Megahertz cycling of ultrafast structural dynamics enabled by nanosecond thermal dissipation

Abstract

Light–matter interactions are of fundamental scientific and technological interest. Ultrafast electron microscopy and diffraction with combined femtosecond-nanometer resolution elucidate the laser-induced dynamics in structurally heterogeneous systems. These measurements, however, remain challenging due to the brightness limitation of pulsed electron sources, leading to an experimental trade-off between resolution and contrast. Larger signals can most directly be obtained by higher repetition rates, which, however, are typically limited to a few kilohertz by the thermal relaxation of thin material films. Here, we combine nanometric electron beam probing with sample support structures tailored to facilitate rapid specimen cooling. Optical cycling of a charge-density wave transformation enables quantifying the mean temperature increase induced by pulsed laser illumination. Varying the excitation fluence and repetition rate, we gauge the impact of excitation confinement and efficient dissipation on the heat diffusion in different sample designs. In particular, a thermally optimized support can dissipate average laser intensities of up to 200 μW/μm2 within a few nanoseconds, allowing for reversible driving and probing of the CDW transition at a repetition rate of 2 MHz. Sample designs tailored to ultrafast measurement schemes will thus extend the capabilities of electron diffraction and microscopy, enabling high-resolution investigations of structural dynamics.