TY - JOUR
T1 - ReaxFF Force Field Development for Gas-Phase hBN Nanostructure Synthesis
AU - Lele, Aditya
AU - Krstic, Predrag
AU - Van Duin, Adri C.T.
N1 - Funding Information:
The authors acknowledge funding support from National Science Foundation (NSF) through the Pennsylvania State University 2D Crystal Consortium–Materials Innovation Platform (2DCC-MIP) under NSF cooperative agreements DMR-1539916 and DMR 2039351.
Publisher Copyright:
© 2022 American Chemical Society. All rights reserved.
PY - 2022/2/3
Y1 - 2022/2/3
N2 - Two-dimensional (2D) hexagonal boron nitride materials are isomorphs of carbon nanomaterials and hold promise for electronics applications owing to their unique properties. Despite the recent advances in synthesis, the current production capacity for boron nitride (BN) nanostructures is far behind that for carbon-based nanostructures. Understanding the growth mechanism of BN nanostructures through modeling and experiments is key to improving this situation. In the current work, we present the development of a ReaxFF-based force field capable of modeling the gas-phase chemistry important for the chemical vapor deposition (CVD) synthesis process. This force field is parameterized to model the boron nitride nanostructure (BNNS) formation in the gas phase using BN and HBNH as precursors. Our ReaxFF simulations show that BN is the best of these two precursors in terms of quality and the size of BNNSs. The BN precursors lead to the formation of closed BNNSs. However, BNNSs are replaced with complex polymeric structures at temperatures of 2500 K and higher due to entropic effects. Compared to the BN precursors, the HBNH precursors form relatively small, flat, and low-quality BNNSs, but this structure is less affected by temperature. Additives like H2 significantly affect the BNNS formation by preventing closed BNNS formation. Our results show the ReaxFF capability in predicting the BN gas-phase chemistry and BNNS formation, thus providing key insights for experimental synthesis.
AB - Two-dimensional (2D) hexagonal boron nitride materials are isomorphs of carbon nanomaterials and hold promise for electronics applications owing to their unique properties. Despite the recent advances in synthesis, the current production capacity for boron nitride (BN) nanostructures is far behind that for carbon-based nanostructures. Understanding the growth mechanism of BN nanostructures through modeling and experiments is key to improving this situation. In the current work, we present the development of a ReaxFF-based force field capable of modeling the gas-phase chemistry important for the chemical vapor deposition (CVD) synthesis process. This force field is parameterized to model the boron nitride nanostructure (BNNS) formation in the gas phase using BN and HBNH as precursors. Our ReaxFF simulations show that BN is the best of these two precursors in terms of quality and the size of BNNSs. The BN precursors lead to the formation of closed BNNSs. However, BNNSs are replaced with complex polymeric structures at temperatures of 2500 K and higher due to entropic effects. Compared to the BN precursors, the HBNH precursors form relatively small, flat, and low-quality BNNSs, but this structure is less affected by temperature. Additives like H2 significantly affect the BNNS formation by preventing closed BNNS formation. Our results show the ReaxFF capability in predicting the BN gas-phase chemistry and BNNS formation, thus providing key insights for experimental synthesis.
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U2 - 10.1021/acs.jpca.1c09648
DO - 10.1021/acs.jpca.1c09648
M3 - Article
C2 - 35049316
AN - SCOPUS:85123614862
SN - 1089-5639
VL - 126
SP - 568
EP - 582
JO - Journal of Physical Chemistry A
JF - Journal of Physical Chemistry A
IS - 4
ER -