Abstract

Modern techniques for the investigation of correlated materials in the time domain combine selective excitation in the THz frequency range with selective probing of coupled structural, electronic and magnetic degrees of freedom using x-ray scattering techniques. Cryogenic sample temperatures are commonly required to prevent thermal occupation of the low energy modes and to access relevant material ground states. Here, we present a chamber optimized for high-field THz excitation and (resonant) x-ray diffraction at sample temperatures between 5 and 500 K. Directly connected to the beamline vacuum and featuring both a Beryllium window and an in-vacuum detector, the chamber covers the full (2–12.7) keV energy range of the femtosecond x-ray pulses available at the Bernina endstation of the SwissFEL free electron laser. Successful commissioning experiments made use of the energy tunability to selectively track the dynamics of the structural, magnetic and orbital order of Ca2RuO4 and Tb2Ti2O7 at the Ru (2.96 keV) and Tb (7.55 keV) L-edges, respectively. THz field amplitudes up to 1.12 MV cm−1 peak field were demonstrated and used to excite the samples at temperatures as low as 5 K.

Highlights

  • One fundamental goal of condensed matter science is to understand and manipulate materials with functionalities that are relevant for technological applications such as high temperature superconductivity, giant magnetoresistance and insulatorto-metal transitions [1, 2]

  • The ground state a material attains under given external conditions depends on the strong interaction between magnetic, electronic and structural degrees of freedom, giving rise to complex energy potentials with multiple local minima corresponding to phases with very different macroscopic properties

  • The design remains compatible with the large x-ray photon energy range of 2–12.7 keV available at the Bernina endstation [70] of SwissFEL [38], which offers element specificity covering absorption edges ranging from M (Dy to U), L (Rb to Tl) and K (P to Se)

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Summary

Introduction

Relevant for technological applications such as high temperature superconductivity, giant magnetoresistance and insulatorto-metal transitions [1, 2]. Because of the central role atomic and electronic order plays in these materials, angle-resolved photoemission spectroscopy, neutron as well as x-ray scattering techniques have become essential tools to determine and study the rich phase diagrams of correlated materials [2,3,4,5], complementing measurement of macroscopic physical quantities. These studies are performed in the adiabatic limit, restricting direct quantitative information on the relevance of individual parameters and their coupling strength. Pioneering work has been conducted over decades with low-count photon sources, investigating coherent lattice motions and structural phase transitions [24,25,26,27,28,29,30,31,32,33]

Time-resolved x-ray diffraction at FELs
Selective excitation
Sample environment
Design concept
Sample holder for THz pump experiments
Grazing incidence sample holder
Cooling
Pump pulse focusing and diagnostics
X-ray diffraction angles
Setup performance
Magnetic and orbital melting in Ca2RuO4
Resonant excitation of a hybrid mode in Tb2Ti2O7
Conclusion
Data availability statement
Full Text
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