Abstract:Time-resolved investigations have begun a new era of chemistry and physics, enabling the monitoring in real time of the dynamics of chemical reactions and matter. Induced transient optical absorption is a basic ultrafast electronic effect, originated by a partial depletion of the valence band, that can be triggered by exposing insulators and semiconductors to sub-picosecond extreme-ultraviolet pulses. Besides its scientific and fundamental implications, this process is very important as it is routinely applied… Show more
“…Pump-probe experiments rely on stable spatial superposition and well-defined time delay between pump and probe beams. The time instant (time zero, 𝑡 0 ) when the pulses are temporary overlapped has to be determined 4,5 . When X-ray FEL (especially based on the self-amplified spontaneous emission (SASE) mode) is used as the probe pulse for pump-probe experiments, there is a femtosecond-scale timing jitter between the arrival times of each FEL pulse.…”
Soft X-ray free-electron lasers (FELs) have gained significant attention as a research tool in X-ray ultrafast spectroscopy due to their ultra-high pulse brightness and ultra-short duration. Combined with an independent optical laser to perform pump-probe experiments with time resolution has wide-ranging application value and can have great impact on ultrafast dynamics research in fields such as energy catalysis, solid state physics, materials science, and biology. However, the inherent temporal and spatial jitter of soft X-ray FEL pulses significantly limits the time resolution in these experiments due to the low level of synchronization between the two independent light sources. Here, we present a spatiotemporal coupling device suitable for soft X-ray FELs. The device uses a self-designed four-blade slit device which is suitable for ultra-high vacuum environments to complete the spatial coupling between the two foci of both the soft X-ray FEL and optical laser, reducing the negative effects caused by spatial jitter of soft X-ray FEL beam spots. Based on this, a wavefrontsplitting scheme is used to reflect and separate approximately 30% of the soft X-ray FEL beam for arrival time diagnosis. Based on the principle of transient decrease in the reflectivity of semiconductor material surfaces induced by X-rays, precise time measurement is achieved on a shot-by-shot basis through spectral encoding. After experiments, the data is rearranged according to the arrival time delay between the two pulses, effectively increasing the time resolution of the pump-probe experiment to the femtosecond scale.
“…Pump-probe experiments rely on stable spatial superposition and well-defined time delay between pump and probe beams. The time instant (time zero, 𝑡 0 ) when the pulses are temporary overlapped has to be determined 4,5 . When X-ray FEL (especially based on the self-amplified spontaneous emission (SASE) mode) is used as the probe pulse for pump-probe experiments, there is a femtosecond-scale timing jitter between the arrival times of each FEL pulse.…”
Soft X-ray free-electron lasers (FELs) have gained significant attention as a research tool in X-ray ultrafast spectroscopy due to their ultra-high pulse brightness and ultra-short duration. Combined with an independent optical laser to perform pump-probe experiments with time resolution has wide-ranging application value and can have great impact on ultrafast dynamics research in fields such as energy catalysis, solid state physics, materials science, and biology. However, the inherent temporal and spatial jitter of soft X-ray FEL pulses significantly limits the time resolution in these experiments due to the low level of synchronization between the two independent light sources. Here, we present a spatiotemporal coupling device suitable for soft X-ray FELs. The device uses a self-designed four-blade slit device which is suitable for ultra-high vacuum environments to complete the spatial coupling between the two foci of both the soft X-ray FEL and optical laser, reducing the negative effects caused by spatial jitter of soft X-ray FEL beam spots. Based on this, a wavefrontsplitting scheme is used to reflect and separate approximately 30% of the soft X-ray FEL beam for arrival time diagnosis. Based on the principle of transient decrease in the reflectivity of semiconductor material surfaces induced by X-rays, precise time measurement is achieved on a shot-by-shot basis through spectral encoding. After experiments, the data is rearranged according to the arrival time delay between the two pulses, effectively increasing the time resolution of the pump-probe experiment to the femtosecond scale.
“…In order to account for possible nonuniformities of the sample, we have excluded the uppermost and the lowermost 5% of the distribution of the measured changes in transmission for each energy and delay. Time zero was calibrated using Si 3 N 4 as usually performed for FEL/Vis pump cross-correlation . It is possible that slight variations in the zero delay from run to run (e.g., changing the photon energy of the FEL) can result in a variation of the delay by up to 100 fs.…”
mentioning
confidence: 99%
“…Time zero was calibrated using Si 3 N 4 as usually performed for FEL/Vis pump cross-correlation. 34 It is possible that slight samples. The spectra of Ce 4+ (dashed green line) and Ce 3+ (dashed blue line) reference samples taken from the literature (30) are also reported.…”
Expanding the activity
of wide bandgap semiconductors from the
UV into the visible range has become a central goal for their application
in green solar photocatalysis. The hybrid plasmonic/semiconductor
system, based on silver nanoparticles (Ag NPs) embedded in a film
of CeO
2
, is an example of a functional material developed
with this aim. In this work, we take advantage of the chemical sensitivity
of free electron laser (FEL) time-resolved soft X-ray absorption spectroscopy
(TRXAS) to investigate the electron transfer process from the Ag NPs
to the CeO
2
film generated by the NPs plasmonic resonance
photoexcitation. Ultrafast changes (<200 fs) of the Ce N
4,5
absorption edge allowed us to conclude that the excited Ag NPs transfer
electrons to the Ce atoms of the CeO
2
film through a highly
efficient electron-based mechanism. These results demonstrate the
potential of FEL-based TRXAS measurements for the characterization
of energy transfer in novel hybrid plasmonic/semiconductor materials.
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