Femtosecond Laser Mass Spectrometry and High Harmonic Spectroscopy of Xylene Isomers

Alharbi, Abdullah; Boguslavskiy, Andrey E.; Austin, Dane; Thiré, Nicolas; Wood, D.; Hawkins, P.; McGrath, Felicity; Johnson, A. S.; Lopez-Quintas, I.; Schmidt, Bruno; Légaré, Francois; Marangos, J. P.; Le, Anh -Thu; Bhardwaj, Ravi

doi:10.1038/s41598-018-22055-9

Title: Femtosecond Laser Mass Spectrometry and High Harmonic Spectroscopy of Xylene Isomers

Journal Article · 28 February 2018 · Scientific Reports

DOI: https://doi.org/10.1038/s41598-018-22055-9 · OSTI ID:1500098

Alharbi, Abdullah ^[1]; Boguslavskiy, Andrey E. ^[2]; Austin, Dane ^[3]; Thiré, Nicolas ^[4]; Wood, D. ^[3]; Hawkins, P. ^[3]; McGrath, Felicity ^[3];

^[3]; Lopez-Quintas, I. ^[5]; Schmidt, Bruno ^[4];

^[4]; Marangos, J. P. ^[3];

^[6]; Bhardwaj, Ravi ^[2]

Univ. of Ottawa, Ottawa, ON (Canada); King Abdulaziz City for Science and Technology (KACST), Riyadh (Saudi Arabia)
Univ. of Ottawa, Ottawa, ON (Canada)
Imperial College London, London (United Kingdom)
INRS-EMT, Varennes (Canada)
Instituto de Química Fisica Rocasolano, Madrid (Spain)
Kansas State Univ., Manhattan, KS (United States)

Structural isomers, molecules having the same chemical formula but with atoms bonded in different order, are hard to identify using conventional spectroscopy and mass spectrometry. They exhibit virtually indistinguishable mass spectra when ionized by electrons. Laser mass spectrometry based on photoionization of the isomers has emerged as a promising alternative but requires shaped ultrafast laser pulses. Here we use transform limited femtosecond pulses to distinguish the isomers using two methods. First, we probe doubly charged parent ions with circularly polarized light. We show that the yield of doubly charged ortho-xylene decreases while para-xylene increases over a range of laser intensities when the laser polarization is changed from linear to circular. Second, we probe high harmonic generation from randomly oriented isomer molecules subjected to an intense laser field. Here we show that the yield of high-order harmonics varies with the positioning of the methyl group in xylene isomers (ortho-, para- and meta-) and is due to differences in the strength of tunnel ionization and the overlap between the angular peaks of ionization and photo-recombination.

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Research Organization:: Kansas State Univ., Manhattan, KS (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: FG02-86ER13491

OSTI ID:: 1500098

Journal Information:: Scientific Reports, Vol. 8, Issue 1; ISSN 2045-2322

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

References (63)

Cross section and asymmetry parameter calculation for sulfur 1s photoionization of SF6 Natalense, Alexandra P. P.; Lucchese, Robert R. The Journal of Chemical Physics, Vol. 111, Issue 12 https://doi.org/10.1063/1.479794	journal	September 1999
Cross section and asymmetry parameter calculation for sulfur 1s photoionization of SF6 Natalense, Alexandra P. P.; Lucchese, Robert R. The Journal of Chemical Physics, Vol. 111, Issue 12 https://doi.org/10.1063/1.479794	journal	September 1999
The latest developments and applications of mass spectrometry in food-safety and quality analysis Wang, Xian; Wang, Shujuan; Cai, Zongwei TrAC Trends in Analytical Chemistry, Vol. 52 https://doi.org/10.1016/j.trac.2013.08.005	journal	December 2013
Quantitative rescattering theory of high-order harmonic generation for polyatomic molecules Le, Anh-Thu; Lucchese, R. R.; Lin, C. D. Physical Review A, Vol. 87, Issue 6 https://doi.org/10.1103/PhysRevA.87.063406	journal	June 2013
Mass Spectrometry in Environmental Analysis [環境分析におけるマススペクトロメトリー] Suzuki, Shigeru Journal of the Mass Spectrometry Society of Japan, Vol. 55, Issue 3 https://doi.org/10.5702/massspec.55.117	journal	January 2007
High-order-harmonic generation from molecular isomers with midinfrared intense laser pulses Le, Anh-Thu; Lucchese, R. R.; Lin, C. D. Physical Review A, Vol. 88, Issue 2 https://doi.org/10.1103/PhysRevA.88.021402	journal	August 2013
Comparing differentiation of xylene isomers by electronic ionization, chemical ionization and self-ion/molecule reactions and the first observation of methyne addition ions for xylene isomers in self-ion/molecule reactions for non-nitrogenated compounds Wu, Hui-Fen; Wu, Wen-Feng Rapid Communications in Mass Spectrometry, Vol. 17, Issue 21 https://doi.org/10.1002/rcm.1203	journal	January 2003
Comparing differentiation of xylene isomers by electronic ionization, chemical ionization and self-ion/molecule reactions and the first observation of methyne addition ions for xylene isomers in self-ion/molecule reactions for non-nitrogenated compounds Wu, Hui-Fen; Wu, Wen-Feng Rapid Communications in Mass Spectrometry, Vol. 17, Issue 21 https://doi.org/10.1002/rcm.1203	journal	January 2003
Photodissociation Dynamics of Small Aromatic Molecules Studied by Multimass Ion Imaging Ni, Chi-Kung; Tseng, Cheng-Ming; Lin, Ming-Fu The Journal of Physical Chemistry B, Vol. 111, Issue 44 https://doi.org/10.1021/jp074904j	journal	November 2007
Photoelectron angular distributions from strong-field ionization of oriented molecules Holmegaard, Lotte; Hansen, Jonas L.; Kalhøj, Line arXiv https://doi.org/10.48550/arxiv.1003.4634	text	January 2010
Accurate retrieval of structural information from laser-induced photoelectron and high-harmonic spectra by few-cycle laser pulses Morishita, Toru; Le, Anh-Thu; Chen, Zhangjin arXiv https://doi.org/10.48550/arxiv.0707.3157	text	January 2007
Mass spectrometry in environmental analysis Medved, Miran Rapid Communications in Mass Spectrometry, Vol. 5, Issue 1 https://doi.org/10.1002/rcm.1290050104	journal	January 1991
Selective Bond Dissociation and Rearrangement with Optimally Tailored, Strong-Field Laser Pulses Levis, Robert J.; Menkir, Getahun M.; Rabitz, Herschel Science, Vol. 292, Issue 5517, p. 709-713 https://doi.org/10.1126/science.1059133	journal	March 2001
High Harmonic Spectroscopy of the Cooper Minimum in Molecules Wong, M. C. H.; Le, A. -T.; Alharbi, A. F. Physical Review Letters, Vol. 110, Issue 3 https://doi.org/10.1103/PhysRevLett.110.033006	journal	January 2013
Environmental Mass Spectrometry Richardson, Susan D. Analytical Chemistry, Vol. 72, Issue 18 https://doi.org/10.1021/ac000755o	journal	September 2000
Mass spectrometry in environmental analysis Medved, Miran Rapid Communications in Mass Spectrometry, Vol. 5, Issue 1 https://doi.org/10.1002/rcm.1290050104	journal	January 1991
Xylene Isomer Mass Spectral Identification through Metal Ion Chemistry in an FTICR Bjarnason, Asgeir Analytical Chemistry, Vol. 68, Issue 21 https://doi.org/10.1021/ac960597u	journal	January 1996
Photoelectron angular distributions from strong-field ionization of oriented molecules Holmegaard, Lotte; Hansen, Jonas L.; Kalhøj, Line Nature Physics, Vol. 6, Issue 6 https://doi.org/10.1038/nphys1666	journal	May 2010
Tomographic imaging of molecular orbitals Itatani, J.; Levesque, J.; Zeidler, D. Nature, Vol. 432, Issue 7019 https://doi.org/10.1038/nature03183	journal	December 2004
Dependence of high-order-harmonic-generation yield on driving-laser ellipticity Möller, Max; Cheng, Yan; Khan, Sabih D. Physical Review A, Vol. 86, Issue 1 https://doi.org/10.1103/PhysRevA.86.011401	journal	July 2012
Calculation of low‐energy elastic cross sections for electron‐CF ₄ scattering Gianturco, F. A.; Lucchese, R. R.; Sanna, N. The Journal of Chemical Physics, Vol. 100, Issue 9 https://doi.org/10.1063/1.467237	journal	May 1994
Multiple ionization of ions and atoms by intense ultrafast laser pulses Suresh, M.; McKenna, J.; Srigengan, B. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 235, Issue 1-4 https://doi.org/10.1016/j.nimb.2005.03.176	journal	July 2005
Infrared and raman spectroscopy Ryczkowski, J. Applied Catalysis A: General, Vol. 132, Issue 1 https://doi.org/10.1016/0926-860x(95)80263-0	journal	November 1995
NMR determination of enantiomeric purity Parker, David. Chemical Reviews, Vol. 91, Issue 7 https://doi.org/10.1021/cr00007a009	journal	November 1991
Accurate Retrieval of Structural Information from Laser-Induced Photoelectron and High-Order Harmonic Spectra by Few-Cycle Laser Pulses Morishita, Toru; Le, Anh-Thu; Chen, Zhangjin Physical Review Letters, Vol. 100, Issue 1 https://doi.org/10.1103/PhysRevLett.100.013903	journal	January 2008
Use of resonant two-photon ionization with supersonic beam mass spectrometry in the discrimination of cresol isomers Tembreull, Roger.; Lubman, David M. Analytical Chemistry, Vol. 56, Issue 11 https://doi.org/10.1021/ac00275a048	journal	August 1984
Environmental Mass Spectrometry Lebedev, Albert T. Annual Review of Analytical Chemistry, Vol. 6, Issue 1 https://doi.org/10.1146/annurev-anchem-062012-092604	journal	June 2013
Control of Chemical Reactions by Feedback-Optimized Phase-Shaped Femtosecond Laser Pulses Assion, A.; Baumert, T.; Bergt, M. Science, Vol. 282, Issue 5390, p. 919-922 https://doi.org/10.1126/science.282.5390.919	journal	October 1998
Use of resonant two-photon ionization with supersonic beam mass spectrometry in the discrimination of cresol isomers Tembreull, Roger.; Lubman, David M. Analytical Chemistry, Vol. 56, Issue 11 https://doi.org/10.1021/ac00275a048	journal	August 1984
Environmental Mass Spectrometry Lebedev, Albert T. Annual Review of Analytical Chemistry, Vol. 6, Issue 1 https://doi.org/10.1146/annurev-anchem-062012-092604	journal	June 2013
Quantitative Mass Spectrometric Identification of Isomers Applying Coherent Laser Control Dela Cruz, Johanna M.; Lozovoy, Vadim V.; Dantus, Marcos The Journal of Physical Chemistry A, Vol. 109, Issue 38, p. 8447-8450 https://doi.org/10.1021/jp0539425	journal	September 2005
An introduction to mass spectrometry applications in biological research Finehout, Erin J.; Lee, Kelvin H. Biochemistry and Molecular Biology Education, Vol. 32, Issue 2 https://doi.org/10.1002/bmb.2004.494032020331	journal	March 2004
A review of drug isomerism and its significance Chhabra, Naveen; Aseri, MadanL; Padmanabhan, Deepak International Journal of Applied and Basic Medical Research, Vol. 3, Issue 1 https://doi.org/10.4103/2229-516X.112233	journal	January 2013
Attosecond imaging of molecular electronic wavepackets Haessler, S.; Caillat, J.; Boutu, W. Nature Physics, Vol. 6, Issue 3 https://doi.org/10.1038/nphys1511	journal	January 2010
Distinction ofortho- andpara-Xylene by Femtosecond-Laser Mass Spectrometry Urbasch, Gunter; Breunig, Hans Georg; Weitzel, Karl-Michael ChemPhysChem, Vol. 8, Issue 15 https://doi.org/10.1002/cphc.200700498	journal	October 2007
High-harmonic spectroscopy of molecular isomers Wong, M. C. H.; Brichta, J. -P.; Spanner, M. Physical Review A, Vol. 84, Issue 5 https://doi.org/10.1103/physreva.84.051403	journal	November 2011
15N NMR Spectroscopy in Structural Analysis Marek, Radex; Lycka, Antonin Current Organic Chemistry, Vol. 6, Issue 1 https://doi.org/10.2174/1385272023374643	journal	January 2002
15N NMR Spectroscopy in Structural Analysis Marek, Radex; Lycka, Antonin Current Organic Chemistry, Vol. 6, Issue 1 https://doi.org/10.2174/1385272023374643	journal	January 2002
Calculation of low‐energy elastic cross sections for electron‐CF ₄ scattering Gianturco, F. A.; Lucchese, R. R.; Sanna, N. The Journal of Chemical Physics, Vol. 100, Issue 9 https://doi.org/10.1063/1.467237	journal	May 1994
Theory of high-harmonic generation by low-frequency laser fields Lewenstein, M.; Balcou, Ph.; Ivanov, M. Yu. Physical Review A, Vol. 49, Issue 3 https://doi.org/10.1103/PhysRevA.49.2117	journal	March 1994
NMR determination of enantiomeric purity Parker, David. Chemical Reviews, Vol. 91, Issue 7 https://doi.org/10.1021/cr00007a009	journal	November 1991
Distinction ofortho- andpara-Xylene by Femtosecond-Laser Mass Spectrometry Urbasch, Gunter; Breunig, Hans Georg; Weitzel, Karl-Michael ChemPhysChem, Vol. 8, Issue 15 https://doi.org/10.1002/cphc.200700498	journal	October 2007
Multiple ionization of ions and atoms by intense ultrafast laser pulses Suresh, M.; McKenna, J.; Srigengan, B. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 235, Issue 1-4 https://doi.org/10.1016/j.nimb.2005.03.176	journal	July 2005
Attosecond imaging of molecular electronic wavepackets Haessler, S.; Caillat, J.; Boutu, W. Nature Physics, Vol. 6, Issue 3 https://doi.org/10.1038/nphys1511	journal	January 2010
Laser mass spectrometry of the Di-, Tri- and tetrachlorobenzenes: Isomer-selective ionization and detection Weickhardt, Christian; Zimmermann, Ralf; Schramm, Karl W. Rapid Communications in Mass Spectrometry, Vol. 8, Issue 5 https://doi.org/10.1002/rcm.1290080508	journal	May 1994
Tomographic imaging of molecular orbitals Itatani, J.; Levesque, J.; Zeidler, D. Nature, Vol. 432, Issue 7019 https://doi.org/10.1038/nature03183	journal	December 2004
An introduction to mass spectrometry applications in biological research Finehout, Erin J.; Lee, Kelvin H. Biochemistry and Molecular Biology Education, Vol. 32, Issue 2 https://doi.org/10.1002/bmb.2004.494032020331	journal	March 2004
Infrared and Raman Spectroscopy Liu, Xinsheng Zeolite Chemistry and Catalysis https://doi.org/10.1007/978-1-4020-9678-5_5	book	January 2009
Probing Proton Dynamics in Molecules on an Attosecond Time Scale Baker, S.; Robinson, J. S.; Haworth, C. A. Science, Vol. 312, Issue 5772 https://doi.org/10.1126/science.1123904	journal	March 2006
Isomer differentiation by combining gas chromatography, selective self-ion/molecule reactions and tandem mass spectrometry in an ion trap mass spectrometer Wu, Hui-Fen; Chuan, Yu-Jie Rapid Communications in Mass Spectrometry, Vol. 17, Issue 10 https://doi.org/10.1002/rcm.1016	journal	January 2003
Isomer differentiation by combining gas chromatography, selective self-ion/molecule reactions and tandem mass spectrometry in an ion trap mass spectrometer Wu, Hui-Fen; Chuan, Yu-Jie Rapid Communications in Mass Spectrometry, Vol. 17, Issue 10 https://doi.org/10.1002/rcm.1016	journal	January 2003
Plasma perspective on strong field multiphoton ionization Corkum, P. B. Physical Review Letters, Vol. 71, Issue 13 https://doi.org/10.1103/PhysRevLett.71.1994	journal	September 1993
Liquid Chromatography-Mass Spectrometry Ohara, Shohei Encyclopedia of Astrobiology https://doi.org/10.1007/978-3-662-44185-5_896	book	January 2015
Quantitative Rescattering Theory for high-order harmonic generation from molecules Le, Anh-Thu; Lucchese, R. R.; Tonzani, S. arXiv https://doi.org/10.48550/arxiv.0903.5354	text	January 2009
Photoelectron angular distributions from strong-field ionization of oriented molecules Holmegaard, Lotte; Hansen, Jonas L.; Kalhøj, Line Nature Physics, Vol. 6, Issue 6 https://doi.org/10.1038/nphys1666	journal	May 2010
Selective Bond Dissociation and Rearrangement with Optimally Tailored, Strong-Field Laser Pulses Levis, Robert J.; Menkir, Getahun M.; Rabitz, Herschel Science, Vol. 292, Issue 5517, p. 709-713 https://doi.org/10.1126/science.1059133	journal	March 2001
Photodissociation Dynamics of Small Aromatic Molecules Studied by Multimass Ion Imaging Ni, Chi-Kung; Tseng, Cheng-Ming; Lin, Ming-Fu The Journal of Physical Chemistry B, Vol. 111, Issue 44 https://doi.org/10.1021/jp074904j	journal	November 2007
Orientation dependence of the ionization of CO and NO in an intense femtosecond two-color laser field Li, H.; Ray, D.; De, S. Physical Review A, Vol. 84, Issue 4 https://doi.org/10.1103/PhysRevA.84.043429	journal	October 2011
Probing molecular chirality on a sub-femtosecond timescale Cireasa, R.; Boguslavskiy, A. E.; Pons, B. Nature Physics, Vol. 11, Issue 8 https://doi.org/10.1038/nphys3369	journal	June 2015
Laser mass spectrometry of the Di-, Tri- and tetrachlorobenzenes: Isomer-selective ionization and detection Weickhardt, Christian; Zimmermann, Ralf; Schramm, Karl W. Rapid Communications in Mass Spectrometry, Vol. 8, Issue 5 https://doi.org/10.1002/rcm.1290080508	journal	May 1994
High harmonic interferometry of multi-electron dynamics in molecules Smirnova, Olga; Mairesse, Yann; Patchkovskii, Serguei Nature, Vol. 460, Issue 7258 https://doi.org/10.1038/nature08253	journal	July 2009
Quantitative rescattering theory for high-order harmonic generation from molecules Le, Anh-Thu; Lucchese, R. R.; Tonzani, S. Physical Review A, Vol. 80, Issue 1 https://doi.org/10.1103/PhysRevA.80.013401	journal	July 2009
Accurate retrieval of structural information from laser-induced photoelectron and high-harmonic spectra by few-cycle laser pulses Morishita, Toru; Le, Anh-Thu; Chen, Zhangjin arXiv https://doi.org/10.48550/arxiv.0707.3157	text	January 2007

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