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Study of carrier transport in MAterials by time-Resolved specTroscopy with ultrashort soft X-ray light

Periodic Reporting for period 2 - SMART-X (Study of carrier transport in MAterials by time-Resolved specTroscopy with ultrashort soft X-ray light)

Période du rapport: 2022-03-01 au 2024-08-31

The challenge of generating efficient, clean, and secure renewable energy is a significant issue facing humanity in the 21st century, identified as a priority in the European Horizon 2020 initiative. The SMART-X doctoral network was established to train scientists in advanced X-ray ultrafast spectroscopy to explore charge carrier dynamics in new materials for energy applications, involving collaboration across seven European countries. This multidisciplinary approach enhances researchers' career prospects by providing them with diverse skills through partnerships with top academic institutions and high-tech companies.
The SMART-X project focused on advancing ultrafast X-ray spectroscopy to analyze electron transport and dynamics, which are vital for developing more efficient solar energy solutions, while also exploring the topological properties of low-dimensional materials for potential applications in nanoelectronics.
SMART-X has made notable progress in ultrafast X-ray spectroscopy by developing new tools and techniques that enhance the understanding of material science. The network has achieved significant advancements in various areas, including the fabrication of high-quality topological Dirac semimetals, the exploration of metal-halide perovskite semiconductors for improved optoelectronic properties, and the refinement of theoretical methods to study ultrafast processes in biological and chemical systems. Additionally, innovations such as the development of tabletop soft X-ray sources and high-speed detection technologies have facilitated high-precision experiments in ultrafast science, culminating in over 70 publications in peer-reviewed journals.
The SMART-X project has been a collaborative initiative focused on enhancing ultrafast X-ray spectroscopy techniques and their applications in materials science, encompassing advancements in methodology, technology, and significant scientific findings across various materials, including perovskites, Dirac semimetals, and organic polymers.
The project has led to notable developments in laser technology for XUV and X-ray ultrafast spectroscopy, particularly through advancements in High Harmonic Generation (HHG). At the Institut de Ciències Fotòniques (ICFO), researchers generated soft X-rays using high-energy pulses, facilitating time-resolved experiments that improved understanding of ultrafast electron dynamics. Similarly, a transient X-ray absorption apparatus developed at Forschungsverbund Berlin e.V. (FVB-MBI) using a Ti:Sapphire laser system, enabled the investigation of various ultrafast dynamics with a broad soft X-ray spectrum.
Efforts to use mid-infrared pumps and soft X-ray probes at the Consiglio Nazionale delle Ricerche (CNR) aimed to study materials like Weyl semimetals and perovskites, achieving high harmonics that enabled detailed transient spectroscopy. At FASTLITE, substantial improvements were made in table-top coherent soft X-ray sources, increasing their competitiveness with larger facilities, and achieving stable carrier-envelope-phase pulses essential for extended experiments. Meanwhile, GREATEYES contributed by creating advanced CMOS-based detectors, including a prototype sCMOS camera, enhancing data acquisition capabilities.
The project also investigated fundamental processes in materials through theoretical and experimental methods. The Centre National de la Recherche Scientifique (CNRS) explored post-collision interactions in Auger spectroscopy, while studies on charge transfer mechanisms in thiophene-based polymers advanced understanding of ultrafast electron dynamics. Elettra Sincrotrone Trieste (ELETTRA) focused on the dynamics of perovskites and developed super-resolution microscopy techniques in the EUV range.

In addition to material investigations, theoretical modeling led by groups at Stockholm University (SU) and the Max-Planck-Gesellschaft zur Förderung der Wissenschaften (MPG) explored ultrafast processes in various systems. This included work on charge transfer dynamics, non-adiabatic processes involving conical intersections, and research into attosecond magnetization dynamics, which revealed notable spin phenomena in non-magnetic materials.
Overall, the SMART-X project significantly advanced the field of ultrafast X-ray spectroscopy, laying the groundwork for future explorations of complex materials and ultrafast processes. Each participating institution contributed to a more comprehensive understanding of electron dynamics, paving the way for novel applications in electronics, energy materials, and beyond.
The SMART-X project has significantly advanced ultrafast X-ray spectroscopy, developing innovative techniques and tools that have pivotal implications for materials science. Key achievements include advancements in high-energy tabletop soft X-ray sources and methodologies, allowing for enhanced experimental precision without reliance on large-scale facilities. For instance, Fastlite's development of an optical parametric chirped-pulse amplifier (OPCPA) has led to stable, high-precision experiments in ultrafast science, enabling effective High Harmonic Generation (HHG) and isolating single X-ray bursts for probing electron dynamics.
Collaborative efforts at the CNR resulted in a broadband XUV source aimed at investigating ultrafast material dynamics, with significant developments in transient absorption spectroscopy geared toward materials such as perovskites. The initial benchmarking of the beamline with silicon provides foundational insights into carrier-lattice interactions. Biegert's team at ICFO has also made strides in table-top X-ray sources for an array of ultrafast dynamics investigations, successfully applying attosecond X-ray absorption spectroscopy to study materials like titanium diselenide.
In addition to spectroscopy innovations, the project tackled advanced materials fabrication, with NCSRD achieving high-quality growth of topological Dirac semimetals and IIT enhancing the understanding of metal-halide perovskite semiconductors. These efforts have culminated in improved optoelectronic properties via controlled defect chemistry and thin-film processes.
Theoretical methods advanced under the SMART-X umbrella have also been crucial, with Kowalewski’s group innovating in soft X-ray spectroscopic techniques to probe ultrafast non-adiabatic processes, while Odelius' team focused on modeling charge transfer dynamics in solution, illuminating the intricacies of ultrafast molecular reactions.
Furthermore, significant strides were made in high-speed X-ray detection; GREATEYES developed prototype sCMOS cameras that offer superior quantum efficiency and energy resolution, further enhancing the capabilities of X-ray spectroscopy.
Overall, the SMART-X project not only deepened our understanding of ultrafast processes in diverse materials but also solidified international collaborations that enhanced knowledge dissemination. The training of 15 PhD students has ensured a sustainable scientific framework, with more than 70 published papers and presentations at leading conferences, marking substantial contributions to the field. These advancements hold promise for future applications in energy conversion, optoelectronics, and molecular electronics, underscoring the project's impact on advancing ultrafast spectroscopy.
some of SMART-X ESRs at the second network symposium