| 研究生: |
楊靖緯 Yang, Jing-Wei |
|---|---|
| 論文名稱: |
利用 hBN 緩衝層進行 Hf₀.₅Zr₀.₅O₂/WSe₂ 異質結構之鐵電介面工程研究 Ferroelectric Interface Engineering in Hafnium Zirconium Oxide/Tungsten Diselenide Heterostructures Using hBN Buffer Layers |
| 指導教授: |
路克史密斯
W. Smith, Luke |
| 學位類別: |
碩士 Master |
| 系所名稱: |
理學院 - 物理學系 Department of Physics |
| 論文出版年: | 2026 |
| 畢業學年度: | 114 |
| 語文別: | 英文 |
| 論文頁數: | 88 |
| 中文關鍵詞: | 負電容 、Hf₀.₅Zr₀.₅O₂ (HZO) 、懸浮式 HZO 薄膜 、六方氮化硼(hBN) 、WSe₂ 、介面工程 、二維場效電晶體 |
| 外文關鍵詞: | negative capacitance, Hf₀.₅Zr₀.₅O₂ (HZO), freestanding HZO thin film, hexagonal boron nitride (hBN), WSe₂, interface engineering, two-dimensional field-effect transistors |
| 相關次數: | 點閱:4 下載:0 |
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隨著人工智慧(AI)、物聯網(IoT)、高效能運算(HPC)及邊緣運算等技術快速發展,現代電子元件對高運算效能與低功耗操作的需求日益提升。然而,傳統矽基金屬氧化物半導體場效電晶體(metal–oxide–semiconductor field-effect transistor, MOSFET)隨著元件持續微縮,逐漸受到短通道效應、漏電流增加及次臨界擺幅(subthreshold swing, SS)60 mV/dec 熱力學極限的限制,使供應電壓與功耗難以進一步降低。近年來,具負電容效應(negative capacitance, NC)的鐵電 Hf0.5Zr0.5O2(HZO)因具有 CMOS 相容性及奈米尺度下仍可維持鐵電性的優勢,被視為實現低功耗電晶體的重要候選材料。此外,二維過渡金屬二硫族化物(2D transition metal dichalcogenides, 2D TMDs)中的 WSe2 具有原子級厚度、優異的靜電控制能力及良好的載子傳輸特性,適合作為下一世代低功耗電晶體通道材料。然而,HZO 與 WSe₂ 整合過程中仍可能面臨介面缺陷(如氧空缺)及費米能階釘扎等問題,進而影響載子注入效率與元件穩定性。
為降低 HZO 薄膜於重複乾式轉移過程中的機械損傷,並提升製程效率與量測一致性,本研究提出一種結合懸浮式(freestanding)HZO 薄膜轉移製程與乾式轉移(dry transfer)二維材料的元件整合策略。預先於基板上設計局部閘極陣列(local gate array), HZO 薄膜轉移後,自陣列中選取一個局部閘極製作 WSe₂ 電晶體,而周圍其他局部閘極則分別製作金屬–絕緣體–金屬(MIM)電容及絕緣體–金屬(IM)結構以進行 PFM 、 SSPFM 等鐵電特性量測,藉此直接驗證 HZO 薄膜於完整元件製程後仍維持良好的鐵電特性。此外,於 HZO 與 WSe₂ 之間引入六方氮化硼(hBN)作為凡得瓦緩衝層,以降低介面缺陷、改善異質結構介面品質,並調控金屬接觸特性。透過光激發光譜(photoluminescence, PL)、原子力顯微鏡(atomic force microscopy, AFM)、壓電響應力顯微鏡(PFM)及溫度依賴電性量測,結合 Arrhenius 分析,以探討有效蕭特基能障與載子傳輸機制,並結合 PFM 結果探討鐵電耦合行為。
實驗結果顯示, HZO 薄膜於轉移製程後仍維持良好的鐵電特性,而 hBN 緩衝層可有效改善 HZO/WSe₂ 異質結構之介面品質,抑制介面缺陷造成的載子捕捉行為,並改善元件穩定性及載子注入特性。此外,本研究透過串聯電容模型分析,指出適當降低 hBN 厚度可改善 HZO 與 WSe2 間的電容匹配(capacitance matching)及靜電耦合。因此,未來若進一步最佳化 hBN 厚度,預期可在維持優異介面品質的同時兼顧穩定負電容操作,有望實現低功耗二維負電容電晶體。
Low-power transistors are essential for next-generation electronic systems, including artificial intelligence (AI), the Internet of Things (IoT), high-performance computing (HPC), and edge computing. However, conventional silicon-based metal–oxide–semiconductor field-effect transistors (MOSFETs) are fundamentally limited by severe short-channel effects, increased leakage current, and the thermionic subthreshold swing (SS) limit of 60 mV/dec, restricting further supply-voltage scaling and power reduction. Recently, ferroelectric hafnium zirconium oxide (Hf₀.₅Zr₀.₅O₂, HZO), owing to its negative capacitance (NC) effect, CMOS compatibility, and robust ferroelectricity at the nanoscale, has emerged as a promising candidate for low-power transistor applications. In addition, two-dimensional transition metal dichalcogenides (2D TMDs), particularly tungsten diselenide (WSe₂), possess an atomically thin body, excellent electrostatic controllability, and favorable carrier transport properties, making them attractive channel materials for next-generation low-power transistors. Nevertheless, interface defects (e.g., oxygen vacancies) and Fermi-level pinning at the HZO/WSe₂ interface remain major challenges that degrade carrier injection efficiency and device stability.
To minimize mechanical damage to HZO thin films caused by repeated dry-transfer processes while improving fabrication efficiency and measurement consistency, this study proposes a device integration strategy that combines freestanding HZO thin-film transfer with the dry transfer of two-dimensional materials. A local gate array was pre-patterned on the substrate prior to HZO transfer. After transferring the HZO thin film, one local gate was selected for WSe₂ field-effect transistor (FET) fabrication, while the surrounding local gates were utilized to fabricate metal–insulator–metal (MIM) capacitors and insulator–metal (IM) structures for ferroelectric characterization using piezoresponse force microscopy (PFM) and switching spectroscopy piezoresponse force microscopy (SSPFM). This design directly verifies that the HZO thin film retains its ferroelectric properties after the complete device fabrication process. Furthermore, a hexagonal boron nitride (hBN) layer was inserted between HZO and WSe₂ as a van der Waals buffer layer to suppress interface defects, improve the heterostructure interface quality, and modulate the metal–semiconductor contact characteristics. Photoluminescence (PL), atomic force microscopy (AFM), piezoresponse force microscopy (PFM), temperature-dependent electrical measurements, and Arrhenius analysis were employed to investigate the effective Schottky barrier and carrier transport mechanisms, while the PFM results were further correlated with the ferroelectric coupling behavior.
The experimental results demonstrate that the transferred HZO thin film retains excellent ferroelectric properties after the complete fabrication process. The hBN buffer layer effectively improves the interface quality of the HZO/WSe₂ heterostructure, suppresses carrier trapping induced by interface defects, and enhances both device stability and carrier injection characteristics. Furthermore, based on a series-capacitance model, this study demonstrates that appropriately reducing the hBN thickness can improve the capacitance matching and electrostatic coupling between the HZO layer and the WSe₂ channel. Therefore, by further optimizing the hBN thickness, stable negative-capacitance operation can be achieved while maintaining excellent interface quality, providing a promising pathway toward the realization of low-power two-dimensional negative-capacitance transistors.
[1] Zheng, F., Meng, W., & Li, L.-J. (2025). Continue the scaling of electronic devices with transition metal dichalcogenide semiconductors. Nano Letters, 25(10), 3683–3691.
[2] Cai, J. (2021, June). CMOS device technology for the next decade [Conference presentation]. 2021 IEEE Symposia on VLSI Technology and Circuits (VLSI), Kyoto, Japan.
[3] Qin, L., Li, C., Wei, Y., Hu, G., Chen, J., Li, Y., Du, C., Xu, Z., Wang, X., & He, J. (2023). Recent developments in negative capacitance gate-all-around field effect transistors: A review. IEEE Access, 11, 14028–14042.
[4] Salahuddin, S., & Datta, S. (2008). Use of negative capacitance to provide voltage amplification for low power nanoscale devices. Nano Letters, 8(2), 405–410.
[5] Khan, A. I., Chatterjee, K., Wang, B., Drapcho, S., You, L., Serrao, C., Rahman, S., Ramesh, R., & Salahuddin, S. (2015). Negative capacitance in a ferroelectric capacitor. Nature Materials, 14, 182–186.
[6] Hoffmann, M., Pešić, M., Slesazeck, S., Schroeder, U., & Mikolajick, T. (2018). On the stabilization of ferroelectric negative capacitance in nanoscale devices. Nanoscale, 10(23), 10891–10899.
[7] Radisavljevic, B., Radenovic, A., Brivio, J., Giacometti, V., & Kis, A. (2011). Single-layer MoS₂ transistors. Nature Nanotechnology, 6, 147–150.
[8] Ghosh, S., Sadaf, M. U. K., Graves, A. R., Zheng, Y., Pannone, A., Ray, S., Cheng, C.-Y., Guevara, J., Redwing, J. M., & Das, S. (2025). High-performance p-type bilayer WSe₂ field effect transistors by nitric oxide doping. Nature Communications, 16, 5649.
[9] Si, M., Jiang, C., Chung, W., Du, Y., Alam, M. A., & Ye, P. D. (2018). Steep-slope WSe₂ negative capacitance field-effect transistor. Nano Letters, 18(6), 3682–3687.
[10] Hoffmann, M., Ravindran, P. V., & Khan, A. I. (2019). Why do ferroelectrics exhibit negative capacitance? Materials, 12(22), 3743.
[11] Khan, A. I., Keshavarzi, A., & Datta, S. (2020). The future of ferroelectric field-effect transistor technology. Nature Electronics, 3, 588–597.
[12] Sales, M. G., Fields, S., Jaszewski, S., Smith, S., Mimura, T., Sarney, W. J., Najmaei, S., Ihlefeld, J. F., & McDonnell, S. (2022). WSe₂ growth on hafnium zirconium oxide by molecular beam epitaxy: The effect of the WSe₂ growth conditions on the ferroelectric properties of HZO. 2D Materials, 9(1), 015001.
[13] Huang, X., Liu, C., & Zhou, P. (2022). 2D semiconductors for specific electronic applications: From device to system. npj 2D Materials and Applications, 6, 51.
[14] Jang, J., Ra, H.-S., Ahn, J., Kim, T. W., Song, S. H., Park, S., Taniguchi, T., Watanabe, K., Lee, K., & Hwang, D. K. (2022). Fermi-level pinning-free WSe₂ transistors via 2D van der Waals metal contacts and their circuits. Advanced Materials, 34(21), 2109899.
[15] Knobloch, T., Uzlu, B., Illarionov, Y. Y., Wang, Z., Otto, M., Filipovic, L., Waltl, M., Neumaier, D., Lemme, M. C., & Grasser, T. (2022). Improving stability in two-dimensional transistors with amorphous gate oxides by Fermi-level tuning. Nature Electronics, 5, 356–366.
[16] Pande, G., Siao, J.-Y., Chen, W.-J., Lee, C.-J., Sankar, R., Chang, Y.-M., Chen, C.-D., Chang, W.-H., Chou, F.-C., & Lin, M.-T. (2020). Ultralow Schottky barriers in hexagonal boron nitride-encapsulated monolayer WSe₂ tunnel field-effect transistors. ACS Applied Materials & Interfaces, 12(16), 18667–18673.
[17] Zhang, Q., Zhang, Y., Luo, Y., & Yin, H. (2024). New structure transistors for advanced technology node CMOS ICs. National Science Review, 11(3), nwae008.
[18] Novoselov, K. S., Geim, A. K., Morozov, S. V., Jiang, D., Zhang, Y., Dubonos, S. V., Grigorieva, I. V., & Firsov, A. A. (2004). Electric field effect in atomically thin carbon films. Science, 306(5696), 666–669.
[19] Novoselov, K. S., Fal'ko, V. I., Colombo, L., Gellert, P. R., Schwab, M. G., & Kim, K. (2012). A roadmap for graphene. Nature, 490, 192–200.
[20] Li, Q. Z., Elliott, P., Dewhurst, J. K., Sharma, S., & Shallcross, S. (2021). Ab initio study of ultrafast charge dynamics in graphene. Physical Review B, 103(3), L081102.
[21] Bussolotti, F., Kawai, H., Ooi, Z. E., Chellappan, V., Thian, D., Pang, A. L. C., & Goh, K. E. J. (2018). Roadmap on finding chiral valleys: Screening 2D materials for valleytronics. Nano Futures, 2(3), 032001.
[22] Zhao, W., Ghorannevis, Z., Chu, L., Toh, M., Kloc, C., Tan, P.-H., & Eda, G. (2013). Evolution of electronic structure in atomically thin sheets of WS₂ and WSe₂. ACS Nano, 7(1), 791–797.
[23] Sahin, H., Tongay, S., Horzum, S., Fan, W., Zhou, J., Li, J., Wu, J., & Peeters, F. M. (2013). Anomalous Raman spectra and thickness-dependent electronic properties of WSe₂. Physical Review B, 87(16), 165409.
[24] Zeng, H., Liu, G.-B., Dai, J., Yan, Y., Zhu, B., He, R., Xie, L., Xu, S., Chen, X., Yao, W., & Cui, X. (2013). Optical signature of symmetry variations and spin-valley coupling in atomically thin tungsten dichalcogenides. Scientific Reports, 3, 1608.
[25] Liu, X., Xing, K., Tang, C. S., Sun, S., Chen, P., Qi, D.-C., Breese, M. B. H., Fuhrer, M. S., Wee, A. T. S., & Yin, X. (2025). Contact resistance and interfacial engineering: Advances in high-performance 2D-TMD based devices. Progress in Materials Science, 148, 101390.
[26] Shuaibu, A., Adeyemi, O. J., Ushiekpan, U. R., Olowomofe, O. G., Akinade, B. J., & Kafayat, O. A. (2019). First principle study of structural, elastic and electronic properties of hexagonal boron nitride (hex-BN) single layer. American Journal of Condensed Matter Physics, 9(1), 1–5.
[27] Fang, N., Toyoda, S., Taniguchi, T., Watanabe, K., & Nagashio, K. (2019). Full energy spectra of interface state densities for n- and p-type MoS₂ field-effect transistors. Advanced Functional Materials, 29(46), 1904465.
[28] Chouprik, A., Negrov, D., Tsymbal, E. Y., & Zenkevich, A. (2021). Defects in ferroelectric HfO₂. Nanoscale, 13(27), 11635–11678.
[29] Chen, T.-A., Chuu, C.-P., Tseng, C.-C., Wen, C.-K., Wong, H.-S. P., Pan, S., Li, R., Chao, T.-A., Chueh, W.-C., Zhang, Y., Fu, Q., Yakobson, B. I., Chang, W.-H., & Li, L.-J. (2020). Wafer-scale single-crystal hexagonal boron nitride monolayers on Cu(111). Nature, 579, 219–223.
[30] Joo, M.-K., Moon, B. H., Ji, H., Han, G. H., Kim, H., Lee, G., Lim, S. C., Suh, D., & Lee, Y. H. (2016). Electron excess doping and effective Schottky barrier reduction on the MoS₂/h-BN heterostructure. Nano Letters, 16(10), 6383–6389.
[31] Allain, A., Kang, J., Banerjee, K., & Kis, A. (2015). Electrical contacts to two-dimensional semiconductors. Nature Materials, 14, 1195–1205.
[32] Dai, S., Li, M., Wu, X., Wu, Y., Li, X., Hao, Y., & Luo, B. (2024). Combinatorial optimization of perovskite-based ferroelectric ceramics for energy storage applications. Journal of Advanced Ceramics, 13(7), 877–910.
[33] Wang, B., Huang, W., Chi, L., Al-Hashimi, M., Marks, T. J., & Facchetti, A. (2018). High-k gate dielectrics for emerging flexible and stretchable electronics. Chemical Reviews, 118(11), 5690–5754.
[34] Jiao, H., Wang, X., Wu, S., Chen, Y., Chu, J., & Wang, J. (2023). Ferroelectric field effect transistors for electronics and optoelectronics. Applied Physics Reviews, 10(1), 011310.
[35] Zagni, N., & Alam, M. A. (2021). Reliability physics of ferroelectric/negative capacitance transistors for memory/logic applications: An integrative perspective. Journal of Materials Research, 36, 4908–4918.
[36] Li, E., He, W., Wang, R., Zhang, C., Zhou, H., Liu, Y., Yuan, Y., Loh, K. P., Chu, J., & Li, W. (2025). Polarity-dependent ferroelectric modulations in two-dimensional hybrid perovskite heterojunction transistors. Nature Communications, 16, 9382.
[37] Palneedi, H., Peddigari, M., Hwang, G.-T., Jeong, D.-Y., & Ryu, J. (2018). High-performance dielectric ceramic films for energy storage capacitors: Progress and outlook. Advanced Functional Materials, 28(42), 1803665.
[38] Hoffmann, M., Slesazeck, S., & Mikolajick, T. (2021). Progress and future prospects of negative capacitance electronics: A materials perspective. APL Materials, 9(2), 020902.
[39] Wang, A., Chen, R., Yun, Y., Xu, J., & Zhang, J. (2025). Review of ferroelectric materials and devices toward ultralow voltage operation. Advanced Functional Materials, 35(7), 2412332.
[40] Chen, H., Tang, L., Liu, L., Chen, Y., Luo, H., Yuan, X., & Zhang, D. (2021). Significant improvement of ferroelectricity and reliability in Hf₀.₅Zr₀.₅O₂ films by inserting an ultrathin Al₂O₃ buffer layer. Applied Surface Science, 542, 148737.
[41] Lin, C.-Y., Chen, B.-C., Liu, Y.-C., Kuo, S.-F., Tsai, H.-C., Chang, Y.-M., Kuo, C.-Y., Chang, C.-F., Chen, J.-H., Chu, Y.-H., Yamamoto, M., Shen, C.-H., Chueh, Y.-L., Chiu, P.-W., Chen, Y.-C., Yang, J.-C., & Lin, Y.-F. (2025). Integration of freestanding hafnium zirconium oxide membranes into two-dimensional transistors as a high-κ ferroelectric dielectric. Nature Electronics, 8, 560–570.
[42] Balke, N., Bdikin, I., Kalinin, S. V., & Kholkin, A. L. (2009). Electromechanical imaging and spectroscopy of ferroelectric and piezoelectric materials: State of the art and prospects for the future. Journal of the American Ceramic Society, 92(8), 1629–1647.
[43] Gu, H., Song, B., Fang, M., Hong, Y., Chen, X., Jiang, H., Ren, W., & Liu, S. (2019). Layer-dependent dielectric and optical properties of centimeter-scale 2D WSe₂: Evolution from a single layer to few layers. Nanoscale, 11(47), 22762–22771.
[44] McCreary, K. M., Hanbicki, A. T., Sivaram, S. V., & Jonker, B. T. (2018). A- and B-exciton photoluminescence intensity ratio as a measure of sample quality for transition metal dichalcogenide monolayers. APL Materials, 6(11), 111106.
[45] Wang, X., Zhu, C., Deng, Y., Duan, R., Chen, J., Zeng, Q., Zhou, J., Fu, Q., You, L., Liu, S., Edgar, J. H., Yu, P., & Liu, Z. (2021). Van der Waals engineering of ferroelectric heterostructures for long-retention memory. Nature Communications, 12, 1109.
[46] Shu, J., Wu, G., Guo, Y., Liu, B., Wei, X., & Chen, Q. (2016). The intrinsic origin of hysteresis in MoS₂ field effect transistors. Nanoscale, 8(5), 3049–3056.
[47] Hao, T., Zeng, B., Sun, Z., Wang, Z., Jiang, Y., Peng, Q., Zheng, S., Zhou, Y., & Liao, M. (2024). Coupling effects of interface charge trapping and polarization switching in HfO₂-based ferroelectric field effect transistors. APL Materials, 12(1), 011108.
[48] Li, J., Si, M., Qu, Y., Lyu, X., Ye, P. D., & Du, Y. (2021). Quantitative characterization of ferroelectric/dielectric interface traps by pulse measurements. IEEE Transactions on Electron Devices, 68(3), 1080–1086.
[49] Jelver, L., Stradi, D., Stokbro, K., & Jacobsen, K. W. (2021). Schottky barrier lowering due to interface states in 2D heterophase devices. Nanoscale Advances, 3(2), 567–574.
[50] Tong, T., He, Y., Gao, Y., Liu, Y., Liao, K., & Li, W. (2024). Reconfigurable dielectric engineered WSe₂/HZO mem-transistor. 2D Materials, 11(4), 045012.
[51] Pang, C.-S., Zhou, R., Liu, X., Wu, P., Hung, T. Y. T., Guo, S., Zaghloul, M. E., Krylyuk, S., Davydov, A. V., Appenzeller, J., & Chen, Z. (2021). Mobility extraction in 2D transition metal dichalcogenide devices—Avoiding contact resistance implicated overestimation. Small, 17(28), 2100940.
[52] Mahlouji, R., Kessels, W. M. M. (E.), Sagade, A. A., & Bol, A. A. (2023). ALD-grown two-dimensional TiSₓ metal contacts for MoS₂ field-effect transistors. Nanoscale Advances, 5(18), 4718–4727.
[53] Vu, Q. A., Fan, S., Lee, S. H., Joo, M.-K., Yu, W. J., & Lee, Y. H. (2018). Near-zero hysteresis and near-ideal subthreshold swing in h-BN encapsulated single-layer MoS₂ field-effect transistors. 2D Materials, 5(3), 031001.
[54] Ali, F., Choi, H., Ali, N., Hassan, Y., Ngo, T. D., Ahmed, F., Park, W.-K., Sun, Z., & Yoo, W. J. (2024). Achieving near-ideal subthreshold swing in p-type WSe₂ field-effect transistors. Advanced Electronic Materials, 10(9), 2400071.
[55] Patoary, N. H., Xie, J., Zhou, G., Al Mamun, F., Sayyad, M., Tongay, S., & Sanchez Esqueda, I. (2023). Improvements in 2D p-type WSe₂ transistors towards ultimate CMOS scaling. Scientific Reports, 13, 3304.