XUV excitation followed by ultrafast non-adiabatic relaxation in PAH molecules as a femto-astrochemistry experiment

A. Marciniak; V. Despré; T. Barillot; A. Rouzée; M. C.E. Galbraith; J. Klei; C. H. Yang; C. T.L. Smeenk; V. Loriot; S. Nagaprasad Reddy; A. G.G.M. Tielens; S. Mahapatra; A. I. Kuleff; M. J.J. Vrakking; F. Lépine

doi:10.1038/ncomms8909

XUV excitation followed by ultrafast non-adiabatic relaxation in PAH molecules as a femto-astrochemistry experiment

A. Marciniak, V. Despré, T. Barillot, A. Rouzée, M. C.E. Galbraith, J. Klei, C. H. Yang, C. T.L. Smeenk, V. Loriot, S. Nagaprasad Reddy, A. G.G.M. Tielens, S. Mahapatra, A. I. Kuleff, M. J.J. Vrakking, F. Lépine

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Abstract

Highly excited molecular species are at play in the chemistry of interstellar media and are involved in the creation of radiation damage in a biological tissue. Recently developed ultrashort extreme ultraviolet light sources offer the high excitation energies and ultrafast time-resolution required for probing the dynamics of highly excited molecular states on femtosecond (fs) (1 fs=10^-15s) and even attosecond (as) (1 as=10^-18s) timescales. Here we show that polycyclic aromatic hydrocarbons (PAHs) undergo ultrafast relaxation on a few tens of femtoseconds timescales, involving an interplay between the electronic and vibrational degrees of freedom. Our work reveals a general property of excited radical PAHs that can help to elucidate the assignment of diffuse interstellar absorption bands in astrochemistry, and provides a benchmark for the manner in which coupled electronic and nuclear dynamics determines reaction pathways in large molecules following extreme ultraviolet excitation.

Original language	English
Article number	7909
Journal	Nature Communications
Volume	6
DOIs	https://doi.org/10.1038/ncomms8909
State	Published - 13 Aug 2015
Externally published	Yes

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Marciniak, A., Despré, V., Barillot, T., Rouzée, A., Galbraith, M. C. E., Klei, J., Yang, C. H., Smeenk, C. T. L., Loriot, V., Reddy, S. N., Tielens, A. G. G. M., Mahapatra, S., Kuleff, A. I., Vrakking, M. J. J., & Lépine, F. (2015). XUV excitation followed by ultrafast non-adiabatic relaxation in PAH molecules as a femto-astrochemistry experiment. Nature Communications, 6, Article 7909. https://doi.org/10.1038/ncomms8909

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title = "XUV excitation followed by ultrafast non-adiabatic relaxation in PAH molecules as a femto-astrochemistry experiment",

abstract = "Highly excited molecular species are at play in the chemistry of interstellar media and are involved in the creation of radiation damage in a biological tissue. Recently developed ultrashort extreme ultraviolet light sources offer the high excitation energies and ultrafast time-resolution required for probing the dynamics of highly excited molecular states on femtosecond (fs) (1 fs=10-15s) and even attosecond (as) (1 as=10-18s) timescales. Here we show that polycyclic aromatic hydrocarbons (PAHs) undergo ultrafast relaxation on a few tens of femtoseconds timescales, involving an interplay between the electronic and vibrational degrees of freedom. Our work reveals a general property of excited radical PAHs that can help to elucidate the assignment of diffuse interstellar absorption bands in astrochemistry, and provides a benchmark for the manner in which coupled electronic and nuclear dynamics determines reaction pathways in large molecules following extreme ultraviolet excitation.",

author = "A. Marciniak and V. Despr{\'e} and T. Barillot and A. Rouz{\'e}e and Galbraith, {M. C.E.} and J. Klei and Yang, {C. H.} and Smeenk, {C. T.L.} and V. Loriot and Reddy, {S. Nagaprasad} and Tielens, {A. G.G.M.} and S. Mahapatra and Kuleff, {A. I.} and Vrakking, {M. J.J.} and F. L{\'e}pine",

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doi = "10.1038/ncomms8909",

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Marciniak, A, Despré, V, Barillot, T, Rouzée, A, Galbraith, MCE, Klei, J, Yang, CH, Smeenk, CTL, Loriot, V, Reddy, SN, Tielens, AGGM, Mahapatra, S, Kuleff, AI, Vrakking, MJJ & Lépine, F 2015, 'XUV excitation followed by ultrafast non-adiabatic relaxation in PAH molecules as a femto-astrochemistry experiment', Nature Communications, vol. 6, 7909. https://doi.org/10.1038/ncomms8909

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AU - Marciniak, A.

AU - Despré, V.

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AU - Rouzée, A.

AU - Galbraith, M. C.E.

AU - Klei, J.

AU - Yang, C. H.

AU - Smeenk, C. T.L.

AU - Loriot, V.

AU - Reddy, S. Nagaprasad

AU - Tielens, A. G.G.M.

AU - Mahapatra, S.

AU - Kuleff, A. I.

AU - Vrakking, M. J.J.

AU - Lépine, F.

PY - 2015/8/13

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XUV excitation followed by ultrafast non-adiabatic relaxation in PAH molecules as a femto-astrochemistry experiment

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