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Register a new userExtreme timescale core-level spectroscopy with tailored XUV pulses
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A new approach for few-femtosecond time-resolved photoelectron spectroscopy in condensed matter that balances the combined needs for both temporal and energy resolution is demonstrated. Here, the method is designed to investigate a prototypical Mott insulator, tantalum disulphide (1T-TaS2), which transforms from its charge-density-wave ordered Mott insulating state to a conducting state in a matter of femtoseconds. The signature to be observed through the phase transition is a charge-density-wave induced splitting of the Ta 4f core-levels, which can be resolved with sub-eV spectral resolution. Combining this spectral resolution with few-femtosecond time resolution enables the collapse of the charge ordered Mott state to be clocked. Precise knowledge of the sub-20-femtosecond dynamics will provide new insight into the physical mechanism behind the collapse and may reveal Mott physics on the timescale of electronic hopping.
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Ionization with ultrashort pulses in the extreme ultraviolet (XUV) regime can be used to prepare an ion in a superposition of spin--orbit substates. In this work, we study the coherence properties of such a superposition, created by ionizing xenon atoms using two phase-locked XUV pulses at different frequencies. In general, if the duration of the driving pulse exceeds the quantum beat period, dephasing will occur. If however, the frequency difference of the two pulses matches the spin--orbit splitting, the coherence can be efficiently increased and dephasing does not occur.
A two-level medium, described by the Maxwell-Bloch (MB) system, is engraved by establishing a standing cavity wave with a linearly polarized electromagnetic field that drives the medium on both ends. A light pulse, polarized along the other direction, then scatters the medium and couples to the cavity standing wave by means of the population inversion density variations. We demonstrate that control of the applied amplitudes of the grating field allows to stop the light pulse and to make it move backward (eventually to drive it freely). A simplified limit model of the MB system with variable boundary driving is obtained as a discrete nonlinear Schroedinger equation with tunable external potential. It reproduces qualitatively the dynamics of the driven light pulse.
A recently developed source of ultraviolet radiation, based on optical soliton propagation in a gas-filled hollow-core photonic crystal fiber, is applied here to angle-resolved photoemission spectroscopy (ARPES). Near-infrared femtosecond pulses of only few {mu}J energy generate vacuum ultraviolet (VUV) radiation between 5.5 and 9 eV inside the gas-filled fiber. These pulses are used to measure the band structure of the topological insulator Bi2Se3 with a signal to noise ratio comparable to that obtained with high order harmonics from a gas jet. The two-order-of-magnitude gain in efficiency promises time-resolved ARPES measurements at repetition rates of hundreds of kHz or even MHz, with photon energies that cover the first Brillouin zone of most materials.
The lack of available table-top extreme ultraviolet (XUV) sources with high enough fluxes and coherence properties have limited the availability of nonlinear XUV and x-ray spectroscopies to free electron lasers (FEL). Here, we demonstrate second harmonic generation (SHG) on a table-top XUV source for the first time by observing SHG at the Ti M2,3-edge with a high harmonic seeded soft x-ray laser (HHG-SXRL) [1,2]. Further, this experiment represents the first SHG experiment in the XUV. First-principles electronic structure calculations are used to confirm the surface specificity and resonant enhancement of the SHG signal. The realization of XUV-SHG on a table-top source with femtosecond temporal resolution opens up tremendous opportunities for the study of element-specific dynamics in multi-component systems where surface, interfacial, and bulk-phase asymmetries play a driving role in smaller-scale labs as opposed to FELs.
The bottleneck for an attosecond science experiment is concluded to be the lack of a high-peak-power isolated attosecond pulse source. Therefore, currently, generating an intense attosecond pulse would be one of the highest priority goals. In this paper, we review a TW-class parallel three-channel waveform synthesizer for generating a gigawatt-scale soft-x-ray isolated attosecond pulse (IAP) using high-order harmonics generation (HHG). Simultaneously, using several stabilization methods, namely, the low-repetition-rate laser carrier-envelope phase stabilization, Mach-Zehnder interferometer, balanced optical cross-correlator, and beam-pointing stabilizer, we demonstrate a stable 50-mJ three-channel optical-waveform synthesizer with a peak power at the multi-TW level. This optical-waveform synthesizer is capable of creating a stable intense optical field for generating an intense continuum harmonic beam thanks to the successful stabilization of all the parameters. Furthermore, the precision control of shot-to-shot reproducible synthesized waveforms is achieved. Through the HHG process employing a loose-focusing geometry, an intense shot-to-shot stable supercontinuum (50-70 eV) is generated in an argon gas cell. This continuum spectrum supports an IAP with a transform-limited duration of 170 as and a submicrojoule pulse energy, which allows the generation of a GW-scale IAP. Another supercontinuum in the soft-x-ray region with higher photon energy of approximately 100-130 eV is also generated in neon gas from the synthesizer. The transform-limited pulse duration is 106 as. According to this work, the enhancement of HHG output through optimized waveform synthesis is experimentally proved. The high-energy multicycle pulse with 10-Hz repetition rate is proved to have the same controllability for optimized waveform synthesis for HHG as few- or subcycle pulses from a 1-kHz laser.
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