title: Discovering chemistry with an ab initio nanoreactor.
abstract: Chemical understanding is driven by the experimental discovery of new compounds and reactivity, and is supported by theory and computation that provide detailed physical insight. Although theoretical and computational studies have generally focused on specific processes or mechanistic hypotheses, recent methodological and computational advances harken the advent of their principal role in discovery. Here we report the development and application of the ab initio nanoreactor--a highly accelerated first-principles molecular dynamics simulation of chemical reactions that discovers new molecules and mechanisms without preordained reaction coordinates or elementary steps. Using the nanoreactor, we show new pathways for glycine synthesis from primitive compounds proposed to exist on the early Earth, which provide new insight into the classic Urey-Miller experiment. These results highlight the emergence of theoretical and computational chemistry as a tool for discovery, in addition to its traditional role of interpreting experimental findings.
authors.affiliation: 1] The PULSE Institute, Stanford University, Stanford, California 94305, USA [2] Department of Chemistry, Stanford University, Stanford, California 94305, USA.
authors.forename: Lee-Ping
authors.initials: LP
authors.lastname: Wang
authors.affiliation: 1] The PULSE Institute, Stanford University, Stanford, California 94305, USA [2] Department of Chemistry, Stanford University, Stanford, California 94305, USA.
authors.forename: Alexey
authors.initials: A
authors.lastname: Titov
authors.affiliation: Department of Chemistry, Stanford University, Stanford, California 94305, USA.
authors.forename: Robert
authors.initials: R
authors.lastname: McGibbon
authors.affiliation: 1] The PULSE Institute, Stanford University, Stanford, California 94305, USA [2] Department of Chemistry, Stanford University, Stanford, California 94305, USA.
authors.forename: Fang
authors.initials: F
authors.lastname: Liu
authors.affiliation: Department of Chemistry, Stanford University, Stanford, California 94305, USA.
authors.forename: Vijay S
authors.initials: VS
authors.lastname: Pande
authors.affiliation: 1] The PULSE Institute, Stanford University, Stanford, California 94305, USA [2] Department of Chemistry, Stanford University, Stanford, California 94305, USA [3] SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA.
authors.forename: Todd J
authors.initials: TJ
authors.lastname: Martínez
mesh_terms: D056004:Molecular Dynamics Simulation; D053758:Nanoparticles / Q000737:chemistry*; D036103:Nanotechnology; D010316:Particle Size