Browse
Submit Data
Databases
API
Help

Dataset Information

35 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

Attosecond time-resolved photoelectron holography.

ABSTRACT: Ultrafast strong-field physics provides insight into quantum phenomena that evolve on an attosecond time scale, the most fundamental of which is quantum tunneling. The tunneling process initiates a range of strong field phenomena such as high harmonic generation (HHG), laser-induced electron diffraction, double ionization and photoelectron holography-all evolving during a fraction of the optical cycle. Here we apply attosecond photoelectron holography as a method to resolve the temporal properties of the tunneling process. Adding a weak second harmonic (SH) field to a strong fundamental laser field enables us to reconstruct the ionization times of photoelectrons that play a role in the formation of a photoelectron hologram with attosecond precision. We decouple the contributions of the two arms of the hologram and resolve the subtle differences in their ionization times, separated by only a few tens of attoseconds.

SUBMITTER: Porat G

PROVIDER: S-EPMC6051996 | biostudies-literature |

REPOSITORIES: biostudies-literature

ACCESS DATA

Json Xml

Similar Datasets

Time-Resolved Photoelectron Spectroscopy of Conical Intersections with Attosecond Pulse Trains.

Project description:Conical Intersections (CIs), which are believed to be ubiquitous in molecular and biological systems, open up ultrafast nonradiative decay channels. A superposition of electronic states is created when a molecule passes through a CI and the nuclear wave packet branches. The resulting electronic coherence can be considered a unique signature of the CI. The involved electronic states can be resolved in the energy domain with photoelectron spectroscopy using a femtosecond pulse as a probe. However, the observation of the created electronic coherence in the time domain requires probe pulses with several electron volts of bandwidth. Attosecond pulses can probe the electronic coherence but are unable to resolve the involved electronic states. In this Letter, we propose to address this restriction by using time-resolved photoelectron spectroscopy with an attosecond pulse train as a probe. We theoretically demonstrate that the resulting photoelectron spectrum may yield energy resolution as well as the information on the created coherences in the time domain.

| S-EPMC8404190 | biostudies-literature

Time-Resolved Photoelectron Spectroscopy Studies of Isoxazole and Oxazole.

Project description:The excited state relaxation pathways of isoxazole and oxazole upon excitation with UV-light were investigated by nonadiabatic ab initio dynamics simulations and time-resolved photoelectron spectroscopy. Excitation of the bright ??*-state of isoxazole predominantly leads to ring-opening dynamics. Both the initially excited ??*-state and the dissociative ??*-state offer a combined barrier-free reaction pathway, such that ring-opening, defined as a distance of more than 2 Å between two neighboring atoms, occurs within 45 fs. For oxazole, in contrast, the excited state dynamics is about twice as slow (85 fs) and the quantum yield for ring-opening is lower. This is caused by a small barrier between the ??*-state and the ??*-state along the reaction path, which suppresses direct ring-opening. Theoretical findings are consistent with the measured time-resolved photoelectron spectra, confirming the timescales and the quantum yields for the ring-opening channel. The results indicate that a combination of time-resolved photoelectron spectroscopy and excited state dynamics simulations can explain the dominant reaction pathways for this class of molecules. As a general rule, we suggest that the antibonding ?*-orbital located between the oxygen atom and a neighboring atom of a five-membered heterocyclic system provides a driving force for ring-opening reactions, which is modified by the presence and position of additional nitrogen atoms.

| S-EPMC7304896 | biostudies-literature

Time resolved photoelectron spectroscopy of thioflavin T photoisomerization: a simulation study.

Project description:The excited state isomerization of thioflavin T (ThT) is responsible for the quenching of its fluorescence in a nonrestricted environment. The fluorescence quantum yield increases substantially upon binding to amyloid fibers. Simulations reveal that the variation of the twisting angle between benzothiazole and benzene groups (φ1) is responsible for the subpicosecond fluorescence quenching. The evolution of the twisting process can be directly probed by photoelectron emission with energies ε ≥ 1.0 eV before the molecule reaches the φ1-twisted configuration (~300 fs).

| S-EPMC3723713 | biostudies-literature

Influence of nuclear dynamics on molecular attosecond photoelectron interferometry.

Project description:In extreme ultraviolet spectroscopy, the photoionization process occurring in a molecule due to the absorption of a single photon can trigger an ultrafast nuclear motion in the cation. Taking advantage of attosecond photoelectron interferometry, where the absorption of the extreme ultraviolet photon is accompanied by the exchange of an additional infrared quantum of light, one can investigate the influence of nuclear dynamics by monitoring the characteristics of the photoelectron spectra generated by the two-color field. Here, we show that attosecond photoelectron interferometry is sensitive to the nuclear response by measuring the two-color photoionization spectra in a mixture of methane (CH4) and deuteromethane (CD4). The effect of the different nuclear evolution in the two isotopologues manifests itself in the modification of the amplitude and contrast of the oscillations of the photoelectron peaks. Our work indicates that nuclear dynamics can affect the coherence properties of the electronic wave packet emitted by photoionization on a time scale as short as a few femtoseconds.

| S-EPMC10468127 | biostudies-literature

Time-resolved electron holography and its application to an ionic liquid specimen.

Project description:Time-resolved electron holography was implemented in a transmission electron microscope by means of electron beam gating with a parallel-plate electrostatic deflector. Stroboscopic observations were performed by accumulating gated electron interference images while applying a periodic modulation voltage to a specimen. Electric polarization in an ionic liquid specimen was observed under applied fields. While a static electric field in the specimen was reduced by the polarization of the material, an applied field modulated at 10 kHz was not screened. This indicates that time-resolved electron holography is capable of determining the frequency limit of dynamic response of polarization in materials. Graphical Abstract.

| S-EPMC10561666 | biostudies-literature

Tracing Photoinduced Hydrogen Migration in Alcohol Dications from Time-Resolved Molecular-Frame Photoelectron Angular Distributions.

Project description:The recent implementation of attosecond and few-femtosecond X-ray pump/X-ray probe schemes in large-scale free-electron laser facilities has opened the way to visualize fast nuclear dynamics in molecules with unprecedented temporal and spatial resolution. Here, we present the results of theoretical calculations showing how polarization-averaged molecular-frame photoelectron angular distributions (PA-MFPADs) can be used to visualize the dynamics of hydrogen migration in methanol, ethanol, propanol, and isopropyl alcohol dications generated by X-ray irradiation of the corresponding neutral species. We show that changes in the PA-MFPADs with the pump-probe delay as a result of intramolecular photoelectron diffraction carry information on the dynamics of hydrogen migration in real space. Although visualization of this dynamics is more straightforward in the smaller systems, methanol and ethanol, one can still recognize the signature of that motion in propanol and isopropyl alcohol and assign a tentative path to it. A possible pathway for a corresponding experiment requires an angularly resolved detection of photoelectrons in coincidence with molecular fragment ions used to define a molecular frame of reference. Such studies have become, in principle, possible since the first XFELs with sufficiently high repetition rates have emerged. To further support our findings, we provide experimental evidence of H migration in ethanol-OD from ion-ion coincidence measurements performed with synchrotron radiation.

| S-EPMC10895665 | biostudies-literature

Simulated and Experimental Time-Resolved Photoelectron Spectra of the Intersystem Crossing Dynamics in 2-Thiouracil.

Project description:We report time-dependent photoelectron spectra recorded with a single-photon ionization setup and extensive simulations of the same spectra for the excited-state dynamics of 2-thiouracil (2TU) in the gas phase. We find that single-photon ionization produces very similar results as two-photon ionization, showing that the probe process does not have a strong influence on the measured dynamics. The good agreement between the single-photon ionization experiments and the simulations shows that the norms of Dyson orbitals allow for qualitatively describing the ionization probabilities of 2TU. This reasonable performance of Dyson norms is attributed to the particular electronic structure of 2TU, where all important neutral and ionic states involve similar orbital transitions and thus the shape of the Dyson orbitals do not strongly depend on the initial neutral and final ionic state. We argue that similar situations should also occur in other biologically relevant thio-nucleobases, and that the time-resolved photoelectron spectra of these bases could therefore be adequately modeled with the techniques employed here.

| S-EPMC6278540 | biostudies-literature

Three-dimensional supercritical resolved light-induced magnetic holography.

Project description:In the era of big data, there exists a growing gap between data generated and storage capacity using two-dimensional (2D) magnetic storage technologies (for example, hard disk drives), because they have reached their performance saturation. 3D volumetric all-optical magnetic holography is emerging rapidly as a promising road map to realizing high-density capacity for its fast magnetization control and subwavelength magnetization volume. However, most of the reported light-induced magnetization confronts the problems of impurely longitudinal magnetization, diffraction-limited spot, and uncontrollable magnetization reversal. To overcome these challenges, we propose a novel 3D light-induced magnetic holography based on the conceptual supercritical design with multibeam combination in the 4? microscopic system. We theoretically demonstrate a 3D deep super-resolved [Formula: see text] purely longitudinal magnetization spot by focusing six coherent circularly polarized beams with two opposing high numerical aperture objectives, which allows 3D magnetic holography with a volumetric storage density of up to 1872 terabit per cubic inches. The number and locations of the super-resolved magnetization spots are controllable, and thus, desired magnetization arrays in 3D volume can be produced with properly designed phase filters. Moreover, flexible magnetization reversals are also demonstrated in multifocal arrays by using different illuminations with opposite light helicity. In addition to data storage, this magnetic holography may find applications in information security, such as identity verification for a credit card with magnetic stripe.

| S-EPMC5640382 | biostudies-literature

Relaxation Dynamics in Photoexcited Chiral Molecules Studied by Time-Resolved Photoelectron Circular Dichroism: Toward Chiral Femtochemistry.

Project description:Unravelling the main initial dynamics responsible for chiral recognition is a key step in the understanding of many biological processes. However, this challenging task requires a sensitive enantiospecific probe to investigate molecular dynamics on their natural femtosecond time scale. Here we show that, in the gas phase, the ultrafast relaxation dynamics of photoexcited chiral molecules can be tracked by recording time-resolved photoelectron circular dichroism (TR-PECD) resulting from the photoionization by a circularly polarized probe pulse. A large forward-backward asymmetry along the probe propagation axis is observed in the photoelectron angular distribution. Its evolution with pump-probe delay reveals ultrafast dynamics that are inaccessible in the angle-integrated photoelectron spectrum or via the usual electron emission anisotropy parameter (β). PECD, which originates from the electron scattering in the chiral molecular potential, appears as a new sensitive observable for ultrafast molecular dynamics in chiral systems.

| S-EPMC5116763 | biostudies-literature

Time-resolved imaging of magnetic vortex dynamics using holography with extended reference autocorrelation by linear differential operator.

Project description:The magnetisation dynamics of the vortex core and Landau pattern of magnetic thin-film elements has been studied using holography with extended reference autocorrelation by linear differential operator (HERALDO). Here we present the first time-resolved x-ray measurements using this technique and investigate the structure and dynamics of the domain walls after excitation with nanosecond pulsed magnetic fields. It is shown that the average magnetisation of the domain walls has a perpendicular component that can change dynamically depending on the parameters of the pulsed excitation. In particular, we demonstrate the formation of wave bullet-like excitations, which are generated in the domain walls and can propagate inside them during the cyclic motion of the vortex core. Based on numerical simulations we also show that, besides the core, there are four singularities formed at the corners of the pattern. The polarisation of these singularities has a direct relation to the vortex core, and can be switched dynamically by the wave bullets excited with a magnetic pulse of specific parameters. The subsequent dynamics of the Landau pattern is dependent on the particular configuration of the polarisations of the core and the singularities.

| S-EPMC5087091 | biostudies-literature

OmicsDI is part of the ELIXIR infrastructure

OmicsDI is an Elixir interoperability service. Learn more ›

Tweets

OmicsDI Databases

PRIDE
PeptideAtlas
MassIVE
JPOST Repository
Physiome Model Repository

EGA
EVA
ENA
LINCS
PAXDB
Cell Collective

MetaboLights
Metabolomics Workbench
MetabolomeExpress
GNPS
BioModels
FAIRDOMHub

ArrayExpress
dbGaP
ExpressionAtlas
GEO
NODE

Information

Databases
Help
API
Contact us
Code on GitHub
Terms of use
Submit Data