TY - JOUR
T1 - Molecular Orientation at the Squalene/Air Interface from Sum Frequency Generation Spectroscopy and Atomistic Modeling
AU - Von Domaros, Michael
AU - Liu, Yangdongling
AU - Butman, Jana L.
AU - Perlt, Eva
AU - Geiger, Franz M.
AU - Tobias, Douglas J.
N1 - Funding Information:
We are grateful to Dr. Paula Olsiewski and the Alfred P. Sloan Foundation for providing us an opportunity and funding to work on this project (G-2017-9796, G-2019-12306, G-2019-12300, and G-2020-13912). M.v.D. and E.P. are supported by independent postdoctoral fellowships from the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation, M.v.D., 409294855; E.P., 391320977). This material is based upon work supported by the National Science Foundation under CNS-1828779. This work made use of the Keck-II and SPID facility of Northwestern University’s NUANCE Center, which has received support from the SHyNE Resource (NSF ECCS-2025633), the International Institute for Nanotechnology (IIN), and Northwestern’s MRSEC program (NSF DMR-1720139). We gratefully acknowledge the help from Dr. Xinqi Chen and Dr. Gajendra Shekhawat with the 3D optical microscopy and AFM, respectively, at the NUANCE Center.
Funding Information:
We are grateful to Dr. Paula Olsiewski and the Alfred P. Sloan Foundation for providing us an opportunity and funding to work on this project (G-2017-9796, G-2019-12306, G-2019-12300, and G-2020-13912). M.v.D. and E.P. are supported by independent postdoctoral fellowships from the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation, M.v.D., 409294855; E.P., 391320977). This material is based upon work supported by the National Science Foundation under CNS-1828779. This work made use of the Keck-II and SPID facility of Northwestern University's NUANCE Center, which has received support from the SHyNE Resource (NSF ECCS-2025633), the International Institute for Nanotechnology (IIN), and Northwestern's MRSEC program (NSF DMR-1720139). We gratefully acknowledge the help from Dr. Xinqi Chen and Dr. Gajendra Shekhawat with the 3D optical microscopy and AFM, respectively, at the NUANCE Center.
Publisher Copyright:
© 2021 American Chemical Society.
PY - 2021/4/22
Y1 - 2021/4/22
N2 - Human skin oils are significant scavengers of atmospheric oxidants in occupied indoor environments, and squalene is a major ozone-active constituent. Here, we present a combined spectroscopic and atomistic modeling approach to elucidate the conformational and orientational preferences of squalene at the air/oil interface and their implications for reactions with ozone. We find that squalene chains have a tendency to align with the surface normal, resulting in different concentrations of the various types of its double bonds and thus different reactivities. We also observe the presence of water at the surface of this hydrophobic compound. Both findings have possible implications for the design and outcomes of kinetic models describing this important aspect of indoor air chemistry.
AB - Human skin oils are significant scavengers of atmospheric oxidants in occupied indoor environments, and squalene is a major ozone-active constituent. Here, we present a combined spectroscopic and atomistic modeling approach to elucidate the conformational and orientational preferences of squalene at the air/oil interface and their implications for reactions with ozone. We find that squalene chains have a tendency to align with the surface normal, resulting in different concentrations of the various types of its double bonds and thus different reactivities. We also observe the presence of water at the surface of this hydrophobic compound. Both findings have possible implications for the design and outcomes of kinetic models describing this important aspect of indoor air chemistry.
UR - http://www.scopus.com/inward/record.url?scp=85104915366&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85104915366&partnerID=8YFLogxK
U2 - 10.1021/acs.jpcb.0c11158
DO - 10.1021/acs.jpcb.0c11158
M3 - Article
C2 - 33835820
AN - SCOPUS:85104915366
SN - 1520-6106
VL - 125
SP - 3932
EP - 3941
JO - Journal of Physical Chemistry B
JF - Journal of Physical Chemistry B
IS - 15
ER -