Advanced EUV/soft X-ray microscopy in the ultrafast regime: imaging functionality of nanomaterials across length scales

Project Information

ULTRAIMAGE

Grant agreement ID: 851154

DOI

10.3030/851154

EC signature date 12 September 2019

Start date 1 June 2021

End date 31 May 2027

Funded under

• EXCELLENT SCIENCE - European Research Council (ERC)

Total cost

€ 1 894 577,00

EU contribution

€ 1 894 577,00

Coordinated by

UNIVERSITA DEGLI STUDI DI PAVIA
Italy

Periodic Reporting for period 3 - ULTRAIMAGE (Advanced EUV/soft X-ray microscopy in the ultrafast regime: imaging functionality of nanomaterials across length scales)

Reporting period: 2024-06-01 to 2025-11-30

Summary of the context and overall objectives of the project

With technology miniaturization, novel materials with functionality activated by light pulses are engineered in the deep nanoscale regime, where bulk macroscopic models can no longer accurately predict heat, charge or spin transport. As a result, smart-materials design represents a complex task. To address this challenge, there is a critical need for new techniques that can image nanoscale processes with high spatial and temporal resolutions, while light-activated functionality occurs, to enable a better understanding of fundamental nanoscale behaviour.

The goal of ULTRAIMAGE is to obtain nanoscale movies of nanostructures’ impulsive response, irradiated by ultrafast laser pulses with extremely high fidelity and in a non-destructive approach, with sub-20nm transverse resolution, 0.5Å axial precision, and ≈10fs temporal resolution. Key to this achievement is the implementation of a unique capability in microscopy, with resolution on nanometer-to-Ångstrom length and femtosecond time scales. This advance is possible through the combination of extreme ultraviolet (EUV) to soft X-ray tabletop coherent light sources with ptychography, a technique for coherent diffractive imaging in which multiple diffraction patterns from overlapping fields of view are processed by iterative algorithms to recover amplitude and phase images of sample and beam, separately.

The proposed research will enable a better understanding of emergent phenomena in soft matter and of fundamental nanoscale behavior, vital to the engineering of next-generation sustainable and cost-effective devices.

Work performed from the beginning of the project to the end of the period covered by the report and main results achieved so far

Scientific and Technical Achievements:
- We established and founded LUXEM, the Laboratory for Ultrafast X-ray and Electron Microscopy. We recruited personnel to the project.
- We carried out the green-field design and implementation of the infrastructure in collaboration with the Department and the HI logistics management. We took care that all technical requirements of the infrastructure, relevant to the project, were faithfully implemented.
- We installed and validated the ultrafast laser and the High-Harmonic Generation (HHG) EUV/soft X-ray source. Fine tuning and optimization are continuously ongoing to adapt the technology to the scientific requirements and objectives of ULTRAIMAGE.
- We carried out an in-depth technology scouting of every single technological component of the experiment, accompanied by extensive simulations and collaboration with industrial partners to achieve custom elements and performances specifically tailored to the scientific objectives of ULTRAIMAGE. This included – among the many – vacuum supplies, EUV optics, HHG and laser technology.
- We purchased and assembled all customs part, we working on a robust automation of the entire apparatus and commissioning it
- We fostered collaboration with the FERMI free-electron laser, through expeditions (beamtimes) that led to pioneering demonstration: the possibility to use of ultrafast XUV ptychography to disentangle the response from chiral compounds and for plasmonic response in nanostructures.
- We established sample provision in a modular approach to their microscopy, with our strategic partners at ETHZ (CH).
- We established a local collaboration with key medical imaging stakeholders at the HI. This platform allows us to develop new (mid and longer-term) possibilities, e.g. real-time imaging of photo-blasting of cancer cells bound to ligated nanoparticles.
- In parallel, we developed a network of international collaboration to guarantee knowledge transfer and implement the action described in WP1. Specifically: 1) Collaboration with the Colorado School of Mines (USA) for the development of ptychographic image reconstruction algorithms; 2) Collaboration with IMDEA Nanociencia (Spain) to carry out the ray-tracing simulations relying on our source parameters. This allowed to: (i) select the optical layout of the microscope, (iii) select the piezo-actuated stages for full in-vacuum automation; (iii) select the detector technology and its actuation; 3) Collaboration with LACUS – EPFL (Switzerland), where a complementary HHG source is available. Technology exchange was fostered by sending our personnel for short-term training periods.
- We were able to consolidate at both National and International levels the impact and relevance of research implemented by ULTRAIMAGE, attracting the collaboration of strategic partners in EUV mirrors fabrication and metrology (Europe, Asia, USA), sample providers (Switzerland). Furthermore, this ERC grant enabled the P.I. to further consolidate her research group, LUXEM, participating in dedicated national funding initiatives to secure funding for projects spinning off the main ERC ULTRAIMAGE. Consequently, an additional Laboratory space in the Physics Department was allocated to LUXEM’s research, to further the implementation and expand the purpose of ULTRAIMAGE.

Dissemination & Communication Achievements:
- We established a cohesive communication platform composed of project and group identity, with associated website, and social networks (LinkedIn and Instagram). These platforms are periodically monitored and kept up-to-date to share the latest events from the project with different stakeholders (scientific community, young researchers, general public & policy makers). We contributed to the partner company's (Dectris) blog with a dedicated article and got ULTRAIMAGE research highlighted in a top national Italian Newspaper, Il Sole24Ore.
- We actively participated in a host of STEM education events with exhibitions and seminars, interviews and videos, i.e. the “European Researchers Night”, "Sumo-Science", “Stati Generali of Regione Lombardia”, “Incontri di Fisica Moderna”, “Fix the Leaky Pipeline: equality in science”, “International Day of Light 2024“, with the aim of consolidating the new ultrafast laser science platform promoted by ULTRAIMAGE via LUXEM in the context of the HI and at the Regional, National and International Levels. Participation to public events was successfully selected to target different stakeholders: scientific community, young researchers, civil society, and policy makers.
- We were invited/participated to Schools and International Conferences to promote our research, our results, and to foster networking with peers. This led to the foundation of a Consortium of Correlative Ultrafast Imaging Methods, which now bridges academic, research and industry partners across 3 continents. This consortium collaborates to achieve: i) characterization of heterogeneity, interfaces, disorder in nanostructured matter; ii) observation of its at & beyond-equilibrium dynamics; iii) prototyping cutting-edge methods and products that can be made available to the public.

The Action was amended to the University of Pavia with starting date 01.06.2021. In the context of the Physics Department at the University of Pavia, Ultrafast Laser Science and – in particular – Ultrafast Microscopy, entered as an entirely brand new research line and did not rely on any pre-existing infrastructure facility nor local network for recruitment. Because of the commitment and dedication of the P.I. the quality of recruited LUXEM Team members, and the unique synergy between LUXEM, the Department of Physics (management, administration, logistics, workshops), the Logistics service of the HI it was possible to achieve all of the above in only 30 months and from the grounds of a complete green-field development.

Progress beyond the state of the art and expected potential impact (including the socio-economic impact and the wider societal implications of the project so far)

The outcome of ULTRAIMAGE is ground-breaking broad impact in fundamental science and in technology in terms of unraveling unprecedented insights of light-activated photonic nanomaterials, and of developing advanced and highly innovative ultrafast microscopic approaches to nanoscience.

The beyond the state of the art key aspects in the ongoing research are:
- Direct visualization of electronic and structural dynamics in bottom-up engineered 2D superlattices.
- Simultaneous observation the short and medium range fundamental structure-properties relationships in a host of photonics systems.
- Better understanding of fundamental nanoscale behaviour in systems too complex to be modeled from first principles.
- Application of cutting-edge techniques of ptychographic coherent diffractive imaging to the ultrafast regime –for the first time with 13nm light–.
- Creation of one of the first laboratories in Europe for the characterisation of functional materials from the nano- to the meso-scale, with Å-to-nm spatial and fs-to as time resolution, further fostered by the synergy with electron-based diffraction and imaging techniques, under development at LUXEM (Laboratory for Ultrafast X-Ray and Electron Microscopy, P.I. G.F.Mancini) or available at the Host Institution (University of Pavia).

All these milestones are being successfully pursued in full compliance with the aims and the overall expected results until the end of the project. ULTRAIMAGE tackles the need for novel strategies in characterisation of functional materials, through the study of their fundamental structure-property relationships. Key to this advance is the development of innovative imaging modalities for functional materials with ultrahigh resolution in both time and space. The proposed line of research addresses main transformative opportunities for discovery science in: (i) mastering hierarchical architectures and beyond-equilibrium matter, (ii) understanding the critical roles of heterogeneity, interfaces, and disorder beyond ideal materials and systems, and (iii) exploiting transformative advances in imaging capabilities across multiple scales, all hot topics in physical chemistry and nano-materials science.

The highly innovative and beyond state-of-the-art of ULTRAIMAGE lies in its promotion of new experimental developments in ultrafast imaging, combining -for the first time- a tabletop 92eV EUV engineered source with advanced coherent diffractive imaging platforms, to visualize complementary aspects of the electronic and morphological structure of materials. Moreover, since in ptychography CDI the image-forming process starts from the collection of Nyquist-sampled diffraction patterns from the specimen, the complete landscape of sample-light interaction in both direct and reciprocal space will be retrieved in a single measurement. ULTRAIMAGE is cutting-edge from a practical and scientific point of view: i) It addresses fundamental questions about materials used in photovoltaics, sensing and electronics; ii) It comes at a time when huge investments are being made worldwide with 13nm sources for nanolithography inspection purposes; iii) It builds on a promising fast-developing experimental technique, which is unique for the study of excited state dynamics that govern functionality across many scientific disciplines.

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