Laboratoire des Solides Irradiés

Through a systematic structural search we found an allotrope of carbon with Cmmm symmetry which we predict to be more stable than graphite for pressures above 10 GPa. This material, which we refer to as Z-carbon, is formed by pure sp(3) bonds and it provides an explanation to several features in experimental x-ray diffraction and Raman spectra of graphite under pressure. The transition from graphite to Z-carbon can occur through simple sliding and buckling of graphene sheets. Our calculations predict that Z-carbon is a transparent wide band-gap semiconductor with a hardness comparable to diamond.

Elastic waves, polarized in the sagittal plane, are investigated in infinite and semi-infinite superlattices made from alternate layers of two isotropic media. By the use of a transfer-matrix method, we obtain explicit equations for the dispersion of the bulk modes as well as of the surface modes of a semi-infinite superlattice. We present a few illustrations of the theory for Al-W superlattices in which the relative thicknesses of the two media or the thickness of the layer at the surface are varied.

We report high-sensitivity microwave measurements of the in-plane penetration depth lambda_{ab} and quasiparticle scattering rate 1/tau in several single crystals of the hole-doped Fe-based superconductor Ba(1-x)K(x)Fe(2)As(2) (x approximately 0.55). While a power-law temperature dependence of lambda_{ab} with a power approximately 2 is found in crystals with large 1/tau, we observe an exponential temperature dependence of the superfluid density consistent with the existence of fully opened two gaps in the cleanest crystal we studied. The difference may be a consequence of different levels of disorder inherent in the crystals. We also find a linear relation between the low-temperature scattering rate and the density of quasiparticles, which shows a clear contrast to the case of d-wave cuprate superconductors with nodes in the gap. These results demonstrate intrinsically nodeless order parameters in the Fe arsenides.

It is shown that new specific effects take place during irradiation of metals with high energy fullerene beams. The observed quasicontinuous damage is confined inside \ensuremath{\sim}20 nm diam cylinders around the projectile paths and is compared to the damage resulting from GeV heavy ion irradiation. The large extension of the highly damaged zones after cluster irradiations might be due to the strong localization of the deposited energy during the slowing-down process.

The experimental valence band photoemission spectrum of semiconductors exhibits multiple satellites that cannot be described by the GW approximation for the self-energy in the framework of many-body perturbation theory. Taking silicon as a prototypical example, we compare experimental high energy photoemission spectra with GW calculations and analyze the origin of the GW failure. We then propose an approximation to the functional differential equation that determines the exact one-body Green's function, whose solution has an exponential form. This yields a calculated spectrum, including cross sections, secondary electrons, and an estimate for extrinsic and interference effects, in excellent agreement with experiment. Our result can be recast as a dynamical vertex correction beyond GW, giving hints for further developments.

Abstract Magneto-optical (MO) effects, viz. magnetically induced changes in light intensity or polarization upon reflection from or transmission through a magnetic sample, were discovered over a century and a half ago. Initially they played a crucially relevant role in unveiling the fundamentals of electromagnetism and quantum mechanics. A more broad-based relevance and wide-spread use of MO methods, however, remained quite limited until the 1960s due to a lack of suitable, reliable and easy-to-operate light sources. The advent of Laser technology and the availability of other novel light sources led to an enormous expansion of MO measurement techniques and applications that continues to this day (see section 1). The here-assembled roadmap article is intended to provide a meaningful survey over many of the most relevant recent developments, advances, and emerging research directions in a rather condensed form, so that readers can easily access a significant overview about this very dynamic research field. While light source technology and other experimental developments were crucial in the establishment of today’s magneto-optics, progress also relies on an ever-increasing theoretical understanding of MO effects from a quantum mechanical perspective (see section 2), as well as using electromagnetic theory and modelling approaches (see section 3) to enable quantitatively reliable predictions for ever more complex materials, metamaterials, and device geometries. The latest advances in established MO methodologies and especially the utilization of the MO Kerr effect (MOKE) are presented in sections 4 (MOKE spectroscopy), 5 (higher order MOKE effects), 6 (MOKE microscopy), 8 (high sensitivity MOKE), 9 (generalized MO ellipsometry), and 20 (Cotton–Mouton effect in two-dimensional materials). In addition, MO effects are now being investigated and utilized in spectral ranges, to which they originally seemed completely foreign, as those of synchrotron radiation x-rays (see section 14 on three-dimensional magnetic characterization and section 16 on light beams carrying orbital angular momentum) and, very recently, the terahertz (THz) regime (see section 18 on THz MOKE and section 19 on THz ellipsometry for electron paramagnetic resonance detection). Magneto-optics also demonstrates its strength in a unique way when combined with femtosecond laser pulses (see section 10 on ultrafast MOKE and section 15 on magneto-optics using x-ray free electron lasers), facilitating the very active field of time-resolved MO spectroscopy that enables investigations of phenomena like spin relaxation of non-equilibrium photoexcited carriers, transient modifications of ferromagnetic order, and photo-induced dynamic phase transitions, to name a few. Recent progress in nanoscience and nanotechnology, which is intimately linked to the achieved impressive ability to reliably fabricate materials and functional structures at the nanoscale, now enables the exploitation of strongly enhanced MO effects induced by light–matter interaction at the nanoscale (see section 12 on magnetoplasmonics and section 13 on MO metasurfaces). MO effects are also at the very heart of powerful magnetic characterization techniques like Brillouin light scattering and time-resolved pump-probe measurements for the study of spin waves (see section 7), their interactions with acoustic waves (see section 11), and ultra-sensitive magnetic field sensing applications based on nitrogen-vacancy centres in diamond (see section 17). Despite our best attempt to represent the field of magneto-optics accurately and do justice to all its novel developments and its diversity, the research area is so extensive and active that there remains great latitude in deciding what to include in an article of this sort, which in turn means that some areas might not be adequately represented here. However, we feel that the 20 sections that form this 2022 magneto-optics roadmap article, each written by experts in the field and addressing a specific subject on only two pages, provide an accurate snapshot of where this research field stands today. Correspondingly, it should act as a valuable reference point and guideline for emerging research directions in modern magneto-optics, as well as illustrate the directions this research field might take in the foreseeable future.

Swift heavy-ion irradiation of elemental metal nanoparticles (NPs) embedded in amorphous SiO(2) induces a spherical to rodlike shape transformation with the direction of NP elongation aligned to that of the incident ion. Large, once-spherical NPs become progressively more rodlike while small NPs below a critical diameter do not elongate but dissolve in the matrix. We examine this shape transformation for ten metals under a common irradiation condition to achieve mechanistic insight into the transformation process. Subtle differences are apparent including the saturation of the elongated NP width at a minimum sustainable, metal-specific value. Elongated NPs of lesser width are unstable and subject to vaporization. Furthermore, we demonstrate the elongation process is governed by the formation of a molten ion-track in amorphous SiO(2) such that upon saturation the elongated NP width never exceeds the molten ion-track diameter.

The cumulant expansion is a powerful approach for including correlation effects in electronic structure calculations beyond the $GW$ approximation. However, the expansion is not generally valid, as current implementations ignore terms that mix particle and hole states and lead to partial occupation numbers of one-electron states. These limitations are corrected here using a cumulant expansion of the retarded one-electron Green's function that includes both particle and hole contributions. The approach provides a consistent framework that improves on the $GW$ approximation to the spectral function without additional computational effort. The method is illustrated with results for the homogeneous electron gas and comparisons to experiment and other methods.

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Using a combination of experimental techniques such as optical absorption, Raman scattering, continuous wave and pulse Electron Spin Resonance (ESR), we characterize a set of γ-irradiated Yb(3+) doped silica glass preforms with different contents of phosphorous and aluminum. We demonstrate that when P is introduced in excess compared to Al, nearly no radiodarkening is induced by γ-rays. On the other hand, when Al>P, a large absorption band is induced by radiation. Thermal annealing experiments reveal the correlation between the decrease of the optical absorption band and the decrease of the Al-Oxygen Hole Center (AlOHC) ESR signal, demonstrating the main role of AlOHC defects in the fiber darkening. HYSCORE (HYperfine Sublevel CORElation) pulse-ESR experiments show a high Al-P nuclear spin coupling when P>Al and no coupling when Al>P. This result suggests that both AlOHC and POHC creation is inhibited by Al-O-P linkages. Confronting our data with previous works, we show that the well-known photodarkening process, meaning losses induced by the IR pump, can also be explained in this framework.

We propose an alternative route to achieve the superconducting state in boron-rich solids, the hole doping of ${\mathrm{B}}_{12}$ icosahedra. For this purpose we consider a prototype metallic phase of ${\mathrm{B}}_{13}{\mathrm{C}}_{2}$. We show that in this compound the boron icosahedral units are mainly responsible for the large phonon frequencies logarithmic average, $65.8\phantom{\rule{0.3em}{0ex}}\text{meV}$, and the moderate electron-phonon coupling $\ensuremath{\lambda}=0.81$. We suggest that this high ${T}_{c}$ could be a general feature of hole-doped boron icosahedral solids. Moreover our calculated moderate value of $\ensuremath{\lambda}$ excludes the formation of bipolarons localized on the icosahedral length scale as suggested by previous authors.

In many-body perturbation theory (MBPT) the self-energy $\ensuremath{\Sigma}=iGW\ensuremath{\Gamma}$ plays a key role since it contains all the many-body effects of the system. The exact self-energy is not known; as a first approximation one can set the vertex function $\ensuremath{\Gamma}$ to unity which leads to the GW approximation. The latter properly describes the high-density regime, where screening is important; in the low-density regime, instead, other approximations are proposed, such as the $T$ matrix, which describes multiple scattering between two particles. Here we combine the two approaches. Starting from the fundamental equations of MBPT, we show how one can derive the $T$-matrix approximation to the self-energy in a common framework with $GW$. This allows us to elucidate several aspects of this formulation, including the origin of, and link between, the electron-hole and the particle-particle $T$ matrix, the derivation of a screened $T$ matrix, and the conversion of the $T$ matrix into a vertex correction. The exactly solvable Hubbard molecule is used for illustration.

We present a method for the evaluation of electronic excitations of advanced materials by reformulating spectral sum-over-states expressions such that only occupied states appear. All empty states are accounted for by one effective energy. Thus we keep the simplicity and precision of the sum-over-states approach while speeding up calculations by more than an order of magnitude. We demonstrate its power by applying it to the $GW$ method, where a huge summation over empty states appears twice (screening and self-energy). The precision is shown for bulk Si and solid and atomic Ar. We then use it to determine the band gap of the technologically important oxide ${\text{SnO}}_{2}$.

We investigate the temporal evolution of the electronic states at the bismuth (111) surface by means of time- and angle-resolved photoelectron spectroscopy. The binding energy of bulklike bands oscillates with the frequency of the A(1g) phonon mode, whereas surface states are insensitive to the coherent displacement of the lattice. A strong dependence of the oscillation amplitude on the electronic wave vector is correctly reproduced by ab initio calculations of electron-phonon coupling. Besides these oscillations, all the electronic states also display a photoinduced shift towards higher binding energy whose dynamics follows the evolution of the electronic temperature.

In this joint experimental and theoretical work, we investigate collective electronic excitations (plasmons) in free-standing, single-layer graphene. The energy- and momentum-dependent electron energy-loss function was measured up to $50\phantom{\rule{0.28em}{0ex}}\mathrm{eV}$ along two independent in-plane symmetry directions ($\ensuremath{\Gamma}M$ and $\ensuremath{\Gamma}K$) over the first Brillouin zone by momentum-resolved electron energy-loss spectroscopy in a transmission electron microscope. We compare our experimental results with corresponding time-dependent density-functional theory calculations. For finite momentum transfers, good agreement with experiments is found if crystal local-field effects are taken into account. In the limit of small and vanishing momentum transfers, we discuss differences between calculations and the experimentally obtained electron energy-loss functions of graphene due to a finite momentum resolution and out-of-plane excitations.

This paper reports the effect of randomness on a quantum spin liquid state of 1T-TaS${}_{2}$ with a two-dimensional perfect triangular lattice. Systematic measurements of heat capacity and thermal conductivity in pure, Se-substituted, and electron-irradiated crystals reveal the microscopic coexistence of localized orphan spins that form random valence bonds and itinerant spinons that appear to form a Fermi surface.

The synthesis and X-ray crystal structure of the ligand L (4,7-dicarbazol-9-yl-[1,10]-phenanthroline) are reported, as well as those of the molecular complex, [Eu(tta)(3)(L)] (1), (tta = 2-thenoyl trifluoroacetylacetonate). Their photophysical properties have been investigated both in solution and in the solid state. It was shown that the ligands used for designing 1 are well-suited for sensitizing the Eu(III) ion emission, thanks to a favorable position of the triplet state as investigated in the Gd(III) complex [Gd(tta)(3)(L)], (2). The low local symmetry of the Eu(III) ion shown by the X-ray crystal structure of 1 is also revealed by luminescence spectroscopy. Because of interesting volatility and solubility properties, 1 is shown to behave as a real molecular material that can be processed both by thermal evaporation and from solution. When doped in poly(methylmethacrylate) (PMMA), 1 forms air-stable and highly red-emitting plastic materials that can be excited in a wide range of wavelengths from the UV to the visible part of the electromagnetic spectrum (250-560 nm). Absolute quantum yields of 80% have been obtained for films comprising 1-3% of 1. Ellipsometry measurements have been introduced to gain information on physical data of 1. They have been performed on thin films of 1 deposited by thermal evaporation and gave access to the refractive index, n, and the absorption coefficient, k, as a function of the wavelength. A value of 1.70 has been found for n at 633 nm. These thin films also show interesting air-stability.

The generation of energetic electron bunches by the interaction of a short, ultraintense (I>10(19) W/cm(2)) laser pulse with "grating" targets has been investigated in a regime of ultrahigh pulse-to-prepulse contrast (10(12)). For incidence angles close to the resonant condition for surface plasmon excitation, a strong electron emission was observed within a narrow cone along the target surface, with energy spectra peaking at 5-8 MeV and total charge of ∼100 pC. Both the energy and the number of emitted electrons were strongly enhanced with respect to simple flat targets. The experimental data are closely reproduced by three-dimensional particle-in-cell simulations, which provide evidence for the generation of relativistic surface plasmons and for their role in driving the acceleration process. Besides the possible applications of the scheme as a compact, ultrashort source of MeV electrons, these results are a step forward in the development of high-field plasmonics.

Abstract The recently discovered kagome superconductors A V 3 Sb 5 ( A = K, Rb, Cs) exhibit unusual charge-density-wave (CDW) orders with time-reversal and rotational symmetry breaking. One of the most crucial unresolved issues is identifying the symmetry of the superconductivity that develops inside the CDW phase. Theory predicts a variety of unconventional superconducting symmetries with sign-changing and chiral order parameters. Experimentally, however, superconducting phase information in A V 3 Sb 5 is still lacking. Here we report the impurity effects in CsV 3 Sb 5 using electron irradiation as a phase-sensitive probe of superconductivity. Our magnetic penetration depth measurements reveal that with increasing impurities, an anisotropic fully-gapped state changes to an isotropic full-gap state without passing through a nodal state. Furthermore, transport measurements under pressure show that the double superconducting dome in the pressure-temperature phase diagram survives against sufficient impurities. These results support that CsV 3 Sb 5 is a non-chiral, anisotropic s -wave superconductor with no sign change both at ambient and under pressure.

Charge doping of iron-pnictide superconductors leads to collective pinning of flux vortices, whereas isovalent doping does not. Moreover, flux pinning in the charge-doped compounds is consistently described by the mean-free path fluctuations introduced by the dopant atoms, allowing for the extraction of the elastic quasiparticle scattering rate. The absence of scattering by dopant atoms in isovalently doped BaFe2(As(1-x)P(x))(2) is consistent with the observation of a linear temperature dependence of the low-temperature penetration depth in this material.