Periodic Reporting for period 3 - MORE-TEM (MOmentum and position REsolved mapping Transmission Electron energy loss Microscope)
Periodo di rendicontazione: 2024-05-01 al 2025-10-31
A major mission of condensed-matter physics is to understand material properties via the knowledge of the energy vs. momentum (q) dispersion and lifetime of fundamental excitations. Unfortunately, none of the available techniques can be applied to emerging nanomaterials. In MORE-TEM, we develop a new spectrometer enabling to map excitations q-resolved with 0.01 Å-1 resolution and q-averaged down to atomic level, at unprecedented 1 meV energy resolution and at variable temperature between 700 K and 4 K. This opens the so-far unexplored possibility to investigate dispersion and lifetime of phonons, plasmons & excitons in nanomaterials including (organic) molecules, 1D nanotubes, 2D materials, heterostructures & nanocrystals in minerals with a few nm of lateral resolution on samples as thin as an atomic monolayer. Mapping out the spatial and q-landscape of primary excitations will allow us to gain control on quantum phases, like charge-density waves and superconductivity, to engineer new materials for energy (e.g. batteries), (opto-)electronic devices in (organic) electronics, and to model the physical & chemical properties of geological systems. This will hugely impact a wide range of applications in physics, chemistry, engineering, environmental-, geo- & material science. MORE-TEM not only implements features of a large-scale facility on a cheaper table-top instrument, but it also pushes q-resolved spectroscopy to the realm of the nanoscale, providing thus a fundamentally new & unique infrastructure for the analysis of nanomaterials.
After selecting the JEOL platform for MORE-TEM. MORE-TEM I was installed in Vienna in 1.10. 2024 and upgraded to MORE-TEM II in 1.1. 2025 and will be upgraded to MORE-TEM III by the CEOS ground potential monochromator based on the design (see graphic sketch below) in Ref. 1 later this year. Till today 49 publications including 17 highlights were published and listed below:
[1] F. Börrnert, et al. Ultramicr., 253, 113805(2023)
[2] F. Macheda, et al. PRB 107, 094308 (2023)
[3] G. Marchese et al.,Nature Physics 20, 88 (2024)
[4] F. Macheda e, PRL 129, 185902 (2022)
[5] A. Siciliano, et al., PRB 107, 174307 (2023)
[6] G. Caldarelli, et al., PRB 106, 024312 (2022)
[7] T. Venanzi et al. PRL 130, 256901(2023)
[8] M. Basini et al. PRB 109, 024309(2024)
[9] M. Basini et al. Nature 628, 534(2024)
[10] J.P. Nery, F. Mauri, PRB 105, 245120 (2022)
[11] S. Mallik et al., Nat. Com. 13, 4625 (2022)
[12] F. Gabriele et al., PR Res, 4, 023112 (2022)
[13] N. Sellati et al. PRB 108, 014503(2023)
[14] W. Cui et al. Adv. Funct. Mat., 32, 2206429 (2022)
[15] J. Hong et al. ACSNano 16, 12328 (2022)
[16] Y.C. Lin et al., Nanolett. 21, 10386 (2021)
[17] R. Senga et al., Nature 603, 68 (2022)
[18] A. Guandalini et al. Nanolett. 23,11835(2023)
[19] A. Guandalini et al. PRBlett. 111, L041401(2025).
[20] C. Schuster et al.,Carbon 234, 11997(2025).
[21] C. Freytag et al.,Small Methods, 2500075(2025)
[22] C. Freytag et al,J. Phys.Chem.C Lett., 16, 4990(2025)
[23] D. de Gon et al., Adv. Opt. Mat. 2500892(2025)
[24] E. Parth et al., Nature Comm. 16, 4797(2025)
[25] YC Lin et al., Nature Comm. 5,425(2024)
[26] Q. Liu et al., ACS Nano 19, 4845(2025)
[27] R. Senga et al., Nature Nano, 20, 740(2025)
[28] M. Unzog et al., PRresearch 7, 013172(2025)
[29] A.V. Krashennikov et al. Nano Lett. 24, 12733 (2024)
[30] F. Macheda et al. PRB 110, 094306(2024)
[31] F. Macheda et al. PRB 110, 115407(2024)
[32] S. P. Villani et al. npj Comput. Mat., 10, 81(2024)
[33] P. Fachin et al PRB 110, L201405(2024)
[34] MJ. Kim et al., Sci. Adv. 10, eadi7598 (2024)
[35] A. Siciliano et al. PRB 110, 134111(2024)
[36] A. Siciliano et al. PRB 110, 144101(2024)
[37] G. Marini et al. Comp. Phys. Comm. 295, 108950(2024)
[38] L. Graziotto et al. Nano Letters 24, 186(2024)
[39] L. Graziotto et al. PRB 109, 075420(2024)
[40] A. Guandalini et al. PRB 111, 075118(2025)
[41] G. Caldarelli et al. PRB 111, 075137(2025)
[42] N. Sellati et al. Nanomat. 14, 1021(2024)
[43] J. Fiore et al. PRB 110, L060504(2024)
[44] N. Sellati et al. PRB 111, 104509(2025)
[45] F. Gabriel et al. PRB 109, 045137(2024)
[46] N. Sellati et al npj Quant. Mat. 10, 46(2025)
[47] L. Benfatto, et al. PRB 108, 134508(2023)
[48] K. Katsumi et al. PRL 132, 256903(2024)
[49] L. Maccari et al. PR. Res, 7, 013160(2025)
[1] F. Börrnert, et al. Ultramicr., 253, 113805(2023)
[2] F. Macheda, et al. PRB 107, 094308 (2023)
[3] G. Marchese et al.,Nature Physics 20, 88 (2024)
[4] F. Macheda e, PRL 129, 185902 (2022)
[5] A. Siciliano, et al., PRB 107, 174307 (2023)
[6] G. Caldarelli, et al., PRB 106, 024312 (2022)
[7] T. Venanzi et al. PRL 130, 256901(2023)
[8] M. Basini et al. PRB 109, 024309(2024)
[9] M. Basini et al. Nature 628, 534(2024)
[10] J.P. Nery, F. Mauri, PRB 105, 245120 (2022)
[11] S. Mallik et al., Nat. Com. 13, 4625 (2022)
[12] F. Gabriele et al., PR Res, 4, 023112 (2022)
[13] N. Sellati et al. PRB 108, 014503(2023)
[14] W. Cui et al. Adv. Funct. Mat., 32, 2206429 (2022)
[15] J. Hong et al. ACSNano 16, 12328 (2022)
[16] Y.C. Lin et al., Nanolett. 21, 10386 (2021)
[17] R. Senga et al., Nature 603, 68 (2022)
[18] A. Guandalini et al. Nanolett. 23,11835(2023)
[19] A. Guandalini et al. PRBlett. 111, L041401(2025).
[20] C. Schuster et al.,Carbon 234, 11997(2025).
[21] C. Freytag et al.,Small Methods, 2500075(2025)
[22] C. Freytag et al,J. Phys.Chem.C Lett., 16, 4990(2025)
[23] D. de Gon et al., Adv. Opt. Mat. 2500892(2025)
[24] E. Parth et al., Nature Comm. 16, 4797(2025)
[25] YC Lin et al., Nature Comm. 5,425(2024)
[26] Q. Liu et al., ACS Nano 19, 4845(2025)
[27] R. Senga et al., Nature Nano, 20, 740(2025)
[28] M. Unzog et al., PRresearch 7, 013172(2025)
[29] A.V. Krashennikov et al. Nano Lett. 24, 12733 (2024)
[30] F. Macheda et al. PRB 110, 094306(2024)
[31] F. Macheda et al. PRB 110, 115407(2024)
[32] S. P. Villani et al. npj Comput. Mat., 10, 81(2024)
[33] P. Fachin et al PRB 110, L201405(2024)
[34] MJ. Kim et al., Sci. Adv. 10, eadi7598 (2024)
[35] A. Siciliano et al. PRB 110, 134111(2024)
[36] A. Siciliano et al. PRB 110, 144101(2024)
[37] G. Marini et al. Comp. Phys. Comm. 295, 108950(2024)
[38] L. Graziotto et al. Nano Letters 24, 186(2024)
[39] L. Graziotto et al. PRB 109, 075420(2024)
[40] A. Guandalini et al. PRB 111, 075118(2025)
[41] G. Caldarelli et al. PRB 111, 075137(2025)
[42] N. Sellati et al. Nanomat. 14, 1021(2024)
[43] J. Fiore et al. PRB 110, L060504(2024)
[44] N. Sellati et al. PRB 111, 104509(2025)
[45] F. Gabriel et al. PRB 109, 045137(2024)
[46] N. Sellati et al npj Quant. Mat. 10, 46(2025)
[47] L. Benfatto, et al. PRB 108, 134508(2023)
[48] K. Katsumi et al. PRL 132, 256903(2024)
[49] L. Maccari et al. PR. Res, 7, 013160(2025)
Selected highlights: As a technological breakthrough CEOS will generate a new device which will be open for almost the whole community due to the goal to develop a retrofit-able monochromator [1]. The design is defined in such a way that it can be used for various types of electron microscopes and it will, in principle, be independent of the vendor of the microscope. Using q integrated EELS a breakthrough in the ability to distinguish different carbon isotopes in the TEM on the single atom level was proven [17]. The theory partner introduced the concept of atomic momentum (q) dependent effective charges ZI(q), a vector quantity associated to each atom I of the unit cell, to describe the phonon cross-section measured by EELS. Interestingly, we discovered that in presence of a strong electron scattering in Ref. [3] we used this concept to extend the definition of Born effective charges, normally used in insulators, to super and bad conducting metals and to simulate the far-IR reflectivity spectra of the extremely high-temperature superconductor, H3S, both in its normal and superconducting phase. This is a breakthrough regarding IR mode detection in metals. For EELS combining high energy and q resolution in the optical range represent a breakthrough regarding the understanding of how to disentangle different quasiparticle excitations was achieved for semiconductors such as 2D layered PdSe2 [15]. For monolayer graphene we were able to study for the first time the gap opening at low q and reveal the intrinsic fermi velocity 18]. Quasi-particle corrections and excitonic effects had to be addressed within the GW approximation and Bethe-Salpeter equation, respectively. Both are essential in the quantitative description. In addition, approaching the optical limit for the first time a vanishing loss function and the importance of kinematic effects were shown [19]. We also report new low-D structures of alkali metal bilayers intercalated in bilayer graphene with degenerated dispersion and possible applications for high-capacity battery materials [25]. An example for nanoscale IR spectroscopy using the finely focused electron beam in TEM is reported [27]. By minimizing the electron dose and damage, the successful discrimination of two different polymers has been done with the distinct vibration energies of hydrogen and deuterium.
All these highlights in the first four years show the pathway to achieve the above-mentioned final goal of the project to develop a revolutionary new research instrument as table top synchrotron combining the utmost combined energy resolution with the concomitant utmost either momentum or spatial resolution at variable temperature.
Regarding the contribution to the discussion of future science policies
PI Thomas Pichler followed in Mai 2023 an invitation to the European Parliament to showcase MORE-TEM as a best practice example of international research collaboration. A follow-up visit of the Ambassador of the EU in Japan, Jean Eric Paquet, was happening in April 2024 at the SANKEN institute of Co-PI Kazu Suenaga in Osaka.
All these highlights in the first four years show the pathway to achieve the above-mentioned final goal of the project to develop a revolutionary new research instrument as table top synchrotron combining the utmost combined energy resolution with the concomitant utmost either momentum or spatial resolution at variable temperature.
Regarding the contribution to the discussion of future science policies
PI Thomas Pichler followed in Mai 2023 an invitation to the European Parliament to showcase MORE-TEM as a best practice example of international research collaboration. A follow-up visit of the Ambassador of the EU in Japan, Jean Eric Paquet, was happening in April 2024 at the SANKEN institute of Co-PI Kazu Suenaga in Osaka.