TY - JOUR
T1 - Following the microscopic pathway to adsorption through chemisorption and physisorption wells
AU - Borodin, Dmitriy
AU - Rahinov, Igor
AU - Shirhatti, Pranav R.
AU - Huang, Meng
AU - Kandratsenka, Alexander
AU - Auerbach, Daniel J.
AU - Zhong, Tianli
AU - Guo, Hua
AU - Schwarzer, Dirk
AU - Kitsopoulos, Theofanis N.
AU - Wodtke, Alec M.
N1 - Publisher Copyright:
© 2020 The Authors.
PY - 2020/9/1
Y1 - 2020/9/1
N2 - Adsorption involves molecules colliding at the surface of a solid and losing their incidence energy by traversing a dynamical pathway to equilibrium. The interactions responsible for energy loss generally include both chemical bond formation (chemisorption) and nonbonding interactions (physisorption). In this work, we present experiments that revealed a quantitative energy landscape and the microscopic pathways underlying a molecule's equilibration with a surface in a prototypical system: CO adsorption on Au(111). Although the minimum energy state was physisorbed, initial capture of the gas-phase molecule, dosed with an energetic molecular beam, was into a metastable chemisorption state. Subsequent thermal decay of the chemisorbed state led molecules to the physisorption minimum. We found, through detailed balance, that thermal adsorption into both binding states was important at all temperatures.
AB - Adsorption involves molecules colliding at the surface of a solid and losing their incidence energy by traversing a dynamical pathway to equilibrium. The interactions responsible for energy loss generally include both chemical bond formation (chemisorption) and nonbonding interactions (physisorption). In this work, we present experiments that revealed a quantitative energy landscape and the microscopic pathways underlying a molecule's equilibration with a surface in a prototypical system: CO adsorption on Au(111). Although the minimum energy state was physisorbed, initial capture of the gas-phase molecule, dosed with an energetic molecular beam, was into a metastable chemisorption state. Subsequent thermal decay of the chemisorbed state led molecules to the physisorption minimum. We found, through detailed balance, that thermal adsorption into both binding states was important at all temperatures.
UR - http://www.scopus.com/inward/record.url?scp=85091192291&partnerID=8YFLogxK
U2 - 10.1126/SCIENCE.ABC9581
DO - 10.1126/SCIENCE.ABC9581
M3 - Article
C2 - 32943520
AN - SCOPUS:85091192291
SN - 0036-8075
VL - 369
SP - 1461
EP - 1465
JO - Science
JF - Science
IS - 6509
M1 - ABC9581
ER -