Capturing the Elusive Water Trimer from the Stepwise Growth of Water on the Surface of the Polycyclic Aromatic Hydrocarbon Acenaphthene

Amanda L. Steber; Cristóbal Pérez; Berhane Temelso; George C. Shields; Anouk M. Rijs; Brooks H. Pate; Zbigniew Kisiel; Melanie Schnell

doi:10.1021/acs.jpclett.7b02695

Capturing the Elusive Water Trimer from the Stepwise Growth of Water on the Surface of the Polycyclic Aromatic Hydrocarbon Acenaphthene

Amanda L. Steber^*, Cristóbal Pérez, Berhane Temelso, George C. Shields, Anouk M. Rijs, Brooks H. Pate, Zbigniew Kisiel, Melanie Schnell

^*Corresponding author for this work

Research output: Contribution to Journal › Article › Academic › peer-review

Abstract

Polycyclic aromatic hydrocarbons (PAHs) are key players in reaction chemistry. While it is postulated that they serve as a basis for ice grains, there has been no direct detection of PAHs in astronomical environments. We aim to investigate the hydration of PAHs to set a foundation for the future exploration of potential ice formation pathways. We report results from chirped pulse Fourier transform microwave spectroscopy and quantum-chemical calculations for the PAH acenaphthene and acenaphthene complexed with up to four water molecules. The acenaphthene-(H₂O)₃ complex is of particular interest as the elusive cyclic water trimer was observed. It appears in a slightly distorted configuration when compared with the pure water trimer. This is explained by hydrogen-bond net cooperativity effects. Binding energies for the complexes are presented. Our results provide insight into the onset of complex aggregation that could be occurring in extraterrestrial environments as part of ice grain formation.

Original language	English
Pages (from-to)	5744-5750
Number of pages	7
Journal	Journal of Physical Chemistry Letters
Volume	8
Issue number	23
DOIs	https://doi.org/10.1021/acs.jpclett.7b02695
Publication status	Published - 7 Dec 2017
Externally published	Yes

Funding

This work was performed as part of our activities within the framework of the ERC Starting grant “Astrorot”, grant agreement number 638027. A.L.S. and A.M.R. were supported by the excellence cluster “The Hamburg Centre for Ultrafast Imaging - Structure, Dynamics and Control of Matter at the Atomic Scale” of the Deutsche Forschungsgemeinschaft via a Louise Johnson Fellowship and a Mildred-Dresselhaus award, respectively. B.T. and G.C.S. acknowledge support by NSF grants CHE-1508556 and CHE-1721511 and by NSF grants CHE-1229354 and CHE-1662030 as part of the MERCURY high-performance computer consortium. Z.K. acknowledges financial support from a grant from the Polish National Science Centre, decision number DEC/2011/02/A/ST2/00298.

Funders	Funder number
Hamburg Centre for Ultrafast Imaging - Structure, Dynamics and Control of Matter
Polish National Science Centre	DEC/2011/02/A/ST2/00298
National Science Foundation	1721511, CHE-1229354, CHE-1508556, 1662030, CHE-1662030, CHE-1721511
Horizon 2020 Framework Programme	638027
European Research Council
Deutsche Forschungsgemeinschaft
Norsk Sykepleierforbund

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title = "Capturing the Elusive Water Trimer from the Stepwise Growth of Water on the Surface of the Polycyclic Aromatic Hydrocarbon Acenaphthene",

abstract = "Polycyclic aromatic hydrocarbons (PAHs) are key players in reaction chemistry. While it is postulated that they serve as a basis for ice grains, there has been no direct detection of PAHs in astronomical environments. We aim to investigate the hydration of PAHs to set a foundation for the future exploration of potential ice formation pathways. We report results from chirped pulse Fourier transform microwave spectroscopy and quantum-chemical calculations for the PAH acenaphthene and acenaphthene complexed with up to four water molecules. The acenaphthene-(H2O)3 complex is of particular interest as the elusive cyclic water trimer was observed. It appears in a slightly distorted configuration when compared with the pure water trimer. This is explained by hydrogen-bond net cooperativity effects. Binding energies for the complexes are presented. Our results provide insight into the onset of complex aggregation that could be occurring in extraterrestrial environments as part of ice grain formation.",

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AU - Steber, Amanda L.

AU - Pérez, Cristóbal

AU - Temelso, Berhane

AU - Shields, George C.

AU - Rijs, Anouk M.

AU - Pate, Brooks H.

AU - Kisiel, Zbigniew

AU - Schnell, Melanie

PY - 2017/12/7

Y1 - 2017/12/7

N2 - Polycyclic aromatic hydrocarbons (PAHs) are key players in reaction chemistry. While it is postulated that they serve as a basis for ice grains, there has been no direct detection of PAHs in astronomical environments. We aim to investigate the hydration of PAHs to set a foundation for the future exploration of potential ice formation pathways. We report results from chirped pulse Fourier transform microwave spectroscopy and quantum-chemical calculations for the PAH acenaphthene and acenaphthene complexed with up to four water molecules. The acenaphthene-(H2O)3 complex is of particular interest as the elusive cyclic water trimer was observed. It appears in a slightly distorted configuration when compared with the pure water trimer. This is explained by hydrogen-bond net cooperativity effects. Binding energies for the complexes are presented. Our results provide insight into the onset of complex aggregation that could be occurring in extraterrestrial environments as part of ice grain formation.

AB - Polycyclic aromatic hydrocarbons (PAHs) are key players in reaction chemistry. While it is postulated that they serve as a basis for ice grains, there has been no direct detection of PAHs in astronomical environments. We aim to investigate the hydration of PAHs to set a foundation for the future exploration of potential ice formation pathways. We report results from chirped pulse Fourier transform microwave spectroscopy and quantum-chemical calculations for the PAH acenaphthene and acenaphthene complexed with up to four water molecules. The acenaphthene-(H2O)3 complex is of particular interest as the elusive cyclic water trimer was observed. It appears in a slightly distorted configuration when compared with the pure water trimer. This is explained by hydrogen-bond net cooperativity effects. Binding energies for the complexes are presented. Our results provide insight into the onset of complex aggregation that could be occurring in extraterrestrial environments as part of ice grain formation.

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Capturing the Elusive Water Trimer from the Stepwise Growth of Water on the Surface of the Polycyclic Aromatic Hydrocarbon Acenaphthene

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