展 (b) 少层GaSe辅助光学微光纤实现高效的二阶非线性过程[82]; (c) 连续波泵浦的InSe集成的微光纤中频率上转换[84]; (d) 填充有GaSe纳米片的HCF结构示意图[85]; (e) GaSe纳米片集成的SCF实现SHG过程[86]
Fig. 6. (a) Enhanced SHG in hybrid WS2-optical-fiber-nanowire structureprepared by transfer method[81]. (b)–(e) Research progress on enhancement of second-order nonlinear process of 2D material-optical fiber integrated structures prepared by solution methods: (b) High-efficiency second-order nonlinear processes in an optical microfibre assisted by few-layer GaSe[82]; (c) continuous-wave pumped frequency upconversions in an InSe-integrated microfiber[84]; (d) schematic of a HCF filled with GaSe nanosheets[85]; (e) SCF with embedded GaSe nanosheets for SHG[86].
图 7 基于转移方法制备的二维材料-片上集成平台中二阶非线性增强的研究进展 (a) Si波导上二维MoSe2中SHG的增强[87]; (b) 单层MoS2与Ti02纳米线集成实现SHG的增强[88]; (c) 少层GaSe与Si3N4微环集成实现高效的SHG和SFG过程[89]; (d) SHG辅助的SnP2Se6光电探测器[90]
Fig. 7. Research progress on enhanced second-order nonlinear process enabled by integrated 2D material - on-chip integrated platforms prepared by transfer methods: (a) Enhanced SHG from two-dimensional MoSe2 on a Si waveguide[87]; (b) enhancement of SHG in a TiO2 nanowire integrated with monolayer MoS2[88]; (c) high-efficiency SHG and SFG in a Si3N4 microring integrated with few-layer GaSe[89]; (d) a schematic of the SHG-assisted SnP2Se6 photodetector[90].
图 9 石墨烯/Si非线性脊形波导中的超快脉冲传播[108] (a) 超快脉冲在石墨烯/Si混合脊形波导中传播的示意图; Si脊形波导 (b-i), 石墨烯/Si脊形波导 (c-i) 以及石墨烯/Si类狭缝波导 (d-i) 的示意图; 飞秒脉冲沿着Si脊形波导 (b-ii), 石墨烯/Si脊形波导 (c-ii) 以及石墨烯/Si类狭缝波导 (d-ii) 传播后的实验测得的以及数值计算的输出光谱
Fig. 9. Ultra-fast pulse propagation in nonlinear graphene/Si ridge waveguide[108]: (a) Schematic of ultra-fast pulse propagation along the hybrid graphene/silicon ridge waveguide; schematic of a Si ridge waveguide (b-i), a graphene/Si ridge waveguide (c-i) and a graphene/Si slot-like ridge waveguide (d-i); experimentally measured and numerically calculated output spectra of the femtosecond pulses propagating along the Si ridge waveguide (b-ii), the graphene/Si ridge waveguide (c-ii), and the graphene/Si slot-like ridge waveguide (d-ii).
图 10 基于转移方法实现片上集成二维材料三阶非线性增强的研究进展 (a) Si-石墨烯微环谐振腔集成实现FWM的增强[111]; (b) Si/石墨烯混合波导实现SPM的增强[110]; (c) GO/Hydex混合波导实现FWM的增强[122]; (d) 二维GO薄膜与Si纳米线集成实现SPM的增强[124]; (e) MoS2置于Si上波导实现光学克尔非线性的增强[130]; (f) 少层WS2与Si3N4波导异质集成实现非线性的增强[132]
Fig. 10. Research progress on third-order nonlinear enhancement of on-chip integrated 2D materials based on transfer methods: (a) Enhanced FWM in a Si-graphene microring resonator[111]; (b) enhanced SPM of graphene/Si hybrid waveguide[110]; (c) enhanced FWM in GO/hydex hybrid waveguide[122]; (d) enhanced SPM in Si nanowires integrated with 2D GO Films[124]; (e) enhanced optical Kerr nonlinearity of MoS2 on Si waveguides[130]; (f) enhancing Si3N4 waveguide nonlinearity with heterogeneous integration of few-layer WS2[132].
图 11 基于直接生长法制备的二阶非线性增强的二维材料-光纤集成平台 (a) 两步生长方法示意图[137]; (b) 光纤中嵌入二维材料实现SHG[138]
Fig. 11. 2D material-optical fiber integrated platforms with enhanced second-order nonlinear process based on direct growth methods: (a) Schematic of the two-step growth method[137]; (b) in-fiber SHG with embedded 2D materials[138].
图 12 基于直接生长法制备的二阶非线性增强的二维材料-波导集成平台 (a) Si3N4波导上直接生长WS2实现SHG增强的示意图[147]; (b) Si波导上直接生长单层MoS2的概念示意图[148]
Fig. 12. Enhanced second-order nonlinear process in 2D material-waveguides integrated platforms based on direct growth methods: (a) Schematic diagram of SHG enhancement of the Si3N4 waveguides with directly grown WS2[147]; (b) concept schematic of Si waveguides with directly grown monolayer MoS2[148].
图 13 基于直接生长法制备的三阶非线性的增强二维材料-光纤集成平台 (a) 嵌入MoS2的HCF中SHG和THG的示意图[137]; (b) 使用原子层厚度的半导体对光纤进行规模化的功能化[149]; (c) 石墨烯-PCF中产生谐波的示意图[150]
Fig. 13. 2D material-fiber integrated platforms with enhanced third-order nonlinear process based on direct growth methods: (a) schematics of SHG and THG in MoS2-embedded HCF[137]; (b) scalable functionalization of optical fibers using atomically thin semiconductors[149]; (c) schematic of harmonic generations in graphene-PCF[150].
表 1 基于Z扫描法测量出的不同二维材料的非线性折射率
${n_2}$ Table 1. Nonlinear refractive index n2 of different 2D materials measured by Z-scan method.
二维材料 厚度 泵浦波长/nm n2 /(m2·W–1) 参考文献 发表年度 气相生长的石墨烯 单层 1550 –10–11 [92] 2012 5—7层 1150—2400 –(0.55-2.5) × 10–13 [93] 2016 化学合成的氧化石墨烯 2 μm 800 7.5 × 10–13 [94] 2014 1 μm 1550 4.5 × 10–14 [95] 2017 气相生长的硫化钼 25 μm 1064 (1.88 ± 0.48) × 10–16 [96] 2016 气相生长的硫化钨 0.75 nm 1040 (1.28 ± 0.03) × 10–14 [97] 2016 气相生长的硒化钨 11.4 nm 1040 (–1.87 ± 0.47) × 10–15 机械剥离的黑磷 15 nm 1030 –1.64 × 10–12 [98] 2018 气相生长的硒化铂 20 层 800 –1.33×10–15 [99] 2020 
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