TY - JOUR
T1 - Gas-phase formation of silicon monoxide via non-adiabatic reaction dynamics and its role as a building block of interstellar silicates
AU - He, Chao
AU - Luo, Yuheng
AU - Doddipatla, Srinivas
AU - Yang, Zhenghai
AU - Millar, Tom J.
AU - Sun, Rui
AU - Kaiser, Ralf I.
N1 - Publisher Copyright:
© 2022 The Royal Society of Chemistry.
PY - 2022/8/8
Y1 - 2022/8/8
N2 - Silicon monoxide (SiO) is classified as a key precursor and fundamental molecular building block to interstellar silicate nanoparticles, which play an essential role in the synthesis of molecular building blocks connected to the Origins of Life. In the cold interstellar medium, silicon monoxide is of critical importance in initiating a series of elementary chemical reactions leading to larger silicon oxides and eventually to silicates. To date, the fundamental formation mechanisms and chemical dynamics leading to gas phase silicon monoxide have remained largely elusive. Here, through a concerted effort between crossed molecular beam experiments and electronic structure calculations, it is revealed that instead of forming highly-stable silicon dioxide (SiO2), silicon monoxide can be formed via a barrierless, exoergic, single-collision event between ground state molecular oxygen and atomic silicon involving non-adiabatic reaction dynamics through various intersystem crossings. Our research affords persuasive evidence for a likely source of highly rovibrationally excited silicon monoxide in cold molecular clouds thus initiating the complex chain of exoergic reactions leading ultimately to a population of silicates at low temperatures in our Galaxy.
AB - Silicon monoxide (SiO) is classified as a key precursor and fundamental molecular building block to interstellar silicate nanoparticles, which play an essential role in the synthesis of molecular building blocks connected to the Origins of Life. In the cold interstellar medium, silicon monoxide is of critical importance in initiating a series of elementary chemical reactions leading to larger silicon oxides and eventually to silicates. To date, the fundamental formation mechanisms and chemical dynamics leading to gas phase silicon monoxide have remained largely elusive. Here, through a concerted effort between crossed molecular beam experiments and electronic structure calculations, it is revealed that instead of forming highly-stable silicon dioxide (SiO2), silicon monoxide can be formed via a barrierless, exoergic, single-collision event between ground state molecular oxygen and atomic silicon involving non-adiabatic reaction dynamics through various intersystem crossings. Our research affords persuasive evidence for a likely source of highly rovibrationally excited silicon monoxide in cold molecular clouds thus initiating the complex chain of exoergic reactions leading ultimately to a population of silicates at low temperatures in our Galaxy.
UR - https://www.scopus.com/pages/publications/85136990102
U2 - 10.1039/d2cp02188a
DO - 10.1039/d2cp02188a
M3 - 文章
C2 - 35971984
AN - SCOPUS:85136990102
SN - 1463-9076
VL - 24
SP - 19761
EP - 19772
JO - Physical Chemistry Chemical Physics
JF - Physical Chemistry Chemical Physics
IS - 33
ER -