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1. X-ray diffractive imaging of controlled gas-phase molecules: Toward imaging of dynamics in the molecular frame

Author

Kierspel, Thomas, Morgan, Andrew, Wiese, Joss, Mullins, Terry, Aquila, Andy, Barty, Anton, Bean, Richard, Boll, Rebecca, Boutet, Sébastien, Bucksbaum, Philip, Chapman, Henry N., Christensen, Lauge, Fry, Alan, Hunter, Mark, Koglin, Jason E., Liang, Mengning, Mariani, Valerio, Natan, Adi, Robinson, Joseph, Rolles, Daniel, Rudenko, Artem, Schnorr, Kirsten, Stapelfeldt, Henrik, Stern, Stephan, Thøgersen, Jan, Yoon, Chun Hong, Wang, Fenglin, and Küpper, Jochen

Subjects
Physics - Atomic and Molecular Clusters, Physics - Chemical Physics
Abstract

We report experimental results on the diffractive imaging of three-dimensionally aligned 2,5-diiodothiophene molecules. The molecules were aligned by chirped near-infrared laser pulses, and their structure was probed at a photon energy of 9.5 keV ($\lambda\approx130 \text{pm}$) provided by the Linac Coherent Light Source. Diffracted photons were recorded on the CSPAD detector and a two-dimensional diffraction pattern of the equilibrium structure of 2,5-diiodothiophene was recorded. The retrieved distance between the two iodine atoms agrees with the quantum-chemically calculated molecular structure to within 5 %. The experimental approach allows for the imaging of intrinsic molecular dynamics in the molecular frame, albeit this requires more experimental data which should be readily available at upcoming high-repetition-rate facilities.

Published
2019
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2. Probing the UV-Induced Photodissociation of CH$_\text{3}$I and C$_\text{6}$H$_\text{3}$F$_\text{2}$I with Femtosecond Time-Resolved Coulomb Explosion Imaging at FLASH

Author

Amini, Kasra, Savelyev, Evgeny, Brauße, Felix, Berrah, Nora, Bomme, Cédric, Brouard, Mark, Burt, Michael, Christensen, Lauge, Düsterer, Stefan, Erk, Benjamin, Höppner, Hauke, Kierspel, Thomas, Krecinic, Faruk, Lauer, Alexandra, Lee, Jason W. L., Müller, Maria, Müller, Erland, Mullins, Terence, Redlin, Harald, Schirmel, Nora, Thøgersen, Jan, Techert, Simone, Toleikis, Sven, Treusch, Rolf, Trippel, Sebastian, Ulmer, Anatoli, Vallance, Claire, Wiese, Joss, Johnsson, Per, Küpper, Jochen, Rudenko, Artem, Rouzée, Arnaud, Stapelfeldt, Henrik, Rolles, Daniel, and Boll, Rebecca

Subjects
Physics - Atomic Physics, Physics - Atomic and Molecular Clusters, Physics - Chemical Physics
Abstract

We explore time-resolved Coulomb explosion induced by intense, extreme ultraviolet (XUV) femtosecond pulses from the FLASH free-electron laser as a method to image photo-induced molecular dynamics in two molecules, iodomethane and 2,6-difluoroiodobenzene. At an excitation wavelength of 267\,nm, the dominant reaction pathway in both molecules is neutral dissociation via cleavage of the carbon--iodine bond. This allows investigating the influence of the molecular environment on the absorption of an intense, femtosecond XUV pulse and the subsequent Coulomb explosion process. We find that the XUV probe pulse induces local inner-shell ionization of atomic iodine in dissociating iodomethane, in contrast to non-selective ionization of all photofragments in difluoroiodobenzene. The results reveal evidence of electron transfer from methyl and phenyl moieties to a multiply charged iodine ion. In addition, indications for ultrafast charge rearrangement on the phenyl radical are found, suggesting that time-resolved Coulomb explosion imaging is sensitive to the localization of charge in extended molecules.

Published
2017
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3. Alignment, Orientation, and Coulomb Explosion of Difluoroiodobenzene Studied with the Pixel Imaging Mass Spectrometry (PImMS) Camera

Author

Amini, Kasra, Boll, Rebecca, Lauer, Alexandra, Burt, Michael, Lee, Jason W L, Christensen, Lauge, Brauße, Felix, Mullins, Terence, Savelyev, Evgeny, Ablikim, Utuq, Berrah, Nora, Bomme, Cédric, Düsterer, Stefan, Erk, Benjamin, Höppner, Hauke, Johnsson, Per, Kierspel, Thomas, Krecinic, Faruk, Küpper, Jochen, Müller, Maria, Müller, Erland, Redlin, Harald, Rouzée, Arnaud, Schirmel, Nora, Thøgersen, Jan, Techert, Simone, Toleikis, Sven, Treusch, Rolf, Trippel, Sebastian, Ulmer, Anatoli, Wiese, Joss, Vallance, Claire, Rudenko, Artem, Stapelfeldt, Henrik, Brouard, Mark, and Rolles, Daniel

Subjects
Physics - Chemical Physics, Quantum Physics
Abstract

Laser-induced adiabatic alignment and mixed-field orientation of 2,6-difluoroiodobenzene (C6H3F2I) molecules are probed by Coulomb explosion imaging following either near-infrared strong-field ionization or extreme-ultraviolet multi-photon inner-shell ionization using free-electron laser pulses. The resulting photoelectrons and fragment ions are captured by a double-sided velocity map imaging spectrometer and projected onto two position-sensitive detectors. The ion side of the spectrometer is equipped with the Pixel Imaging Mass Spectrometry (PImMS) camera, a time-stamping pixelated detector that can record the hit positions and arrival times of up to four ions per pixel per acquisition cycle. Thus, the time-of-flight trace and ion momentum distributions for all fragments can be recorded simultaneously. We show that we can obtain a high degree of one- and three-dimensional alignment and mixed- field orientation, and compare the Coulomb explosion process induced at both wavelengths.

Published
2017
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4. Strongly aligned gas-phase molecules at Free-Electron Lasers

Author

Kierspel, Thomas, Wiese, Joss, Mullins, Terry, Robinson, Joseph, Aquila, Andy, Barty, Anton, Bean, Richard, Boll, Rebecca, Boutet, Sébastien, Bucksbaum, Philip, Chapman, Henry N., Christensen, Lauge, Fry, Alan, Hunter, Mark, Koglin, Jason E., Liang, Mengning, Mariani, Valerio, Morgan, Andrew, Natan, Adi, Petrovic, Vladimir, Rolles, Daniel, Rudenko, Artem, Schnorr, Kirsten, Stapelfeldt, Henrik, Stern, Stephan, Thøgersen, Jan, Yoon, Chun Hong, Wang, Fenglin, Trippel, Sebastian, and Küpper, Jochen

Subjects
Physics - Atomic and Molecular Clusters
Abstract

We demonstrate a novel experimental implementation to strongly align molecules at full repetition rates of free-electron lasers. We utilized the available in-house laser system at the coherent x-ray imaging beamline at the Linac Coherent Light Source. Chirped laser pulses, i. e., the direct output from the regenerative amplifier of the Ti:Sa chirped pulse amplification laser system, were used to strongly align 2,5-diiodothiophene molecules in a molecular beam. The alignment laser pulses had pulse energies of a few mJ and a pulse duration of 94 ps. A degree of alignment of $\left<\cos^2\!\theta_{2D}\right>$ = 0.85 was measured, limited by the intrinsic temperature of the molecular beam rather than by the available laser system. With the general availability of synchronized chirped-pulse-amplified near-infrared laser systems at short-wavelength laser facilities, our approach allows for the universal preparation of molecules tightly fixed in space for experiments with x-ray pulses., Comment: 10 pages, 5 figures

Published
2015
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5. X-ray diffractive imaging of controlled gas-phase molecules: Toward imaging of dynamics in the molecular frame.

Author

Kierspel, Thomas, Morgan, Andrew, Wiese, Joss, Mullins, Terry, Aquila, Andy, Barty, Anton, Bean, Richard, Boll, Rebecca, Boutet, Sébastien, Bucksbaum, Philip, Chapman, Henry N., Christensen, Lauge, Fry, Alan, Hunter, Mark, Koglin, Jason E., Liang, Mengning, Mariani, Valerio, Natan, Adi, Robinson, Joseph, and Rolles, Daniel

Subjects
MOLECULAR dynamics, X-ray imaging, COHERENCE (Optics), LIGHT sources, MOLECULES, DIFFRACTIVE scattering
Abstract

We report experimental results on the diffractive imaging of three-dimensionally aligned 2,5-diiodothiophene molecules. The molecules were aligned by chirped near-infrared laser pulses, and their structure was probed at a photon energy of 9.5 keV (λ ≈ 130 pm) provided by the Linac Coherent Light Source. Diffracted photons were recorded on the Cornell–SLAC pixel array detector, and a two-dimensional diffraction pattern of the equilibrium structure of 2,5-diiodothiophene was recorded. The retrieved distance between the two iodine atoms agrees with the quantum-chemically calculated molecular structure to be within 5%. The experimental approach allows for the imaging of intrinsic molecular dynamics in the molecular frame, albeit this requires more experimental data, which should be readily available at upcoming high-repetition-rate facilities. [ABSTRACT FROM AUTHOR]

Published
2020
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6. Communication: Three-fold covariance imaging of laser-induced Coulomb explosions.

Author

Pickering, James D., Amini, Kasra, Brouard, Mark, Burt, Michael, Bush, Ian J., Christensen, Lauge, Lauer, Alexandra, Nielsen, Jens H., Slater, Craig S., and Stapelfeldt, Henrik

Subjects
COULOMB explosion, IMAGING systems, LASER photochemistry, MOLECULAR structure, DIPHENYL, MASS spectrometry
Abstract

We apply a three-fold covariance imaging method to analyse previously acquired data [C. S. Slater et al., Phys. Rev. A 89, 011401(R) (2014)] on the femtosecond laser-induced Coulomb explosion of spatially pre-aligned 3,5-dibromo-3',5'-difluoro-4'-cyanobiphenyl molecules. The data were acquired using the "Pixel Imaging Mass Spectrometry" camera. We show how three-fold covariance imaging of ionic photofragment recoil trajectories can be used to provide new information about the parent ion's molecular structure prior to its Coulomb explosion. In particular, we show how the analysis may be used to obtain information about molecular conformation and provide an alternative route for enantiomer determination. [ABSTRACT FROM AUTHOR]

Published
2016
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7. Photodissociation of Aligned $CH_3I$ and $C_{6}H_{3}F_{2}I$ Molecules Probed with Time-Resolved Coulomb Explosion Imaging by Site-Selective XUV Ionization

Author

Amini, Kasra, Savelyev, Evgeny, Brauße, Felix, Berrah, Nora, Bomme, Cedric, Brouard, Mark, Burt, Michael, Christensen, Lauge, Düsterer, Stefan, Erk, Benjamin, Höppner, Hauke, Kierspel, Thomas, Krecinic, Faruk, Lauer, Alexandra, Lee, Jason W. L., Müller, Maria, Mueller, Erland, Mullins, Terence, Redlin, Harald, Schirmel, Nora, Thøgersen, Jan, Techert, Simone, Toleikis, Sven, Treusch, Rolf, Trippel, Sebastian, Ulmer, Anatoli, Vallance, Claire, Wiese, Joss, Johnsson, Per, Küpper, Jochen, Rudenko, Artem, Rouzée, Arnaud, Stapelfeldt, Henrik, Rolles, Daniel, and Boll, Rebecca

Abstract

Structural dynamics 5(1), 014301 - (2018). doi:10.1063/1.4998648, We explore time-resolved Coulomb explosion induced by intense, extreme ultraviolet (XUV) femtosecond pulses from a free-electron laser as a method to image photo-induced molecular dynamics in two molecules, iodomethane and 2,6-difluoroiodobenzene. At an excitation wavelength of 267 nm, the dominant reaction pathway in both molecules is neutral dissociation via cleavage of the carbon–iodine bond. This allows investigating the influence of the molecular environment on the absorption of an intense, femtosecond XUV pulse and the subsequent Coulomb explosion process. We find that the XUV probe pulse induces local inner-shell ionization of atomic iodine in dissociating iodomethane, in contrast to non-selective ionization of all photofragments in difluoroiodobenzene. The results reveal evidence of electron transfer from methyl and phenyl moieties to a multiply charged iodine ion. In addition, indications for ultrafast charge rearrangement on the phenyl radical are found, suggesting that time-resolved Coulomb explosion imaging is sensitive to the localization of charge in extended molecules., Published by AIP Publishing LLC, Melville, NY

Published
2018
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8. Probing the UV-Induced Photodissociation of CH3I and C6H3F2I with Femtosecond Time-Resolved Coulomb Explosion Imaging at FLASH

Author

Savelyev, Evgeny, Amini, Kasra, Brauße, Felix, Berrah, Nora, Bomme, Cédric, Brouard, Mark, Burt, Michael, Christensen, Lauge, Düsterer, Stefan, Erk, Benjamin, Höppner, Hauke, Kierspel, Thomas, Krecinic, Faruk, Lauer, Alexandra, Lee, Jason W. L., Müller, Maria, Müller, Erland, Mullins, Terence, Redlin, Harald, Schirmel, Nora, Thøgersen, Jan, Techert, Simone, Toleikis, Sven, Treusch, Rolf, Trippel, Sebastian, Ulmer, Anatoli, Vallance, Claire, Wiese, Joss, Johnsson, Per, Küpper, Jochen, Rudenko, Artem, Rouzée, Arnaud, Stapelfeldt, Henrik, Rolles, Daniel, and Boll, Rebecca

Subjects
physics.chem-ph, Physics::Atomic and Molecular Clusters, physics.atm-clus, Physics::Chemical Physics, physics.atom-ph
Abstract

We explore time-resolved Coulomb explosion induced by intense, extreme ultraviolet (XUV) femtosecond pulses from the FLASH free-electron laser as a method to image photo-induced molecular dynamics in two molecules, iodomethane and difluoroiodobenzene. At an excitation wavelength of 267 nm, the dominant reaction pathway in both molecules is neutral cleavage of the carbon--iodine bond, which allows studying the influence of the molecular environment on the XUV absorption and the subsequent Coulomb explosion process. The XUV probe pulse induces local inner-shell ionization of atomic iodine in dissociating iodomethane, in contrast to non-selective ionization of all photofragments in difluoroiodobenzene. The resulting signals reveal evidence of electron transfer from methyl and phenyl moieties to a multiply charged iodine ion. In addition, we find indications for ultrafast charge rearrangement on the phenyl radical, suggesting that time-resolved Coulomb explosion imaging is sensitive to the localization of charge in extended molecules.

Published
2017

9. Jitter-correction for IR/UV-XUV pump-probe experiments at the FLASH free-electron laser

Author

Savelyev, Evgeny, Boll, Rebecca, Bomme, Cédric, Schirmel, Nora, Redlin, Harald, Erk, Benjamin, Düsterer, Stefan, Mueller, Erland, Höppner, Hauke, Toleikis, Sven, Müller, Jost, Kristin Czwalinna, Marie, Treusch, Rolf, Kierspel, Thomas, Mullins, Terence, Trippel, Sebastian, Wiese, Joss, Küpper, Jochen, Brauβe, Felix, Krecinic, Faruk, Rouzée, Arnaud, Rudawski, Piotr, Johnsson, Per, Amini, Kasra, Lauer, Alexandra, Burt, Michael, Brouard, Mark, Christensen, Lauge, Thøgersen, Jan, Stapelfeldt, Henrik, Berrah, Nora, Müller, Maria, Ulmer, Anatoli, Techert, Simone, Rudenko, Artem, and Rolles, Daniel

Subjects
time-resolved ion imaging, free-electron laser, velocity map imaging, pump-probe experiments, photodissociation, ddc:530, 530 Physik
Abstract

New journal of physics 19(4), 043009(2017). doi:10.1088/1367-2630/aa652d, In pump-probe experiments employing a free-electron laser (FEL) in combination with a synchronized optical femtosecond laser, the arrival-time jitter between the FEL pulse and the optical laser pulse often severely limits the temporal resolution that can be achieved. Here, we present a pump-probe experiment on the UV-induced dissociation of 2,6-difluoroiodobenzene $(C_{6}H_{3}F_{2}I)$ molecules performed at the FLASH FEL that takes advantage of recent upgrades of the FLASH timing and synchronization system to obtain high-quality data that are not limited by the FEL arrival-time jitter. We discuss in detail the necessary data analysis steps and describe the origin of the time-dependent effects in the yields and kinetic energies of the fragment ions that we observe in the experiment., Published by IOP Publ. , Bad Honnef

Published
2017
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10. Photodissociation of aligned CH3I and C6H3F2I molecules probed with time-resolved Coulomb explosion imaging by site-selective extreme ultraviolet ionization

Author

Amini, Kasra, primary, Savelyev, Evgeny, additional, Brauße, Felix, additional, Berrah, Nora, additional, Bomme, Cédric, additional, Brouard, Mark, additional, Burt, Michael, additional, Christensen, Lauge, additional, Düsterer, Stefan, additional, Erk, Benjamin, additional, Höppner, Hauke, additional, Kierspel, Thomas, additional, Krecinic, Faruk, additional, Lauer, Alexandra, additional, Lee, Jason W. L., additional, Müller, Maria, additional, Müller, Erland, additional, Mullins, Terence, additional, Redlin, Harald, additional, Schirmel, Nora, additional, Thøgersen, Jan, additional, Techert, Simone, additional, Toleikis, Sven, additional, Treusch, Rolf, additional, Trippel, Sebastian, additional, Ulmer, Anatoli, additional, Vallance, Claire, additional, Wiese, Joss, additional, Johnsson, Per, additional, Küpper, Jochen, additional, Rudenko, Artem, additional, Rouzée, Arnaud, additional, Stapelfeldt, Henrik, additional, Rolles, Daniel, additional, and Boll, Rebecca, additional

Published
2018
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12. Alignment, orientation, and Coulomb explosion of difluoroiodobenzene studied with the pixel imaging mass spectrometry (PImMS) camera

Author

Amini, Kasra, primary, Boll, Rebecca, additional, Lauer, Alexandra, additional, Burt, Michael, additional, Lee, Jason W. L., additional, Christensen, Lauge, additional, Brauβe, Felix, additional, Mullins, Terence, additional, Savelyev, Evgeny, additional, Ablikim, Utuq, additional, Berrah, Nora, additional, Bomme, Cédric, additional, Düsterer, Stefan, additional, Erk, Benjamin, additional, Höppner, Hauke, additional, Johnsson, Per, additional, Kierspel, Thomas, additional, Krecinic, Faruk, additional, Küpper, Jochen, additional, Müller, Maria, additional, Müller, Erland, additional, Redlin, Harald, additional, Rouzée, Arnaud, additional, Schirmel, Nora, additional, Thøgersen, Jan, additional, Techert, Simone, additional, Toleikis, Sven, additional, Treusch, Rolf, additional, Trippel, Sebastian, additional, Ulmer, Anatoli, additional, Wiese, Joss, additional, Vallance, Claire, additional, Rudenko, Artem, additional, Stapelfeldt, Henrik, additional, Brouard, Mark, additional, and Rolles, Daniel, additional

Published
2017
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16. Strong eld ionization of naphthalene: angular shifts and molecular potential

Author

Dimitrovski, Darko, Maurer, Jochen, Christensen, Lauge, Madsen, Lars Bojer, and Stapelfeldt, Henrik

Subjects
Physics::Atomic and Molecular Clusters, Physics::Atomic Physics, Physics::Chemical Physics
Abstract

We analyze the photoelectron momentum distributions from strong eld ionization of xed-in-space naphthalene molecules by circularly polarized laser pulses. By direct comparison between experiment and theory, we show that the angular shifts in the photoelectron momentum distributions are very sensitive to the exact form of the molecular potential.

Published
2013

17. Strongly aligned gas-phase molecules at free-electron lasers

Author

Kierspel, Thomas, primary, Wiese, Joss, additional, Mullins, Terry, additional, Robinson, Joseph, additional, Aquila, Andy, additional, Barty, Anton, additional, Bean, Richard, additional, Boll, Rebecca, additional, Boutet, Sébastien, additional, Bucksbaum, Philip, additional, Chapman, Henry N, additional, Christensen, Lauge, additional, Fry, Alan, additional, Hunter, Mark, additional, Koglin, Jason E, additional, Liang, Mengning, additional, Mariani, Valerio, additional, Morgan, Andrew, additional, Natan, Adi, additional, Petrovic, Vladimir, additional, Rolles, Daniel, additional, Rudenko, Artem, additional, Schnorr, Kirsten, additional, Stapelfeldt, Henrik, additional, Stern, Stephan, additional, Thøgersen, Jan, additional, Yoon, Chun Hong, additional, Wang, Fenglin, additional, Trippel, Sebastian, additional, and Küpper, Jochen, additional

Published
2015
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20. Dynamic Stark Control of Torsional Motion by a Pair of Laser Pulses

Author

Christensen, Lauge, primary, Nielsen, Jens H., additional, Brandt, Christian B., additional, Madsen, Christian B., additional, Madsen, Lars Bojer, additional, Slater, Craig S., additional, Lauer, Alexandra, additional, Brouard, Mark, additional, Johansson, Mikael P., additional, Shepperson, Benjamin, additional, and Stapelfeldt, Henrik, additional

Published
2014
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21. Covariance imaging experiments using a pixel-imaging mass-spectrometry camera

Author

Slater, Craig S., primary, Blake, Sophie, additional, Brouard, Mark, additional, Lauer, Alexandra, additional, Vallance, Claire, additional, John, Jaya John, additional, Turchetta, Renato, additional, Nomerotski, Andrei, additional, Christensen, Lauge, additional, Nielsen, Jens H., additional, Johansson, Mikael P., additional, and Stapelfeldt, Henrik, additional

Published
2014
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22. Imaging molecular structure through femtosecond photoelectron diffraction on aligned and oriented gas-phase molecules

Author

Boll, Rebecca, primary, Rouzée, Arnaud, additional, Adolph, Marcus, additional, Anielski, Denis, additional, Aquila, Andrew, additional, Bari, Sadia, additional, Bomme, Cédric, additional, Bostedt, Christoph, additional, Bozek, John D., additional, Chapman, Henry N., additional, Christensen, Lauge, additional, Coffee, Ryan, additional, Coppola, Niccola, additional, De, Sankar, additional, Decleva, Piero, additional, Epp, Sascha W., additional, Erk, Benjamin, additional, Filsinger, Frank, additional, Foucar, Lutz, additional, Gorkhover, Tais, additional, Gumprecht, Lars, additional, Hömke, André, additional, Holmegaard, Lotte, additional, Johnsson, Per, additional, Kienitz, Jens S., additional, Kierspel, Thomas, additional, Krasniqi, Faton, additional, Kühnel, Kai-Uwe, additional, Maurer, Jochen, additional, Messerschmidt, Marc, additional, Moshammer, Robert, additional, Müller, Nele L. M., additional, Rudek, Benedikt, additional, Savelyev, Evgeny, additional, Schlichting, Ilme, additional, Schmidt, Carlo, additional, Scholz, Frank, additional, Schorb, Sebastian, additional, Schulz, Joachim, additional, Seltmann, Jörn, additional, Stener, Mauro, additional, Stern, Stephan, additional, Techert, Simone, additional, Thøgersen, Jan, additional, Trippel, Sebastian, additional, Viefhaus, Jens, additional, Vrakking, Marc, additional, Stapelfeldt, Henrik, additional, Küpper, Jochen, additional, Ullrich, Joachim, additional, Rudenko, Artem, additional, and Rolles, Daniel, additional

Published
2014
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23. Resonance-enhanced multiple ionization of krypton at an x-ray free-electron laser

Author

Rudek, Benedikt, primary, Rolles, Daniel, additional, Son, Sang-Kil, additional, Foucar, Lutz, additional, Erk, Benjamin, additional, Epp, Sascha, additional, Boll, Rebecca, additional, Anielski, Denis, additional, Bostedt, Christoph, additional, Schorb, Sebastian, additional, Coffee, Ryan, additional, Bozek, John, additional, Trippel, Sebastian, additional, Marchenko, Tatiana, additional, Simon, Marc, additional, Christensen, Lauge, additional, De, Sankar, additional, Wada, Shin-ichi, additional, Ueda, Kiyoshi, additional, Schlichting, Ilme, additional, Santra, Robin, additional, Ullrich, Joachim, additional, and Rudenko, Artem, additional

Published
2013
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24. Coulomb explosion imaging of small organic molecules at LCLS

Author

Erk, Benjamin, primary, Rudenko, Artem, additional, Rolles, Daniel, additional, Rudek, Benedikt, additional, Foucar, Lutz, additional, Epp, Sascha, additional, Cryle, Max, additional, Schlichting, Ilme, additional, Bostedt, Christoph, additional, Schorb, Sebastian, additional, Bozek, John, additional, Rouzee, Arnaud, additional, Hundertmark, Axel, additional, Marchenko, Tatiana, additional, Simon, Mark, additional, Filsinger, Frank, additional, Christensen, Lauge, additional, De, Shankar, additional, Trippel, Sebastian, additional, Wada, Shinichi, additional, Ueda, Kiyoshi, additional, Schroeter, Claus Dieter, additional, and Ullrich, Joachim, additional

Published
2012
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26. X-ray diffractive imaging of controlled gas-phase molecules: Toward imaging of dynamics in the molecular frame

Author

Kierspel, Thomas, Morgan, Andrew, Wiese, Joss, Mullins, Terence, Aquila, Andrew, Barty, Anton, Bean, Richard, Boll, Rebecca, Boutet, Sebastien, Bucksbaum, Philip, Chapman, Henry N., Christensen, Lauge, Fry, Alan, Hunter, Mark, Koglin, Jason, Liang, Mengning, Mariani, Valerio, Natan, Adi, Robinson, Joseph, Rolles, Daniel, Rudenko, Artem, Schnorr, Kirsten, Stapelfeldt, Henrik, Stern, Stephan, Thøgersen, Jan, Yoon, Chun Hong, Wang, Fenglin, and Küpper, Jochen

Subjects
3. Good health
Abstract

The journal of chemical physics 152(8), 084307 (2020). doi:10.1063/1.5133963, We report experimental results on the diffractive imaging of three-dimensionally aligned 2,5-diiodothiophene molecules. The molecules were aligned by chirped near-infrared laser pulses, and their structure was probed at a photon energy of 9.5 keV (λ ≈ 130 pm) provided by the Linac Coherent Light Source. Diffracted photons were recorded on the Cornell–SLAC pixel array detector, and a two-dimensional diffraction pattern of the equilibrium structure of 2,5-diiodothiophene was recorded. The retrieved distance between the two iodine atoms agrees with the quantum-chemically calculated molecular structure to be within 5%. The experimental approach allows for the imaging of intrinsic molecular dynamics in the molecular frame, albeit this requires more experimental data, which should be readily available at upcoming high-repetition-rate facilities., Published by American Institute of Physics, Melville, NY

27. Photodissociation of aligned CH3I and C6H3F2I molecules probed with time-resolved Coulomb explosion imaging by site-selective extreme ultraviolet ionization.

Author

Amini, Kasra, Savelyev, Evgeny, Brauße, Felix, Berrah, Nora, Bomme, Cédric, Brouard, Mark, Burt, Michael, Christensen, Lauge, Düsterer, Stefan, Erk, Benjamin, Höppner, Hauke, Kierspel, Thomas, Krecinic, Faruk, Lauer, Alexandra, Lee, Jason W. L., Müller, Maria, Müller, Erland, Mullins, Terence, Redlin, Harald, and Schirmel, Nora

Subjects
PHOTODISSOCIATION, METHYL iodide, ULTRAVIOLET radiation
Abstract

We explore time-resolved Coulomb explosion induced by intense, extreme ultraviolet (XUV) femtosecond pulses from a free-electron laser as a method to image photo-induced molecular dynamics in two molecules, iodomethane and 2,6-difluoroiodobenzene. At an excitation wavelength of 267 nm, the dominant reaction pathway in both molecules is neutral dissociation via cleavage of the carbon–iodine bond. This allows investigating the influence of the molecular environment on the absorption of an intense, femtosecond XUV pulse and the subsequent Coulomb explosion process. We find that the XUV probe pulse induces local inner-shell ionization of atomic iodine in dissociating iodomethane, in contrast to non-selective ionization of all photofragments in difluoroiodobenzene. The results reveal evidence of electron transfer from methyl and phenyl moieties to a multiply charged iodine ion. In addition, indications for ultrafast charge rearrangement on the phenyl radical are found, suggesting that time-resolved Coulomb explosion imaging is sensitive to the localization of charge in extended molecules. [ABSTRACT FROM AUTHOR]

Published
2018
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28. Photodissociation of aligned CH 3 I and C 6 H 3 F 2 I molecules probed with time-resolved Coulomb explosion imaging by site-selective extreme ultraviolet ionization.

Author

Amini K, Savelyev E, Brauße F, Berrah N, Bomme C, Brouard M, Burt M, Christensen L, Düsterer S, Erk B, Höppner H, Kierspel T, Krecinic F, Lauer A, Lee JWL, Müller M, Müller E, Mullins T, Redlin H, Schirmel N, Thøgersen J, Techert S, Toleikis S, Treusch R, Trippel S, Ulmer A, Vallance C, Wiese J, Johnsson P, Küpper J, Rudenko A, Rouzée A, Stapelfeldt H, Rolles D, and Boll R

Abstract

We explore time-resolved Coulomb explosion induced by intense, extreme ultraviolet (XUV) femtosecond pulses from a free-electron laser as a method to image photo-induced molecular dynamics in two molecules, iodomethane and 2,6-difluoroiodobenzene. At an excitation wavelength of 267 nm, the dominant reaction pathway in both molecules is neutral dissociation via cleavage of the carbon-iodine bond. This allows investigating the influence of the molecular environment on the absorption of an intense, femtosecond XUV pulse and the subsequent Coulomb explosion process. We find that the XUV probe pulse induces local inner-shell ionization of atomic iodine in dissociating iodomethane, in contrast to non-selective ionization of all photofragments in difluoroiodobenzene. The results reveal evidence of electron transfer from methyl and phenyl moieties to a multiply charged iodine ion. In addition, indications for ultrafast charge rearrangement on the phenyl radical are found, suggesting that time-resolved Coulomb explosion imaging is sensitive to the localization of charge in extended molecules.

Published
2018
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