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X-ray free-electron laser based dark-field X-ray microscopy - a simulation-based study

MetadataDetails
Publication Date2022-01-19
JournalJournal of Applied Crystallography
AuthorsTheodor S. Holstad, Trygve Magnus Réder, Mads Carlsen, Erik Knudsen, Leora E. Dresselhaus‐Marais
InstitutionsTechnical University of Denmark, SLAC National Accelerator Laboratory
Citations12
AnalysisFull AI Review Included

Technical Documentation & Analysis: Ultrafast DFXM in Diamond

Section titled “Technical Documentation & Analysis: Ultrafast DFXM in Diamond”

This document analyzes the research paper “X-ray free-electron laser based dark-field X-ray microscopy: a simulation-based study” and outlines how 6CCVD’s advanced MPCVD diamond materials and customization services are essential for replicating and extending this cutting-edge research in ultrafast dynamics.


This simulation study validates the feasibility of using Dark-Field X-ray Microscopy (DFXM) combined with X-ray Free-Electron Lasers (XFEL) and a pump-probe scheme to visualize phonon dynamics (strain waves) in single crystal diamond (SCD).

  • Core Achievement: Numerical demonstration that single-pulse DFXM imaging of longitudinal strain waves in SCD is feasible using LCLS/XCS specifications.
  • Time Resolution Breakthrough: The proposed methodology enables a potential nine orders of magnitude improvement in time resolution, moving DFXM from milliseconds to the femtosecond regime (35 fs pulse duration).
  • Material Requirement: The experiment relies critically on high-quality, precisely oriented SCD substrates coated with a specific Ti/Au metalization stack to generate the strain wave via laser heating.
  • Strain Sensitivity: Simulations show visibility of strain pulses with a maximum amplitude of approximately 4 x 10-4.
  • Future Applications: Opens the door to studying ultrafast phenomena such as strain wave interaction with defects (dislocations, twin walls), rapid material failure, and diffusionless phase transformations.
  • 6CCVD Value Proposition: 6CCVD is uniquely positioned to supply the required high-purity, low-mosaic Optical Grade SCD substrates with precise custom metalization (Ti/Au) and crystallographic orientation.

The following hard data points were extracted from the simulation parameters for the proposed XFEL-based DFXM experiment:

ParameterValueUnitContext
Sample MaterialDiamond Single CrystalN/ASCD Substrate
Sample Dimensions0.6 x 1 x 2mmRequired size for simulation
Metalization (Adhesion)15nmTi (Titanium) adhesion layer
Metalization (Heating)600nmAu (Gold) heating layer
XFEL Photon Energy10keVLCLS/XCS Instrument specification
XFEL Pulse Duration35fsUltrafast probe pulse duration
Pump Laser Pulse Duration100fsOptical laser heating pulse
Pump Laser Wavelength800nmUsed for thermal excitation
Pump Laser Fluence0.8J cm-2Energy density on Au film
Maximum Strain Magnitude4 x 10-4N/AAmplitude of simulated strain pulse
Diamond Sound Speed (cs)18km s-1Longitudinal sound wave velocity
Objective Magnification (M)27.9N/AX-ray objective (CRL)
Detector Pixel Size (Effective)466 x 664nmIn the observation plane

The simulation demonstrates a successful pump-probe DFXM experiment based on the following critical steps and material parameters:

  1. Substrate Selection: Use of a high-quality Single Crystal Diamond (SCD) with (110), (110), and (001) facets, specifically oriented for Bragg scattering from the {111} planes (2Ξ0 = 35.04°).
  2. Surface Preparation: The (110) facet is coated with a bilayer metal stack: a 15 nm Titanium (Ti) adhesion layer followed by a 600 nm Gold (Au) layer.
  3. Strain Wave Generation (Pump): A 100 fs optical laser pulse (800 nm, 0.8 J cm-2) heats the Au film, causing impulsive thermal expansion which launches a longitudinal strain wave into the diamond crystal.
  4. Strain Wave Modeling: A one-dimensional thermomechanical model (udkm1Dsim) is used to compute the resulting temperature profile and subsequent crystal lattice dynamics.
  5. DFXM Imaging (Probe): A 35 fs XFEL pulse (10 keV) probes the crystal at picosecond time delays, generating a Bragg-scattered beam.
  6. Image Acquisition: The diffracted beam is magnified by a Compound Refractive Lens (CRL) objective (M = 27.9) and projected onto a 2D CMOS detector.
  7. Contrast Optimization: Simulations explored both geometrical optics and wave-optics formalisms, confirming that rocking-type weak-beam contrast provides the clearest visualization of the strain wave profile.

6CCVD is an expert supplier of MPCVD diamond materials and custom fabrication services, perfectly aligned to meet the stringent requirements of XFEL-based DFXM experiments. We provide the foundational materials necessary to transition these simulations into successful experimental reality.

To replicate or extend this research, the following 6CCVD materials are required:

Research Requirement6CCVD Material RecommendationTechnical Rationale
High-Purity SubstrateOptical Grade Single Crystal Diamond (SCD)Essential for minimizing intrinsic defects (e.g., nitrogen vacancies) and achieving the low mosaic spread (simulated at 200 ”rad) necessary for precise Bragg condition alignment.
Ultrafast Strain GenerationCustom Metalized SCDThe Ti/Au stack is critical. 6CCVD provides high-adhesion, uniform metalization layers (15 nm Ti / 600 nm Au) directly onto the specified SCD facet.
Future High-Energy ApplicationsHeavy Boron-Doped Diamond (BDD)For experiments requiring conductive substrates or alternative pump-probe mechanisms, BDD offers robust electrical and thermal properties.

The success of this DFXM technique hinges on precise material engineering and alignment, areas where 6CCVD excels:

  • Custom Dimensions & Orientation: The paper specifies a 0.6 x 1 x 2 mm sample with specific facets ((110), (110), (001)). 6CCVD offers custom laser cutting and shaping of SCD plates up to 125mm, ensuring the exact dimensions and crystallographic orientation required for goniometer mounting and Bragg geometry.
  • Advanced Metalization Services: We offer in-house deposition of the exact Ti/Au bilayer stack used for the thermal pump mechanism. Our capabilities include Au, Pt, Pd, Ti, W, and Cu metalization, allowing researchers to explore different adhesion layers or heating materials.
  • Ultra-Smooth Surface Finish: DFXM requires minimal surface interference. 6CCVD guarantees Ra < 1 nm polishing on SCD, ensuring optimal optical laser absorption and minimizing scattering noise in the X-ray probe beam.
  • Thickness Control: We provide SCD substrates with precise thickness control from 0.1 ”m up to 500 ”m, allowing researchers to optimize the X-ray penetration depth and Field of View (FoV) for specific XFEL energies.

6CCVD’s in-house PhD team specializes in the material science of diamond for extreme environments and advanced optics. We can assist researchers in:

  • Material Selection: Optimizing SCD grade (e.g., low nitrogen, low birefringence) for specific XFEL beamline parameters (e.g., 10 keV X-rays).
  • Metalization Recipe Development: Fine-tuning adhesion and heating layer thicknesses for optimal strain wave amplitude and longevity.
  • Crystallographic Alignment: Ensuring precise facet cutting and orientation necessary for complex Bragg scattering geometries (e.g., {111} reflection).

For custom specifications or material consultation, visit 6ccvd.com or contact our engineering team directly.

View Original Abstract

Dark-field X-ray microscopy (DFXM) is a nondestructive full-field imaging technique providing three-dimensional mapping of microstructure and local strain fields in deeply embedded crystalline elements. This is achieved by placing an objective lens in the diffracted beam, giving a magnified projection image. So far, the method has been applied with a time resolution of milliseconds to hours. In this work, the feasibility of DFXM at the picosecond time scale using an X-ray free-electron laser source and a pump-probe scheme is considered. Thermomechanical strain-wave simulations are combined with geometrical optics and wavefront propagation optics to simulate DFXM images of phonon dynamics in a diamond single crystal. Using the specifications of the XCS instrument at the Linac Coherent Light Source as an example results in simulated DFXM images clearly showing the propagation of a strain wave.