Molecular Growth of PANH Via Intermolecular Coulombic Decay

Overview

Journal Sci Adv

Specialties Biology
Science

Date 2023 Jul 26

PMID 37494436

Authors

Saroj Barik

Nihar Ranjan Behera

Saurav Dutta

Rajesh Kumar Kushawaha

Y Sajeev

Raghunath O Ramabhadran

G Aravind

Affiliations

Soon will be listed here.

Abstract

Nitrogen-bearing polycyclic aromatic hydrocarbons (PANHs) are ubiquitous in space. They are considered precursors to advanced biomolecules identified in meteorites. However, their chemical evolution into biomolecules in photodestructive astrophysical mediums remains a paradox. Here, we show that light can efficiently initiate the molecular mass growth of PANHs. Ultraviolet-photoexcited quinoline monomers, the smallest PANH, were observed to associate and intermolecular Coulombic decay between the associating monomers formed the cations of quinoline-dimer. Molecular rearrangements in the dimer cation lead to a dominant formation of cations heavier than quinoline. The enrichment of these heavier cations over all the other cations reveals the efficiency of this route for the mass growth of PANHs in space. This mechanism also leads to a highly reactive unsaturated PANH-ring via CH loss, a hitherto unknown channel in any photon-driven process. The occurrence of this efficient pathway toward complex molecules points to a rich chemistry in dense interstellar clouds.

References

Burns L, Vazquez-Mayagoitia A, Sumpter B, Sherrill C . Density-functional approaches to noncovalent interactions: a comparison of dispersion corrections (DFT-D), exchange-hole dipole moment (XDM) theory, and specialized functionals. J Chem Phys. 2011; 134(8):084107. DOI: 10.1063/1.3545971. View

Salama F, Galazutdinov G, Krelowski J, Allamandola L, Musaev F . Polycyclic aromatic hydrocarbons and the diffuse interstellar bands: a survey. Astrophys J. 2001; 526 Pt 1:265-73. DOI: 10.1086/307978. View

Snow T, Le Page V, Keheyan Y, Bierbaum V . The interstellar chemistry of PAH cations. Nature. 1998; 391(6664):259-60. DOI: 10.1038/34602. View

Huber R, Margreiter M, Fuchs J, von Grafenstein S, Tautermann C, Liedl K . Heteroaromatic π-stacking energy landscapes. J Chem Inf Model. 2014; 54(5):1371-9. PMC: 4037317. DOI: 10.1021/ci500183u. View

Doddipatla S, Galimova G, Wei H, Thomas A, He C, Yang Z . Low-temperature gas-phase formation of indene in the interstellar medium. Sci Adv. 2021; 7(1). PMC: 7775774. DOI: 10.1126/sciadv.abd4044. View

Allamandola L, Tielens A, Barker J . Interstellar polycyclic aromatic hydrocarbons: the infrared emission bands, the excitation/emission mechanism, and the astrophysical implications. Astrophys J Suppl Ser. 1989; 71:733-75. DOI: 10.1086/191396. View

Parker D, Kaiser R . On the formation of nitrogen-substituted polycyclic aromatic hydrocarbons (NPAHs) in circumstellar and interstellar environments. Chem Soc Rev. 2016; 46(2):452-463. DOI: 10.1039/c6cs00714g. View

Soliman A, Hamid A, Attah I, Momoh P, Samy El-Shall M . Formation of nitrogen-containing polycyclic cations by gas-phase and intracluster reactions of acetylene with the pyridinium and pyrimidinium ions. J Am Chem Soc. 2012; 135(1):155-66. DOI: 10.1021/ja3068116. View

Kuleff A, Gokhberg K, Kopelke S, Cederbaum L . Ultrafast interatomic electronic decay in multiply excited clusters. Phys Rev Lett. 2010; 105(4):043004. DOI: 10.1103/PhysRevLett.105.043004. View

10.

Riley K, Pitonak M, cerny J, Hobza P . On the Structure and Geometry of Biomolecular Binding Motifs (Hydrogen-Bonding, Stacking, X-H···π): WFT and DFT Calculations. J Chem Theory Comput. 2015; 6(1):66-80. DOI: 10.1021/ct900376r. View

11.

Barik S, Dutta S, Behera N, Kushawaha R, Sajeev Y, Aravind G . Ambient-light-induced intermolecular Coulombic decay in unbound pyridine monomers. Nat Chem. 2022; 14(10):1098-1102. DOI: 10.1038/s41557-022-01002-2. View

12.

Bouwman J, Sztaray B, Oomens J, Hemberger P, Bodi A . Dissociative photoionization of quinoline and isoquinoline. J Phys Chem A. 2015; 119(7):1127-36. DOI: 10.1021/jp5121993. View

13.

Jiang Y, Wu Y, Deng J, Wang Z . Antiaromaticity-aromaticity transition of cyclo[16]carbon upon metal encapsulation. Phys Chem Chem Phys. 2021; 23(14):8817-8824. DOI: 10.1039/d0cp06256a. View

14.

Jahnke T, Hergenhahn U, Winter B, Dorner R, Fruhling U, Demekhin P . Interatomic and Intermolecular Coulombic Decay. Chem Rev. 2020; 120(20):11295-11369. PMC: 7596762. DOI: 10.1021/acs.chemrev.0c00106. View

15.

Salama F, Allamandola L . Is a pyrene-like molecular ion the cause of the 4,430-angstroms diffuse interstellar absorption band?. Nature. 1992; 358(6381):42-3. DOI: 10.1038/358042a0. View

16.

Gatchell M, Ameixa J, Ji M, Stockett M, Simonsson A, Denifl S . Survival of polycyclic aromatic hydrocarbon knockout fragments in the interstellar medium. Nat Commun. 2021; 12(1):6646. PMC: 8599666. DOI: 10.1038/s41467-021-26899-0. View

17.

Sandford S, Nuevo M, Bera P, Lee T . Prebiotic Astrochemistry and the Formation of Molecules of Astrobiological Interest in Interstellar Clouds and Protostellar Disks. Chem Rev. 2020; 120(11):4616-4659. DOI: 10.1021/acs.chemrev.9b00560. View

18.

McGuire B, Loomis R, Burkhardt A, Lee K, Shingledecker C, Charnley S . Detection of two interstellar polycyclic aromatic hydrocarbons via spectral matched filtering. Science. 2021; 371(6535):1265-1269. DOI: 10.1126/science.abb7535. View