Abstract
Understanding the emergent electronic structure in twisted atomically thin layers has led to the exciting field of twistronics. However, practical applications of such systems are challenging since the specific angular correlations between the layers must be precisely controlled and the layers have to be single crystalline with uniform atomic ordering. Here, an alternative, simple, and scalable approach is suggested, where nanocrystallinetwo-dimensional (2D) film on 3D substrates yields twisted-interface-dependent properties. Ultrawide-bandgap hexagonal boron nitride (h-BN) thin films are directly grown on high in-plane lattice mismatched wide-bandgap silicon carbide (4H-SiC) substrates to explore the twist-dependent structure-property correlations. Concurrently, nanocrystalline h-BN thin film shows strong non-linear second-harmonic generation and ultra-low cross-plane thermal conductivity at room temperature, which are attributed to the twisted domain edges between van der Waals stacked nanocrystals with random in-plane orientations. First-principles calculations based on time-dependent density functional theory manifest strong even-order optical nonlinearity in twisted h-BN layers. This work unveils that directly deposited 2D nanocrystalline thin film on 3D substrates could provide easily accessible twist-interfaces, therefore enabling a simple and scalable approach to utilize the 2D-twistronics integrated in 3D material devices for next-generation nanotechnology.
| Original language | English |
|---|---|
| Article number | 2304624 |
| Journal | Advanced Materials |
| Volume | 35 |
| Issue number | 47 |
| DOIs | |
| State | Published - Nov 23 2023 |
Funding
This work was sponsored partly by the Army Research Office and was accomplished under Cooperative Agreement Number W911NF‐19‐2‐0269. The views and conclusions contained in this document are those of the authors and should not be interpreted as representing the official policies, either expressed or implied, of the Army Research Office or the U.S. Government. The U.S. Government is authorized to reproduce and distribute reprints for Government purposes notwithstanding any copyright notation herein. This work was sponsored by the Department of the Navy, Office of Naval Research under ONR award no. N00014‐22‐1‐ 2357. R.X. and H.Z. were supported by the Welch Foundation C‐2128. T.L. and Y.Z. were supported as part of ULTRA, an Energy Frontier Research Center funded by the US Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), under award no. DE‐SC0021230. G.A.A. was sponsored by the National Science Foundation Graduate Research Fellowship under grant no. 1650114 and by the GEM Associate Ph.D. Fellowship. This work was also supported by the Cluster of Excellence “CUI: Advanced Imaging of Matter” of the Deutsche Forschungsgemeinschaft (DFG)—EXC 2056—project ID 390715994, and SFB‐925 “Light Induced Dynamics and Control of Correlated Quantum Systems”—project 170620586 of the Deutsche Forschungsgemeinschaft (DFG) and Grupos Consolidados (IT1453‐22). The authors acknowledge support from the Max Planck‐New York City Center for non‐equilibrium quantum phenomena. This work was performed, in part, at the Cornell NanoScale Facility, a member of the National Nanotechnology Coordinated Infrastructure (NNCI), which was supported by the National Natural Science Foundation of China (grant no. NNCI2025233). Scanning transmission electron microscopy experiments were performed as part of a user proposal at the Center for Nanophase Materials Sciences (CNMS), a U.S. Department of Energy, Office of Science User Facility. This work was sponsored partly by the Army Research Office and was accomplished under Cooperative Agreement Number W911NF-19-2-0269. The views and conclusions contained in this document are those of the authors and should not be interpreted as representing the official policies, either expressed or implied, of the Army Research Office or the U.S. Government. The U.S. Government is authorized to reproduce and distribute reprints for Government purposes notwithstanding any copyright notation herein. This work was sponsored by the Department of the Navy, Office of Naval Research under ONR award no. N00014-22-1- 2357. R.X. and H.Z. were supported by the Welch Foundation C-2128. T.L. and Y.Z. were supported as part of ULTRA, an Energy Frontier Research Center funded by the US Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), under award no. DE-SC0021230. G.A.A. was sponsored by the National Science Foundation Graduate Research Fellowship under grant no. 1650114 and by the GEM Associate Ph.D. Fellowship. This work was also supported by the Cluster of Excellence “CUI: Advanced Imaging of Matter” of the Deutsche Forschungsgemeinschaft (DFG)—EXC 2056—project ID 390715994, and SFB-925 “Light Induced Dynamics and Control of Correlated Quantum Systems”—project 170620586 of the Deutsche Forschungsgemeinschaft (DFG) and Grupos Consolidados (IT1453-22). The authors acknowledge support from the Max Planck-New York City Center for non-equilibrium quantum phenomena. This work was performed, in part, at the Cornell NanoScale Facility, a member of the National Nanotechnology Coordinated Infrastructure (NNCI), which was supported by the National Natural Science Foundation of China (grant no. NNCI2025233). Scanning transmission electron microscopy experiments were performed as part of a user proposal at the Center for Nanophase Materials Sciences (CNMS), a U.S. Department of Energy, Office of Science User Facility.
| Funders | Funder number |
|---|---|
| Center for Nanophase Materials Sciences | |
| Max Planck-New York City Center | |
| Max Planck‐New York City Center | |
| National Science Foundation | 1650114 |
| Office of Naval Research | N00014‐22‐1‐ 2357 |
| U.S. Department of Energy | |
| Army Research Office | W911NF‐19‐2‐0269 |
| Welch Foundation | C‐2128 |
| Office of Science | |
| Basic Energy Sciences | DE‐SC0021230 |
| U.S. Navy | |
| Deutsche Forschungsgemeinschaft | 390715994, SFB‐925, 170620586, IT1453‐22 |
| National Natural Science Foundation of China | NNCI2025233 |
Keywords
- h-BN films
- nano-domains
- second harmonic generation
- thermal conductivity
- time-dependent density functional theory
- twist-interfaces
