Showing papers by "Marc J. J. Vrakking published in 2013"

Probing Time-Dependent Molecular Dipoles on the Attosecond Time Scale

Abstract: Photoinduced molecular processes start with the interaction of the instantaneous electric field of the incident light with the electronic degrees of freedom. This early attosecond electronic motion impacts the fate of the photoinduced reactions. We report the first observation of attosecond time scale electron dynamics in a series of small-and medium-sized neutral molecules (N-2, CO2, and C2H4), monitoring time-dependent variations of the parent molecular ion yield in the ionization by an attosecond pulse, and thereby probing the time-dependent dipole induced by a moderately strong near-infrared laser field. This approach can be generalized to other molecular species and may be regarded as a first example of molecular attosecond Stark spectroscopy. (Less)

Femtosecond photoelectron diffraction on laser-aligned molecules: Towards time-resolved imaging of molecular structure

Abstract: We demonstrate an experimental method to record snapshot diffraction images of polyatomic gas-phase molecules, which can, in a next step, be used to probe time-dependent changes in the molecular geometry during photochemical reactions with femtosecond temporal and angstrom spatial resolution. Adiabatically laser-aligned 1-ethynyl-4-fluorobenzene (C${}_{8}$H${}_{5}$F) molecules were imaged by diffraction of photoelectrons with kinetic energies between 31 and 62 eV, created from core ionization of the fluorine ($1s$) level by $\ensuremath{\approx}80$ fs x-ray free-electron-laser pulses. Comparison of the experimental photoelectron angular distributions with density functional theory calculations allows relating the diffraction images to the molecular structure.

Hydrogen Atoms under Magnification: Direct Observation of the Nodal Structure of Stark States

Abstract: To describe the microscopic properties of matter, quantum mechanics uses wave functions, whose structure and time dependence is governed by the Schrodinger equation. In atoms the charge distributions described by the wave function are rarely observed. The hydrogen atom is unique, since it only has one electron and, in a dc electric field, the Stark Hamiltonian is exactly separable in terms of parabolic coordinates (η, ξ, φ). As a result, the microscopic wave function along the ξ coordinate that exists in the vicinity of the atom, and the projection of the continuum wave function measured at a macroscopic distance, share the same nodal structure. In this Letter, we report photoionization microscopy experiments where this nodal structure is directly observed. The experiments provide a validation of theoretical predictions that have been made over the last three decades.

Coulomb explosion of diatomic molecules in intense XUV fields mapped by partial covariance

Abstract: Single-shot time-of-flight spectra for Coulomb explosion of N2 and I2 molecules have been recorded at the Free Electron LASer in Hamburg (FLASH) and have been analysed using a partial covariance mapping technique. The partial covariance analysis unravels a detailed picture of all significant Coulomb explosion pathways, extending up to the N 4+ ‐N 5+ channel for nitrogen and up to the I 8+ ‐I 9+ channel for iodine. The observation of the latter channel is unexpected if only sequential ionization processes from the ground state ions are considered. The maximum kinetic energy release extracted from the covariance maps for each dissociation channel shows that Coulomb explosion of nitrogen molecules proceeds much faster than that of the iodine. The N2 ionization dynamics is modelled using classical trajectory simulations in good agreement with the outcome of the experiments. The results suggest that covariance mapping of the Coulomb explosion can be used to measure the intensity and pulse duration of free-electron lasers.

Interference in the angular distribution of photoelectrons in superimposed XUV and optical laser fields

Abstract: The angular distribution of photoelectrons ejected during the ionization of Ne atoms by extreme ultraviolet (XUV) free-electron laser radiation in the presence of an intense near infrared (NIR) dressing field was investigated experimentally and theoretically. A highly nonlinear process with absorption and emission of more than ten NIR photons results in the formation of numerous sidebands. The amplitude of the sidebands varies strongly with the emission angle and the angular distribution pattern reveals clear signatures of interferences between the different angular momenta for the outgoing electron in the multi-photon process. As a specific feature, the central photoelectron line is characterized at the highest NIR fields by an angular distribution, which is peaked perpendicularly to both the XUV and NIR polarization directions. Experimental results are reproduced by a theoretical model based on the strong field approximation.

Towards imaging of ultrafast molecular dynamics using FELs

Abstract: The dissociation dynamics induced by a 100 fs, 400 nm laser pulse in a rotationally cold Br-2 sample was characterized by Coulomb explosion imaging (CEI) using a time-delayed extreme ultra-violet (XUV) FEL pulse, obtained from the Free electron LASer in Hamburg (FLASH). The momentum distribution of atomic fragments resulting from the 400 nm-induced dissociation was measured with a velocity map imaging spectrometer and used to monitor the internuclear distance as the molecule dissociated. By employing the simultaneously recorded in-house timing electro-optical sampling data, the time resolution of the final results could be improved to 300 fs, compared to the inherent 500 fs time-jitter of the FEL pulse. Before dissociation, the Br-2 molecules were transiently 'fixed in space' using laser-induced alignment. In addition, similar alignment techniques were used on CO2 molecules to allow the measurement of the photoelectron angular distribution (PAD) directly in the molecular frame (MF). Our results on MFPADs in aligned CO2 molecules, together with our investigation of the dissociation dynamics of the Br-2 molecules with CEI, show that information about the evolving molecular structure and electronic geometry can be retrieved from such experiments, therefore paving the way towards the study of complex non-adiabatic dynamics in molecules through XUV time-resolved photoion and photoelectron spectroscopy.

Reconstruction of attosecond electron wave packets using quantum state holography

Abstract: We present a method for performing quantum state holography, with which we completely characterize the amplitude and phase of an attosecond electron wave packet. Our approach is an extension of a recent publication [J. Mauritsson et al., Phys. Rev. Lett. 105, 053001 (2010)] in which we demonstrated experimentally that the energies and amplitudes of an attosecond electron wave packet can be characterized using attosecond electron interferometry. Here we show theoretically that attosecond electron interferometry can be extended to retrieve the phases of all the states that make up the wave packet. We demonstrate the feasibility of our method by analyzing a wave packet created by a shake-up process. We show that our method can successfully retrieve arbitrary phases and/or lifetimes added to the component eigenstates.

Carrier-envelope phase stable few-cycle pulses at 400 kHz for electron-ion coincidence experiments.

Abstract: Coincident electron-ion detection after photoionization in a "reaction microscope" is a very powerful tool to study atomic and molecular dynamics. However, the implementation of this tool in the field of attosecond science has so far been rather limited, due to the lack of high repetition rate laser sources capable of delivering few-cycle pulses with sufficient energy per pulse. In this article, the development of a Non-collinear Optical Parametric Amplifier (NOPA) capable of delivering Carrier-Envelope Phase (CEP) stable pulses with sub-6 fs duration and pulse energies in the few-µJ range is presented. The potential of combining the high repetition rate source and a reaction microscope operating at this high frequency is demonstrated in a proof-of-principle experiment on strong field ionization of Ar atoms.

Photoelectron angular distributions for the two-photon ionization of helium by ultrashort extreme ultraviolet free-electron laser pulses

Abstract: The two-photon ionization of helium atoms by ultrashort extreme-ultraviolet free-electron laser pulses, produced by the SPring-8 Compact SASE Source test accelerator, was investigated at photon energies of 20.3, 21.3, 23.0 and 24.3 eV. The angular distribution of photoelectrons generated by two-photon ionization is obtained using a velocity map imaging spectrometer. The phase-shift differences and amplitude ratios of the outgoing s and d continuum wave packets are extracted from the photoelectron angular distributions. The obtained values of the phase-shift differences are distinct from scattering phase-shift differences when the photon energy is tuned to a resonance with an excited level or Rydberg manifold. The difference stems from the co-presence of resonant and non-resonant path contributions in the two-photon ionization by femtosecond pulses. Since the relative contribution of both paths can be controlled in principle by the pulse shape, these results illustrate a new way to tailor the continuum wave packet.

Photoelectron angular distributions for the two-photon sequential double ionization of xenon by ultrashort extreme ultraviolet free electron laser pulses

Abstract: Xenon atoms are double-ionized by sequential two-photon absorption by ultrashort extreme ultraviolet free-electron laser pulses with a photon energy of 23.0 and 24.3 eV, produced by the SPring-8 Compact SASE Source test accelerator. The angular distributions of photoelectrons generated by two-photon double ionization are obtained using velocity map imaging. The results are reproduced reasonably well by the present theoretical calculations within the multi-configurational Dirac-Fock approach.

Photoelectron imaging of XUV photoionization of CO2 by 13–40 eV synchrotron radiation

Abstract: Valence band photoionization of CO2 has been studied by photoelectron spectroscopy using a velocity map imaging spectrometer and synchrotron radiation. The measured data allow retrieving electronic and vibrational branching ratios, vibrationally resolved asymmetry parameters, and the total electron yield which includes multiple strong resonances. Additionally, the spectrum of low kinetic energy electrons has been studied in the resonant region, and the evolution with photon energy of one of the forbidden transitions present in the slow photoelectrons spectrum has been carefully analyzed, indicating that in the presence of auto-ionizing resonances the vibrational populations of the ion are significantly redistributed.

The ELI-ALPS secondary sources: A getaway to scientific excellence

Abstract: The essence of ELI-ALPS, the laser driven secondary sources ranging from X-ray and X-UV to THz with duration as short as tens of attoseconds, are designed to be available for users from 2016.

Special issue on ultrafast electron and molecular dynamics

Abstract: Your invitation to submit. Journal of Physics. B: Atomic Molecular and Optical Physics (JPhysB) is delighted to announce a forthcoming special issue on ultrafast electron and molecular dynamics to appear in 2014, and invites you to submit a paper. Within the last decade, a number of novel approaches have emerged, both experimental and theoretical, that allow the investigation of (time-resolved) molecular dynamics in novel ways not anticipated before. Experimentally, the introduction of novel light sources such as high-harmonic generation and XUV/x-ray free electron lasers, and the emergence of novel detection strategies, such as time-resolved electron/x-ray diffraction and the fully coincident detection of electrons and fragment ions in reaction microscopes, has significantly expanded the arsenal of available techniques, and has taken studies of molecular dynamics into new domains of spectroscopic, spatial and temporal resolution, the latter including first explorations into the attosecond domain. Along the way, particular types of molecular dynamics, such as dynamics around conical intersections, have gained an increased prominence, sparked by an emerging realization about the essential role that this dynamics plays in relaxation pathways in important bio-molecular systems. The progress on the theoretical side has been no less impressive. Novel generations of supercomputers and a series of novel computational strategies have allowed nearly exact calculations in small molecules, as well as highly successful approximate calculations in large, polyatomic molecules. Frequent and intensive collaborations involving both theory and experiment have been essential for the progress that has been accomplished. The special issue 'Ultrafast electron and molecular dynamics' seeks to provide an overview of some of the most important developments in the field, while at the same time indicating how studies of (time-resolved) molecular dynamics are likely to evolve in the coming years. You are invited to submit your article by 1 December 2013.

Observation of ultrafast electron dynamics in N 2 molecules induced by attosecond pulses

Abstract: We used velocity-map imaging to measure ultrafast electron dynamics in N 2 initiated by attosecond pulses. A time-to-space mapping of autoionization channel is demonstrated. A sub-cycle oscillatory dynamics related to quantum interference is also observed.

Ultrafast Relaxation Dynamics of Highly-excited States in N2 Molecules Excited by Femtosecond XUV Pulses

Abstract: We used velocity-map-imaging to measure electronic and nuclear dynamics in N2 molecules excited by a train of attosecond pulses. A time-to-space mapping of autoionization channel is demonstrated. It is found that the autoionization becomes energetically allowed when the two nuclei are still very close (~ 3 A) and that it can be coherently manipulated by a strong femtosecond infrared pulse.

Ultrafast dynamics of highly-excited states in N 2 molecules excited by attoseconds pulses

Abstract: The ultrafast dynamics induced by photo-ionization in atoms and molecules plays an important role in a number of fundamental physical and chemical phenomena [1]. Understanding the coupling of electronic and nuclear degrees of freedom as well as the electron correlations immediately following, or accompanying, optical excitation is particularly important and requires the use of ultrafast methods [2,3].

Attosecond molecular electron dynamics

Abstract: Using attosecond light sources based on high-harmonic generation (HHG), pump-probe experiments can be performed where electron dynamics is studied on its natural timescale, providing insight into the fundamental role that electrons play in photo-induced processes. The tutorial will present first applications in molecular science.