PhD subjects

In view of the challenges posed by global warming, some fundamental research is focusing on optimizing the properties of materials for gas capture (e.g. CO2), filtration, desalination or the conversion of water to H2 by photocatalysis. Two-dimensional materials (graphene, MoS2, hBN, etc.) nanostructured by ion irradiation have recently shown unique and original properties to improve the efficiency of these processes. The introduction of surface modifications to these materials can be used to tailor their properties to specific requirements. Irradiation by fast heavy ions, such as those produced on the GANIL facility, or by low-energy ions produced on CIMAP's PELIICAEN device, induces surface modifications on the nanometric scale.

In this thesis, we propose to gain a better understanding of the processes involved in ion-beam structuration and the modification of 2D material properties as a function of the influence of different irradiation parameters on the local radiation-induced modifications.

The last few decades of condensed matter research have seen the emergence of a rich new physics, based on the notion of "spin liquids". Interest in these new states of matter stems from the fact that they exhibit large-scale quantum entanglement, a property that is fundamental to quantum computation. By directly exploiting this notion of entanglement, a quantum computer would enable revolutionary approaches to certain classes of problems, compared with conventional computers.

The study of spin liquids is therefore a key technological issue, and the aim of this thesis project is to contribute to this fundamental research effort.

Attosecond science focuses on the study of dynamics in matter at ultimate timescales, using light pulses of attosecond (10-18 s) duration. Our laboratory has pioneered the development and use of these pulses to investigate the ultrafast response of matter. In particular, we operate several platforms dedicated to attosecond spectroscopy of solids.

During this PhD project, we will develop original attosecond experiments aimed at elucidating the dynamics of one of the most important and intriguing degree of freedom of solids: the spins of its electrons. This quantity is responsible for the magnetic properties of materials, with applications ranging from data storage devices to spintronic components. Typically, existing devices use electric currents to convey and manipulate information.
Here, we aim to answer one apparently simple question: can we use a laser field, instead of a current, to control the electronic spins of a solid? While this would have the concrete potential of orders-of-magnitude faster operation, answering this question first requires fascinating fundamental investigations. Indeed, the response of magnetic materials at optical frequencies – below 10 fs – is almost completely unknown to this day. We propose to address this problem by performing experiments that combine spin sensitivity and attosecond resolution for the first time. By carefully shaping attosecond pulses and using state-of-the art detection schemes, we aim to establish a technique called attosecond magnetic dichroism, which will reveal the spin response of materials on the timescale of the electric field of light. We will first focus on simple tridimensional ferromagnetic and antiferromagnetic systems, before evolving towards their bi-dimensional counterparts. Indeed, so-called 2D materials are expected to provide enhanced, or even fundamentally novel light-spin interactions. By understanding how light interacts with electronic spins in 2D, we will provide key elements towards the integration of future low-dimensionality spintronic components.

The student will acquire practical knowledge about experimental ultrafast optics and of time resolved spectroscopy of condensed matter, especially magnetic materials. He/she will become an expert in attosecond physics and technology, as well as acquire valuable skills in complex data acquisition and analysis.

The central topic of the thesis is a recently proposed form of matter called altermagnetism. In common with simple antiferromagnets these are magnetic materials supporting long-range magnetic order with no net moment. In simple antiferromagnets the up and down spin electronic bands are degenerate. But in altermagnets they are not. One way of thinking about these materials is that they are nonmagnetic in real space but magnetic in momentum space thus combining features of ferromagnets and antiferromagnets. These materials have generated a great deal of interest in the spintronics community. Roughly speaking this community has, for a long time, been interested in antiferromagnets that support spin currents because antiferromagnets are insensitive to stray fields and can support faster device switching than in typical ferromagnets. Altermagnets have the potential to realize the dreams of antiferromagnetic spintronics. At the same time, altermagnets are of fundamental interest in condensed matter physics. It turns out that altermagnetism is grounded in a peculiar type of symmetry breaking described by the theory of spin groups.

The goal of this thesis project is to extend our understanding of spin groups in condensed matter especially in the direction of altermagnetism and topological materials.

Summary :
The student will develop attosecond spectroscopy techniques making use of the new high reprate Ytterbium laser sources. The ultrafast photoemission dynamics will be studied to reveal in real time the processes of electron scattering/rearrangement as well as electron-ion quantum entanglement, using the charged-particle coincidence techniques.

Detailed summary :
In recent years, there has been spectacular progress in the generation of attosecond (1 as=10-18 s) pulses, rewarded by the 2023 Nobel Prize [1]. These ultrashort pulses are generated from the strong nonlinear interaction of short intense laser pulses with gas jets [2]. A new laser technology based on Ytterbium is emerging, with stability 5 times higher and reprate 10 times higher than the current Titanium:Sapphire technology. These new capabilities represent a revolution for the field.
This opens new prospects for the exploration of matter at the electron intrinsic timescale. Attosecond spectroscopy thus allows studying in real time the quantum process of photoemission, shooting the 3D movie of electronic wavepacket ejection [3,4], and studying quantum decoherence resulting from, e.g., electron-ion entanglement [5].
The first objective of the thesis work is to develop on the ATTOLab laser platform the attosecond spectroscopies using the new Ytterbium laser sources. The second objective is to take advantage of charged particle coincidence techniques, enabled by the high reprate, to study the dynamics of photoemission and quantum entanglement with unprecedented precision.
The student will be trained in ultrafast optics, atomic and molecular physics, quantum optics, and will acquire a broad mastery of XUV and charged-particle spectroscopy techniques.

References :
[1] https://www.nobelprize.org/prizes/physics/2023/summary/
[2] Y. Mairesse, et al., Science 302, 1540 (2003)
[3] V. Gruson, et al., Science 354, 734 (2016)
[4] A. Autuori, et al., Science Advances 8, eabl7594 (2022)
[5] C. Bourassin-Bouchet, et al., Phys. Rev. X 10, 031048 (2020)

The combined demands of increasing energy production and the need to reduce fossil fuels to limit global warming have paved the way for an urgent need for clean energy harvesting technologies. One interesting solution is to use solar energy to produce fuels. Thus, low-cost materials such as semiconductors have been intensively studied for photocatalytic reactions. Among them, 1D nanostructures hold promise due to their interesting properties (high specific and accessible surfaces, confined environments, better charge separation). Imogolite, a natural hollow nanotube clay belongs to this category. Although it is not directly photoactive in the visible light range (high band gap), it exhibits a permanent wall polarization due to its intrinsic curvature. This property makes it a potentially useful co-photocatalyst for charge separation. Moreover, this nanotube belongs to a family sharing the same local structure with different curved morphologies (nanosphere and nanotile). In addition, several modifications of these materials are possible (wall doping with metals, coupling with metal nanoparticles, functionalization of the internal cavity) allowing tuning band gap. The proof of concept (i.e., photocatalytic nanoreactor) was only obtained for the nanotube form.

This phD project aims to study the whole family (nanotube, nanosphere, and nanotile, with various functionalizations) as nanoreactors for reduction reactions of protons and CO2 triggered under irradiation.

The objective of the thesis project is to analyze the physicochemical processes resulting from the extreme dose rates that can now be obtained in water with the ultra-short (fs) pulses of relativistic electrons produced by laser-plasma acceleration. Indeed, first measurements show that these processes are probably not equivalent to those obtained with longer pulses (µs) in the FLASH effect used in radiotherapy. To achieve this, we propose to analyze the dynamics of formation/recombination of the hydrated electron, an emblematic species of water radiolysis, to qualify and quantify the dose rate effect over increasingly shorter times. This will be done in three stages in support of the necessary and now accessible technological progress, to have a dose per pulse sufficient to directly detect the hydrated electron. First, with the existing UHI100 facility, using the scavenging of the hydrated electron by producing a stable species; then producing a less stable but detectable species in real time and increasing the repetition rate of the electron source. Finally, by using an innovative concept named a “hybrid target”, based on a plasma mirror as an electron injector coupled to a laser-plasma accelerator, delivering larger doses with a narrower energy spectrum, we will be able to develop pump-probe detection allowing access to the shortest times, and to the formation in clusters of ionization, of the hydrated electron and measuring its initial yield.

### Context
The context of this PhD thesis deals with laser plasma electron accelerators (LPA), which can be obtained by focusing a high-power laser into a gas medium. At focus, the laser field is so intense that it quasi-instantly ionizes matter into an undersense plasma, in which it can propagate. During laser propagation, the ponderomotive laser pressure expels plasma electrons from its path, forming a cavity void of electrons in its wake. This cavity, called ‘bubble’, can sustain accelerating fields (100GV/m) that are roughly three orders of magnitude larger than what can be provided by Radiofrequency cavities, which equip the current generation of conventional accelerators. These accelerating structures can trap some plasma electrons and accelerate them at relativistic energies (few GeVs) over distances of a few centimeters. This offers the prospect of producing much more compact and affordable accelerators, with the following goals: (i) democratizing their usage for existing applications currently reserved to only a few installations in the world (ii) enabling new applications in strategic sectors (fundamental research, industry, medicine, defense).

Among the applications for which a strong international competition exist we remark:

> The usage of these accelerators to provide the first high-energy (100 MeV) electron radiotherapy machine for medical treatmes

> The usage of these accelerators as a building block of a future large scale TeV electron/positron collider for high-energy physics

> The usage of these accelerators to develop a compact and mobile relativistic muon source to perform active muon tomography. Such a tool would be a major asset for industrial applications (e.g., safety diagnostic of nuclear reactors), and for defense applications (non-proliferation). It is worth to mention that in these two sectors the american agency DARPA has already funded an ambitious program ( Muons for Science and Security, MuS2) in 2022, with the aim of providing a first conceptual report of a relativistic moun source based on a plasma accelerator (cf. https://www.darpa.mil/news-events/2022-07-22).

### Challenges:

In order to enable the aforementioned applications, strong limitations of current laser-plasma accelerators need to be addressed. An important limitation is the low amount of charge at high-energies (100 MeV – few GeV) provided by these accelerators. The main reason behind the low accelerated charge is the fact that present-day injection techniques are based on the injection of electrons from the gas, whose density is very low. In order to address this limitation, we have recently proposed a new injection concept based on a remarkable physical system called “plasma-mirror”. This concept relies on the use of a hybrid solid-gas target. When impinging on such a target, the high-power laser fully ionizes the solid and the gas. The solid part is so dense that it can reflect the incident laser, forming a so-called ‘plasma mirror’. In the gas part, the laser propagates and drives a LPA. Upon reflection on the plasma mirror, ultra-dense electron bunches can be highly-precisely injected into the bubble of the LPA formed by the reflected laser field. As the solid offers orders of magnitude more charge than the gas medium and as charge is injected from a highly-localized region from the plasma (plane), it has the potential to level up the injected charge in LPAs while keeping a high electron beam quality.

The PHI group is an international leader in the study and control of these systems. In collaboration with LOA, by using a 100TW-class laser, we have demonstrated that this new concept allows for a significant increase of the accelerated charge while preserving the quality of the beam.

### Goals

The first objective of this PhD thesis will be to develop a multi-GeV laser-plasma accelerator based on a plasma-mirror injection on Petawatt-class laser installations like the APOLLON laser facility. With a Petawatt-class laser this accelerator should produce electrons beams at 4 GeV with a total charge of hundreds of pC and a few % energy spread. Such a beam quality would represent a substantial progress in the domain.

The second objective will be to send this electron beam into a high-Z converter in order to generate muons/anti-muons pairs. Our estimations show that we could obtain roughly 10^4 relativistic muons per shot, which would allow for the radiography of a high-Z material in a few minutes.

This PhD subject foresees:
> Theoretical/numerical modeling activities based on our exascale code WarpX (to model the laser-plasma accelerator) and on the Geant4 code (for the modeling of the high-Z converter).

> Experimental activities (high-intensity laser-plasma interaction, detection of relativistic muons)


The project involves several partner laboratories:

> The Laboratoire d’Optique Appliquée for the laser-plasma acceleration activities (A. Leblanc)

> The Lawrence Berkeley National Lab for code development activities (WarpX, J.L Vay)

> The CEA-IRFU for the detection part (micromegas technology, O. Limousin)


For the experimental part, we will use several laser facilities:

> The UHI100 laser installation for the setup and testing of the laser-plasma accelerator at reduced power

> The APOLLON installation for the setup and testing of the plasma accelerator with a PW-class laser. A first experience implementing the concept of a plasma-mirror injector at the PW-level is scheduled for May 2024 in the framework of a collaboration between CEA and LOA. Following this experiment, we will perform a second experiment (2025-2026) to generate muons on APOLLON or other laser facilities in Europe (e.g., the ELI installations).