Browse
Submit Data
Databases
API
Help

Dataset Information

0 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

An investigation of electron-phonon coupling via phonon dispersion measurements in graphite using angle-resolved photoelectron spectroscopy.

ABSTRACT: Electron-phonon coupling (EPC) plays an important role in solid state physics. Here, we demonstrate an experimental method that enables investigation of the elemental processes of the indirect transition, in which EPC participates in photoexcitation in solids, by resolving the energy and momentum of phonons and electrons simultaneously. For graphite, we used angle-resolved photoelectron spectroscopy to observe electron emission at the Γ-point being scattered from the K-point by a phonon. Energy conservation during phonon emission implies that the step-like structure in the spectrum is near the Fermi level, and angle-resolved measurements revealed phonon dispersions that contribute to EPC because of parallel momentum conservation. The observed phonon branch depends on the photon energy, i.e., the final photoexcitation state; this dependency is partly explained by the selection rule, which is determined by the electron state symmetry for the initial, intermediate, and final states and the phonon.

SUBMITTER: Tanaka S

PROVIDER: S-EPMC3805971 | biostudies-other | 2013

REPOSITORIES: biostudies-other

ACCESS DATA

Json Xml

Similar Datasets

Novel Electron-Phonon Relaxation Pathway in Graphite Revealed by Time-Resolved Raman Scattering and Angle-Resolved Photoemission Spectroscopy.

Project description:Time dynamics of photoexcited electron-hole pairs is important for a number of technologies, in particular solar cells. We combined ultrafast pump-probe Raman scattering and photoemission to directly follow electron-hole excitations as well as the G-phonon in graphite after an excitation by an intense laser pulse. This phonon is known to couple relatively strongly to electrons. Cross-correlating effective electronic and phonon temperatures places new constraints on model-based fits. The accepted two-temperature model predicts that G-phonon population should start to increase as soon as excited electron-hole pairs are created and that the rate of increase should not depend strongly on the pump fluence. Instead we found that the increase of the G-phonon population occurs with a delay of ~65 fs. This time-delay is also evidenced by the absence of the so-called self-pumping for G phonons. It decreases with increased pump fluence. We show that these observations imply a new relaxation pathway: Instead of hot carriers transferring energy to G-phonons directly, the energy is first transferred to optical phonons near the zone boundary K-points, which then decay into G-phonons via phonon-phonon scattering. Our work demonstrates that phonon-phonon interactions must be included in any calculations of hot carrier relaxation in optical absorbers even when only short timescales are considered.

| S-EPMC5244369 | biostudies-literature

Local Berry curvature signatures in dichroic angle-resolved photoelectron spectroscopy from two-dimensional materials.

Project description:Topologically nontrivial two-dimensional materials hold great promise for next-generation optoelectronic applications. However, measuring the Hall or spin-Hall response is often a challenge and practically limited to the ground state. An experimental technique for tracing the topological character in a differential fashion would provide useful insights. In this work, we show that circular dichroism angle-resolved photoelectron spectroscopy provides a powerful tool that can resolve the topological and quantum-geometrical character in momentum space. In particular, we investigate how to map out the signatures of the momentum-resolved Berry curvature in two-dimensional materials by exploiting its intimate connection to the orbital polarization. A spin-resolved detection of the photoelectrons allows one to extend the approach to spin-Chern insulators. The present proposal can be extended to address topological properties in materials out of equilibrium in a time-resolved fashion.

| S-EPMC7048418 | biostudies-literature

Determination of interatomic coupling between two-dimensional crystals using angle-resolved photoemission spectroscopy.

Project description:Lack of directional bonding between two-dimensional crystals like graphene or monolayer transition metal dichalcogenides provides unusual freedom in the selection of components for vertical van der Waals heterostructures. However, even for identical layers, their stacking, in particular the relative angle between their crystallographic directions, modifies properties of the structure. We demonstrate that the interatomic coupling between two two-dimensional crystals can be determined from angle-resolved photoemission spectra of a trilayer structure with one aligned and one twisted interface. Each of the interfaces provides complementary information and together they enable self-consistent determination of the coupling. We parametrise interatomic coupling for carbon atoms by studying twisted trilayer graphene and show that the result can be applied to structures with different twists and number of layers. Our approach demonstrates how to extract fundamental information about interlayer coupling in a stack of two-dimensional crystals and can be applied to many other van der Waals interfaces.

| S-EPMC7367817 | 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 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 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

Hole-phonon coupling effect on the band dispersion of organic molecular semiconductors.

Project description:The dynamic interaction between the traveling charges and the molecular vibrations is critical for the charge transport in organic semiconductors. However, a direct evidence of the expected impact of the charge-phonon coupling on the band dispersion of organic semiconductors is yet to be provided. Here, we report on the electronic properties of rubrene single crystal as investigated by angle resolved ultraviolet photoelectron spectroscopy. A gap opening and kink-like features in the rubrene electronic band dispersion are observed. In particular, the latter results in a large enhancement of the hole effective mass (> 1.4), well above the limit of the theoretical estimations. The results are consistent with the expected modifications of the band structures in organic semiconductors as introduced by hole-phonon coupling effects and represent an important experimental step toward the understanding of the charge localization phenomena in organic materials.The charge transport properties in organic semiconductors are affected by the impact of molecular vibrations, yet it has been challenging to quantify them to date. Here, Bussolotti et al. provide direct experimental evidence on the band dispersion modified by molecular vibrations in a rubrene single crystal.

| S-EPMC5539254 | biostudies-literature

Nonadiabatic exciton-phonon coupling in Raman spectroscopy of layered materials.

Project description:We present an ab initio computational approach for the calculation of resonant Raman intensities, including both excitonic and nonadiabatic effects. Our diagrammatic approach, which we apply to two prototype, semiconducting layered materials, allows a detailed analysis of the impact of phonon-mediated exciton-exciton scattering on the intensities. In the case of bulk hexagonal boron nitride, this scattering leads to strong quantum interference between different excitonic resonances, strongly redistributing oscillator strength with respect to optical absorption spectra. In the case of MoS2, we observe that quantum interference effects are suppressed by the spin-orbit splitting of the excitons.

| S-EPMC7413722 | biostudies-literature

Unraveling intrinsic correlation effects with angle-resolved photoemission spectroscopy.

Project description:Interaction effects can change materials properties in intriguing ways, and they have, in general, a huge impact on electronic spectra. In particular, satellites in photoemission spectra are pure many-body effects, and their study is of increasing interest in both experiment and theory. However, the intrinsic spectral function is only a part of a measured spectrum, and it is notoriously difficult to extract this information, even for simple metals. Our joint experimental and theoretical study of the prototypical simple metal aluminum demonstrates how intrinsic satellite spectra can be extracted from measured data using angular resolution in photoemission. A nondispersing satellite is detected and explained by electron-electron interactions and the thermal motion of the atoms. Additional nondispersing intensity comes from the inelastic scattering of the outgoing photoelectron. The ideal intrinsic spectral function, instead, has satellites that disperse both in energy and in shape. Theory and the information extracted from experiment describe these features with very good agreement.

| S-EPMC7682325 | biostudies-literature

Four-dimensional vibrational spectroscopy for nanoscale mapping of phonon dispersion in BN nanotubes.

Project description:Directly mapping local phonon dispersion in individual nanostructures can advance our understanding of their thermal, optical, and mechanical properties. However, this requires high detection sensitivity and combined spatial, energy and momentum resolutions, thus has been elusive. Here, we demonstrate a four-dimensional electron energy loss spectroscopy technique, and present position-dependent phonon dispersion measurements in individual boron nitride nanotubes. By scanning the electron beam in real space while monitoring both the energy loss and the momentum transfer, we are able to reveal position- and momentum-dependent lattice vibrations at nanometer scale. Our measurements show that the phonon dispersion of multi-walled nanotubes is locally close to hexagonal-boron nitride crystals. Interestingly, acoustic phonons are sensitive to defect scattering, while optical modes are insensitive to small voids. This work not only provides insights into vibrational properties of boron nitride nanotubes, but also demonstrates potential of the developed technique in nanoscale phonon dispersion measurements.

| S-EPMC7896073 | 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