TY - JOUR
T1 - Why an integrated approach between search algorithms and chemical intuition is necessary?
AU - Thimmakondu, Venkatesan S.
AU - Sinjari, Aland
AU - Inostroza, Diego
AU - Vairaprakash, Pothiappan
AU - Thirumoorthy, Krishnan
AU - Roy, Saikat
AU - Anoop, Anakuthil
AU - Tiznado, William
N1 - Publisher Copyright:
© 2022 The Royal Society of Chemistry
PY - 2022/4/27
Y1 - 2022/4/27
N2 - Though search algorithms are appropriate tools for identifying low-energy isomers, fixing several constraints seems to be a fundamental prerequisite to successfully running any structural search program. This causes some potential setbacks as far as identifying all possible isomers, close to the lowest-energy isomer, for any elemental composition. The number of explored candidates, the choice of method, basis set, and availability of CPU time needed to analyze the various initial test structures become necessary restrictions in resolving the issues of structural isomerism reasonably. While one could arrive at new structures through chemical intuition, reproducing or achieving those exact same structures requires increasing the number of variables in any given program, which causes further constraints in exploring the potential energy surface in a reasonable amount of time. Thus, it is emphasized here that an integrated approach between search algorithms and chemical intuition is necessary by taking the C12O2Mg2 system as an example. Our initial search through the AUTOMATON program yielded 1450 different geometries. However, through chemical intuition, we found eighteen new geometries within 40.0 kcal mol−1 at the PBE0-D3/def2-TZVP level. These results indirectly emphasize that an integrated approach between search algorithms and chemical intuition is necessary to further our knowledge in chemical space for any given elemental composition.
AB - Though search algorithms are appropriate tools for identifying low-energy isomers, fixing several constraints seems to be a fundamental prerequisite to successfully running any structural search program. This causes some potential setbacks as far as identifying all possible isomers, close to the lowest-energy isomer, for any elemental composition. The number of explored candidates, the choice of method, basis set, and availability of CPU time needed to analyze the various initial test structures become necessary restrictions in resolving the issues of structural isomerism reasonably. While one could arrive at new structures through chemical intuition, reproducing or achieving those exact same structures requires increasing the number of variables in any given program, which causes further constraints in exploring the potential energy surface in a reasonable amount of time. Thus, it is emphasized here that an integrated approach between search algorithms and chemical intuition is necessary by taking the C12O2Mg2 system as an example. Our initial search through the AUTOMATON program yielded 1450 different geometries. However, through chemical intuition, we found eighteen new geometries within 40.0 kcal mol−1 at the PBE0-D3/def2-TZVP level. These results indirectly emphasize that an integrated approach between search algorithms and chemical intuition is necessary to further our knowledge in chemical space for any given elemental composition.
UR - http://www.scopus.com/inward/record.url?scp=85131449747&partnerID=8YFLogxK
U2 - 10.1039/d2cp00315e
DO - 10.1039/d2cp00315e
M3 - Article
AN - SCOPUS:85131449747
SN - 1463-9076
VL - 24
SP - 11680
EP - 11686
JO - Physical Chemistry Chemical Physics
JF - Physical Chemistry Chemical Physics
IS - 19
ER -