https://iopscience.iop.org/article/10.1088/1361-6455/aac6ac/pdf

Attosecond physics phenomena at nanometric tips

Time-resolved hard x-ray photoelectron spectroscopy (trHAXPES) is established using the x-ray free-electron laser SACLA. The technique extends time-resolved photoemission into the hard x-ray regime and, as a core-level spectroscopy, combines element and atomic-site specificity and sensitivity to the chemical environment with femtosecond time resolution and bulk (sub-surface) sensitivity. The viability of trHAXPES using 8 keV x-ray free-electron-laser radiation is demonstrated by a systematic investigation of probe and pump pulse-induced vacuum space-charge effects on the V 1s emission of VO2 and the Ti 1s emission of SrTiO3. The time and excitation energy dependencies of the measured spectral shifts and broadenings are compared to the results of N-body numerical simulations and simple analytic (mean-field) models. Good agreement between the experimental and calculated results is obtained. In particular, the characteristic temporal evolution of the pump pulse-induced spectral shift is shown to provide an effective means to determine the temporal overlap of pump and probe pulses. trHAXPES opens a new avenue in the study of ultrafast atomic-site specific electron and chemical dynamics in materials and at buried interfaces.

http://iopscience.iop.org/article/10.1088/1367-2630/16/12/123045/pdf

Time-resolved HAXPES at SACLA: probe and pump pulse-induced space-charge effects

Low-energy electron transmission through thin-film molecular and biomolecular solids.

With its direct correspondence to electronic structure, angle-resolved photoemission spectroscopy (ARPES) is a ubiquitous tool for the study of solids. When extended to the temporal domain, time-resolved (TR)-ARPES offers the potential to move beyond equilibrium properties, exploring both the unoccupied electronic structure as well as its dynamical response under ultrafast perturbation. Historically, ultrafast extreme ultraviolet sources employing high-order harmonic generation (HHG) have required compromises that make it challenging to achieve a high energy resolution—which is highly desirable for many TR-ARPES studies—while producing high photon energies and a high photon flux. We address this challenge by performing HHG inside a femtosecond enhancement cavity, realizing a practical source for TR-ARPES that achieves a flux of over 1011 photons/s delivered to the sample, operates over a range of 8–40 eV with a repetition rate of 60 MHz. This source enables TR-ARPES studies with a temporal and energy resolution of 190 fs and 22 meV, respectively. To characterize the system, we perform ARPES measurements of polycrystalline Au and MoTe2, as well as TR-ARPES studies on graphite.

Cavity-enhanced high harmonic generation for extreme ultraviolet time- and angle-resolved photoemission spectroscopy.

With its direct correspondence to electronic structure, angle-resolved photoemission spectroscopy (ARPES) is a ubiquitous tool for the study of solids. When extended to the temporal domain, time-resolved (TR)-ARPES offers the potential to move beyond equilibrium properties, exploring both the unoccupied electronic structure as well as its dynamical response under ultrafast perturbation. Historically, ultrafast extreme ultraviolet (XUV) sources employing high-order harmonic generation (HHG) have required compromises that make it challenging to achieve a high energy resolution - which is highly desirable for many TR-ARPES studies - while producing high photon energies and a high photon flux. We address this challenge by performing HHG inside a femtosecond enhancement cavity (fsEC), realizing a practical source for TR-ARPES that achieves a flux of over 10$^{11}$ photons/s delivered to the sample, operates over a range of 8-40 eV with a repetition rate of 60 MHz. This source enables TR-ARPES studies with a temporal and energy resolution of 190 fs and 22 meV, respectively. To characterize the system, we perform ARPES measurements of polycrystalline Au and MoTe$_2$, as well as TR-ARPES studies on graphite.

Cavity-enhanced high harmonic generation for XUV time-resolved ARPES

The experimental results of multiphoton electron emission from Cu and W induced by 2-eV 100-fs laser pulses with $s$ and $p$ polarizations at incidence angles between 0\ifmmode^\circ\else\textdegree\fi{} and 85\ifmmode^\circ\else\textdegree\fi{} and different intensities are reported. The data show a third-order nonlinear photoemission process for Cu and a fourth-order behavior for W. For both metals the electron emission is higher for the polarization in the incidence plane, with a maximum value at the pseudo-Brewster angle, while the electron yield as a function of the incidence angle exhibits an unambiguous dependence on the bulk absorption coefficient and it can be accounted for on the basis of the Fresnel equations.

/pdf/multiphoton-electron-emission-from-cu-and-w-an-angle-lubsbr2fo6.pdf

Alberto Lumachi

Papers

Multiphoton electron emission from Cu and W: An angle-resolved study