Ultrafast electron localization and screening in a transition metal dichalcogenide.

The coupling of light to electrical charge carriers in semiconductors is the foundation of many technological applications. Attosecond transient absorption spectroscopy measures simultaneously how excited electrons and the vacancies they leave behind dynamically react to the applied optical fields. In compound semiconductors, these dynamics can be probed via any of their atomic constituents with core-level transitions into valence and conduction band. Typically, the atomic species forming the compound contribute comparably to the relevant electronic properties of the material. One therefore expects to observe similar dynamics, irrespective of the choice of atomic species via which it is probed. Here, we show in the two-dimensional transition metal dichalcogenide semiconductor MoSe2, that through a selenium-based core-level transition we observe charge carriers acting independently from each other, while when probed through molybdenum, the collective, many-body motion of the carriers dominates. Such unexpectedly contrasting behavior can be explained by a strong localization of electrons around molybdenum atoms following absorption of light, which modifies the local fields acting on the carriers. We show that similar behavior in elemental titanium metal [M. Volkov et al., Nat. Phys. 15, 1145-1149 (2019)] carries over to transition metal-containing compounds and is expected to play an essential role for a wide range of such materials. Knowledge of independent particle and collective response is essential for fully understanding these materials.

Charge Density Wave Melting in One-Dimensional Wires with Femtosecond Subgap Excitation.

Charge density waves (CDWs) are symmetry-broken ground states that commonly occur in low-dimensional metals due to strong electron-electron and/or electron-phonon coupling. The nonequilibrium carrier distribution established via photodoping with femtosecond laser pulses readily quenches these ground states and induces an ultrafast insulator-to-metal phase transition. To date, CDW melting has been mainly investigated in the single-photon regime with pump photon energies bigger than the gap size. The recent development of strong-field midinfrared sources now enables the investigation of CDW dynamics following subgap excitation. Here we excite prototypical one-dimensional indium wires with a CDW gap of ∼300 meV with midinfrared pulses at ℏω=190 meV with MV/cm field strength and probe the transient electronic structure with time- and angle-resolved photoemission spectroscopy. We find that the CDW gap is filled on a timescale short compared to our temporal resolution of 300 fs and that the band structure changes are completed within ∼1 ps. Supported by a minimal theoretical model we attribute our findings to multiphoton absorption across the CDW gap.

Attosecond dynamical Franz-Keldysh effect in polycrystalline diamond.

Short, intense laser pulses can be used to access the transition regime between classical and quantum optical responses in dielectrics. In this regime, the relative roles of inter- and intraband light-driven electronic transitions remain uncertain. We applied attosecond transient absorption spectroscopy to investigate the interaction between polycrystalline diamond and a few-femtosecond infrared pulse with intensity below the critical intensity of optical breakdown. Ab initio time-dependent density functional theory calculations, in tandem with a two-band parabolic model, accounted for the experimental results in the framework of the dynamical Franz-Keldysh effect and identified infrared induction of intraband currents as the main physical mechanism responsible for the observations.

Attosecond nonlinear polarization and light-matter energy transfer in solids.

Electric-field-induced charge separation (polarization) is the most fundamental manifestation of the interaction of light with matter and a phenomenon of great technological relevance. Nonlinear optical polarization produces coherent radiation in spectral ranges inaccessible by lasers and constitutes the key to ultimate-speed signal manipulation. Terahertz techniques have provided experimental access to this important observable up to frequencies of several terahertz. Here we demonstrate that attosecond metrology extends the resolution to petahertz frequencies of visible light. Attosecond polarization spectroscopy allows measurement of the response of the electronic system of silica to strong (more than one volt per ångström) few-cycle optical (about 750 nanometres) fields. Our proof-of-concept study provides time-resolved insight into the attosecond nonlinear polarization and the light-matter energy transfer dynamics behind the optical Kerr effect and multi-photon absorption. Timing the nonlinear polarization relative to the driving laser electric field with sub-30-attosecond accuracy yields direct quantitative access to both the reversible and irreversible energy exchange between visible-infrared light and electrons. Quantitative determination of dissipation within a signal manipulation cycle of only a few femtoseconds duration (by measurement and ab initio calculation) reveals the feasibility of dielectric optical switching at clock rates above 100 terahertz. The observed sub-femtosecond rise of energy transfer from the field to the material (for a peak electric field strength exceeding 2.5 volts per ångström) in turn indicates the viability of petahertz-bandwidth metrology with a solid-state device.

Ultrafast dynamics. Attosecond band-gap dynamics in silicon.

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.

Nonadiabatic generation of coherent phonons.

The time-dependent density functional theory (TDDFT) is the leading computationally feasible theory to treat excitations by strong electromagnetic fields. Here the theory is applied to coherent optical phonon generation produced by intense laser pulses. We examine the process in the crystalline semimetal antimony (Sb), where nonadiabatic coupling is very important. This material is of particular interest because it exhibits strong phonon coupling and optical phonons of different symmetries can be observed. The TDDFT is able to account for a number of qualitative features of the observed coherent phonons, despite its unsatisfactory performance on reproducing the observed dielectric functions of Sb. A simple dielectric model for nonadiabatic coherent phonon generation is also examined and compared with the TDDFT calculations.