19 research outputs found
Ion-photoelectron entanglement in photoionization with chirped laser pulses
The investigation of coherent dynamics induced by photoionization of atoms or molecules by extreme ultra-violet (XUV) attosecond laser pulses requires careful consideration of the degree of ion + photoelectron entanglement that results from the photoionization process. Here, we consider coherent H2+ vibrational dynamics induced by photoionization of neutral H2 by a chirped attosecond laser pulse. We show that chirping the attosecond laser pulse leads to ion + photoelectron entanglement and the transition from a pure to a mixed state. This transition is characterized by evaluating the purity, which is close to unity for a transform-limited attosecond laser pulse and which decreases to a value that is determined by the number of vibrational states populated in the photoionization process for increasing values of the chirp parameter. In the calculations, the vibrational dynamics is probed by calculating time-delayed dissociation of the H2+ cation by a short ultra-violet (UV) laser pulse. Independent of the magnitude of the chirp, the coherent vibrational dynamics can be recovered by recording the XUV-UV delay-dependent kinetic energy release in coincidence with the kinetic energy of the accompanying photoelectron
Phase-locking of time-delayed attosecond XUV pulse pairs
We present a setup for the generation of phase-locked attosecond extreme ultraviolet (XUV) pulse pairs. The attosecond pulse pairs are generated by high harmonic generation (HHG) driven by two phase-locked near-infrared (NIR) pulses that are produced using an actively stabilized Mach-Zehnder interferometer compatible with near-single cycle pulses. The attosecond XUV pulses can be delayed over a range of 400 fs with a sub-10-as delay jitter. We validate the precision and the accuracy of the setup by XUV optical interferometry and by retrieving the energies of Rydberg states of helium in an XUV pump–NIR probe photoelectron spectroscopy experiment
Probing Time-Dependent Molecular Dipoles on the Attosecond Time Scale
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 (N2, 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
High power, high repetition rate laser-based sources for attosecond science
Within the last two decades attosecond science has been established as a novel research field providing insights into the ultrafast electron dynamics that follows a photoexcitation or photoionization process. Enabled by technological advances in ultrafast laser amplifiers, attosecond science has been in turn, a powerful engine driving the development of novel sources of intense ultrafast laser pulses. This article focuses on the development of high repetition rate laser-based sources delivering high energy pulses with a duration of only a few optical cycles, for applications in attosecond science. In particular, a high power, high repetition rate optical parametric chirped pulse amplification system is described, which was developed to drive an attosecond pump-probe beamline targeting photoionization experiments with electron-ion coincidence detection at high acquisition rates
Recombination dynamics of clusters in intense extreme-ultraviolet and near- infrared fields
We investigate electron-ion recombination processes in clusters exposed to
intense extreme-ultraviolet (XUV) or near-infrared (NIR) pulses. Using the
technique of reionization of excited atoms from recombination (REAR), recently
introduced in Schütte et al (2014 Phys. Rev. Lett. 112 253401), a large
population of excited atoms, which are formed in the nanoplasma during cluster
expansion, is identified under both ionization conditions. For intense XUV
ionization of clusters, we find that the significance of recombination
increases for increasing cluster sizes. In addition, larger fragments are
strongly affected by recombination as well, as shown for the case of dimers.
We demonstrate that for mixed Ar–Xe clusters exposed to intense NIR pulses,
excited atoms and ions are preferentially formed in the Xe core. As a result
of electron-ion recombination, higher charge states of Xe are efficiently
suppressed, leading to an overall reduced expansion speed of the cluster core
in comparison to the shell
Visualizing the Coupling between Red and Blue Stark States Using Photoionization Microscopy
In nonhydrogenic atoms in a dc electric field, the finite size of the ionic
core introduces a coupling between quasibound Stark states that leads to
avoided crossings between states that would otherwise cross. Near an avoided
crossing, the interacting states may have decay amplitudes that cancel each
other, decoupling one of the states from the ionization continuum. This well-
known interference narrowing effect, observed as a strongly electric field-
dependent decrease in the ionization rate, was previously observed in several
atoms. Here we use photoionization microscopy to visualize interference
narrowing in helium atoms, thereby explicitly revealing the mechanism by which
Stark states decay. The interference narrowing allows measurements of the
nodal patterns of red Stark states, which are otherwise not observable due to
their intrinsic short lifetime
Attosecond investigation of extreme-ultraviolet multi-photon multi-electron ionization
Multi-electron dynamics in atoms and molecules very often occur on sub- to few-femtosecond time scales. The available intensities of extreme-ultraviolet (XUV) attosecond pulses have previously allowed the time-resolved investigation of two-photon, two-electron interactions. Here we study double and triple ionization of argon atoms involving the absorption of up to five XUV photons using a pair of intense attosecond pulse trains (APTs). By varying the time delay between the two APTs with attosecond precision and the spatial overlap with nanometer precision, we obtain information on complex nonlinear multi-photon ionization pathways. Our experimental and numerical results show that Ar2+ is predominantly formed by a sequential two-photon process, whereas the delay dependence of the Ar3+ ion yield exhibits clear signatures of the involvement of a simultaneous two-photon absorption process. Our experiment suggests that it is possible to investigate multi-electron dynamics using attosecond pulses for both pumping and probing the dynamics
Generation and characterization of isolated attosecond pulses at 100  kHz repetition rate
The generation of coherent light pulses in the extreme ultraviolet (XUV) spectral region with attosecond pulse durations constitutes the foundation of the field of attosecond science. Twenty years after the first demonstration of isolated attosecond pulses, they continue to be a unique tool enabling the observation and control of electron dynamics in atoms, molecules, and solids. It has long been identified that an increase in the repetition rate of attosecond light sources is necessary for many applications in atomic and molecular physics, surface science, and imaging. Although high harmonic generation (HHG) at repetition rates exceeding 100 kHz, showing a continuum in the cutoff region of the XUV spectrum, was already demonstrated in 2013, the number of photons per pulse was insufficient to perform pulse characterization via attosecond streaking, let alone to perform a pump-probe experiment. Here we report on the generation and full characterization of XUV attosecond pulses via HHG driven by near-single-cycle pulses at a repetition rate of 100 kHz. The high number of 106 XUV photons per pulse on target enables attosecond electron streaking experiments through which the XUV pulses are determined to consist of a dominant single attosecond pulse. These results open the door for attosecond pump-probe spectroscopy studies at a repetition rate 1 or 2 orders of magnitude above current implementations
towards time-resolved imaging of molecular structure
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 (C8H5F) 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 ≈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
XUV excitation followed by ultrafast non-adiabatic relaxation in PAH molecules as a femto-astrochemistry experiment
15Highly excited molecular species are at play in the chemistry of interstellar media and are involved in the creation of radiation damage in a biological tissue. Recently developed ultrashort extreme ultraviolet light sources offer the high excitation energies and ultrafast time-resolution required for probing the dynamics of highly excited molecular states on femtosecond (fs) (1 fs=10−15s) and even attosecond (as) (1 as=10−18 s) timescales. Here we show that polycyclic aromatic hydrocarbons (PAHs) undergo ultrafast relaxation on a few tens of femtoseconds timescales, involving an interplay between the electronic and vibrational degrees of freedom. Our work reveals a general property of excited radical PAHs that can help to elucidate the assignment of diffuse interstellar absorption bands in astrochemistry, and provides a benchmark for the manner in which coupled electronic and nuclear dynamics determines reaction pathways in large molecules following extreme ultraviolet excitation.openopenMarciniak, A.*; Despré, V.; Barillot, T.; Rouzée, A.; Galbraith, M.C.E.; Klei, J.; Yang, C.-H.; Smeenk, C.T.L.; Loriot, V.; Reddy, S. Nagaprasad; Tielens, A.G.G.M.; Mahapatra, S.; Kuleff, A.I.; Vrakking, M.J.J.; Lépine, F.Marciniak, A.; Despré, V.; Barillot, T.; Rouzée, A.; Galbraith, M. C. E.; Klei, J.; Yang, C. -H.; Smeenk, C. T. L.; Loriot, V.; Reddy, S. Nagaprasad; Tielens, A. G. G. M.; Mahapatra, S.; Kuleff, A. I.; Vrakking, M. J. J.; Lépine, F