Electron transfer from valence to conduction band states in semiconductors is the basis of modern electronics. Here, attosecond extreme ultraviolet (XUV) spectroscopy is used to resolve this process in silicon in real time. Electrons injected into the conduction band by few-cycle laser pulses alter the silicon XUV absorption spectrum in sharp steps synchronized with the laser electric field oscillations. The observed ~450-attosecond step rise time provides an upper limit for the carrier-induced band-gap reduction and the electron-electron scattering time in the conduction band. This electronic response is separated from the subsequent band-gap modifications due to lattice motion, which occurs on a time scale of 60 ± 10 femtoseconds, characteristic of the fastest optical phonon. Quantum dynamical simulations interpret the carrier injection step as light-field–induced electron tunneling.

Understanding excited carrier dynamics in semiconductors is crucial for the development of photovoltaics and efficient photonic devices. However, overlapping spectral features in optical pump-probe spectroscopy often render assignments of separate electron and hole carrier dynamics ambiguous. Here, ultrafast electron and hole dynamics in germanium nanocrystalline thin films are directly and simultaneously observed by ultrafast transient absorption spectroscopy in the extreme ultraviolet at the germanium M4,5 edge. We decompose the spectra into contributions of electronic state blocking and photo-induced band shifts at a carrier density of 8 × 1020 cm−3. Separate electron and hole relaxation times are observed as a function of hot carrier energies. A first-order electron and hole decay of ∼1 ps suggests a Shockley–Read–Hall recombination mechanism. The simultaneous observation of electrons and holes with extreme ultraviolet transient absorption spectroscopy paves the way for investigating few- to sub-femtosecond dynamics of both holes and electrons in complex semiconductor materials and across junctions.

Semiconductor alloys containing silicon and germanium are of growing importance for compact and highly efficient photonic devices due to their favorable properties for direct integration into silicon platforms and wide tunability of optical parameters. Here, we report the simultaneous direct and energy-resolved probing of ultrafast electron and hole dynamics in a silicon-germanium alloy with the stoichiometry Si0.25Ge0.75 by extreme ultraviolet transient absorption spectroscopy. Probing the photoinduced dynamics of charge carriers at the germanium M4,5-edge (∼30 eV) allows the germanium atoms to be used as reporter atoms for carrier dynamics in the alloy. The photoexcitation of electrons across the direct and indirect band gap into conduction band (CB) valleys and their subsequent hot carrier relaxation are observed and compared to pure germanium, where the Ge direct false(ΔEgap,Ge,direct=0.8 eVfalse) and Si0.25Ge0.75 indirect gaps (ΔEgap,Si0.25Ge0.75,indirect=0.95 eV) are comparable in energy. In the alloy, comparable carrier lifetimes are observed for the X, L, and Γ valleys in the conduction band. A midgap feature associated with electrons accumulating in trap states near the CB edge following intraband thermalization is observed in the Si0.25Ge0.75 alloy. The successful implementation of the reporter atom concept for capturing the dynamics of the electronic bands by site-specific probing in solids opens a route to study carrier dynamics in more complex materials with femtosecond and sub-femtosecond temporal resolution.

Sub-cycle photoelectron streaking from silver plasmonic nanospheres is simulated using few-cycle laser pulses tuned both on and off the plasmon resonance (376 nm vs 800 nm, respectively) to initiate the plasmon. Phase-locked, isolated attosecond XUV pulses induce photoemission from the nanospheres, and two different types of streaking of the photoelectrons occur simultaneously due to the laser and plasmon electric fields. Streaking is simulated over a wide range of excitation pulse intensities, and final velocity distributions for the photoelectrons emitted at different times are calculated. The resulting velocity distributions exhibit several characteristics attributable to the plasmon electric field. The dipole moment amplitude can be reconstructed using velocity map imaging or time-of-flight photoelectron velocity measurements without separate measurement of the laser electric field or deconvolution using an assumed streaking trace shape. These results indicate that photoelectron experiments in table-top set-ups can provide unprecedented spatio-temporal information about sub-cycle plasmon dynamics in metallic nanostructures.

Few-cycle laser pulses with wavelengths centered at 400 nm and 800 nm are simultaneously obtained through wavelength separation of ultrashort, spectrally broadened Vis-NIR laser pulses spanning 350-1100 nm wavelengths. The 400 nm and 800 nm pulses are separately compressed, yielding pulses with 4.4 fs and 3.8 fs duration, respectively. The pulse energy exceeds 5 μJ for the 400 nm pulses and 750 μJ for the 800 nm pulses. Intense 400 nm few-cycle pulses have a broad range of applications in nonlinear optical spectroscopy, which include the study of photochemical dynamics, semiconductors, and photovoltaic materials on few-femtosecond to attosecond time scales. The ultrashort 400 nm few-cycle pulses generated here not only extend the spectral range of the optical pulse for NIR-XUV attosecond pump-probe spectroscopy but also pave the way for two-color, three-pulse, multidimensional optical-XUV spectroscopy experiments.