Electron microscopy can visualize the structure of complex materials with atomic and subatomic resolution, but investigations of reaction dynamics and light-matter interaction call for time resolution as well, ideally on a level below the oscillation period of light. Here, we report the use of the optical cycles of a continuous-wave laser to bunch the electron beam inside a transmission electron microscope into electron pulses that are shorter than half a cycle of light. The pulses arrive at the target at almost the full average brightness of the electron source and in synchrony to the optical cycles, providing attosecond time resolution of spectroscopic features. The necessary modifications are simple and can turn almost any electron microscope into an attosecond instrument that may be useful for visualizing the inner workings of light-matter interaction on the basis of the atoms and the cycles of light.

Ultrafast transmission changes around the fundamental trion resonance are studied after exciting a 𝑝-shell exciton in a negatively charged II-VI quantum dot. The biexcitonic induced absorption reveals quantum beats between hot trion states at 133 GHz. While interband dephasing is dominated by relaxation of the 𝑃shell hole within 390 fs, trionic coherence remains stored in the spin system for 85 ps due to Pauli blocking of the triplet electron. The complex spectro-temporal evolution of transmission is explained analytically by solving the Maxwell-Liouville equations. Pump and probe polarizations provide full control over amplitude and phase of the quantum beats.

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We present an ultrafast spectroscopy system designed for temporal and spectral resolution of transient transmission changes after excitation of single electrons in solid-state quantum structures. The system is designed for optimum long-term stability, offering the option of hands-off operation over several days. Pump and probe pulses are generated in a versatile Er:fiber laser system where visible photon energies may be tuned independently from 1.90 eV to 2.51 eV in three parallel branches. Bandwidth-limited pulse durations between 100 fs and 10 ps are available. The solid-state quantum systems under investigation are mounted in a closed-cycle superconducting magnet cryostat providing temperatures down to 1.6 K and magnetic fields of up to 9 T. The free-standing cryomagnet is coupled to the laser system by means of a highbandwidth active beam steering unit to eliminate residual low-frequency mechanical vibrations of the pulse tube coolers. High-NA objective lenses inside the sample chamber are employed for focusing femtosecond laser pulses onto the sample and recollection of the transmission signal. The transmitted probe light is dispersed in a grating monochromator equipped with a liquid nitrogen-cooled CCD camera, enabling a frame rate of 559 Hz. In order to eliminate spurious background effects due to low-frequency changes in the thermal equilibrium of the sample, we operate with a lock-in scheme where, instead of the pump amplitude, the pump-probe timing is modulated. This feature is provided without any mechanical action by an electro-optic timing unit inside the femtosecond Er:fiber system. The performance of the instrument is tested with spectrally resolved pump-probe measurements on a single negatively charged CdSe/ZnSe quantum dot under a magnetic field of 9 T. Selective initialization and readout of charge and spin states is carried out via two different femtosecond laser pulses. High-quality results on subpicosecond intraband relaxation dynamics after single-electron excitation motivate a broad variety of future experiments in ultrafast quantum optics and few-fermion quantum dynamics.

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