Fully anharmonic infrared cascade spectra of polycyclic aromatic hydrocarbons

Mackie, Cameron J.; Chen, Tao; Candian, Alessandra; Lee, Timothy J.; Tielens, Alexander G.  G.  M.

doi:10.1063/1.5038725

Fully anharmonic infrared cascade spectra of polycyclic aromatic hydrocarbons

Journal Article · Tue Oct 02 00:00:00 EDT 2018 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.5038725· OSTI ID:1572785

Mackie, Cameron J. ^[1]; Chen, Tao ^[2]; ^[3]; ^[4]; Tielens, Alexander G. G. M. ^[3]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division; Leiden Univ. (Netherlands). Leiden Observatory
Leiden Univ. (Netherlands). Leiden Observatory; Royal Inst. of Technology, Stockholm (Sweden). Dept. of Theoretical Chemistry and Biology, School of Biotechnology
Leiden Univ. (Netherlands). Leiden Observatory
NASA Ames Research Center (ARC), Moffett Field, Mountain View, CA (United States)

The infrared (IR) emission of polycyclic aromatic hydrocarbons (PAHs) permeates our universe; astronomers have detected the IR signatures of PAHs around many interstellar objects. The IR emission of interstellar PAHs differs from their emission as seen under conditions on Earth as they emit through a collisionless cascade down through their excited vibrational states from high internal energies. The difficulty in reproducing interstellar conditions in the laboratory results in a reliance on theoretical techniques. However, the size and complexity of PAHs require careful consideration when producing the theoretical spectra. In this work, we outline the theoretical methods necessary to lead to fully theoretical IR cascade spectra of PAHs including: an anharmonic second order vibrational perturbation theory treatment, the inclusion of Fermi resonances through polyads, and the calculation of anharmonic temperature band shifts and broadenings (including resonances) through a Wang-Landau approach. We also suggest a simplified scheme to calculate vibrational emission spectra that retain the essential characteristics of the full IR cascade treatment and can directly transform low temperature absorption spectra in IR cascade spectra. Finally, we show that past astronomical models were in error in assuming a 15 cm^-1 correction was needed to account for anharmonic emission effects.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1572785

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 13 Vol. 149; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

References (56)

Anharmonic molecular force fields: Anharmonic molecular force fields Császár, Attila G. Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 2, Issue 2 https://doi.org/10.1002/wcms.75	journal	July 2011
Infrared spectroscopy of matrix-isolated polycyclic aromatic compounds and their ions. 7. Phenazine, a dual substituted polycyclic aromatic nitrogen heterocycle Mattioda, A. L.; Hudgins, D. M.; Bauschlicher, C. W. Advances in Space Research, Vol. 36, Issue 2 https://doi.org/10.1016/j.asr.2005.03.127	journal	January 2005
On-line database of the spectral properties of polycyclic aromatic hydrocarbons Malloci, Giuliano; Joblin, Christine; Mulas, Giacomo Chemical Physics, Vol. 332, Issue 2-3 https://doi.org/10.1016/j.chemphys.2007.01.001	journal	February 2007
Time-resolved infrared emission spectra of naphthalene under gas phase laboratory and astrophysical conditions Parneix, P.; Basire, M.; Calvo, F. Computational and Theoretical Chemistry, Vol. 990 https://doi.org/10.1016/j.comptc.2011.12.014	journal	June 2012
Synthesis of carbon nanotubes using polycyclic aromatic hydrocarbons as carbon sources in an arc discharge Lai, H. J.; Lin, M. C. C.; Yang, M. H. Materials Science and Engineering: C, Vol. 16, Issue 1-2 https://doi.org/10.1016/s0928-4931(01)00303-4	journal	October 2001
Vibrational spectra of furan, pyrrole, and thiophene from a density functional theory anharmonic force field Burcl, Rudolf; Handy, Nicholas C.; Carter, Stuart Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, Vol. 59, Issue 8 https://doi.org/10.1016/s1386-1425(02)00421-3	journal	June 2003
Accurate ab initio quartic force field for trans-HNNH and treatment of resonance polyads Martin, Jan M. L.; Taylor, Peter R. Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, Vol. 53, Issue 8 https://doi.org/10.1016/s1386-1425(96)01869-0	journal	July 1997
The gas-phase infrared spectra of phenanthrene-h10 and phenanthrene-d10 Cané, Elisabetta; Miani, Andrea; Palmieri, Paolo Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, Vol. 53, Issue 11 https://doi.org/10.1016/s1386-1425(97)00103-0	journal	October 1997
High-Quality Large-Area Graphene from Dehydrogenated Polycyclic Aromatic Hydrocarbons Wan, Xi; Chen, Kun; Liu, Danqing Chemistry of Materials, Vol. 24, Issue 20 https://doi.org/10.1021/cm301993z	journal	October 2012
Development and Validation of the B3LYP/N07D Computational Model for Structural Parameter and Magnetic Tensors of Large Free Radicals Barone, Vincenzo; Cimino, Paola; Stendardo, Emiliano Journal of Chemical Theory and Computation, Vol. 4, Issue 5 https://doi.org/10.1021/ct800034c	journal	April 2008
A Review on Polycyclic Aromatic Hydrocarbon (PAH) Emissions from Energy Generation Mastral, Ana M.; Callén, María S. Environmental Science & Technology, Vol. 34, Issue 15 https://doi.org/10.1021/es001028d	journal	August 2000
Infrared Spectroscopy of Matrix-Isolated Polycyclic Aromatic Compounds and Their Ions. 6. Polycyclic Aromatic Nitrogen Heterocycles Mattioda, A. L.; Hudgins, D. M.; Bauschlicher, C. W. The Journal of Physical Chemistry A, Vol. 107, Issue 10 https://doi.org/10.1021/jp021938c	journal	March 2003
Anharmonic Force Fields of Naphthalene- h ₈ and Naphthalene- d ₈ Cané, Elisabetta; Miani, Andrea; Trombetti, Agostino The Journal of Physical Chemistry A, Vol. 111, Issue 33 https://doi.org/10.1021/jp071610p	journal	August 2007
Temperature Effects on the Rovibrational Spectra of Pyrene-Based PAHs Calvo, F.; Basire, M.; Parneix, P. The Journal of Physical Chemistry A, Vol. 115, Issue 32 https://doi.org/10.1021/jp202935p	journal	August 2011
On the Nature of Interlayer Interactions in a System of Two Graphene Fragments Berashevich, Julia; Chakraborty, Tapash The Journal of Physical Chemistry C, Vol. 115, Issue 50 https://doi.org/10.1021/jp2095032	journal	November 2011
Temperature and Anharmonic Effects on the Infrared Absorption Spectrum from a Quantum Statistical Approach: Application to Naphthalene Basire, M.; Parneix, P.; Calvo, F. The Journal of Physical Chemistry A, Vol. 113, Issue 25 https://doi.org/10.1021/jp901104x	journal	June 2009
Theoretical Infrared Spectra for Polycyclic Aromatic Hydrocarbon Neutrals, Cations, and Anions Langhoff, Stephen R. The Journal of Physical Chemistry, Vol. 100, Issue 8 https://doi.org/10.1021/jp952074g	journal	January 1996
Infrared Spectroscopy of Matrix-Isolated Polycyclic Aromatic Hydrocarbon Cations. 4. The Tetracyclic PAH Isomers Chrysene and 1,2-Benzanthracene Hudgins, Douglas M.; Allamandola, L. J. The Journal of Physical Chemistry A, Vol. 101, Issue 19 https://doi.org/10.1021/jp9609794	journal	May 1997
Infrared Spectroscopy of Matrix Isolated Polycyclic Aromatic Hydrocarbons. 1. PAHs Containing Two to Four Rings Hudgins, Douglas M.; Sandford, Scott A. The Journal of Physical Chemistry A, Vol. 102, Issue 2 https://doi.org/10.1021/jp9834816	journal	January 1998
Infrared Spectroscopy of Matrix Isolated Polycyclic Aromatic Hydrocarbons. 2. PAHs Containing Five or More Rings Hudgins, Douglas M.; Sandford, Scott A. The Journal of Physical Chemistry A, Vol. 102, Issue 2 https://doi.org/10.1021/jp983482y	journal	January 1998
High-resolution infrared absorption spectroscopy of thermally excited naphthalene. Measurements and calculations of anharmonic parameters and vibrational interactions Pirali, O.; Vervloet, M.; Mulas, G. Physical Chemistry Chemical Physics, Vol. 11, Issue 18 https://doi.org/10.1039/b814037e	journal	January 2009
The anharmonic quartic force field infrared spectra of hydrogenated and methylated PAHs Mackie, Cameron J.; Candian, Alessandra; Huang, Xinchuan Physical Chemistry Chemical Physics, Vol. 20, Issue 2 https://doi.org/10.1039/c7cp06546a	journal	January 2018
High-resolution IR absorption spectroscopy of polycyclic aromatic hydrocarbons in the 3 μ m region: role of hydrogenation and alkylation Maltseva, Elena; Mackie, Cameron J.; Candian, Alessandra Astronomy & Astrophysics, Vol. 610 https://doi.org/10.1051/0004-6361/201732102	journal	February 2018
The CH out-of-plane bending modes of PAH molecules in astrophysical environments Hony, S.; Van Kerckhoven, C.; Peeters, E. Astronomy & Astrophysics, Vol. 370, Issue 3 https://doi.org/10.1051/0004-6361:20010242	journal	May 2001
The profiles of the aromatic infrared bands explained with molecular carriers Pech, C.; Joblin, C.; Boissel, P. Astronomy & Astrophysics, Vol. 388, Issue 2 https://doi.org/10.1051/0004-6361:20020416	journal	May 2002
Modeling the anharmonic infrared Emission Spectra of PAHs: Application to the Pyrene Cation Basire, M.; Parneix, P.; Pino, T. EAS Publications Series, Vol. 46 https://doi.org/10.1051/eas/1146009	journal	January 2011
Self—Consistent Molecular Orbital Methods. XII. Further Extensions of Gaussian—Type Basis Sets for Use in Molecular Orbital Studies of Organic Molecules Hehre, W. J.; Ditchfield, R.; Pople, J. A. The Journal of Chemical Physics, Vol. 56, Issue 5, p. 2257-2261 https://doi.org/10.1063/1.1677527	journal	March 1972
Quantum anharmonic densities of states using the Wang–Landau method Basire, M.; Parneix, P.; Calvo, F. The Journal of Chemical Physics, Vol. 129, Issue 8 https://doi.org/10.1063/1.2965905	journal	August 2008
A second-order perturbation theory route to vibrational averages and transition properties of molecules: General formulation and application to infrared and vibrational circular dichroism spectroscopies Bloino, Julien; Barone, Vincenzo The Journal of Chemical Physics, Vol. 136, Issue 12 https://doi.org/10.1063/1.3695210	journal	March 2012
Density‐functional thermochemistry. III. The role of exact exchange Becke, Axel D. The Journal of Chemical Physics, Vol. 98, Issue 7, p. 5648-5652 https://doi.org/10.1063/1.464913	journal	April 1993
The anharmonic force field of ethylene, C ₂ H ₄ , by means of accurate ab initio calculations Martin, Jan M. L.; Lee, Timothy J.; Taylor, Peter R. The Journal of Chemical Physics, Vol. 103, Issue 7 https://doi.org/10.1063/1.469681	journal	August 1995
The gas-phase infrared spectra of anthracene-h10 and anthracene-d10 Cané, Elisabetta; Miani, Andrea; Palmieri, Paolo The Journal of Chemical Physics, Vol. 106, Issue 22 https://doi.org/10.1063/1.474033	journal	June 1997
The anharmonic quartic force field infrared spectra of three polycyclic aromatic hydrocarbons: Naphthalene, anthracene, and tetracene Mackie, Cameron J.; Candian, Alessandra; Huang, Xinchuan The Journal of Chemical Physics, Vol. 143, Issue 22 https://doi.org/10.1063/1.4936779	journal	December 2015
The anharmonic quartic force field infrared spectra of five non-linear polycyclic aromatic hydrocarbons: Benz[a]anthracene, chrysene, phenanthrene, pyrene, and triphenylene Mackie, Cameron J.; Candian, Alessandra; Huang, Xinchuan The Journal of Chemical Physics, Vol. 145, Issue 8 https://doi.org/10.1063/1.4961438	journal	August 2016
Beyond the x - K relations : Calculations of 1–1 and 2–2 resonance constants with application to HCN and DCN Lehmann, Kevin K. Molecular Physics, Vol. 66, Issue 6 https://doi.org/10.1080/00268978900100751	journal	April 1989
Polycyclic aromatic hydrocarbons and the unidentified infrared emission bands - Auto exhaust along the Milky Way Allamandola, L. J.; Tielens, A. G. G. M.; Barker, J. R. The Astrophysical Journal, Vol. 290 https://doi.org/10.1086/184435	journal	March 1985
Anharmonicity and the interstellar polycyclic aromatic hydrocarbon infrared emission spectrum Barker, John R.; Allamandola, L. J.; Tielens, A. G. G. M. The Astrophysical Journal, Vol. 315 https://doi.org/10.1086/184861	journal	April 1987
Infrared emission from a polycyclic aromatic hydrocarbon (PAH) excited by ultraviolet laser Cherchneff, Isabelle; Barker, John R. The Astrophysical Journal, Vol. 341 https://doi.org/10.1086/185448	journal	June 1989
Infrared emission spectra of benzene and naphthalene - Implications for the interstellar polycyclic aromatic hydrocarbon hypothesis Brenner, Jerrell; Barker, John R. The Astrophysical Journal, Vol. 388 https://doi.org/10.1086/186325	journal	March 1992
Interstellar polycyclic aromatic hydrocarbons - The infrared emission bands, the excitation/emission mechanism, and the astrophysical implications Allamandola, L. J.; Tielens, G. G. M.; Barker, J. R. The Astrophysical Journal Supplement Series, Vol. 71 https://doi.org/10.1086/191396	journal	September 1989
Simulated Infrared Emission Spectra of Highly Excited Polyatomic Molecules: A Detailed Model of the PAH‐UIR Hypothesis Cook, D. J.; Saykally, R. J. The Astrophysical Journal, Vol. 493, Issue 2 https://doi.org/10.1086/305156	journal	February 1998
The Infrared Spectra of Very Large, Compact, Highly Symmetric, Polycyclic Aromatic Hydrocarbons (PAHs) Bauschlicher, Jr., Charles W.; Peeters, Els; Allamandola, Louis J. The Astrophysical Journal, Vol. 678, Issue 1 https://doi.org/10.1086/533424	journal	May 2008
The Infrared Spectroscopy of Compact Polycyclic Aromatic Hydrocarbons Containing up to 384 Carbons Ricca, Alessandra; Bauschlicher, Charles W.; Boersma, Christiaan The Astrophysical Journal, Vol. 754, Issue 1 https://doi.org/10.1088/0004-637x/754/1/75	journal	July 2012
High-Resolution ir Absorption Spectroscopy of Polycyclic Aromatic Hydrocarbons: the Realm of Anharmonicity Maltseva, Elena; Petrignani, Annemieke; Candian, Alessandra The Astrophysical Journal, Vol. 814, Issue 1 https://doi.org/10.1088/0004-637x/814/1/23	journal	November 2015
The nasa ames pah ir Spectroscopic Database Version 2.00: Updated Content, web Site, and On(Off)Line Tools Boersma, C.; Bauschlicher, C. W.; Ricca, A. The Astrophysical Journal Supplement Series, Vol. 211, Issue 1 https://doi.org/10.1088/0067-0049/211/1/8	journal	February 2014
The 11.2 μm emission of PAHs in astrophysical objects Candian, A.; Sarre, P. J. Monthly Notices of the Royal Astronomical Society, Vol. 448, Issue 3 https://doi.org/10.1093/mnras/stv192	journal	March 2015
Efficient, Multiple-Range Random Walk Algorithm to Calculate the Density of States Wang, Fugao; Landau, D. P. Physical Review Letters, Vol. 86, Issue 10 https://doi.org/10.1103/physrevlett.86.2050	journal	March 2001
Single Photon Infrared Emission Spectroscopy of the Gas Phase Pyrene Cation: Support for a Polycyclic Aromatic Hydrocarbon Origin of the Unidentified Infrared Emission Bands Kim, H. -S.; Wagner, D. R.; Saykally, R. J. Physical Review Letters, Vol. 86, Issue 25 https://doi.org/10.1103/physrevlett.86.5691	journal	June 2001
A new approach to Monte Carlo simulations in statistical physics: Wang-Landau sampling Landau, D. P.; Tsai, Shan-Ho; Exler, M. American Journal of Physics, Vol. 72, Issue 10 https://doi.org/10.1119/1.1707017	journal	October 2004
Interstellar Polycyclic Aromatic Hydrocarbon Molecules Tielens, A. G. G. M. Annual Review of Astronomy and Astrophysics, Vol. 46, Issue 1 https://doi.org/10.1146/annurev.astro.46.060407.145211	journal	September 2008
Efficient, Multiple-Range Random Walk Algorithm to Calculate the Density of States Landau, D. P.; Wang, Fugao The American Physical Society https://doi.org/10.17877/de290r-16192	text	January 2001
HIGH-RESOLUTION IR ABSORPTION SPECTROSCOPY OF POLYCYCLIC AROMATIC HYDROCARBONS IN THE 3 μ m REGION: ROLE OF PERIPHERY Maltseva, Elena; Petrignani, Annemieke; Candian, Alessandra The Astrophysical Journal, Vol. 831, Issue 1 https://doi.org/10.3847/0004-637x/831/1/58	journal	October 2016
The infrared spectra of very large, compact, highly symmetric, polycyclic aromatic hydrocarbons (PAHs) Bauschlicher,, Charles W.; Peeters, Els; Allamandola, Louis J. arXiv https://doi.org/10.48550/arxiv.0802.1071	text	January 2008
On the nature of interlayer interactions in a system of two graphene fragments Berashevich, Julia; Chakraborty, Tapash arXiv https://doi.org/10.48550/arxiv.1107.5299	preprint	January 2011
On-line database of the spectral properties of polycyclic aromatic hydrocarbons Malloci, G.; Joblin, C.; Mulas, G. arXiv https://doi.org/10.48550/arxiv.astro-ph/0701254	text	January 2007
An efficient, multiple range random walk algorithm to calculate the density of states Wang, Fugao; Landau, D. P. arXiv https://doi.org/10.48550/arxiv.cond-mat/0011174	text	January 2000

Cited By (2)

Anharmonicity and the infrared emission spectrum of highly excited polycyclic aromatic hydrocarbons Chen, Tao; Mackie, Cameron; Candian, Alessandra Astronomy & Astrophysics, Vol. 618 https://doi.org/10.1051/0004-6361/201833731	journal	October 2018
The infrared bands of polycyclic aromatic hydrocarbons in the 1.6–1.7 μ m wavelength region Chen, Tao; Luo, Yi; Li, Aigen Astronomy & Astrophysics, Vol. 632 https://doi.org/10.1051/0004-6361/201936310	journal	December 2019

Similar Records

HIGH-RESOLUTION IR ABSORPTION SPECTROSCOPY OF POLYCYCLIC AROMATIC HYDROCARBONS: THE REALM OF ANHARMONICITY

Journal Article · Thu Nov 19 23:00:00 EST 2015 · Astrophysical Journal · OSTI ID:22521405

Anharmonicity and the infrared emission spectrum of highly excited polycyclic aromatic hydrocarbons

Journal Article · Mon Oct 01 00:00:00 EDT 2018 · Astronomy and Astrophysics · OSTI ID:1616065

Anharmonicity and the interstellar polycyclic aromatic hydrocarbon infrared emission spectrum

Journal Article · Tue Mar 31 23:00:00 EST 1987 · Astrophys. J.; (United States) · OSTI ID:6269512

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Fully anharmonic infrared cascade spectra of polycyclic aromatic hydrocarbons

Citation Formats

References (56)

Cited By (2)

Similar Records

Related Subjects