Transient lensing from a photoemitted electron gas imaged by ultrafast electron microscopy.

Understanding and controlling ultrafast charge carrier dynamics is of fundamental importance in diverse fields of (quantum) science and technology. Here, we create a three-dimensional hot electron gas through two-photon photoemission from a copper surface in vacuum. We employ an ultrafast electron microscope to record movies of the subsequent electron dynamics on the picosecond-nanosecond time scale. After a prompt Coulomb explosion, the subsequent dynamics is characterized by a rapid oblate-to-prolate shape transformation of the electron gas, and periodic and long-lived electron cyclotron oscillations inside the magnetic field of the objective lens. In this regime, the collective behavior of the oscillating electrons causes a transient, mean-field lensing effect and pronounced distortions in the images. We derive an analytical expression for the time-dependent focal length of the electron-gas lens, and perform numerical electron dynamics and probe image simulations to determine the role of Coulomb self-fields and image charges. This work inspires the visualization of cyclotron dynamics inside two-dimensional electron-gas materials and enables the elucidation of electron/plasma dynamics and properties that could benefit the development of high-brightness electron and X-ray sources.

Multidimensional Large Amplitude Dynamics in the Pyridine-Water Complex.

Aqueous pyridine plays an important role in a variety of catalytic processes aimed at harnessing solar energy. In this work, the pyridine-water interaction is studied by microwave spectroscopy and density functional theory calculations. Water forms a hydrogen bond to the nitrogen with the oxygen tilted slightly toward either of the ortho-hydrogens of the pyridine, and a tunneling motion involving in-plane rocking of the water interconverts the resulting equivalent structures. A pair of tunneling states with severely perturbed rotational spectra is identified and their energy separation, ΔE, is inferred from the perturbations and confirmed by direct measurement. Curiously, values of ΔE are 10404.45 and 13566.94 MHz for the H2O and D2O complexes, respectively, revealing an inverted isotope effect upon deuteration. Small splittings in some transitions suggest an additional internal motion making this complex an interesting challenge for theoretical treatments of large amplitude motion. The results underscore the significant effect of the ortho-hydrogens on the intermolecular interaction of pyridine.