Probing solvation and reactivity in ionized polycyclic aromatic hydrocarbon-water clusters with photoionization mass spectrometry and electronic structure calculations

doi:10.1039/c8fd00229k

	Probing solvation and reactivity in ionized polycyclic aromatic hydrocarbon-water clusters with photoionization mass spectrometry and electronic structure calculations
	Xu, Bo 2; Stein, Tamar 1,4; Ablikim, Utuq 2; Jiang, Ling 3; Hendrix, Josie 1; Head-Gordon, Martin 1,2; Ahmed, Musahid 2
刊名	FARADAY DISCUSSIONS
	2019-07-01
卷号	217 页码:414-433
ISSN号	1359-6640
DOI	10.1039/c8fd00229k
通讯作者	Ahmed, Musahid(mahmed@lbl.gov)
英文摘要	Polycyclic aromatic hydrocarbons (PAHs) may comprise up to 20% of the carbon budget in our galaxy and most PAHs condense onto water-rich icy grain mantles. Benzene-water clusters have been invoked as model systems for studying the photo-processing of water ice mantles containing PAHs. However, there is a paucity of information on larger aromatics, where the extended pi cloud could affect photo-processing. In this study, tunable vacuum ultraviolet (VUV) photoionization of naphthalene-water clusters N-x(H2O)(y) (N denotes naphthalene) is performed using synchrotron radiation and analyzed by reflectron time-of-flight mass spectrometry. Naphthalene clusters up to x = 4 are generated as are naphthalene-water clusters up to y = 25. At low photon energy (<11 eV), the naphthalene moiety is ionized and there is no proton transfer from N+ to the water sub-cluster, which is very different from the benzene-water system. Protonated products, N[(H2O)(x)H](+) and OH radical addition product (NOH)[(H2O)(x)H](+) are generated above 11 eV, suggesting that water sub-clusters dominate the dynamics at high photon energies. Ab initio calculations are performed to decipher the experimental results. Energetics of the neutral structures N(H2O)(1-4) and their photoionized counterparts are calculated, including ionization on the N moiety as well as on the water sub-cluster. Energy decomposition analysis (EDA) is performed to understand trends in the binding between the naphthalene and the water sub-cluster in the ionized species.
资助项目	Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy (DOE), through the Gas Phase Chemical Physics Program of the Chemical Sciences Division[DE-AC02-05CH11231] ; National Aeronautics and Space Administration (NASA) through the NASA Astrobiology Institute[NNH13ZDA017C]
WOS关键词	INFRARED-SPECTROSCOPY ; PROTON-TRANSFER ; RADICAL-CATION ; EXCITED-STATES ; BENZENE ; NAPHTHALENE ; IONIZATION ; ENERGETICS ; ENERGIES ; ICES
WOS研究方向	Chemistry
语种	英语
出版者	ROYAL SOC CHEMISTRY
WOS记录号	WOS:000476809000021
资助机构	Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy (DOE), through the Gas Phase Chemical Physics Program of the Chemical Sciences Division ; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy (DOE), through the Gas Phase Chemical Physics Program of the Chemical Sciences Division ; National Aeronautics and Space Administration (NASA) through the NASA Astrobiology Institute ; National Aeronautics and Space Administration (NASA) through the NASA Astrobiology Institute ; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy (DOE), through the Gas Phase Chemical Physics Program of the Chemical Sciences Division ; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy (DOE), through the Gas Phase Chemical Physics Program of the Chemical Sciences Division ; National Aeronautics and Space Administration (NASA) through the NASA Astrobiology Institute ; National Aeronautics and Space Administration (NASA) through the NASA Astrobiology Institute ; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy (DOE), through the Gas Phase Chemical Physics Program of the Chemical Sciences Division ; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy (DOE), through the Gas Phase Chemical Physics Program of the Chemical Sciences Division ; National Aeronautics and Space Administration (NASA) through the NASA Astrobiology Institute ; National Aeronautics and Space Administration (NASA) through the NASA Astrobiology Institute ; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy (DOE), through the Gas Phase Chemical Physics Program of the Chemical Sciences Division ; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy (DOE), through the Gas Phase Chemical Physics Program of the Chemical Sciences Division ; National Aeronautics and Space Administration (NASA) through the NASA Astrobiology Institute ; National Aeronautics and Space Administration (NASA) through the NASA Astrobiology Institute
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/173889]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者	Ahmed, Musahid
作者单位	1.Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA 2.Lawrence Berkeley Natl Lab, Chem Sci Div, Berkeley, CA 94720 USA 3.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, 457 Zhongshan Rd, Dalian 116023, Peoples R China 4.Hebrew Univ Jerusalem, Fritz Haber Res Ctr Mol Dynam, IL-9190401 Jerusalem, Israel
推荐引用方式 GB/T 7714	Xu, Bo,Stein, Tamar,Ablikim, Utuq,et al. Probing solvation and reactivity in ionized polycyclic aromatic hydrocarbon-water clusters with photoionization mass spectrometry and electronic structure calculations[J]. FARADAY DISCUSSIONS,2019,217:414-433.
APA	Xu, Bo.,Stein, Tamar.,Ablikim, Utuq.,Jiang, Ling.,Hendrix, Josie.,...&Ahmed, Musahid.(2019).Probing solvation and reactivity in ionized polycyclic aromatic hydrocarbon-water clusters with photoionization mass spectrometry and electronic structure calculations.FARADAY DISCUSSIONS,217,414-433.
MLA	Xu, Bo,et al."Probing solvation and reactivity in ionized polycyclic aromatic hydrocarbon-water clusters with photoionization mass spectrometry and electronic structure calculations".FARADAY DISCUSSIONS 217(2019):414-433.