TY - JOUR
T1 - Accurate rovibrational energies of ozone isotopologues up to J = 10 utilizing artificial neural networks
AU - Petty, Corey
AU - Spada, Rene F.K.
AU - Machado, Francisco B.C.
AU - Poirier, Bill
N1 - Funding Information:
F.B.C.M. acknowledges the Fundacão de Amparo à Pesquisa do Estado de São Paulo (FAPESP) under Grant Nos. 2014/14470-1, 2016/05615-1, and 2017/07707-3 and Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq) under Grant Nos. 307052/2016-8 and 404337/2016-3. B.P. acknowledges both a research grant (Grant No. CHE-1665370) and a CRIF MU instrumentation grant (Grant No. CHE-0840493) from the National Science Foundation, a research grant (Grant No. NNX13AJ49G-EXO) from NASA Astrobiology, and the FAPESP/Texas Tech University SPRINT program (Project No. 2016/50485-9) for travel support. All authors are grateful for the computational resources and support provided by the Texas Tech University High Performance Computing Center and the Texas Advanced Computing Center. Calculations presented in this paper were performed using the ScalIT suite of parallel codes.
Funding Information:
F.B.C.M. acknowledges the Fundacão de Amparo à Pesquisa do Estado de São Paulo (FAPESP) under Grant Nos. 2014/14470-1, 2016/05615-1, and 2017/07707-3 and Con-selho Nacional de Desenvolvimento Científico e Tecnológico (CNPq) under Grant Nos. 307052/2016-8 and 404337/2016-3. B.P. acknowledges both a research grant (Grant No. CHE-1665370) and a CRIF MU instrumentation grant (Grant No. CHE-0840493) from the National Science Foundation, a research grant (Grant No. NNX13AJ49G-EXO) from NASA Astrobiology, and the FAPESP/Texas Tech University SPRINT program (Project No. 2016/50485-9) for travel support. All authors are grateful for the computational resources and support provided by the Texas Tech University High Performance Computing Center and the Texas Advanced Computing Center. Calculations presented in this paper were performed using the ScalIT suite of parallel codes.
Publisher Copyright:
© 2018 Author(s).
PY - 2018/7/14
Y1 - 2018/7/14
N2 - In recent years, ozone and its isotopologues have been a topic of interest in many fields of research, due to its importance in atmospheric chemistry and its anomalous isotopic enrichment - or the so-called “mass-independent fractionation.” In the field of potential energy surface (PES) creation, debate over the existence of a potential barrier just under the dissociation threshold (referred to as a “potential reef”) has plagued research for some years. Recently, Dawes and co-workers [Dawes, Lolur, Li, Jiang, and Guo (DLLJG) J. Chem. Phys. 139, 201103 (2013)] created a highly accurate global PES, for which the reef is found to be replaced with a (monotonic) “plateau.” Subsequent dynamical calculations on this “DLLJG” PES have shown improved agreement with experiment, particularly the vibrational spectrum. However, it is well known that reaction dynamics is also highly influenced by the rovibrational states, especially in cases like ozone that assume a Lindemann-type mechanism. Accordingly, we present the first significant step toward a complete characterization of the rovibrational spectrum for various isotopologues of ozone, computed using the DLLJG PES together with the ScalIT suite of parallel codes. Additionally, artificial neural networks are used in an innovative fashion - not to construct the PES function per se but rather to greatly speed up its evaluation.
AB - In recent years, ozone and its isotopologues have been a topic of interest in many fields of research, due to its importance in atmospheric chemistry and its anomalous isotopic enrichment - or the so-called “mass-independent fractionation.” In the field of potential energy surface (PES) creation, debate over the existence of a potential barrier just under the dissociation threshold (referred to as a “potential reef”) has plagued research for some years. Recently, Dawes and co-workers [Dawes, Lolur, Li, Jiang, and Guo (DLLJG) J. Chem. Phys. 139, 201103 (2013)] created a highly accurate global PES, for which the reef is found to be replaced with a (monotonic) “plateau.” Subsequent dynamical calculations on this “DLLJG” PES have shown improved agreement with experiment, particularly the vibrational spectrum. However, it is well known that reaction dynamics is also highly influenced by the rovibrational states, especially in cases like ozone that assume a Lindemann-type mechanism. Accordingly, we present the first significant step toward a complete characterization of the rovibrational spectrum for various isotopologues of ozone, computed using the DLLJG PES together with the ScalIT suite of parallel codes. Additionally, artificial neural networks are used in an innovative fashion - not to construct the PES function per se but rather to greatly speed up its evaluation.
UR - http://www.scopus.com/inward/record.url?scp=85049902644&partnerID=8YFLogxK
U2 - 10.1063/1.5036602
DO - 10.1063/1.5036602
M3 - Article
C2 - 30007387
AN - SCOPUS:85049902644
VL - 149
JO - The Journal of Chemical Physics
JF - The Journal of Chemical Physics
SN - 0021-9606
IS - 2
M1 - 024307
ER -