publication . Other literature type . Article . Preprint . 2019

Spectroscopic Signature of Chemical Bond Dissociation Revealed by Calculated Core-Electron Spectra

Ludger Inhester; Zheng Li; Xiaolei Zhu; Nikita Medvedev; Thomas J. A. Wolf;
English
  • Published: 07 Nov 2019
  • Publisher: Deutsches Elektronen-Synchrotron, DESY, Hamburg
  • Country: Germany
Abstract
The advent of ultrashort soft x-ray pulse sources permits the use of established gas phase spectroscopy methods to investigate ultrafast photochemistry in isolated molecules with element and site specificity. In the present study, we simulate excited state wavepacket dynamics of a prototypical process, the ultrafast photodissociation of methyl iodide. Based on the simulation, we calculate time-dependent excited state carbon edge photoelectron and Auger electron spectra. We observe distinct signatures in both types of spectra and show their direct connection to C-I bond dissociation and charge rearrangement processes in the molecule. We demonstrate at the CH$_3$I...
Subjects
arXiv: Physics::Chemical PhysicsPhysics::Atomic and Molecular Clusters
free text keywords: 530, Physics - Chemical Physics, ddc:530, General Materials Science, Photodissociation, Chemistry, Core electron, Molecule, Chemical bond, Methyl iodide, chemistry.chemical_compound, Ultrashort pulse, Photochemistry, Auger electron spectroscopy, Molecular physics, Spectroscopy
45 references, page 1 of 3

(1) Cheng, Y.-C.; Fleming, G. R. Dynamics of Light Harvesting in Photosynthesis. Ann. Rev. Phys. Chem. 2009, 60, 241-262.

(2) Polli, D.; Altoè, P.; Weingart, O.; Spillane, K. M.; Manzoni, C.; Brida, D.; Tomasello, G.; Orlandi, G.; Kukura, P.; Mathies, R. A. et al. Conical Intersection Dynamics of the Primary Photoisomerization Event in Vision. Nature 2010, 467, 440-443. [OpenAIRE]

(3) Wolf, T.; Kuhlman, T. S.; Schalk, O.; Martinez, T.; Møller, K. B.; Stolow, A.; Unterreiner, A.- N. Hexamethylcyclopentadiene: Time-Resolved Photoelectron Spectroscopy and Ab Initio Multiple Spawning Simulations. Phys. Chem. Chem. Phys. 2014, 16, 11770-11779.

(4) Horton, S. L.; Liu, Y.; Forbes, R.; Makhija, V.; Lausten, R.; Stolow, A.; Hockett, P.; Marquetand, P.; Rozgonyi, T.; Weinacht, T. Excited State Dynamics of CH2I2 and CH2BrI Studied with UV Pump VUV Probe Photoelectron Spectroscopy. J. Chem. Phys. 2019, 150, 174201.

(5) Coates, M. R.; Larsen, M. A. B.; Forbes, R.; Neville, S. P.; Boguslavskiy, A. E.; Wilkinson, I.; Sølling, T. I.; Lausten, R.; Stolow, A.; Schuurman, M. S. Vacuum Ultraviolet Excited State Dynamics of the Smallest Ring, Cyclopropane. II. Time-Resolved Photoelectron Spectroscopy and Ab Initio Dynamics. J. Chem. Phys. 2018, 149, 144311.

(6) MacDonell, R. J.; Schalk, O.; Geng, T.; Thomas, R. D.; Feifel, R.; Hansson, T.; Schuurman, M. S. Excited State Dynamics of Acrylonitrile: Substituent Effects at Conical Intersections Interrogated via Time-Resolved Photoelectron Spectroscopy and Ab Initio Simulation. J. Chem. Phys. 2016, 145, 114306.

(7) Schalk, O.; Geng, T.; Thompson, T.; Baluyot, N.; Thomas, R. D.; Tapavicza, E.; Hansson, T. Cyclohexadiene Revisited: A Time-Resolved Photoelectron Spectroscopy and Ab Initio Study. J. Phys. Chem. A 2016, 120, 2320-2329.

(8) Warne, E. M.; Downes-Ward, B.; Woodhouse, J.; Parkes, M. A.; Bellshaw, D.; Springate, E.; Majchrzak, P.; Zhang, Y.; Karras, G.; Wyatt, A. S. et al. Photodissociation Dynamics of CH3I Probed via Multiphoton Ionisation Photoelectron Spectroscopy. Phys. Chem. Chem. Phys. 2019, 21, 11142-11149.

(9) Emma, P.; Akre, R.; Arthur, J.; Bionta, R.; Bostedt, C.; Bozek, J.; Brachmann, A.; Bucksbaum, P.; Coffee, R.; Decker, F.-J. et al. First Lasing and Operation of an Ångstrom-Wavelength Free-Electron Laser. Nat. Photonics 2010, 4, 641-647.

(10) Pertot, Y.; Schmidt, C.; Matthews, M.; Chauvet, A.; Huppert, M.; Svoboda, V.; von Conta, A.; Tehlar, A.; Baykusheva, D.; Wolf, J.-P. et al. Time-Resolved x-Ray Absorption Spectroscopy with a Water Window High-Harmonic Source. Science 2017, 355, 264-267. [OpenAIRE]

(11) Attar, A. R.; Bhattacherjee, A.; Pemmaraju, C. D.; Schnorr, K.; Closser, K. D.; Prendergast, D.; Leone, S. R. Femtosecond X-Ray Spectroscopy of an Electrocyclic Ring-Opening Reaction. Science 2017, 356, 54-59.

(12) Teichmann, S. M.; Silva, F.; Cousin, S. L.; Hemmer, M.; Biegert, J. 0.5-keV Soft X-Ray Attosecond Continua. Nat. Commun. 2016, 7, 11493.

(13) Johnson, A. S.; Austin, D. R.; Wood, D. A.; Brahms, C.; Gregory, A.; Holzner, K. B.; Jarosch, S.; Larsen, E. W.; Parker, S.; Strüber, C. S. et al. High-Flux Soft x-Ray Harmonic Generation from Ionization-Shaped Few-Cycle Laser Pulses. Sci. Adv. 2018, 4, eaar3761.

(14) Allaria, E.; Appio, R.; Badano, L.; Barletta, W. A.; Bassanese, S.; Biedron, S. G.; Borga, A.; Busetto, E.; Castronovo, D.; Cinquegrana, P. et al. Highly Coherent and Stable Pulses from the FERMI Seeded Free-Electron Laser in the Extreme Ultraviolet. Nat. Photonics 2012, 6, 699-704. [OpenAIRE]

(15) Ackermann, W.; Asova, G.; Ayvazyan, V.; Azima, A.; Baboi, N.; Bähr, J.; Balandin, V.; Beutner, B.; Brandt, A.; Bolzmann, A. et al. Operation of a Free-Electron Laser from the Extreme Ultraviolet to the Water Window. Nat. Photonics 2007, 1, 336-342.

45 references, page 1 of 3
Abstract
The advent of ultrashort soft x-ray pulse sources permits the use of established gas phase spectroscopy methods to investigate ultrafast photochemistry in isolated molecules with element and site specificity. In the present study, we simulate excited state wavepacket dynamics of a prototypical process, the ultrafast photodissociation of methyl iodide. Based on the simulation, we calculate time-dependent excited state carbon edge photoelectron and Auger electron spectra. We observe distinct signatures in both types of spectra and show their direct connection to C-I bond dissociation and charge rearrangement processes in the molecule. We demonstrate at the CH$_3$I...
Subjects
arXiv: Physics::Chemical PhysicsPhysics::Atomic and Molecular Clusters
free text keywords: 530, Physics - Chemical Physics, ddc:530, General Materials Science, Photodissociation, Chemistry, Core electron, Molecule, Chemical bond, Methyl iodide, chemistry.chemical_compound, Ultrashort pulse, Photochemistry, Auger electron spectroscopy, Molecular physics, Spectroscopy
45 references, page 1 of 3

(1) Cheng, Y.-C.; Fleming, G. R. Dynamics of Light Harvesting in Photosynthesis. Ann. Rev. Phys. Chem. 2009, 60, 241-262.

(2) Polli, D.; Altoè, P.; Weingart, O.; Spillane, K. M.; Manzoni, C.; Brida, D.; Tomasello, G.; Orlandi, G.; Kukura, P.; Mathies, R. A. et al. Conical Intersection Dynamics of the Primary Photoisomerization Event in Vision. Nature 2010, 467, 440-443. [OpenAIRE]

(3) Wolf, T.; Kuhlman, T. S.; Schalk, O.; Martinez, T.; Møller, K. B.; Stolow, A.; Unterreiner, A.- N. Hexamethylcyclopentadiene: Time-Resolved Photoelectron Spectroscopy and Ab Initio Multiple Spawning Simulations. Phys. Chem. Chem. Phys. 2014, 16, 11770-11779.

(4) Horton, S. L.; Liu, Y.; Forbes, R.; Makhija, V.; Lausten, R.; Stolow, A.; Hockett, P.; Marquetand, P.; Rozgonyi, T.; Weinacht, T. Excited State Dynamics of CH2I2 and CH2BrI Studied with UV Pump VUV Probe Photoelectron Spectroscopy. J. Chem. Phys. 2019, 150, 174201.

(5) Coates, M. R.; Larsen, M. A. B.; Forbes, R.; Neville, S. P.; Boguslavskiy, A. E.; Wilkinson, I.; Sølling, T. I.; Lausten, R.; Stolow, A.; Schuurman, M. S. Vacuum Ultraviolet Excited State Dynamics of the Smallest Ring, Cyclopropane. II. Time-Resolved Photoelectron Spectroscopy and Ab Initio Dynamics. J. Chem. Phys. 2018, 149, 144311.

(6) MacDonell, R. J.; Schalk, O.; Geng, T.; Thomas, R. D.; Feifel, R.; Hansson, T.; Schuurman, M. S. Excited State Dynamics of Acrylonitrile: Substituent Effects at Conical Intersections Interrogated via Time-Resolved Photoelectron Spectroscopy and Ab Initio Simulation. J. Chem. Phys. 2016, 145, 114306.

(7) Schalk, O.; Geng, T.; Thompson, T.; Baluyot, N.; Thomas, R. D.; Tapavicza, E.; Hansson, T. Cyclohexadiene Revisited: A Time-Resolved Photoelectron Spectroscopy and Ab Initio Study. J. Phys. Chem. A 2016, 120, 2320-2329.

(8) Warne, E. M.; Downes-Ward, B.; Woodhouse, J.; Parkes, M. A.; Bellshaw, D.; Springate, E.; Majchrzak, P.; Zhang, Y.; Karras, G.; Wyatt, A. S. et al. Photodissociation Dynamics of CH3I Probed via Multiphoton Ionisation Photoelectron Spectroscopy. Phys. Chem. Chem. Phys. 2019, 21, 11142-11149.

(9) Emma, P.; Akre, R.; Arthur, J.; Bionta, R.; Bostedt, C.; Bozek, J.; Brachmann, A.; Bucksbaum, P.; Coffee, R.; Decker, F.-J. et al. First Lasing and Operation of an Ångstrom-Wavelength Free-Electron Laser. Nat. Photonics 2010, 4, 641-647.

(10) Pertot, Y.; Schmidt, C.; Matthews, M.; Chauvet, A.; Huppert, M.; Svoboda, V.; von Conta, A.; Tehlar, A.; Baykusheva, D.; Wolf, J.-P. et al. Time-Resolved x-Ray Absorption Spectroscopy with a Water Window High-Harmonic Source. Science 2017, 355, 264-267. [OpenAIRE]

(11) Attar, A. R.; Bhattacherjee, A.; Pemmaraju, C. D.; Schnorr, K.; Closser, K. D.; Prendergast, D.; Leone, S. R. Femtosecond X-Ray Spectroscopy of an Electrocyclic Ring-Opening Reaction. Science 2017, 356, 54-59.

(12) Teichmann, S. M.; Silva, F.; Cousin, S. L.; Hemmer, M.; Biegert, J. 0.5-keV Soft X-Ray Attosecond Continua. Nat. Commun. 2016, 7, 11493.

(13) Johnson, A. S.; Austin, D. R.; Wood, D. A.; Brahms, C.; Gregory, A.; Holzner, K. B.; Jarosch, S.; Larsen, E. W.; Parker, S.; Strüber, C. S. et al. High-Flux Soft x-Ray Harmonic Generation from Ionization-Shaped Few-Cycle Laser Pulses. Sci. Adv. 2018, 4, eaar3761.

(14) Allaria, E.; Appio, R.; Badano, L.; Barletta, W. A.; Bassanese, S.; Biedron, S. G.; Borga, A.; Busetto, E.; Castronovo, D.; Cinquegrana, P. et al. Highly Coherent and Stable Pulses from the FERMI Seeded Free-Electron Laser in the Extreme Ultraviolet. Nat. Photonics 2012, 6, 699-704. [OpenAIRE]

(15) Ackermann, W.; Asova, G.; Ayvazyan, V.; Azima, A.; Baboi, N.; Bähr, J.; Balandin, V.; Beutner, B.; Brandt, A.; Bolzmann, A. et al. Operation of a Free-Electron Laser from the Extreme Ultraviolet to the Water Window. Nat. Photonics 2007, 1, 336-342.

45 references, page 1 of 3
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publication . Other literature type . Article . Preprint . 2019

Spectroscopic Signature of Chemical Bond Dissociation Revealed by Calculated Core-Electron Spectra

Ludger Inhester; Zheng Li; Xiaolei Zhu; Nikita Medvedev; Thomas J. A. Wolf;