Based on its high activation energy, YARP excluded Ga-hydride from further exploration, whereas Ga-n-butyl and Ga-vinyl were included as active nodes for further reaction exploration. The high activation energy of β-hydrogen elimination forming Ga-hydride has also been observed in our previous studies using conventional periodic DFT. The second step of exploration identifies Ga- n-butenyl (from Ga-vinyl, ∆G † = 53.2 kcal/mol), acetylene (formed with Ga-ethyl from Ga-vinyl, ∆G † = 51.4 kcal/mol), Ga-hexyl (from Ga-butyl, ∆G † = 61.3 kcal/mol), 1-butene (formed with Ga-ethyl from Ga-butyl, ∆G † = 36.0 kcal/mol) and butane (formed with Ga-vinyl from Ga-butyl, ∆G † = 76.4 kcal/mol) as intended products. Notably, the lowest barrier step yielding 1-butene constitutes a rediscovery by the algorithm of the classic Cossee-Arlman mechanism that has previously been studied as the likely pathway for major product formation in this system. Based on the activation energies of the reactions at this iteration, Ga-n-butenyl was included as a new active node for further exploration (node 7), Ga-n-hexyl was classified as a terminal node (node 13) due to its size, and 1-butene was added to the free-olefin list as a candidate for further reactions with the active nodes, Ga-ethyl (node 0) and Ga-vinyl (node 1). YARP recursively explored the reaction space via the same approach that was employed in the first and second iteration until all reactions within the prescribed constraints had been explored. All reactions explored with ∆G † < 80 kcal/mol are presented in Figure . 2 and detailed geometries of each node can be found in the SI.