Fluorescence intensity correlations enable 3D imaging without sample rotations

TL;DR

This paper introduces a novel lensless 3D imaging method using fluorescence intensity correlations excited by ultrashort X-ray pulses, enabling structural analysis without sample rotation, applicable to non-periodic specimens.

Contribution

The study demonstrates that fluorescence intensity correlations can provide 3D structural information of non-periodic objects without sample rotation, overcoming limitations of traditional X-ray fluorescence imaging.

Findings

Successfully imaged 3D structures without sample rotation

Recorded multiple specimen projections from a single orientation

Confirmed fluorescence reflects real-space structural changes

Abstract

Lensless X-ray imaging provides element-specific nanoscale insights into thick samples beyond the reach of conventional light and electron microscopy. Coherent diffraction imaging (CDI) methods, such as ptychographic tomography, can recover three-dimensional (3D) nanoscale structures but require extensive sample rotation, adding complexity to experiments. X-ray elastic-scattering patterns from a single sample orientation are highly directional and provide limited 3D information about the structure. In contrast to X-ray elastic scattering, X-ray fluorescence is emitted mostly isotropically. However, first-order spatial coherence has traditionally limited nanoscale fluorescence imaging to single-crystalline samples. Here, we demonstrate that intensity correlations of X-ray fluorescence excited by ultrashort X-ray pulses contain 3D structural information of non-periodic, stationary objects. In our experiment, we illuminated a vanadium foil within a sub-200 nm X-ray laser beam focus. Without changing the sample orientation, we recorded 16 distinct specimen projections using detector regions covering different photon incidence angles relative to the X-ray free-electron laser (FEL) beam. The projections varied systematically as the fluorescing volume was translated along an astigmatism, confirming that FEL-induced fluorescence reflects real-space structural changes. Our results establish a new approach for lensless 3D imaging of non-periodic specimens using fluorescence intensity correlations, with broad implications for materials science, chemistry, and nanotechnology.