High-κ monocrystalline dielectrics for low-power two-dimensional electronics
Source abstract
Abstract
The downscaling of complementary metal-oxide-semiconductor technology has produced breakthroughs in electronics, but more extreme scaling has hit a wall of device performance degradation. One key challenge is the development of insulators with high dielectric constant, wide bandgap and high tunnel masses. Here, we show that two-dimensional monocrystalline gadolinium pentoxide, which is devised through combining particle swarm optimization algorithm and theoretical calculations and synthesized via van der Waals epitaxy, could exhibit a high dielectric constant of ~25.5 and a wide bandgap simultaneously. A desirable equivalent oxide thickness down to 1 nm with an ultralow leakage current of ~10-4 A cm-2 even at 5 MV cm-1 is achieved. The molybdenum disulfide transistors gated by gadolinium pentoxide exhibit high on/off ratios over 108 and near-Boltzmann-limit subthreshold swing at an operation voltage of 0.5 V. We also constructed inverter circuits with high gain and nanowatt power consumption. This reliable approach to integrating ultrathin monocrystalline insulators paves the way to future nanoelectronics.
Source: europepmc · Quality: candidate unverified · Source record ↗
Research context
OpenAlex topics: Electronic and Structural Properties of Oxides · Semiconductor materials and devices · Ga2O3 and related materials
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (56)
Show source-provided references
1. Liu, Y. et al. Promises and prospects of two-dimensional transistors. Nature 591, 43–53 (2021).10.1038/s41586-021-03339-z ↗
2. Datta, S., Chakraborty, W. & Radosavljevic, M. Toward attojoule switching energy in logic transistors. Science 378, 733–740 (2022).10.1126/science.ade7656 ↗
3. Choi, Y. K. et al. Ultrathin-body SOI MOSFET for deep-sub-tenth micron era. IEEE Electron Device Lett. 21, 254–255 (2000).10.1109/55.841313 ↗
4. Zhang, Y. et al. A single-crystalline native dielectric for two-dimensional semiconductors with an equivalent oxide thickness below 0.5 nm. Nat. Electron. 5, 643–649 (2022).10.1038/s41928-022-00824-9 ↗
5. Hisamoto, D. et al. FinFET—a self-aligned double-gate MOSFET scalable to 20 nm. IEEE Trans. Electron Devices 47, 2320–2325 (2000).10.1109/16.887014 ↗
6. Robertson, J. High dielectric constant gate oxides for metal oxide Si transistors. Rep. Prog. Phys. 69, 327–396 (2006).10.1088/0034-4885/69/2/R02 ↗
7. Wang, S. et al. Two-dimensional devices and integration towards the silicon lines. Nat. Mater. 21, 1225–1239 (2022).10.1038/s41563-022-01383-2 ↗
8. Zhang, C. et al. Single-crystalline van der Waals layered dielectric with high dielectric constant. Nat. Mater. 22, 832–837 (2023).10.1038/s41563-023-01502-7 ↗
9. Le Bahers, T., Rérat, M. & Sautet, P. Semiconductors used in photovoltaic and photocatalytic devices: assessing fundamental properties from DFT. J. Phys. Chem. C 118, 5997–6008 (2014).10.1021/jp409724c ↗
10. Luo, P. et al. Molybdenum disulfide transistors with enlarged van der Waals gaps at their dielectric interface via oxygen accumulation. Nat. Electron. 5, 849–858 (2022).10.1038/s41928-022-00877-w ↗
11. Robertson, J. & Wallace, R. M. High-K materials and metal gates for CMOS applications. Mater. Sci. Eng. R. Rep. 88, 1–41 (2015).10.1016/j.mser.2014.11.001 ↗
12. Hong, S. et al. Ultralow-dielectric-constant amorphous boron nitride. Nature 582, 511–514 (2020).10.1038/s41586-020-2375-9 ↗
13. Huang, J.-K. et al. High-κ perovskite membranes as insulators for two-dimensional transistors. Nature 605, 262–267 (2022).10.1038/s41586-022-04588-2 ↗
14. Zou, X. et al. Interface engineering for high-performance top-gated MoS2 field-effect transistors. Adv. Mater. 26, 6255–6261 (2014).10.1002/adma.201402008 ↗
15. Li, W. et al. Uniform and ultrathin high-κ gate dielectrics for two-dimensional electronic devices. Nat. Electron. 2, 563–571 (2019).10.1038/s41928-019-0334-y ↗
16. Xu, Y. et al. Scalable integration of hybrid high-κ dielectric materials on two-dimensional semiconductors. Nat. Mater. 22, 1078–1084 (2023).10.1038/s41563-023-01626-w ↗
17. Illarionov, Y. Y. et al. Insulators for 2D nanoelectronics: the gap to bridge. Nat. Commun. 11, 3385 (2020).10.1038/s41467-020-16640-8 ↗
18. Wang, B. et al. High-k gate dielectrics for emerging flexible and stretchable electronics. Chem. Rev. 118, 5690–5754 (2018).10.1021/acs.chemrev.8b00045 ↗
19. Cheisson, T. & Schelter, E. J. Rare earth elements: Mendeleev’s bane, modern marvels. Science 363, 489–493 (2019).10.1126/science.aau7628 ↗
20. Voncken, J. H. L. The Rare Earth Elements: An Introduction (Springer, 2016).10.1007/978-3-319-26809-5 ↗
21. Merchant, A. et al. Scaling deep learning for materials discovery. Nature 624, 80–85 (2023).10.1038/s41586-023-06735-9 ↗
22. Zhao, Y. et al. α-Fe2O3 as a versatile and efficient oxygen atom transfer catalyst in combination with H2O as the oxygen source. Nat. Catal. 4, 684–691 (2021).10.1038/s41929-021-00659-1 ↗
23. Cheng, R. et al. Ultrathin single-crystalline CdTe nanosheets realized via van der Waals epitaxy. Adv. Mater. 29, 1703122 (2017).10.1002/adma.201703122 ↗
24. Yang, K. et al. Ultrathin high-κ antimony oxide single crystals. Nat. Commun. 11, 2502 (2020).
25. Zavabeti, A. et al. A liquid metal reaction environment for the room-temperature synthesis of atomically thin metal oxides. Science 358, 332–335 (2017).10.1126/science.aao4249 ↗
26. Liu, K. et al. A wafer-scale van der Waals dielectric made from an inorganic molecular crystal film. Nat. Electron. 4, 906–913 (2021).10.1038/s41928-021-00683-w ↗
27. Chen, J. et al. Vertically grown ultrathin Bi2SiO5 as high-κ single-crystalline gate dielectric. Nat. Commun. 14, 4406 (2023).
28. McPherson, J., Kim, J., Shanware, A., Mogul, H. & Rodriguez, J. Proposed universal relationship between dielectric breakdown and dielectric constant. In Digest. International Electron Devices Meeting 633–636 (IEEE, 2002).10.1109/IEDM.2002.1175919 ↗
29. Kang, L. et al. Electrical characteristics of highly reliable ultrathin hafnium oxide gate dielectric. IEEE Electron Device Lett. 21, 181–183 (2000).10.1109/55.830975 ↗
30. Sokolov, N. S. et al. Low-leakage MIS structures with 1.5-6 nm CaF2 insulating layer on Si(111). Microelectron. Eng. 84, 2247–2250 (2007).10.1016/j.mee.2007.04.065 ↗
31. Sire, C., Blonkowski, S., Gordon, M. J. & Baron, T. Statistics of electrical breakdown field in HfO2 and SiO2 films from millimeter to nanometer length scales. Appl. Phys. Lett. 91, 242905 (2007).10.1063/1.2822420 ↗
32. Zhang, L. et al. ALD preparation of high-k HfO2 thin films with enhanced energy density and efficient electrostatic energy storage. RSC Adv. 7, 8388–8393 (2017).10.1039/C6RA27847G ↗
33. Baumert, B. A. et al. Characterization of sputtered barium strontium titanate and strontium titanate-thin films. J. Appl. Phys. 82, 2558–2566 (1997).10.1063/1.366066 ↗
34. Kim, S. M. et al. Synthesis of large-area multilayer hexagonal boron nitride for high material performance. Nat. Commun. 6, 8662 (2015).
35. Zhou, C. et al. Enhanced polarization switching characteristics of HfO2 ultrathin films via acceptor–donor co-doping. Nat. Commun. 15, 2893 (2024).10.1038/s41467-024-47194-8 ↗
36. Nukala, P. et al. Reversible oxygen migration and phase transitions in hafnia-based ferroelectric devices. Science 372, 630–635 (2021).10.1126/science.abf3789 ↗
37. Jiang, Y. et al. Enabling ultra-low-voltage switching in BaTiO3. Nat. Mater. 21, 779–785 (2022).10.1038/s41563-022-01266-6 ↗
38. Hu, Y. et al. Ferroelastic-switching-driven large shear strain and piezoelectricity in a hybrid ferroelectric. Nat. Mater. 20, 612–617 (2021).10.1038/s41563-020-00875-3 ↗
39. Wang, X. et al. Van der Waals engineering of ferroelectric heterostructures for long-retention memory. Nat. Commun. 12, 1109 (2021).
40. Wang, L. et al. A general one-step plug-and-probe approach to top-gated transistors for rapidly probing delicate electronic materials. Nat. Nanotechnol. 17, 1206–1213 (2022).10.1038/s41565-022-01221-1 ↗
41. Yang, A. J. et al. Van der Waals integration of high-κ perovskite oxides and two-dimensional semiconductors. Nat. Electron. 5, 233–240 (2022).10.1038/s41928-022-00753-7 ↗
42. Illarionov, Y. Y. et al. Ultrathin calcium fluoride insulators for two-dimensional field-effect transistors. Nat. Electron. 2, 230–235 (2019).10.1038/s41928-019-0256-8 ↗
43. Peimyoo, N. et al. Laser-writable high-k dielectric for van der Waals nanoelectronics. Sci. Adv. 5, eaau0906 (2019).10.1126/sciadv.aau0906 ↗
44. Lu, Z. et al. Wafer-scale high-κ dielectrics for two-dimensional circuits via van der Waals integration. Nat. Commun. 14, 2340 (2023).
45. Jin, Y. et al. Controllable oxidation of ZrS2 to prepare high‐κ, single‐crystal m‐ZrO2 for 2D electronics. Adv. Mater. 35, 2212079 (2023).10.1002/adma.202212079 ↗
46. Radisavljevic, B., Radenovic, A., Brivio, J., Giacometti, V. & Kis, A. Single-layer MoS2 transistors. Nat. Nanotechnol. 6, 147–150 (2011).10.1038/nnano.2010.279 ↗
47. Wang, Y. et al. CALYPSO: a method for crystal structure prediction. Comput. Phys. Commun. 183, 2063–2070 (2012).10.1016/j.cpc.2012.05.008 ↗
48. Stewart, J. J. P. MOPAC: a semiempirical molecular orbital program. J. Comput. Aided Mol. Des. 4, 1–103 (1990).10.1007/BF00128336 ↗
49. Hostaš, J., Řezáč, J. & Hobza, P. On the performance of the semiempirical quantum mechanical PM6 and PM7 methods for noncovalent interactions. Chem. Phys. Lett. 568, 161–166 (2013).10.1016/j.cplett.2013.02.069 ↗
50. Dieter, K. M. & Stewart, J. J. P. Calculation of vibrational frequencies using molecular trajectories. J. Mol. Struct. THEOCHEM 163, 143–149 (1988).10.1016/0166-1280(88)80386-5 ↗
51. Kresse, G. & Furthmüller, J. Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. Phys. Rev. B 54, 11169 (1996).10.1103/PhysRevB.54.11169 ↗
52. Blöchl, P. E. Projector augmented-wave method. Phys. Rev. B 50, 17953 (1994).10.1103/PhysRevB.50.17953 ↗
53. Perdew, J. P., Burke, K. & Ernzerhof, M. Generalized gradient approximation made simple. Phys. Rev. Lett. 77, 3865 (1996).10.1103/PhysRevLett.77.3865 ↗
54. Heyd, J. & Scuseria, G. E. Efficient hybrid density functional calculations in solids: assessment of the Heyd–Scuseria–Ernzerhof screened Coulomb hybrid functional. J. Chem. Phys. 121, 1187–1192 (2004).10.1063/1.1760074 ↗
55. Grimme, S. Semiempirical GGA‐type density functional constructed with a long‐range dispersion correction. J. Comput. Chem. 27, 1787–1799 (2006).10.1002/jcc.20495 ↗
56. Sipe, J. E. & Ghahramani, E. Nonlinear optical response of semiconductors in the independent-particle approximation. Phys. Rev. B 48, 11705 (1993).10.1103/PhysRevB.48.11705 ↗