Perspective on Mechanism Development and Structure‐Activity Relationships for Gas‐Phase Atmospheric Chemistry

TY - JOUR

T1 - Perspective on Mechanism Development and Structure‐Activity Relationships for Gas‐Phase Atmospheric Chemistry

AU - Rickard, Andrew Robert

AU - Vereecken, L.

AU - Aumont, B.

AU - Barnes, I

AU - Bozzelli, J. W.

AU - Goldman, M. J.

AU - Green, W. H.

AU - Madronich, S.

AU - McGillen, M.

AU - Mellouki, A.

AU - Orlando, J. J.

AU - Wallington, Timothy J.

AU - Picquet-Varrault, B.

AU - Stockwell , W. R.

AU - Carter, W. P. L.

N1 - © 2018, Wiley Periodicals, Inc. This is an author-produced version of the published paper. Uploaded in accordance with the publisher’s self-archiving policy. Further copying may not be permitted; contact the publisher for details.

PY - 2018/4/12

Y1 - 2018/4/12

N2 - This perspective gives our views on general aspects and future directions of gas‐phase atmospheric chemical kinetic mechanism development, emphasizing on the work needed for the sustainable development of chemically detailed mechanisms that reflect current kinetic, mechanistic, and theoretical knowledge. Current and future mechanism development efforts and research needs are discussed, including software‐aided autogeneration and maintenance of kinetic models as a future‐proof approach for atmospheric model development. There is an overarching need for the evaluation and extension of structure‐activity relationships (SARs) that predict the properties and reactions of the many multifunctionalized compounds in the atmosphere that are at the core of detailed mechanisms, but for which no direct chemical data are available. Here, we discuss the experimental and theoretical data needed to support the development of mechanisms and SARs, the types of SARs relevant to atmospheric chemistry, the current status and limitations of SARs for various types of atmospheric reactions, the status of thermochemical estimates needed for mechanism development, and our outlook for the future. The authors have recently formed a SAR evaluation working group to address these issues.

AB - This perspective gives our views on general aspects and future directions of gas‐phase atmospheric chemical kinetic mechanism development, emphasizing on the work needed for the sustainable development of chemically detailed mechanisms that reflect current kinetic, mechanistic, and theoretical knowledge. Current and future mechanism development efforts and research needs are discussed, including software‐aided autogeneration and maintenance of kinetic models as a future‐proof approach for atmospheric model development. There is an overarching need for the evaluation and extension of structure‐activity relationships (SARs) that predict the properties and reactions of the many multifunctionalized compounds in the atmosphere that are at the core of detailed mechanisms, but for which no direct chemical data are available. Here, we discuss the experimental and theoretical data needed to support the development of mechanisms and SARs, the types of SARs relevant to atmospheric chemistry, the current status and limitations of SARs for various types of atmospheric reactions, the status of thermochemical estimates needed for mechanism development, and our outlook for the future. The authors have recently formed a SAR evaluation working group to address these issues.

KW - CHEMICAL MECHANISM

KW - ATMOSPHERIC CHEMISTRY

KW - structure activity relationships

U2 - 10.1002/kin.21172

DO - 10.1002/kin.21172

M3 - Article

SN - 0538-8066

VL - 50

SP - 435

EP - 469

JO - International journal of chemical kinetics

JF - International journal of chemical kinetics

IS - 6

ER -