Dynamical diffraction formalism for imaging time-dependent diffuse scattering from coherent phonons with Dark-Field X-ray Microscopy

TL;DR

This paper introduces a dynamical diffraction formalism for Dark-Field X-ray Microscopy that enables frequency-resolved imaging of coherent phonon decay in bulk materials, overcoming previous resolution limits.

Contribution

It develops a new theoretical approach using Takagi-Taupin formalism to study time-dependent diffuse scattering from phonons with DFXM, enhancing frequency and spatial resolution.

Findings

Demonstrates how to observe long-lived intensity oscillations in phonon dynamics.

Establishes spatial and reciprocal space resolution limits for DFXM phonon studies.

Proposes experimental strategies for optimizing phonon excitation and detection.

Abstract

Coherent acoustic phonons, whose damping sets the upper bound of quality factors in acoustic resonators, play a critical role in advanced telecommunication and quantum information technologies. Yet, probing their decay in the GHz regime remains challenging using conventional surface-based techniques. Dark-field X-ray microscopy (DFXM) offers a solution by enabling through-depth, non-destructive and full-field imaging of strain fields and dislocations inside bulk materials with high spatial and angular resolution. We previously used kinematic diffraction theory to describe DFXM signals based on how the Bragg peak shifts due to the strain wave, allowing us to reconstruct the frequency spectrum of coherent phonons as a function of depth through the sample. The approach of tracking the Bragg peak shifts to study phonon dynamics, however, places an upper-bound to the highest phonon frequency that can be studied, determined by the spatial resolution of the measurement. In this work, we discuss how coherent phonon dynamics can be studied with DFXM from time-dependent intensity oscillation sidebands. This approach simultaneously allows studying coherent phonon dynamics in real and reciprocal space, overcoming frequency resolution limits imposed by the real-space resolution of Bragg-peak tracking. Using Takagi-Taupin dynamical diffraction formalism, we establish the spatial and reciprocal space resolution achievable for studying the coherent phonon dynamics and evaluate conditions for observing long-lived intensity oscillations. We close by proposing experimental strategies to optimize excitation bandwidths and reciprocal-space selectivity. The formalism in the paper enables the design of DFXM experiments for quantitative, frequency-resolved measurements of acoustic phonon decay and phonon-defect interactions in bulk crystalline materials.