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Boosting laboratory photoelectron spectroscopy by megahertz high-order harmonics

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Boosting laboratory photoelectron spectroscopy by megahertz high-order harmonics
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Since the discovery of the photoelectric effect, photoelectron spectroscopy has evolved into the most powerful technique for studying the electronic structure of materials. Moreover, the recent combination of photoelectron experiments with attosecond light sources using high-order harmonic generation (HHG) allows direct observation of electron dynamics in real time. However, the efficiency of these experiments is greatly limited by space-charge effects at typically low repetition rates of photoexcitation. Here, we demonstrate HHG-based laboratory photoemission experiments at a photoelectron count rate of 1 × 105 electrons/s and characterize the main features of the electronic band structure of Ag(001) within several seconds without significant degradation by the space-charge effects. The combination of a compact HHG light source at megahertz repetition rates with the efficient collection of photoelectrons using time-of-flight spectroscopy may allow rapid investigation of electronic bands in a flexible laboratory environment and pave the way for an efficient design of attosecond spectroscopy and microscopy.
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Transcript: English(auto-generated)
In this paper, we present laboratory photoelectron spectroscopy experiments using a high-order harmonic lysos. My name is Michel Hout and I present our experimental setup for the high-order harmonic generation. As driving a laser, we use a fiber-based laser system which you can see on this side.
It's an infrared laser with a pulse energy of 14 microjoule and a repetition rate of about 1 MHz. With just a few optical components, we guide the laser beam into the ultrahigh vacuum chamber where the high-order harmonic generation takes place. The laser beam is focused into a gas jet there and we can have a closer look at the generation now.
In our generation chamber, the gas comes from the top through a capillary and the laser is focused just at the tip of the capillary into the gas jet. There the generation of the high-order harmonic light takes place and afterwards there is a monochromator with a toroidal grating where we can select the energy to do photo emission.
To characterize the generated spectrum of the high-order harmonics, we turn the monochromator grating slowly within few degrees and measure the photoelectron signal. We observe a harmonic spectrum from 14 to 40 eV generated from an argon jet.
Whereas from a single jet, the harmonic spectrum is narrower but can provide higher photon flux. By using the broad photon energy range generated from argon, we
can perform photoelectron spectroscopy on a silver surface at different photon energies. For photoelectron spectroscopy, we use a time-of-flight spectrometer and this allows us to map the energy as well as the momentum in two directions, in kx and ky directions.
So if we have a dispersion like this, we can also see this for example in the ky direction and then we take a look at slides of constant energy.
For example like this, and we measure this on a silver surface. Using the higher photon flux generated from signal, we can recognize the D-band complex of silver in a short measurement within 10 seconds. This proof of principle experiments are not significantly influenced by the space charge
effects because of the high repetition rate of our light source at 1 MHz. In order to compare with other photomission experiments, we present in this paper an overview.
This summary shows the number of emitted photoelectrons per second as a function of the repetition rate of the light source. The red color indicates the energy broadening in a model calculation for space charge effects. Conventional photomission experiments using high-order harmonics work at few kHz repetition rates.
Therefore, significant degradation due to large space charge effects has been observed. In our experiments, we work at much higher repetition rate with a moderate photon flux.
Our experimental condition can be nearly optimal for photoelectron spectroscopy measurements using a time-of-flight spectrometer. Thank you for your attention.