Structural as well as magnetization studies have been carried out on graphite samples irradiated by neutrons over 50 years in the CIRUS research reactor at Trombay. Neutron diffraction studies reveal that the defects in irradiated graphite samples are not well annealed and remain significant up to high temperatures much greater than 653 K where the Wigner energy is completely released. We infer that the remnant defects may be intralayer Frenkel defects, which do not store large energy, unlike the interlayer Frenkel defects that store the Wigner energy. Magnetization studies on the irradiated graphite show ferromagnetic behavior even at 300 K and a large additional paramagnetic contribution at 5 K. Ab-initio calculations based on the spin-polarized density-functional theory show that the magnetism in defected graphite is essentially confined on to a single 2-coordinated carbon atom that is located around a vacancy in the hexagonal layer.
Recent theories and experiments have suggested hydrodynamic phonon transport features in graphite at unusually high temperatures. Here, we report a pico-second pump-probe thermal reflectance measurement of heat pulse propagation in graphite. The measurement results reveal transient lattice cooling near the adiabatic center of a 15 $μ$m diameter ring-shape pump beam at temperatures between 80 and 120 K. While such lattice cooling has not been reported in recent diffraction measurements of second sound in graphite, the observation here is consistent with both hydrodynamic phonon transport theory…
We have investigated the variation in the magnetization of highly ordered pyrolytic graphite (HOPG) after neutron irradiation, which introduces defects in the bulk sample and consequently gives rise to a large magnetic signal. We observe strong paramagnetism in HOPG, increasing with the neutron fluence. We correlate the induced paramagnetism with structural defects by comparison with density-functional theory calculations. In addition to the in-plane vacancies, the trans-planar defects also contribute to the magnetization. The lack of any magnetic order between the local moments is possibly du…
Basing on experimental data on irradiation-induced deformation of graphite we introduced a concept of diffuse domain structure developed in reactor graphite produced by extrusion. Such domains are considered as random continuous deviations of local graphite texture from the global one. We elucidate the origin of domain structure and estimate the size and the degree of orientational ordering of its domains. Using this concept we explain the well known radiation-induced size effect observed in reactor graphite. We also propose a method for converting the experimental data on shape-change of fini…
We provide evidence that proton irradiation of energy 2.25 MeV on highly-oriented pyrolytic graphite samples triggers ferro- or ferrimagnetism. Measurements performed with a superconducting quantum interferometer device (SQUID) and magnetic force microscopy (MFM) reveal that the magnetic ordering is stable at room temperature.
The energetic evaluations of graphite-to-diamond transition by electron irradiation are performed. The heat conduction problem is solved for the diamond synthesis when a pulse-periodic source of energy is located within a graphite cylinder; time dependences of temperature and pressure are found. It is shown, that the temperatures and pressures implemented in graphite are sufficient for graphite-to-diamond transition under electron bombardment.
Effect of the femtosecond and nanosecond UV laser irradiation (below the ablation threshold) of graphite-like hexagonal boron nitride (hBN) has been studied. Experiments were carried out with the compacted powder under high vacuum at room temperature using excimer KrF laser (248 nm). In the nanosecond operation mode, the laser-induced fluorescence spectra are found strongly modified depending on the integrated doze, which is attributed to a progressive enrichment of the surface layer by elemental boron. A slow sample recovery after the laser irradiation has been observed. On the other hand, in…
In this work we have investigated the changes of the magnetic properties of highly oriented pyrolytic graphite samples after irradiation either with $\sim 3 \times 10^{14}$ protons or $ 3.5 \times 10^{13} ... 3.5 \times 10^{14}$ iron ions with energies in the MeV range. Our results show that iron and proton irradiations can produce similar paramagnetic contributions depending on the implantation temperature. However, only protons induce a ferromagnetic effect.
In this chapter we review the magnetic effects produced by proton irradiation on graphite, disordered carbon and fullerene films. The advantage of proton irradiation is twofold: it enables us to make an impurity analysis simultaneously to the implantation of hydrogen. In this chapter we will review the main effects obtained after proton irradiation in different carbon-based structures. This chapter is organized as follows. In section 2 we provide the main characteristics of our irradiation facility. In this section we show an example of element analysis obtained in one of the graphite samples …
We have experimentally investigated the expansion mechanism induced by laser irradiation of H2SO4 intercalated graphite. Intercalated graphite materials irradiated by laser allows to study reactions occurring in confined chemical conditions. We find that the laser-assisted reaction process is characterized by a threshold temperature of about 140°C followed by a fast rate of heating which produces a large amount of overheated gases and causes a violent expansion of the graphite crystal. We investigate the morphological changes undergone by irradiated graphite filaments using a combination of th…
Laser excitation has emerged as a means to expose hidden states of matter and promote phase transitions on demand. Such laser induced transformations are often rendered possible owing to the delivery of spatially and/or temporally manipulated light, carrying energy quanta well above the thermal background. Here, we report time-resolved broadband femtosecond (fs) transient absorption measurements on thin flakes of Weyl semimetal candidate $T_d$-MoTe$_2$ subjected to various levels and schemes of fs-photoexcitation. Our results reveal that impulsive fs-laser irradiation alters the interlayer beh…
In this paper we show how single layer graphene can be utilized to study swift heavy ion (SHI) modifications on various substrates. The samples were prepared by mechanical exfoliation of bulk graphite onto SrTiO$_3$, NaCl and Si(111), respectively. SHI irradiations were performed under glancing angles of incidence and the samples were analysed by means of atomic force microscopy in ambient conditions. We show that graphene can be used to check whether the irradiation was successful or not, to determine the nominal ion fluence and to locally mark SHI impacts. In case of samples prepared in situ…
Graphite has been used as neutron moderator or reflector in many nuclear reactors. The irradiation of graphite in a nuclear reactor results in a complex population of defects. Heating of the irradiated graphite at high temperatures results in annihilation of the defects with release of an unusually large energy, called the Wigner energy. From various experiments on highly irradiated graphite samples from CIRUS reactor at Trombay and ab-initio simulations, we have for the first time identified various 2-, 3- and 4-coordinated topological structures in defected graphite, and provided microscopic…
We have prepared magnetic graphite samples bombarded by protons at low temperatures and low fluences to attenuate the large thermal annealing produced during irradiation. An overall optimization of sample handling allowed us to find Curie temperatures $ T_c \gtrsim 350$ K at the used fluences. The magnetization versus temperature shows unequivocally a linear dependence, which can be interpreted as due to excitations of spin waves in a two dimensional Heisenberg model with a weak uniaxial anisotropy.
We investigate the dependence of the electrical resistivity of $\sim 60 $nm thick single crystalline graphite samples on the defect concentration produced by proton irradiation at very low fluences. We show that the resistivity decreases few percent at room temperature after inducing defects at concentrations as low as $\sim 0.1 $ppm due to the increase in the carrier density, in agreement with theoretical estimates. The overall results indicate that the carrier densities measured in graphite are not intrinsic but related to defects and impurities.
Recently, magnetic order in highly oriented pyrolytic graphite (HOPG) induced by proton broad- and microbeam irradiation was discovered. Theoretical models propose that hydrogen could play a major role in the magnetism mechanism. We analysed the hydrogen distribution of pristine as well as irradiated HOPG samples, which were implanted to micrometer-sized spots as well as extended areas with various doses of 2.25 MeV protons at the Leipzig microprobe LIPSION. For this we used the sensitive 3D hydrogen microscopy system at the Munich microprobe SNAKE. The background hydrogen level in pristine HO…
Understanding radiation-induced defect formation in carbon materials is crucial for nuclear technology and for the manufacturing of nanostructures with desired properties. Using first principles molecular dynamics, we perform a systematic study of the non-equilibrium processes of radiation damage in graphite. Our study reveals a rich variety of defect structures (vacancies, interstitials, intimate interstitial-vacancy pairs, and in-plane topological defects) with formation energies of 5--15 eV. We clarify the mechanisms underlying their creation and find unexpected preferences for particular s…
We have fabricated Pt-containing granular metals by focused electron beam induced deposition from the $(CH_3)_3CH_3C_5H_4Pt$ precursor gas. The granular metals are made of platinum nanocrystallites embedded in a carbonaceous matrix. We have exposed the as-grown nanocomposites to low energy electron beam irradiation and we have measured the electrical conductivity as a function of the irradiation dose. Postgrowth electron beam irradiation transforms the matrix microstructure and thus the strength of the tunneling coupling between Pt nanocrystallites. For as-grown samples (weak tunnel coupling r…
A few atomic layers of helium adsorbed on graphite have been attracting much attention as one of the ideal quantum systems in two dimension. Although previous reports on neutron diffraction have shown fundamental structural information in these systems, there still remain many open questions. Here, we propose surface crystal truncation rod (CTR) scatterings using synchrotron radiation X-rays as a promising method to reveal surface and interface structures of helium films on graphite at temperatures below 2 K, based on the preliminary experimental results on a monolayer of He-4 on a thin graphi…
In this work we have studied systematically the changes in the magnetic behavior of highly oriented pyrolytic graphite (HOPG) samples after proton irradiation in the MeV energy range. Superconducting quantum interferometer device (SQUID) results obtained from samples with thousands of localized spots of micrometer size as well on samples irradiated with a broad beam confirm previously reported results. Both, the para- and ferromagnetic contributions depend strongly on the irradiation details. The results indicate that the magnetic moment at saturation of spots of micrometer size is of the orde…
We demonstrate that X-ray irradiation can be used to induce an insulator-metal transition in Si-doped Al$_{0.35}$Ga$_{0.65}$As, a semiconductor with {\it DX} centers. The excitation mechanism of the {\it DX} centers into their shallow donor state was revealed by studying the photoconductance along with fluorescence. The photoconductance as a function of incident X-ray energy exhibits an edge both at the Ga and As K-edge, implying that core-hole excitation of Ga and As are efficient primary steps for the excitation of {\it DX} centers. A high quantum yield ($\gg 1$) suggests that the excitation…
We show, using ab initio total energy density functional theory, that the so-called Wigner defects, an interstitial carbon atom right besides a vacancy, which are present in irradiated graphite can also exist in bundles of carbon nanotubes. Due to the geometrical structure of a nanotube, however, this defect has a rather low formation energy, lower than the vacancy itself, suggesting that it may be one of the most important defects that are created after electron or ion irradiation. Moreover, they form a strong link between the nanotubes in bundles, increasing their shear modulus by a sizeable…
Modification induced by 110 MeV Ni ion irradiated thin film samples of C60 on Si and quartz substrates were studied at various fluences. The pristine and irradiated samples were investigated using Raman spectroscopy, electrical conductivity and optical absorption spectroscopy. The Raman data and band gap measurements indicate that swift ions at low fluences result in formations that involve multiple molecular units like dimer or polymer. High fluence irradiation resulted in sub-molecular formations and amorphous semiconducting carbon, indicating overall damage of the fullerene molecules. These…
We investigate native point defects and rare-earth (co)dopants in SrAl$_2$O$_4$ using hybrid density-functional defect calculations. Europium (Eu) and dysprosium (Dy) are found to be mixed valence and energetically most favorable at the Sr lattice sites. However, unlike Eu where both Eu$^{2+}$ and Eu$^{3+}$ can be realized in synthesis, Dy is stable predominantly as Dy$^{3+}$, and the divalent Dy$^{2+}$ may only be photogenerated under irradiation. On the basis of an analysis of Eu-related band-defect (including charge-transfer) and interconfigurational $5d$-$4f$ optical transitions, we assign…
We report a significant and persistent enhancement of the conductivity in free-standing non intentionnaly doped InAs nanowires upon irradiation in ultra high vacuum. Combining four-point probe transport measurements performed on nanowires with different surface chemistries, field-effect based measurements and numerical simulations of the electron density, the change of the conductivity is found to be caused by the increase of the surface free carrier concentration. Although an electron beam of a few keV, typically used for the inspection and the processing of materials, propagates through the …
Interplay of Cl Substitution and He$^{+}$ Irradiation in CrSBr$_{1-x}$Cl$_{x}$
J. Heyrovský Institute of Physical Chemistry, Czech Academy of Sciences（捷克科学院 J. 赫鲁夫斯基物理化学研究所）；Faculty of Mathematics and Physics, Charles University（查理大学数学与物理学院）；University of Chemistry and Technology Prague（布拉格化工大学）；Institute for Ion Beam Physics and Materials Research, Helmholtz-Zentrum Dresden-Rossendorf（德累斯顿-罗斯多夫亥姆霍兹中心离子束物理与材料研究所）
The irradiation with fast ions with kinetic energies of > 10 MeV leads to the deposition of a high amount of energy along their trajectory (up to several ten keV/nm). The energy is mainly transferred to the electronic subsystem and induces different secondary processes of excitations which result in significant material modifications. A new setup to study these ion induced effects on surfaces will be described in this paper. The setup combines a variable irradiation chamber with different techniques of surface characterizations like scanning probe microscopy, time-of-flight secondary ion and n…
