Ultrafast magnetic scattering on ferrimagnets enabled by a bright Yb-based soft x-ray source
G. Fan, Katherine Légaré, Vincent Cardin, Xinhua Xie, Reza Safaei, Edgar Kaksis, G. Andriukaitis, A. Pugžlys, Bruno E. Schmidt, Jean‐Pierre Wolf, M. Hehn, G. Malinowski, Boris Vodungbo, Emmanuelle Jal, J. Lüning, Nicolas Jaouen, Gaia Giovannetti, Francesca Calegari, Zhensheng Tao, Andrius Baltuška, François Légaré, Tadas Balčiūnas
Abstract
Development of ultrafast table-top x-ray sources that can map various spin, orbital, and electronic configurations and reordering processes on their natural time and length scales is an essential topic for modern condensed matter physics as well as ultrafast science. In this work, we demonstrate spatiotemporally resolved resonant magnetic scattering (XRMS) to probe the inner-shell 4d electrons of a rare-earth (RE) composite ferrimagnetic system using a bright <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mo>></mml:mo> </mml:mrow> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mn>200</mml:mn> </mml:mrow> </mml:mrow> <mml:mspace width="thickmathspace"/> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mi mathvariant="normal">e</mml:mi> <mml:mi mathvariant="normal">V</mml:mi> </mml:mrow> </mml:mrow> </mml:math> soft x-ray high harmonic generation (HHG) source, which is relevant for future energy-efficient, high-speed spintronic applications. The XRMS is enabled by direct driving of the HHG process with power-scalable, high-energy Yb laser technology. The optimally phase-matched broadband plateau of the HHG offers a record photon flux ( <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mo>></mml:mo> </mml:mrow> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mn>2</mml:mn> </mml:mrow> </mml:mrow> <mml:mo>×</mml:mo> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mn>1</mml:mn> </mml:mrow> </mml:mrow> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:msup> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mn>0</mml:mn> </mml:mrow> </mml:mrow> <mml:mn>9</mml:mn> </mml:msup> </mml:mrow> <mml:mspace width="thickmathspace"/> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mi mathvariant="normal">p</mml:mi> <mml:mi mathvariant="normal">h</mml:mi> <mml:mi mathvariant="normal">o</mml:mi> <mml:mi mathvariant="normal">t</mml:mi> <mml:mi mathvariant="normal">o</mml:mi> <mml:mi mathvariant="normal">n</mml:mi> <mml:mi mathvariant="normal">s</mml:mi> </mml:mrow> </mml:mrow> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mo>/</mml:mo> </mml:mrow> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mi mathvariant="normal">s</mml:mi> </mml:mrow> </mml:mrow> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mo>/</mml:mo> </mml:mrow> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mn>1</mml:mn> </mml:mrow> </mml:mrow> <mml:mi mathvariant="normal">%</mml:mi> </mml:math> bandwidth) with excellent spatial coherence and covers the entire resonant energy range of RE’s <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:msub> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mi mathvariant="normal">N</mml:mi> </mml:mrow> </mml:mrow> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mn>4</mml:mn> <mml:mo>,</mml:mo> <mml:mn>5</mml:mn> </mml:mrow> </mml:msub> </mml:mrow> </mml:math> edges. We verify the underlying physics of our x-ray generation strategy through the analysis of microscopic and macroscopic processes. Using a CoTb alloy as a prototypical ferrimagnetic system, we retrieve the spin dynamics, and resolve a fast demagnetization time of <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mn>500</mml:mn> </mml:mrow> </mml:mrow> <mml:mspace width="thickmathspace"/> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mo>±</mml:mo> </mml:mrow> </mml:mrow> <mml:mspace width="thickmathspace"/> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mn>126</mml:mn> </mml:mrow> </mml:mrow> <mml:mspace width="thickmathspace"/> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mi mathvariant="normal">f</mml:mi> <mml:mi mathvariant="normal">s</mml:mi> </mml:mrow> </mml:mrow> </mml:math> , concomitant with an expansion of the domain periodicity, corresponding to a domain wall velocity of <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mo>∼</mml:mo> </mml:mrow> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mn>750</mml:mn> </mml:mrow> </mml:mrow> <mml:mspace width="thickmathspace"/> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mi mathvariant="normal">m</mml:mi> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mo>/</mml:mo> </mml:mrow> <mml:mi mathvariant="normal">s</mml:mi> </mml:mrow> </mml:mrow> </mml:math> . The results confirm that, far from cross-contamination of low-energy absorption edges in multi-element systems, the highly localized states of <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mn>4</mml:mn> <mml:mi mathvariant="normal">d</mml:mi> </mml:mrow> </mml:mrow> </mml:math> electrons associated with the <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"> <mml:msub> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mi mathvariant="normal">N</mml:mi> </mml:mrow> </mml:mrow> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mn>4</mml:mn> <mml:mo>,</mml:mo> <mml:mn>5</mml:mn> </mml:mrow> </mml:mrow> </mml:msub> </mml:math> edges can provide high-quality core-level magnetic information on par with what can be obtained at the <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mi mathvariant="normal">M</mml:mi> </mml:mrow> </mml:mrow> </mml:math> edges, which is currently accessible only at large-scale x-ray facilities. The analysis also indicates the rich material-, composition-, and probing-energy-dependent driving mechanism of RE-associated multicomponent systems. Considering the rapid emergence of high-power Yb lasers combined with novel nonlinear compression technology, this work indicates potential for next-generation high-performance soft x-ray HHG-based sources in future extremely photon-hungry applications on the table-top scale, such as probing electronic motion in biologically relevant molecules in their physiological environment (liquid phase), and advanced coherent imaging of nano-engineered devices with <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mn>5</mml:mn> </mml:mrow> </mml:mrow> <mml:mo>∼</mml:mo> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mn>8</mml:mn> </mml:mrow> </mml:mrow> <mml:mspace width="thickmathspace"/> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mi mathvariant="normal">n</mml:mi> <mml:mi mathvariant="normal">m</mml:mi> </mml:mrow> </mml:mrow> </mml:math> resolution.