Anomalous gate-tunable capacitance in Van der Waals heterostructures

Linshang Chen; Haoran Long; Heng Wu; Rui Mei; Zhengyu Su; Mengjie Feng; Jiang-Bin Wu; Kenji Watanabe; Takashi Taniguchi; Xuewei Cao; Zhongming Wei; Ping-Heng Tan; Yanmeng Shi

doi:10.1088/1674-4926/26040034

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Anomalous gate-tunable capacitance in Van der Waals heterostructures

Linshang Chen^{1, 2}, Haoran Long^{1, 2}, Heng Wu^{1, 2}, Rui Mei^{1, 2}, Zhengyu Su^{1, 2}, Mengjie Feng¹, Jiang-Bin Wu¹, Kenji Watanabe^{4, 5}, Takashi Taniguchi^{4, 5}, Xuewei Cao³, Zhongming Wei^{1, 2,}, Ping-Heng Tan^{1, 2,} and Yanmeng Shi^{1, 2,}

+ Author Affiliations

1. State Key Laboratory of Semiconductor Physics and Chip Technologies, Institute of Semiconductors, Chinese Academy of Sciences, Beijing 100083, China
2. Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China
3. School of Physics, Nankai University, Tianjin 300071, China
4. Research Center for Functional Materials, National Institute for Materials Science, Tsukuba, Japan
5. International Center for Material Nanoarchitectonics, National Institute for Materials Science, Tsukuba, Japan

Author Bio:

Linshang Chen got his bachelor’s degree in 2022 and his master’s degree in 2025 from Nankai University. Now he is a doctoral student at Institute of Semiconductors under the supervision of Prof. Yanmeng Shi on quantum transports in low-dimensional systems.

Zhongming Wei received his B.S. from Wuhan University (China) in 2005, and Ph.D. from Institute of Chemistry, Chinese Academy of Sciences in 2010 under the supervision of Prof. Daoben Zhu. From August 2010 to January 2015, he worked as a postdoctoral fellow and then Assistant Professor in Prof. Thomas Bjørnholm's group at University of Copenhagen, Denmark. Currently, he is working as a Professor at Institute of Semiconductors, Chinese Academy of Sciences. His research interests include low-dimensional semiconductors and their (opto-)electronic devices.(https://www.jos.ac.cn/article/doi/10.1088/1674-4926/44/1/010101).

Ping-Heng Tan is a Professor at the State Key Laboratory of Semiconductor Physics and Chip Technologies, Institute of Semiconductors, Chinese Academy of Sciences. He obtained BS (1996) in Physics from Peking University, PhD (2001) from Institute of Semiconductors, Chinese Academy of Sciences. He worked at Walter Schottky Institute, Technische Universitaet Muenchen as a Postdoc Research Associate from 2001−2003. He was a KC-Wong Royal Society Fellow at Cambridge University from 2006−2007. His current research is on two-dimensional layered materials, nanocarbon materials and low-dimensional semiconductor materials. He was supported by National Science Fund for Distinguished Young Scholars in 2012.(https://www.jos.ac.cn/en/article/doi/10.1088/1674-4926/26010049).

Corresponding author: Zhongming Wei, zmwei@semi.ac.cn; Ping-Heng Tan, phtan@semi.ac.c; Yanmeng Shi, ymshi@semi.ac.cn

DOI: 10.1088/1674-4926/26040034CSTR: 32376.14.1674-4926.26040034

Abstract: The ferroelectricity emerging in non-polar graphene/hexagonal boron nitride (hBN) heterostructures has drawn considerable attention because of its fascinating properties and promising high-frequency electrical polarization switching. Yet, the underlying mechanism is still under debate. Here in twisted double bilayer graphene (TDBLG) aligned with its neighboring hBN, we observed two types of hysteresis - delayed hysteresis in top gate induced by the anomalous screening, and advanced hysteresis in back gate caused by the anomalous gate-tunable capacitance. To investigate the role played by moiré potential in the anomalous hysteresis, we studied a moiréless graphene heterostructure. Unexpectedly, we observed exactly the same phenomena in this control device. Our findings suggest that the anomalous ferroelectricity in graphene/hBN heterostructures may originate from the dielectric material hBN, calling for further structural investigations on hBN. Further analysis indicates that those hysteresis can be asymmetric and scalable with applied external electric fields, distinct from conventional ferroelectric switching with well-defined coercive fields. The observation of gate-tunable capacitance provides more insights in the mysterious ferroelectricity in graphene/hBN heterostructures, and should enable new design of memory devices such as memcapacitor based on tunable capacitance.

Keywords: graphene, two-dimensional materials, van der Waals heterostructures, electrical hysteresis, anomalous screening

References

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Fig. 1. (Color online) Two types of hysteresis in TDBLG device. (a) Schematic of dual-gate TDBLG device. (b) Four-terminal longitudinal resistance R_xx as a function of top gate voltage V_tg, for forward (blue) and backward (orange) scans, respectively, when V_bg = 0. (c) Four-terminal longitudinal resistance as a function of back gate voltage V_bg, for forward (blue) and backward (orange) scans, respectively when V_tg = 0.

DownLoad: Full-Size Img PowerPoint

Fig. 2. (Color online) Layer-specific anomalous screening and hysteretic transport behaviour as a function of top gate voltage. (a, b) Four-terminal longitudinal resistance mappings R_xx(V_tg, V_bg) for forward (a) and backward scans (b) of V_tg. Black arrows indicate the fast-scan directions of V_tg and stepping direction of V_bg. (c) The resistance difference between (a) and (b). (d) Carrier density extracted from Hall effect measurement as a function of V_tgwhen V_bg = 0. The fitted top gate capacitance C_tg in normal regime is ≈ 5.3 × 10⁻⁴ F·m⁻².

DownLoad: Full-Size Img PowerPoint

Fig. 3. (Color online) The anomalous gating and hysteretic transport behaviour as a function of back gate voltage. (a, b) Dual-gate mapping of four-terminal longitudinal resistance R_xx(V_bg, V_tg) for forward (a) and backward (b) scans of V_bg. The black arrows indicate the sweeping and stepping directions of gate voltages. (c) The resistance difference between (a) and (b). (d, e) Hall carrier density as a function of V_bg when V_bg sweep limit is between (−10V, +10V) and the system is stuck in the anomalous region (d), and when V_bg sweep limit is between (−80V, +80V) (e). Scattered lines are experimental data, and dash lines are linear fittings. The fitted effective capacitance C_effective in (d) is ≈ 1.7 × 10⁻⁴ F·m⁻² (magenta dash line). The fitted effective capacitance C_effective in (e) is ≈ 1.7 × 10⁻⁴ F·m⁻² (cyan dash lines) and ≈ 0.85 × 10⁻⁴ F·m⁻² (magenta dash lines). (f) R_xx (n_ext) when D_ext = 0.1 V·nm⁻¹, showing no hysteresis. (g) The resistance difference mapping ΔR_xx (D_ext, n_ext) between forward and backward scans of D_ext.

DownLoad: Full-Size Img PowerPoint

Fig. 4. (Color online) Anomalous screening and gate-tunable capacitance in a moiréless MLG device. (a) Schematic (left) and the optical microscope picture of the moiréless MLG device structure. Scale bar is 10 μm. (b, c) The different hysteretic behaviours as a function of V_tg (b) and V_bg (c). (d, e) The dependence of n_Hall on V_tg (d) and V_bg (e). The fitted top gate capacitance in (d) is C_tg ≈ 3.6 × 10⁻⁴ F·m⁻² (magenta dash line). The fitted effective capacitances of back gate in (e) are C_effective ≈ 2 × 10⁻⁴ F·m⁻² (cyan dash line) and ≈ 0.68 × 10⁻⁴ F·m⁻² (magenta dash line). (f) Line traces of R_xx (n_ext) at D_ext = 0 and 0.33 V·nm⁻¹ (left) R_xx (D_ext) (right). The data is taken at T = 200 K.

DownLoad: Full-Size Img PowerPoint

Fig. 5. (Color online) Unconventional hysteresis loops in moiréless MLG device. (a) Asymmetric and scalable hysteresis loops obtained over different V_tg ranges: (−6, −2V) and (−6, 0V) on the hole-doped side (left), and (+2, +6V) and (0, +6V) on the electron-doped side (right). (b) Asymmetric and scalable hysteresis loops obtained over different V_bg ranges: (−15, −5V), (−22, +2V) and (−35, +20V) in the left panel, and (+5, +15V), (−2, +22V) and (−20, +35V) in the right panel. Blue and orange symbols indicate forward and backward gate sweeps, respectively.

DownLoad: Full-Size Img PowerPoint

[1]	Woods C R, Ares P, Nevison-Andrews H, et al. Charge-polarized interfacial superlattices in marginally twisted hexagonal boron nitride. Nat Commun, 2021, 12: 347 doi: 10.1038/s41467-020-20667-2
[2]	Yasuda K, Wang X R, Watanabe K, et al. Stacking-engineered ferroelectricity in bilayer boron nitride. Science, 2021, 372(6549): 1458 doi: 10.1126/science.abd3230
[3]	Vizner Stern M, Waschitz Y, Cao W, et al. Interfacial ferroelectricity by van der Waals sliding. Science, 2021, 372(6549): 1462 doi: 10.1126/science.abe8177
[4]	Rogée L, Wang L J, Zhang Y, et al. Ferroelectricity in untwisted heterobilayers of transition metal dichalcogenides. Science, 2022, 376(6596): 973 doi: 10.1126/science.abm5734
[5]	Fei Z Y, Zhao W J, Palomaki T A, et al. Ferroelectric switching of a two-dimensional metal. Nature, 2018, 560(7718): 336 doi: 10.1038/s41586-018-0336-3
[6]	Sui F R, Jin M, Zhang Y Y, et al. Sliding ferroelectricity in van der Waals layered γ-InSe semiconductor. Nat Commun, 2023, 14: 36 doi: 10.1038/s41467-022-35490-0
[7]	Deb S, Cao W, Raab N, et al. Cumulative polarization in conductive interfacial ferroelectrics. Nature, 2022, 612(7940): 465 doi: 10.1038/s41586-022-05341-5
[8]	Meng P, Wu Y Z, Bian R J, et al. Sliding induced multiple polarization states in two-dimensional ferroelectrics. Nat Commun, 2022, 13: 7696 doi: 10.1038/s41467-022-35339-6
[9]	Wang X R, Yasuda K, Zhang Y, et al. Interfacial ferroelectricity in rhombohedral-stacked bilayer transition metal dichalcogenides. Nat Nanotechnol, 2022, 17(4): 367 doi: 10.1038/s41565-021-01059-z
[10]	Weston A, Castanon E G, Enaldiev V, et al. Interfacial ferroelectricity in marginally twisted 2D semiconductors. Nat Nanotechnol, 2022, 17(4): 390 doi: 10.1038/s41565-022-01072-w
[11]	Zheng Z R, Ma Q, Bi Z, et al. Unconventional ferroelectricity in moiré heterostructures. Nature, 2020, 588(7836): 71 doi: 10.1038/s41586-020-2970-9
[12]	Niu R R, Li Z X, Han X Y, et al. Giant ferroelectric polarization in a bilayer graphene heterostructure. Nat Commun, 2022, 13: 6241 doi: 10.1038/s41467-022-34104-z
[13]	Klein D R, Xia L Q, MacNeill D, et al. Electrical switching of a bistable moiré superconductor. Nat Nanotechnol, 2023, 18(4): 331 doi: 10.1038/s41565-022-01314-x
[14]	Ren L L, Dong B J. Ferroelectric polarization in an h-BN-encapsulated 30°-twisted bilayer–graphene heterostructure. Magnetochemistry, 2023, 9(5): 116 doi: 10.3390/magnetochemistry9050116
[15]	Zheng Z R, Wang X Q, Zhu Z Y, et al. Electronic ratchet effect in a moiré system: signatures of excitonic ferroelectricity. arXiv preprint, 2023, doi: 10.48550/arXiv.2306.03922
[16]	Zhang L, Ding J, Xiang H X, et al. Electronic ferroelectricity in monolayer graphene moiré superlattices. Nat Commun, 2024, 15: 10905 doi: 10.1038/s41467-024-55281-z
[17]	Jiang S Q, Du R J, Jiang J W, et al. The interplay of ferroelectricity and magneto-transport in non-magnetic moiré superlattices. Nat Commun, 2025, 16: 5640 doi: 10.1038/s41467-025-60783-5
[18]	Lin F R, Xuan X Y, Cao Z H, et al. Room temperature ferroelectricity in monolayer graphene sandwiched between hexagonal boron nitride. Nat Commun, 2025, 16: 1189 doi: 10.1038/s41467-025-56065-9
[19]	Yan X D, Zheng Z R, Sangwan V K, et al. Moiré synaptic transistor with room-temperature neuromorphic functionality. Nature, 2023, 624(7992): 551 doi: 10.1038/s41586-023-06791-1
[20]	Wang P F, Chen M Y, Xie Y Q, et al. Moiré synaptic transistor for homogeneous-architecture reservoir computing. Chin Phys Lett, 2023, 40(11): 117201 doi: 10.1088/0256-307X/40/11/117201
[21]	Singh A, Xu S G, Sarsfield P J, et al. Stacking-induced ferroelectricity in tetralayer graphene. Nano Lett, 2026, 26(14): 4642 doi: 10.1021/acs.nanolett.6c00118
[22]	Maffione G, Farrar L S, Kapfer M, et al. Twist-angle-controlled anomalous gating in bilayer graphene/BN heterostructures. Nat Mater, 2026, doi: 10.1038/s41563-026-02667-7
[23]	Niu R R, Li Z X, Han X Y, et al. Ferroelectricity with concomitant Coulomb screening in van der Waals heterostructures. Nat Nanotechnol, 2025, 20(3): 346 doi: 10.1038/s41565-024-01846-4
[24]	Zhang T Y, Wang Y Y, Xue H X, et al. Observation of unconventional ferroelectricity in non-moiré graphene on hexagonal boron nitride boundaries and interfaces. arXiv preprint, 2026, doi: 10.48550/arXiv.2601.05621
[25]	Waters D, Waleffe D, Thompson E, et al. Anomalous hysteresis in graphite/boron nitride transistors. Nano Lett, 2025, 25(21): 8768 doi: 10.1021/acs.nanolett.5c01799
[26]	Liu X M, Hao Z Y, Khalaf E, et al. Tunable spin-polarized correlated states in twisted double bilayer graphene. Nature, 2020, 583(7815): 221 doi: 10.1038/s41586-020-2458-7
[27]	Shen C, Chu Y B, Wu Q S, et al. Correlated states in twisted double bilayer graphene. Nat Phys, 2020, 16(5): 520 doi: 10.1038/s41567-020-0825-9
[28]	Cao Y, Rodan-Legrain D, Rubies-Bigorda O, et al. Tunable correlated states and spin-polarized phases in twisted bilayer–bilayer graphene. Nature, 2020, 583(7815): 215 doi: 10.1038/s41586-020-2260-6
[29]	Chen S W, He M H, Zhang Y H, et al. Electrically tunable correlated and topological states in twisted monolayer–bilayer graphene. Nat Phys, 2021, 17(3): 374 doi: 10.1038/s41567-020-01062-6
[30]	He M H, Li Y H, Cai J Q, et al. Symmetry breaking in twisted double bilayer graphene. Nat Phys, 2021, 17(1): 26 doi: 10.1038/s41567-020-1030-6
[31]	Park J M, Cao Y, Watanabe K, et al. Tunable strongly coupled superconductivity in magic-angle twisted trilayer graphene. Nature, 2021, 590(7845): 249 doi: 10.1038/s41586-021-03192-0
[32]	Bistritzer R, MacDonald A H. Moiré bands in twisted double-layer graphene. Proc Natl Acad Sci U S A, 2011, 108(30): 12233 doi: 10.1073/pnas.1108174108
[33]	Jindal A, Saha A, Li Z Z, et al. Coupled ferroelectricity and superconductivity in bilayer Td-MoTe₂. Nature, 2023, 613(7942): 48 doi: 10.1038/s41586-022-05521-3
[34]	Du R J, Xiao J K, Zhang D, et al. Ferroelectricity in twisted double bilayer graphene. 2D Mater, 2024, 11(2), 025015
[35]	Yang L, Ding S P, Gao J H, et al. Atypical sliding and moiré ferroelectricity in pure multilayer graphene. Phys Rev Lett, 2023, 131(9): 096801 doi: 10.1103/PhysRevLett.131.096801
[36]	Garcia-Ruiz A, Enaldiev V, McEllistrim A, et al. Mixed-stacking few-layer graphene as an elemental weak ferroelectric material. Nano Lett, 2023, 23(10): 4120 doi: 10.1021/acs.nanolett.2c04723
[37]	Martinez-Rincon J, Di Ventra M, Pershin Y V. Solid-state memcapacitive system with negative and diverging capacitance. Phys Rev B, 2010, 81(19): 195430 doi: 10.1103/PhysRevB.81.195430

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Received: 18 June 2026 Revised: 01 July 2026 Online: Accepted Manuscript: 17 September 2026

Article Navigation > Journal of Semiconductors > 2026 > Accepted Manuscript

Linshang Chen, Haoran Long, Heng Wu, Rui Mei, Zhengyu Su, Mengjie Feng, Jiang-Bin Wu, Kenji Watanabe, Takashi Taniguchi, Xuewei Cao, Zhongming Wei, Ping-Heng Tan, Yanmeng Shi. Anomalous gate-tunable capacitance in Van der Waals heterostructures[J]. Journal of Semiconductors, 2026, In Press. doi: 10.1088/1674-4926/26040034 ****L S Chen, H R Long, H Wu, R Mei, Z Y Su, M J Feng, J - B Wu, K Watanabe, T K S T N G chi, X W Cao, Z M Wei, P - H Tan, and Y M Shi, Anomalous gate-tunable capacitance in Van der Waals heterostructures[J]. J. Semicond., 2026, accepted doi: 10.1088/1674-4926/26040034

Citation:

L S Chen, H R Long, H Wu, R Mei, Z Y Su, M J Feng, J - B Wu, K Watanabe, T K S T N G chi, X W Cao, Z M Wei, P - H Tan, and Y M Shi, Anomalous gate-tunable capacitance in Van der Waals heterostructures[J]. J. Semicond., 2026, accepted doi: 10.1088/1674-4926/26040034

Citation:

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Anomalous gate-tunable capacitance in Van der Waals heterostructures

DOI: 10.1088/1674-4926/26040034

CSTR: 32376.14.1674-4926.26040034

Linshang Chen^{1, 2},
Haoran Long^{1, 2},
Heng Wu^{1, 2},
Rui Mei^{1, 2},
Zhengyu Su^{1, 2},
Mengjie Feng¹,
Jiang-Bin Wu¹,
Kenji Watanabe^{4, 5},
Takashi Taniguchi^{4, 5},
Xuewei Cao³,
Zhongming Wei^{1, 2,},
Ping-Heng Tan^{1, 2,},
Yanmeng Shi^{1, 2,}

1.
State Key Laboratory of Semiconductor Physics and Chip Technologies, Institute of Semiconductors, Chinese Academy of Sciences, Beijing 100083, China
2.
Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China
3.
School of Physics, Nankai University, Tianjin 300071, China
4.
Research Center for Functional Materials, National Institute for Materials Science, Tsukuba, Japan
5.
International Center for Material Nanoarchitectonics, National Institute for Materials Science, Tsukuba, Japan

More Information

Linshang Chen got his bachelor’s degree in 2022 and his master’s degree in 2025 from Nankai University. Now he is a doctoral student at Institute of Semiconductors under the supervision of Prof. Yanmeng Shi on quantum transports in low-dimensional systems
Zhongming Wei received his B.S. from Wuhan University (China) in 2005, and Ph.D. from Institute of Chemistry, Chinese Academy of Sciences in 2010 under the supervision of Prof. Daoben Zhu. From August 2010 to January 2015, he worked as a postdoctoral fellow and then Assistant Professor in Prof. Thomas Bjørnholm's group at University of Copenhagen, Denmark. Currently, he is working as a Professor at Institute of Semiconductors, Chinese Academy of Sciences. His research interests include low-dimensional semiconductors and their (opto-)electronic devices.(https://www.jos.ac.cn/article/doi/10.1088/1674-4926/44/1/010101)
Ping-Heng Tan is a Professor at the State Key Laboratory of Semiconductor Physics and Chip Technologies, Institute of Semiconductors, Chinese Academy of Sciences. He obtained BS (1996) in Physics from Peking University, PhD (2001) from Institute of Semiconductors, Chinese Academy of Sciences. He worked at Walter Schottky Institute, Technische Universitaet Muenchen as a Postdoc Research Associate from 2001−2003. He was a KC-Wong Royal Society Fellow at Cambridge University from 2006−2007. His current research is on two-dimensional layered materials, nanocarbon materials and low-dimensional semiconductor materials. He was supported by National Science Fund for Distinguished Young Scholars in 2012.(https://www.jos.ac.cn/en/article/doi/10.1088/1674-4926/26010049)
Corresponding author: zmwei@semi.ac.cn; phtan@semi.ac.c; ymshi@semi.ac.cn
Received Date: 2026-06-18
Revised Date: 2026-07-01

Available Online: 2026-09-17

Abstract

Abstract

The ferroelectricity emerging in non-polar graphene/hexagonal boron nitride (hBN) heterostructures has drawn considerable attention because of its fascinating properties and promising high-frequency electrical polarization switching. Yet, the underlying mechanism is still under debate. Here in twisted double bilayer graphene (TDBLG) aligned with its neighboring hBN, we observed two types of hysteresis - delayed hysteresis in top gate induced by the anomalous screening, and advanced hysteresis in back gate caused by the anomalous gate-tunable capacitance. To investigate the role played by moiré potential in the anomalous hysteresis, we studied a moiréless graphene heterostructure. Unexpectedly, we observed exactly the same phenomena in this control device. Our findings suggest that the anomalous ferroelectricity in graphene/hBN heterostructures may originate from the dielectric material hBN, calling for further structural investigations on hBN. Further analysis indicates that those hysteresis can be asymmetric and scalable with applied external electric fields, distinct from conventional ferroelectric switching with well-defined coercive fields. The observation of gate-tunable capacitance provides more insights in the mysterious ferroelectricity in graphene/hBN heterostructures, and should enable new design of memory devices such as memcapacitor based on tunable capacitance.
- graphene,
- two-dimensional materials,
- van der Waals heterostructures,
- electrical hysteresis,
- anomalous screening

Supplementary materials to this article can be found online at https://doi.org/10.1088/1674-4926/26040034.

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