We detect macroscopic currents driven by intense light fields in a photoconductive antenna, which we switch on using ultrafast vacuum ultraviolet light pulses. By comparing these currents with the vector potential of the incident light, we can follow nonequilibrium inter- and intra-band carrier dynamics with attosecond resolution.
X-ray absorption fine-structure (XAFS) spectroscopy is a well-established technique capable of extracting information about a material’s electronic and lattice structure with atomic resolution. While the near-edge region (XANES) of a XAFS spectrum provides information about the electronic configuration, structural information is extracted from the extended XAFS (EXAFS) spectrum, consisting of several hundreds of eV above the absorption edge. With the advent of high harmonic sources, reaching photon energies in soft x-ray (SXR) region, it now becomes possible to connect the spectroscopic capabilities of XAFS to the unprecedented attosecond temporal resolution of a high harmonic source allowing the observation of electronic and lattice dynamics in real time [1,2].
Layered materials, such the transition-metal dichalcogenide TiS2 or graphite, are an emerging class of materials with attractive structural and electronic properties as they can be thinned to a single atomic layer with electron mobilities resembling that of a metal, semiconductor, or semi-metal.
In this work, we utilized broadband water-window-covering attosecond SXR pulses (300 as, ranging from 200
- 550 eV) capable of accessing orbital-specific K- and L-edges of such layered materials to perform transient XAFS
with attosecond time resolution [3,4].
[1] Teichmann, S. et al, "0.5-keV soft x-ray attosecond continua", Nat. Commun. 7, 11493 (2016).
[2] Cousin S. et al, "Attosecond streaking in the water window: a new regime of attosecond pulse characterization", Phys. Rev. X, 7, 041030 (2017).
[3] Buades, B. et al., “Dispersive soft x-ray absorption fine-structure spectroscopy in graphite with an attosecond pulse”, Optica 5 (5), 502 (2018).
[4] Buades, B. et al., “Attosecond-resolved petahertz carrier motion in semi-metallic TiS2”, arXiv: 1808.06493 (2018).
If the energy of a photon exceeds the band-gap of a material, an electron can be promoted from the valence into the conduction band with a probability described by the linear absorption coefficient. For photons with energies below the bandgap, the medium is transparent. However, even large band-gap materials that are transparent for visible light in the linear regime can become absorptive in the presence of strong electric fields either through multi-photon, or via tunneling transitions.
To study the intricate dynamics of these excitation pathways we developed Attosecond Polarization Sampling (APS). This method resolves the light-matter energy transfer dynamics with attosecond temporal resolution and allows real-time recording of the evolution of both the linear and nonlinear polarization wave driven by the external electric field inside a material.
In APS, the laser electric field E(t) is recorded after passage through the sample in two different settings: First, we attenuate the laser pulses before sending them through the material (here: 10 μm fused silica (SiO2)), ensuring only linear effects occur. In the second step, we use intensities close to the damage threshold of SiO2 so that both linear and non-linear interaction occurs. Comparison of the two electric fields yields slight differences in the instantaneous temporal phase of the pulse carrying information about the time evolution of the induced nonlinear polarization wave.
The observed phase shifts record the field amplitude dependency of the nonlinear refractive index due to the Kerr-effect including its response time and can be directly related to the degree of light-field induced conduction band population. Consequently, these measurements, as shown in Fig. 1, allow to determine the amount of energy exchanged between light-field and sample with sub-optical-cycle time resolution. In the case of strong-field illumination of SiO2 we find that the nonlinear energy transfer has a strong reversible component occurring only during short time intervals around the field crests of the strong laser field and corresponding to the non-permanent transfer of electrons into conduction band-states.
Build-up and immediate decay of this transient conduction band population are the result of a bi-directional energy transfer between field and matter and conform to the assumption of energy absorption from the field during the first half of the laser pulse and re-emission of energy into the same field within the duration of the few-cycle laser pulses.
Most interestingly, we find settings where the transient energy exchange yields a significant modification of the optical and electronic material properties for femtosecond time intervals but no lasting energy transfer (i.e. residual conduction band population) is observable. This ultrafast, dissipation free switching of material properties might turn useful for a future all-optical, ultrafast and loss-free signal metrology.
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