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1. A localized view on molecular dissociation via electron-ion partial covariance

Author

Allum, Felix, Music, Valerija, Inhester, Ludger, Boll, Rebecca, Erk, Benjamin, Schmidt, Philipp, Baumann, Thomas M., Brenner, Günter, Burt, Michael, Demekhin, Philipp V., Dörner, Simon, Ehresmann, Arno, Galler, Andreas, Grychtol, Patrik, Heathcote, David, Kargin, Denis, Larsson, Mats, Lee, Jason W. L., Li, Zheng, Manschwetus, Bastian, Marder, Lutz, Mason, Robert, Meyer, Michael, Otto, Huda, Passow, Christopher, Pietschnig, Rudolf, Ramm, Daniel, Schubert, Kaja, Schwob, Lucas, Thomas, Richard D., Vallance, Claire, Vidanović, Igor, von Korff Schmising, Clemens, Wagner, René, Walter, Peter, Zhaunerchyk, Vitali, Rolles, Daniel, Bari, Sadia, Brouard, Mark, Ilchen, Markus, Allum, Felix, Music, Valerija, Inhester, Ludger, Boll, Rebecca, Erk, Benjamin, Schmidt, Philipp, Baumann, Thomas M., Brenner, Günter, Burt, Michael, Demekhin, Philipp V., Dörner, Simon, Ehresmann, Arno, Galler, Andreas, Grychtol, Patrik, Heathcote, David, Kargin, Denis, Larsson, Mats, Lee, Jason W. L., Li, Zheng, Manschwetus, Bastian, Marder, Lutz, Mason, Robert, Meyer, Michael, Otto, Huda, Passow, Christopher, Pietschnig, Rudolf, Ramm, Daniel, Schubert, Kaja, Schwob, Lucas, Thomas, Richard D., Vallance, Claire, Vidanović, Igor, von Korff Schmising, Clemens, Wagner, René, Walter, Peter, Zhaunerchyk, Vitali, Rolles, Daniel, Bari, Sadia, Brouard, Mark, and Ilchen, Markus

Abstract

Inner-shell photoelectron spectroscopy provides an element-specific probe of molecular structure, as core-electron binding energies are sensitive to the chemical environment. Short-wavelength femtosecond light sources, such as Free-Electron Lasers (FELs), even enable time-resolved site-specific investigations of molecular photochemistry. Here, we study the ultraviolet photodissociation of the prototypical chiral molecule 1-iodo-2-methylbutane, probed by extreme-ultraviolet (XUV) pulses from the Free-electron LASer in Hamburg (FLASH) through the ultrafast evolution of the iodine 4d binding energy. Methodologically, we employ electron-ion partial covariance imaging as a technique to isolate otherwise elusive features in a two-dimensional photoelectron spectrum arising from different photofragmentation pathways. The experimental and theoretical results for the time-resolved electron spectra of the 4d3/2 and 4d5/2 atomic and molecular levels that are disentangled by this method provide a key step towards studying structural and chemical changes from a specific spectator site.

Published
2022
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2. UV-induced dissociation of CH2BrI probed by intense femtosecond XUV pulses

Author

Kockert, Hansjochen, Lee, Jason W. L., Allum, Felix, Amini, Kasra, Bari, Sadia, Bomme, Cedric, Brausse, Felix, Brouard, Mark, Burt, Michael, de Miranda, Barbara Cunha, Duesterer, Stefan, Eng-Johnsson, Per, Erk, Benjamin, Geleoc, Marie, Geneaux, Romain, Gentleman, Alexander S., Guillemin, Renaud, Goldsztejn, Gildas, Holland, David M. P., Ismail, Iyas, Journel, Loic, Kierspel, Thomas, Kuepper, Jochen, Lahl, Jan, Mackenzie, Stuart R., Maclot, Sylvain, Manschwetus, Bastian, Mereshchenko, Andrey S., Mullins, Terence, Olshin, Pavel K., Palaudoux, Jerome, Penent, Francis, Piancastelli, Maria Novella, Rompotis, Dimitrios, Rouzee, Arnaud, Ruchon, Thierry, Rudenko, Artem, Schirmel, Nora, Simon, Marc, Techert, Simone, Travnikova, Oksana, Trippel, Sebastian, Vallance, Claire, Wang, Enliang, Wiese, Joss, Ziaee, Farzaneh, Marchenko, Tatiana, Rolles, Daniel, Boll, Rebecca, Kockert, Hansjochen, Lee, Jason W. L., Allum, Felix, Amini, Kasra, Bari, Sadia, Bomme, Cedric, Brausse, Felix, Brouard, Mark, Burt, Michael, de Miranda, Barbara Cunha, Duesterer, Stefan, Eng-Johnsson, Per, Erk, Benjamin, Geleoc, Marie, Geneaux, Romain, Gentleman, Alexander S., Guillemin, Renaud, Goldsztejn, Gildas, Holland, David M. P., Ismail, Iyas, Journel, Loic, Kierspel, Thomas, Kuepper, Jochen, Lahl, Jan, Mackenzie, Stuart R., Maclot, Sylvain, Manschwetus, Bastian, Mereshchenko, Andrey S., Mullins, Terence, Olshin, Pavel K., Palaudoux, Jerome, Penent, Francis, Piancastelli, Maria Novella, Rompotis, Dimitrios, Rouzee, Arnaud, Ruchon, Thierry, Rudenko, Artem, Schirmel, Nora, Simon, Marc, Techert, Simone, Travnikova, Oksana, Trippel, Sebastian, Vallance, Claire, Wang, Enliang, Wiese, Joss, Ziaee, Farzaneh, Marchenko, Tatiana, Rolles, Daniel, and Boll, Rebecca

Abstract

The ultraviolet (UV)-induced dissociation and photofragmentation of gas-phase CH2BrI molecules induced by intense femtosecond extreme ultraviolet (XUV) pulses at three different photon energies are studied by multi-mass ion imaging. Using a UV-pump-XUV-probe scheme, charge transfer between highly charged iodine ions and neutral CH2Br radicals produced by C-I bond cleavage is investigated. In earlier charge-transfer studies, the center of mass of the molecules was located along the axis of the bond cleaved by the pump pulse. In the present case of CH2BrI, this is not the case, thus inducing a rotation of the fragment. We discuss the influence of the rotation on the charge transfer process using a classical over-the-barrier model. Our modeling suggests that, despite the fact that the dissociation is slower due to the rotational excitation, the critical interatomic distance for charge transfer is reached faster. Furthermore, we suggest that charge transfer during molecular fragmentation may be modulated in a complex way.

Published
2022
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3. UV-induced dissociation of CH2BrI probed by intense femtosecond XUV pulses

Author

Kockert, Hansjochen, Lee, Jason W. L., Allum, Felix, Amini, Kasra, Bari, Sadia, Bomme, Cedric, Brausse, Felix, Brouard, Mark, Burt, Michael, de Miranda, Barbara Cunha, Duesterer, Stefan, Eng-Johnsson, Per, Erk, Benjamin, Geleoc, Marie, Geneaux, Romain, Gentleman, Alexander S., Guillemin, Renaud, Goldsztejn, Gildas, Holland, David M. P., Ismail, Iyas, Journel, Loic, Kierspel, Thomas, Kuepper, Jochen, Lahl, Jan, Mackenzie, Stuart R., Maclot, Sylvain, Manschwetus, Bastian, Mereshchenko, Andrey S., Mullins, Terence, Olshin, Pavel K., Palaudoux, Jerome, Penent, Francis, Piancastelli, Maria Novella, Rompotis, Dimitrios, Rouzee, Arnaud, Ruchon, Thierry, Rudenko, Artem, Schirmel, Nora, Simon, Marc, Techert, Simone, Travnikova, Oksana, Trippel, Sebastian, Vallance, Claire, Wang, Enliang, Wiese, Joss, Ziaee, Farzaneh, Marchenko, Tatiana, Rolles, Daniel, Boll, Rebecca, Kockert, Hansjochen, Lee, Jason W. L., Allum, Felix, Amini, Kasra, Bari, Sadia, Bomme, Cedric, Brausse, Felix, Brouard, Mark, Burt, Michael, de Miranda, Barbara Cunha, Duesterer, Stefan, Eng-Johnsson, Per, Erk, Benjamin, Geleoc, Marie, Geneaux, Romain, Gentleman, Alexander S., Guillemin, Renaud, Goldsztejn, Gildas, Holland, David M. P., Ismail, Iyas, Journel, Loic, Kierspel, Thomas, Kuepper, Jochen, Lahl, Jan, Mackenzie, Stuart R., Maclot, Sylvain, Manschwetus, Bastian, Mereshchenko, Andrey S., Mullins, Terence, Olshin, Pavel K., Palaudoux, Jerome, Penent, Francis, Piancastelli, Maria Novella, Rompotis, Dimitrios, Rouzee, Arnaud, Ruchon, Thierry, Rudenko, Artem, Schirmel, Nora, Simon, Marc, Techert, Simone, Travnikova, Oksana, Trippel, Sebastian, Vallance, Claire, Wang, Enliang, Wiese, Joss, Ziaee, Farzaneh, Marchenko, Tatiana, Rolles, Daniel, and Boll, Rebecca

Abstract

The ultraviolet (UV)-induced dissociation and photofragmentation of gas-phase CH2BrI molecules induced by intense femtosecond extreme ultraviolet (XUV) pulses at three different photon energies are studied by multi-mass ion imaging. Using a UV-pump-XUV-probe scheme, charge transfer between highly charged iodine ions and neutral CH2Br radicals produced by C-I bond cleavage is investigated. In earlier charge-transfer studies, the center of mass of the molecules was located along the axis of the bond cleaved by the pump pulse. In the present case of CH2BrI, this is not the case, thus inducing a rotation of the fragment. We discuss the influence of the rotation on the charge transfer process using a classical over-the-barrier model. Our modeling suggests that, despite the fact that the dissociation is slower due to the rotational excitation, the critical interatomic distance for charge transfer is reached faster. Furthermore, we suggest that charge transfer during molecular fragmentation may be modulated in a complex way.

Published
2022
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4. UV-induced dissociation of CH2BrI probed by intense femtosecond XUV pulses

Author

Kockert, Hansjochen, Lee, Jason W. L., Allum, Felix, Amini, Kasra, Bari, Sadia, Bomme, Cedric, Brausse, Felix, Brouard, Mark, Burt, Michael, de Miranda, Barbara Cunha, Duesterer, Stefan, Eng-Johnsson, Per, Erk, Benjamin, Geleoc, Marie, Geneaux, Romain, Gentleman, Alexander S., Guillemin, Renaud, Goldsztejn, Gildas, Holland, David M. P., Ismail, Iyas, Journel, Loic, Kierspel, Thomas, Kuepper, Jochen, Lahl, Jan, Mackenzie, Stuart R., Maclot, Sylvain, Manschwetus, Bastian, Mereshchenko, Andrey S., Mullins, Terence, Olshin, Pavel K., Palaudoux, Jerome, Penent, Francis, Piancastelli, Maria Novella, Rompotis, Dimitrios, Rouzee, Arnaud, Ruchon, Thierry, Rudenko, Artem, Schirmel, Nora, Simon, Marc, Techert, Simone, Travnikova, Oksana, Trippel, Sebastian, Vallance, Claire, Wang, Enliang, Wiese, Joss, Ziaee, Farzaneh, Marchenko, Tatiana, Rolles, Daniel, Boll, Rebecca, Kockert, Hansjochen, Lee, Jason W. L., Allum, Felix, Amini, Kasra, Bari, Sadia, Bomme, Cedric, Brausse, Felix, Brouard, Mark, Burt, Michael, de Miranda, Barbara Cunha, Duesterer, Stefan, Eng-Johnsson, Per, Erk, Benjamin, Geleoc, Marie, Geneaux, Romain, Gentleman, Alexander S., Guillemin, Renaud, Goldsztejn, Gildas, Holland, David M. P., Ismail, Iyas, Journel, Loic, Kierspel, Thomas, Kuepper, Jochen, Lahl, Jan, Mackenzie, Stuart R., Maclot, Sylvain, Manschwetus, Bastian, Mereshchenko, Andrey S., Mullins, Terence, Olshin, Pavel K., Palaudoux, Jerome, Penent, Francis, Piancastelli, Maria Novella, Rompotis, Dimitrios, Rouzee, Arnaud, Ruchon, Thierry, Rudenko, Artem, Schirmel, Nora, Simon, Marc, Techert, Simone, Travnikova, Oksana, Trippel, Sebastian, Vallance, Claire, Wang, Enliang, Wiese, Joss, Ziaee, Farzaneh, Marchenko, Tatiana, Rolles, Daniel, and Boll, Rebecca

Abstract

The ultraviolet (UV)-induced dissociation and photofragmentation of gas-phase CH2BrI molecules induced by intense femtosecond extreme ultraviolet (XUV) pulses at three different photon energies are studied by multi-mass ion imaging. Using a UV-pump-XUV-probe scheme, charge transfer between highly charged iodine ions and neutral CH2Br radicals produced by C-I bond cleavage is investigated. In earlier charge-transfer studies, the center of mass of the molecules was located along the axis of the bond cleaved by the pump pulse. In the present case of CH2BrI, this is not the case, thus inducing a rotation of the fragment. We discuss the influence of the rotation on the charge transfer process using a classical over-the-barrier model. Our modeling suggests that, despite the fact that the dissociation is slower due to the rotational excitation, the critical interatomic distance for charge transfer is reached faster. Furthermore, we suggest that charge transfer during molecular fragmentation may be modulated in a complex way.

Published
2022
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5. UV-induced dissociation of CH2BrI probed by intense femtosecond XUV pulses

Author

Kockert, Hansjochen, Lee, Jason W. L., Allum, Felix, Amini, Kasra, Bari, Sadia, Bomme, Cedric, Brausse, Felix, Brouard, Mark, Burt, Michael, de Miranda, Barbara Cunha, Duesterer, Stefan, Eng-Johnsson, Per, Erk, Benjamin, Geleoc, Marie, Geneaux, Romain, Gentleman, Alexander S., Guillemin, Renaud, Goldsztejn, Gildas, Holland, David M. P., Ismail, Iyas, Journel, Loic, Kierspel, Thomas, Kuepper, Jochen, Lahl, Jan, Mackenzie, Stuart R., Maclot, Sylvain, Manschwetus, Bastian, Mereshchenko, Andrey S., Mullins, Terence, Olshin, Pavel K., Palaudoux, Jerome, Penent, Francis, Piancastelli, Maria Novella, Rompotis, Dimitrios, Rouzee, Arnaud, Ruchon, Thierry, Rudenko, Artem, Schirmel, Nora, Simon, Marc, Techert, Simone, Travnikova, Oksana, Trippel, Sebastian, Vallance, Claire, Wang, Enliang, Wiese, Joss, Ziaee, Farzaneh, Marchenko, Tatiana, Rolles, Daniel, Boll, Rebecca, Kockert, Hansjochen, Lee, Jason W. L., Allum, Felix, Amini, Kasra, Bari, Sadia, Bomme, Cedric, Brausse, Felix, Brouard, Mark, Burt, Michael, de Miranda, Barbara Cunha, Duesterer, Stefan, Eng-Johnsson, Per, Erk, Benjamin, Geleoc, Marie, Geneaux, Romain, Gentleman, Alexander S., Guillemin, Renaud, Goldsztejn, Gildas, Holland, David M. P., Ismail, Iyas, Journel, Loic, Kierspel, Thomas, Kuepper, Jochen, Lahl, Jan, Mackenzie, Stuart R., Maclot, Sylvain, Manschwetus, Bastian, Mereshchenko, Andrey S., Mullins, Terence, Olshin, Pavel K., Palaudoux, Jerome, Penent, Francis, Piancastelli, Maria Novella, Rompotis, Dimitrios, Rouzee, Arnaud, Ruchon, Thierry, Rudenko, Artem, Schirmel, Nora, Simon, Marc, Techert, Simone, Travnikova, Oksana, Trippel, Sebastian, Vallance, Claire, Wang, Enliang, Wiese, Joss, Ziaee, Farzaneh, Marchenko, Tatiana, Rolles, Daniel, and Boll, Rebecca

Abstract

The ultraviolet (UV)-induced dissociation and photofragmentation of gas-phase CH2BrI molecules induced by intense femtosecond extreme ultraviolet (XUV) pulses at three different photon energies are studied by multi-mass ion imaging. Using a UV-pump-XUV-probe scheme, charge transfer between highly charged iodine ions and neutral CH2Br radicals produced by C-I bond cleavage is investigated. In earlier charge-transfer studies, the center of mass of the molecules was located along the axis of the bond cleaved by the pump pulse. In the present case of CH2BrI, this is not the case, thus inducing a rotation of the fragment. We discuss the influence of the rotation on the charge transfer process using a classical over-the-barrier model. Our modeling suggests that, despite the fact that the dissociation is slower due to the rotational excitation, the critical interatomic distance for charge transfer is reached faster. Furthermore, we suggest that charge transfer during molecular fragmentation may be modulated in a complex way.

Published
2022
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6. UV-induced dissociation of CH2BrI probed by intense femtosecond XUV pulses

Author

Kockert, Hansjochen, Lee, Jason W. L., Allum, Felix, Amini, Kasra, Bari, Sadia, Bomme, Cedric, Brausse, Felix, Brouard, Mark, Burt, Michael, de Miranda, Barbara Cunha, Duesterer, Stefan, Eng-Johnsson, Per, Erk, Benjamin, Geleoc, Marie, Geneaux, Romain, Gentleman, Alexander S., Guillemin, Renaud, Goldsztejn, Gildas, Holland, David M. P., Ismail, Iyas, Journel, Loic, Kierspel, Thomas, Kuepper, Jochen, Lahl, Jan, Mackenzie, Stuart R., Maclot, Sylvain, Manschwetus, Bastian, Mereshchenko, Andrey S., Mullins, Terence, Olshin, Pavel K., Palaudoux, Jerome, Penent, Francis, Piancastelli, Maria Novella, Rompotis, Dimitrios, Rouzee, Arnaud, Ruchon, Thierry, Rudenko, Artem, Schirmel, Nora, Simon, Marc, Techert, Simone, Travnikova, Oksana, Trippel, Sebastian, Vallance, Claire, Wang, Enliang, Wiese, Joss, Ziaee, Farzaneh, Marchenko, Tatiana, Rolles, Daniel, Boll, Rebecca, Kockert, Hansjochen, Lee, Jason W. L., Allum, Felix, Amini, Kasra, Bari, Sadia, Bomme, Cedric, Brausse, Felix, Brouard, Mark, Burt, Michael, de Miranda, Barbara Cunha, Duesterer, Stefan, Eng-Johnsson, Per, Erk, Benjamin, Geleoc, Marie, Geneaux, Romain, Gentleman, Alexander S., Guillemin, Renaud, Goldsztejn, Gildas, Holland, David M. P., Ismail, Iyas, Journel, Loic, Kierspel, Thomas, Kuepper, Jochen, Lahl, Jan, Mackenzie, Stuart R., Maclot, Sylvain, Manschwetus, Bastian, Mereshchenko, Andrey S., Mullins, Terence, Olshin, Pavel K., Palaudoux, Jerome, Penent, Francis, Piancastelli, Maria Novella, Rompotis, Dimitrios, Rouzee, Arnaud, Ruchon, Thierry, Rudenko, Artem, Schirmel, Nora, Simon, Marc, Techert, Simone, Travnikova, Oksana, Trippel, Sebastian, Vallance, Claire, Wang, Enliang, Wiese, Joss, Ziaee, Farzaneh, Marchenko, Tatiana, Rolles, Daniel, and Boll, Rebecca

Abstract

The ultraviolet (UV)-induced dissociation and photofragmentation of gas-phase CH2BrI molecules induced by intense femtosecond extreme ultraviolet (XUV) pulses at three different photon energies are studied by multi-mass ion imaging. Using a UV-pump-XUV-probe scheme, charge transfer between highly charged iodine ions and neutral CH2Br radicals produced by C-I bond cleavage is investigated. In earlier charge-transfer studies, the center of mass of the molecules was located along the axis of the bond cleaved by the pump pulse. In the present case of CH2BrI, this is not the case, thus inducing a rotation of the fragment. We discuss the influence of the rotation on the charge transfer process using a classical over-the-barrier model. Our modeling suggests that, despite the fact that the dissociation is slower due to the rotational excitation, the critical interatomic distance for charge transfer is reached faster. Furthermore, we suggest that charge transfer during molecular fragmentation may be modulated in a complex way.

Published
2022
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8. Coulomb explosion imaging of CH3I and CH2CII photodissociation dynamics

Author

Allum, Felix, Burt, Michael, Amini, Kasra, Boll, Rebecca, Kockert, Hansjochen, Olshin, Pavel K., Bari, Sadia, Bomme, Cedric, Brausse, Felix, de Miranda, Barbara Cunha, Duesterer, Stefan, Erk, Benjamin, Geleoc, Marie, Geneaux, Romain, Gentleman, Alexander S., Goldsztejn, Gildas, Guillemin, Renaud, Holland, David M. P., Ismail, Iyas, Johnsson, Per, Journel, Loic, Kuepper, Jochen, Lahl, Jan, Lee, Jason W. L., Maclot, Sylvain, Mackenzie, Stuart R., Manschwetus, Bastian, Mereshchenko, Andrey S., Mason, Robert, Palaudoux, Jerome, Piancastelli, Maria Novella, Penent, Francis, Rompotis, Dimitrios, Rouzee, Arnaud, Ruchon, Thierry, Rudenko, Artem, Savelyev, Evgeny, Simon, Marc, Schirmel, Nora, Stapelfeldt, Henrik, Techert, Simone, Travnikova, Oksana, Trippel, Sebastian, Underwood, Jonathan G., Vallance, Claire, Wiese, Joss, Ziaee, Farzaneh, Brouard, Mark, Marchenko, Tatiana, Rolles, Daniel, Allum, Felix, Burt, Michael, Amini, Kasra, Boll, Rebecca, Kockert, Hansjochen, Olshin, Pavel K., Bari, Sadia, Bomme, Cedric, Brausse, Felix, de Miranda, Barbara Cunha, Duesterer, Stefan, Erk, Benjamin, Geleoc, Marie, Geneaux, Romain, Gentleman, Alexander S., Goldsztejn, Gildas, Guillemin, Renaud, Holland, David M. P., Ismail, Iyas, Johnsson, Per, Journel, Loic, Kuepper, Jochen, Lahl, Jan, Lee, Jason W. L., Maclot, Sylvain, Mackenzie, Stuart R., Manschwetus, Bastian, Mereshchenko, Andrey S., Mason, Robert, Palaudoux, Jerome, Piancastelli, Maria Novella, Penent, Francis, Rompotis, Dimitrios, Rouzee, Arnaud, Ruchon, Thierry, Rudenko, Artem, Savelyev, Evgeny, Simon, Marc, Schirmel, Nora, Stapelfeldt, Henrik, Techert, Simone, Travnikova, Oksana, Trippel, Sebastian, Underwood, Jonathan G., Vallance, Claire, Wiese, Joss, Ziaee, Farzaneh, Brouard, Mark, Marchenko, Tatiana, and Rolles, Daniel

Abstract

The photodissociation dynamics of CH3I and CH2CII at 272 nm were investigated by time-resolved Coulomb explosion imaging, with an intense non-resonant 815nmprobe pulse. Fragment ion momenta over a widem/z range were recorded simultaneously by coupling a velocity map imaging spectrometer with a pixel imaging mass spectrometry camera. For both molecules, delay-dependent pump-probe features were assigned to ultraviolet-induced carbon-iodine bond cleavage followed by Coulomb explosion. Multi-mass imaging also allowed the sequential cleavage of both carbon-halogen bonds in CH2ClI to be investigated. Furthermore, delay-dependent relative fragment momenta of a pair of ions were directly determined using recoil-frame covariance analysis. These results are complementary to conventional velocity map imaging experiments and demonstrate the application of time-resolved Coulomb explosion imaging to photoinduced real-time molecular motion.

Published
2018
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9. Time-resolved inner-shell photoelectron spectroscopy : From a bound molecule to an isolated atom

Author

Brasse, Felix, Goldsztejn, Gildas, Amini, Kasra, Boll, Rebecca, Bari, Sadia, Bomme, Cedric, Brouard, Mark, Burt, Michael, de Miranda, Barbara Cunha, Duesterer, Stefan, Erk, Benjamin, Geleoc, Marie, Geneaux, Romain, Gentleman, Alexander S., Guillemin, Renaud, Ismail, Iyas, Johnsson, Per, Journel, Loic, Kierspel, Thomas, Kockert, Hansjochen, Kuepper, Jochen, Lablanquie, Pascal, Lahl, Jan, Lee, Jason W. L., Mackenzie, Stuart R., Maclot, Sylvain, Manschwetus, Bastian, Mereshchenko, Andrey S., Mullins, Terence, Olshin, Pavel K., Palaudoux, Jerome, Patchkovskii, Serguei, Penent, Francis, Piancastelli, Maria Novella, Rompotis, Dimitrios, Ruchon, Thierry, Rudenko, Artem, Savelyev, Evgeny, Schirmel, Nora, Techert, Simone, Travnikova, Oksana, Trippel, Sebastian, Underwood, Jonathan G., Vallance, Claire, Wiese, Joss, Simon, Marc, Holland, David M. P., Marchenko, Tatiana, Rouzee, Arnaud, Rolles, Daniel, Brasse, Felix, Goldsztejn, Gildas, Amini, Kasra, Boll, Rebecca, Bari, Sadia, Bomme, Cedric, Brouard, Mark, Burt, Michael, de Miranda, Barbara Cunha, Duesterer, Stefan, Erk, Benjamin, Geleoc, Marie, Geneaux, Romain, Gentleman, Alexander S., Guillemin, Renaud, Ismail, Iyas, Johnsson, Per, Journel, Loic, Kierspel, Thomas, Kockert, Hansjochen, Kuepper, Jochen, Lablanquie, Pascal, Lahl, Jan, Lee, Jason W. L., Mackenzie, Stuart R., Maclot, Sylvain, Manschwetus, Bastian, Mereshchenko, Andrey S., Mullins, Terence, Olshin, Pavel K., Palaudoux, Jerome, Patchkovskii, Serguei, Penent, Francis, Piancastelli, Maria Novella, Rompotis, Dimitrios, Ruchon, Thierry, Rudenko, Artem, Savelyev, Evgeny, Schirmel, Nora, Techert, Simone, Travnikova, Oksana, Trippel, Sebastian, Underwood, Jonathan G., Vallance, Claire, Wiese, Joss, Simon, Marc, Holland, David M. P., Marchenko, Tatiana, Rouzee, Arnaud, and Rolles, Daniel

Abstract

Due to its element and site specificity, inner-shell photoelectron spectroscopy is a widely used technique to probe the chemical structure of matter. Here, we show that time-resolved inner-shell photoelectron spectroscopy can be employed to observe ultrafast chemical reactions and the electronic response to the nuclear motion with high sensitivity. The ultraviolet dissociation of iodomethane (CH3I) is investigated by ionization above the iodine 4d edge, using time-resolved inner-shell photoelectron and photoion spectroscopy. The dynamics observed in the photoelectron spectra appear earlier and are faster than those seen in the iodine fragments. The experimental results are interpreted using crystal-field and spin-orbit configuration interaction calculations, and demonstrate that time-resolved inner-shell photoelectron spectroscopy is a powerful tool to directly track ultrafast structural and electronic transformations in gas-phase molecules.

Published
2018
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10. Coulomb-explosion imaging of concurrent CH2BrI photodissociation dynamics

Author

Burt, Michael, Boll, Rebecca, Lee, Jason W. L., Amini, Kasra, Kockert, Hansjochen, Vallance, Claire, Gentleman, Alexander S., Mackenzie, Stuart R., Bari, Sadia, Bomme, Cedric, Duesterer, Stefan, Erk, Benjamin, Manschwetus, Bastian, Mueller, Erland, Rompotis, Dimitrios, Savelyev, Evgeny, Schirmel, Nora, Techert, Simone, Treusch, Rolf, Kuepper, Jochen, Trippel, Sebastian, Wiese, Joss, Stapelfeldt, Henrik, de Miranda, Barbara Cunha, Guillemin, Renaud, Ismail, Iyas, Journel, Loic, Marchenko, Tatiana, Palaudoux, Jerome, Penent, Francis, Piancastelli, Maria Novella, Simon, Marc, Travnikova, Oksana, Brausse, Felix, Goldsztejn, Gildas, Rouzee, Arnaud, Geleoc, Marie, Geneaux, Romain, Ruchon, Thierry, Underwood, Jonathan, Holland, David M. P., Mereshchenko, Andrey S., Olshin, Pavel K., Johnsson, Per, Maclot, Sylvain, Lahl, Jan, Rudenko, Artem, Ziaee, Farzaneh, Brouard, Mark, Rolles, Daniel, Burt, Michael, Boll, Rebecca, Lee, Jason W. L., Amini, Kasra, Kockert, Hansjochen, Vallance, Claire, Gentleman, Alexander S., Mackenzie, Stuart R., Bari, Sadia, Bomme, Cedric, Duesterer, Stefan, Erk, Benjamin, Manschwetus, Bastian, Mueller, Erland, Rompotis, Dimitrios, Savelyev, Evgeny, Schirmel, Nora, Techert, Simone, Treusch, Rolf, Kuepper, Jochen, Trippel, Sebastian, Wiese, Joss, Stapelfeldt, Henrik, de Miranda, Barbara Cunha, Guillemin, Renaud, Ismail, Iyas, Journel, Loic, Marchenko, Tatiana, Palaudoux, Jerome, Penent, Francis, Piancastelli, Maria Novella, Simon, Marc, Travnikova, Oksana, Brausse, Felix, Goldsztejn, Gildas, Rouzee, Arnaud, Geleoc, Marie, Geneaux, Romain, Ruchon, Thierry, Underwood, Jonathan, Holland, David M. P., Mereshchenko, Andrey S., Olshin, Pavel K., Johnsson, Per, Maclot, Sylvain, Lahl, Jan, Rudenko, Artem, Ziaee, Farzaneh, Brouard, Mark, and Rolles, Daniel

Abstract

The dynamics following laser-induced molecular photodissociation of gas-phase CH2BrI at 271.6 nm were investigated by time-resolved Coulomb-explosion imaging using intense near-IR femtosecond laser pulses. The observed delay-dependent photofragment momenta reveal that CH2BrI undergoes C-I cleavage, depositing 65.6% of the available energy into internal product states, and that absorption of a second UV photon breaks the C-Br bond of C(H)2Br. Simulations confirm that this mechanism is consistent with previous data recorded at 248 nm, demonstrating the sensitivity of Coulomb-explosion imaging as a real-time probe of chemical dynamics.

Published
2017
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