Ever since Ernest Rutherford first scattered α-particles from gold foils1, collision experiments have revealed unique insights into atoms, nuclei, and elementary particles2. In solids, many-body correlations also lead to characteristic resonances3, called quasiparticles, such as excitons, dropletons4, polarons, or Cooper pairs. Their structure and dynamics define spectacular macroscopic phenomena, ranging from Mott insulating states via spontaneous spin and charge order to high-temperature superconductivity5. Fundamental research would immensely benefit from quasiparticle colliders, but the notoriously short lifetimes of quasiparticles6 have challenged practical solutions. Here we exploit lightwave-driven charge transport7–24, the backbone of attosecond science9–13, to explore ultrafast quasiparticle collisions directly in the time domain: A femtosecond optical pulse creates excitonic electron–hole pairs in the layered dichalcogenide tungsten diselenide while a strong terahertz field accelerates and collides the electrons with the holes. The underlying wave packet dynamics, including collision, pair annihilation, quantum interference and dephasing, are detected as light emission in high-order spectral sidebands17–19 of the optical excitation. A full quantum theory explains our observations microscopically. This approach opens the door to collision experiments with a broad variety of complex quasiparticles and suggests a promising new way of sub-femtosecond pulse generation.
As conventional electronics is approaching its ultimate limits1, nanoscience has urgently sought for novel fast control concepts of electrons at the fundamental quantum level2. Lightwave electronics3 – the foundation of attosecond science4 – utilizes the oscillating carrier wave of intense light pulses to control the translational motion of the electron’s charge faster than a single cycle of light5–15. Despite being particularly promising information carriers, the internal quantum attributes of spin16 and valley pseudospin17–19 have not been switchable on the subcycle scale20–21. Here we demonstrate lightwave-driven changes of the valley pseudospin and introduce distinct signatures in the optical read out. Photogenerated electron–hole pairs in a monolayer of tungsten diselenide are accelerated and collided by a strong lightwave. The emergence of high odd-order sidebands and anomalous changes in their polarization direction directly attest to the ultrafast pseudospin dynamics. Quantitative computations combining density-functional theory with a non-perturbative quantum many-body approach assign the polarization of the sidebands to a lightwave-induced change of the valley pseudospin and confirm that the process is coherent and adiabatic. Our work opens the door to systematic valleytronic logic at optical clock rates.
Intense multiterahertz fields of order megavolts per centimeter are used to coherently promote optically dark and dense paraexcitons in Cu2O from the 1s into the 2p state. The nonlinear field response of the intraexcitonic degrees of freedom is directly monitored in the time domain via ultrabroadband electro-optic sampling. The experimental results are analyzed with a microscopic many-body theory, identifying up to two internal Rabi cycles. The effects of population inversion and ponderomotive contributions are disentangled.
An experiment-theory comparison is presented to demonstrate terahertz-induced extreme-nonlinear transients in a GaAs/AlGaAs quantum-well system. The terahertz-pump and optical-probe experiments show pronounced spectral modulations of the light- and heavy-hole excitonic resonances. Excellent agreement with the results of microscopic many-body calculations is obtained, identifying clear ponderomotive contributions and the generation of terahertz harmonics.
Detailed electronic many-body configurations are extracted from quantitatively measured time-resolved nonlinear absorption spectra of resonantly excited GaAs quantum wells. The microscopic theory assigns the observed spectral changes to a unique mixture of electron-hole plasma, exciton, and polarization effects. Strong transient gain is observed only under cocircular pump-probe conditions and is attributed to the transfer of pump-induced coherences to the probe.
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