Here we report the experimental evidence of the interactions between the excitations of the $π\toπ^*$ optical transition and the image potential states (IPS) of highly oriented pyrolitic graphite (HOPG). By using non-linear angle resolved photoelectron spectroscopy (NL-ARPES) we show that the IPS photoemission intensity, the effective mass, and the linewidth exhibit a strong variation when the photon energy is tuned across the $π\toπ^*$ saddle points in the 3.1 - 4.5 eV photon energy range. A model based on the self-energy formalism is proposed to correlate the effective mass and the linewidth variations to transient many body effects, when a high carriers density (in the $10^{20}$ cm$^{-3}$ range) is created by the absorption of a coherent light pulse. This finding brings a clear evidence of a high IPS-bulk coupling in graphite and opens the way for exploiting the IPS as a sensitive, nonperturbing probe for the many-body dynamics in materials.
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 propose a two-pulse excitation to efficiently photoinduced a novel $sp^3$-bonded nano-domain with a frozen shear in a graphite crystal. This $sp^3$ structure is known to be well stabilized by shear displacement between neighboring two graphite layers. This shear motion is generated only as a transient and unfrozen one by the first visible laser pulse, shone over the graphite crystal. While, the second pulse is proved to freeze it before it disappears, resulting in an efficient interlayer $σ$ ($sp^3$) bond formation.
The double-resonance (DR) Raman process is a signature of all sp2 carbon material and provide fundamental information of the electronic structure and phonon dispersion in graphene, carbon nanotubes and different graphite-type materials. We have performed in this work the study of different DR Raman bands of rhombohedral graphite using five different excitation laser energies and obtained the dispersion of the different DR features by changing the laser energy. Results are compared with those of Bernal graphite and shows that rhombohedral graphite exhibit a richer DR Raman spectrum. For example…
A new type of plasmarons formed by the compound of photoelectrons and acoustic surface plasmon excitations is investigated in the system p(2x2)-K/Graphite. The physics behind these types of plasmarons, e-plasmarons, is different from the ones recently found in graphene where the loss feature is argued to result from the photohole-plasmon interaction, h-plasmarons. Based on first principles methods we calculate the dispersion of e-plasmaron excitation rate which yields a broad feature below the parabolic quantum-well band with a peak about 0.4 eV below the quantum well band in the Gamma-point.
Time-resolved Raman spectroscopy has been applied to probe the anharmonic coupling and electron-phonon interaction of optical phonons in graphite. From the decay of the transient anti-Stokes scattering of the G-mode following ultrafast excitation, we measured a lifetime of 2.2+/-0.1ps for zone-center optical phonons. We also observed a transient stiffening of G-mode phonons, an effect attributed to the reduction of the electron-phonon coupling for high electronic temperatures.
We present an analysis of deep-UV Raman measurements of graphite, graphene and carbon nanotubes. For excitation energies above the strong optical absorption peak at the $M$ point in the Brillouin zone ($\approx 4.7\,\text{eV}$), we partially suppress double-resonant scattering processes and observe the two-phonon density of states of carbon nanomaterials. The measured peaks are assigned to contributions from LO, TO, and LA phonon branches, supported by calculations of the phonon dispersion. Moreover, we gain access to the infrared-active $E_{1u}$ mode in graphite. By lowering the excitation en…
Using the classical molecular dynamics and the semiempirical Brenner's potential, we theoretically study the interlayer sigma bond formation, as cooperative and nonlinear phenomena induced by visible light excitations of a graphite crystal. We have found several cases, wherein the excitations of certain lattice sites result in new interlayer bonds even at non-excited sites. We have also found that, a new interlayer bond is easier to be formed around a bond, if it is already existing. As many more sites are going to be excited, the number of interlayer bonds increases nonlinearly with the numbe…
The optical conductivity of graphite in quantizing magnetic fields is analytically evaluated for frequencies in the range of 10--300 meV, where the electron relaxation processes can be neglected and the low-energy excitations at the "Dirac lines" are more essential. The conductivity peaks are explained in terms of the electron transitions in graphite. Conductivity calculated per one graphite layer tends on average to the universal conductivity of graphene while the frequency is larger than the Landau spacing. The (semi)metal-insulator transformation is possible under doping in high magnetic fi…
We use polarized magneto-Raman scattering to study purely electronic excitations and the electron-phonon coupling in bulk graphite. At a temperature of 4.2 K and in magnetic fields up to 28 T we observe $K$-point electronic excitations involving Landau bands with $Δ|n|=0$ and with $Δ|n|=\pm2$ that can be selected by controlling the angular momentum of the excitation laser and of the scattered light. The magneto-phonon effect involving the $E_{2g}$ optical phonon and $K$-point inter Landau bands electronic excitations with $Δ|n|=\pm1$ is revealed and analyzed within a model taking into account …
Ultrafast dynamics of graphite is investigated by time-resolved photoemission spectroscopy. We observe spectral features of direct photoexcitations, non-thermal electron distributions, and recovery dynamics occurring with two time scales having distinct pump-power dependences. Additionally, we find an anomalous increase of the spectral intensity around the Fermi level, and we attribute this to spectral broadenings due to coupled optical phonons in the transient. The fingerprints of the coupled optical phonons occur from the temporal region where the electronic temperature is still not definabl…
The micro-Raman scattering response of a graphene-like location on the surface of bulk natural graphite is investigated both at $T=\unit{4.2}{K}$ and at room temperature in magnetic fields up to 29 T. Two different polarization configurations, co-circular and crossed-circular, are employed in order to determine the Raman scattering selection rules. Several distinct series of electronic excitations are observed and we discuss their characteristic shapes and amplitudes. In particular, we report a clear splitting of the signals associated with the inter-Landau level excitations $-n\rightarrow+n$.…
The electron energy-loss function of graphite is studied for momentum transfers q beyond the first Brillouin zone. We find that near Bragg reflections the spectra can change drastically for very small variations in q. The effect is investigated by means of first principle calculations in the random phase approximation and confirmed by inelastic x-ray scattering measurements of the dynamic structure factor S(q,ω). We demonstrate that this effect is governed by crystal local field effects and the stacking of graphite. It is traced back to a strong coupling between excitations at small and large …
Due to the absence of matching carbon atoms at honeycomb centers with carbon atoms in adjacent graphene sheets, theorists predicted that a sliding process is needed to form AA, AB, or ABC stacking when directly converting graphite into sp3 bonded diamond. Here, using twisted bilayer graphene, which naturally provides AA and AB stacking configurations, we report the ultrafast formation of a transient 2D diamond-like structure (which is not observed in aligned graphene) under femtosecond laser irradiation. This photo-induced phase transition is evidenced by the appearance of new bond lengths of …
Novel phenomena in magnetically-intercalated graphite has been a subject of much research, pioneered and promoted by M.~S. and G.~Dresselhaus and many others in the 1980s. Among the most enigmatic findings of that era was a dramatic, roller-coaster-like behavior of the magnetoresistivity in EuC$_6$ compound, in which magnetic Eu$^{2+}$ ions form a triangular lattice that is commensurate to graphite honeycomb planes. In this study, we provide a long-awaited {\it microscopic} explanation of this behavior, demonstrating that the resistivity of EuC$_6$ is dominated by spin excitations in Eu-planes…
Radio-frequency compressed ultrafast electron diffraction has been used to probe the coherent and incoherent coupling of impulsive electronic excitation at 1.55 eV (800 nm) to optical and acoustic phonon modes directly from the perspective of the lattice degrees of freedom. A bi-exponential suppression of diffracted intensity due to relaxation of the electronic system into incoherent phonons is observed, with the 250 fs fast contribution dominated by coupling to the $E_{2g2}$ optical phonon mode at the $Γ$-point ($Γ-E_{2g2}$) and $A_1^{'}$ optical phonon mode at the $K$-point ($K-A_1^{'}$). Bo…
Two-particle spectroscopy with correlated electron pairs is used to establish the causal link between the secondary electron spectrum, the $(π+σ)-$plasmon peak and the unoccupied band structure of highly oriented pyrolitic graphite. The plasmon spectrum is resolved with respect to the involved interband transitions and clearly exhibits final state effects, in particular due to the energy gap between the interlayer resonances along the $Γ$A-direction. The corresponding final state effects can also be identified in the secondary electron spectrum. Interpretation of the results is performed on th…
The magneto-optical properties of simple hexagonal graphite exhibit rich beating oscillations, which are dominated by the field strength and photon energy. The former has a strong effect on the intensity, the energy range of the beating and the number of groups, and the latter modulates the total group numbers of the oscillation structures. The single-particle and collective excitations are simultaneously presented in the magnetoreflectance spectra and can be precisely distinguished. For the loss function and reflectance, the beating pattern of the first group displays stronger intensities and…
We synthesize and study the structural and optical properties of nanocrystalline graphene monofluoride and graphite monofluoride, which are carbon-based wide bandgap materials. Using laser excitations 2.41 - 5.08 eV, we identify six emission modes of graphite monofluoride, spanning the visible spectrum from red to violet. The energy and linewidth of the modes point to defect-induced midgap states as the source of the photoemission. We discuss possible candidates. Our findings open the window to electro-optical applications of graphene fluoride.
Time-dependent and constituent-specific spectral changes in soft near edge X-ray spectroscopy (XAS) of an [Fe/MgO]$_8$ metal/insulator heterostructure upon laser excitation are analyzed at the O K-edge with picosecond time resolution. The oxygen absorption edge of the insulator features a uniform intensity decrease of the fine structure at elevated phononic temperatures, which can be quantified by a simple simulation and fitting procedure presented here. Combining X-ray absorption spectroscopy with ultrafast electron diffraction measurements and ab initio calculations demonstrate that the tran…
We combine tunable mid-infrared (MIR) pump pulses with time- and angle-resolved two-photon photoemission to study ultrafast photoexcitation of the topological surface state (TSS) of Sb$_{2}$Te$_{3}$. It is revealed that MIR pulses permit a direct excitation of the unoccupied TSS owing to an optical coupling across the Dirac point. The novel optical coupling provokes asymmetric transient populations of the TSS at ${\pm}k_{||}$, which mirrors a macroscopic photoexcited electric surface current. By observing the decay of the asymmetric population, we directly demonstrate the dynamics of the long-…
The nature of low energy plasmon excitations plays an important role in understanding the low energy electronic properties and coupling mechanism of different superconducting compounds such as CaC$_6$. Recent ab-initio studies predict a charge carrier intraband plasmon in keeping with a low energy acoustic plasmon. Here, we have studied the low-energy electronic excitations of CaC$_6$ using high-resolution electron energy-loss spectroscopy in transmission at low temperatures. The analysis of the core-level excitations leads to the conclusion that hybridization between graphite and calcium stat…
We generate in-plane magnetoelastic waves in nickel films using the all-optical transient grating technique. When performed on amorphous glass substrates, two dominant magnetoelastic excitations can be resonantly driven by the underlying elastic distortions, the Rayleigh Surface Acoustic Wave and the Surface Skimming Longitudinal Wave. An applied field, oriented in the sample plane, selectively tunes the coupling between magnetic precession and one of the elastic waves, thus demonstrating selective excitation of coexisting, large amplitude magnetoelastic waves. Analytical calculations based on…
Low-energy electronic properties of ABC-stacked graphite are studied by the tight-binding model. There are linear and parabolic bands with and without degeneracy. They show strongly anisotropic dispersions. ABC-stacked grahite is a semimetal due to slight overlapping near the Fermi level beween conduction and valence bands. The interlayer interactions could change the energy dispersion, state degeneracy, and positions of band-crossing and band-edge state. Density of states exhibit a shoulder structure, owing to band-edge states near or at high symmetric points. Low-frequency Coulomb excitation…
The transient evolution of carriers in an intrinsic graphene under ultrafast excitation, which is caused by the collisionless interband transitions, is studied theoretically. The energy relaxation due to the quasielastic acoustic phonon scattering and the interband generation-recombination transitions due to thermal radiation are analyzed. The distributions of carriers are obtained for the limiting cases when carrier-carrier scattering is negligible and when the intercarrier scattering imposes the quasiequilibrium distribution. The transient optical response (differential reflectivity and tran…
Time-dependent density functional theory (TDDFT) simulations of transient core-level spectroscopies require a balanced treatment of both valence- and core-electron excitations. To this end, tuned range-separated hybrid exchange-correlation functionals within the generalized Kohn-Sham scheme offer a computationally efficient means of simultaneously improving the accuracy of valence and core excitation energies in TDDFT by mitigating delocalization errors across multiple length-scales. In this work range-separated hybrid functionals are employed in conjunction with the velocity-gauge formulation…
The exciton-phonon coupling in highly oriented pyrolytic graphite is studied using resonant inelastic X-ray scattering (RIXS) spectroscopy. With ~ 70 meV energy resolution, multiple low energy excitations associated with coupling to phonons can be clearly resolved in RIXS spectra. Using resonance dependence and the closed form for RIXS cross-section without considering the intermediate state mixing of phonon modes, the dimensionless coupling constant g is determined to be 5 and 0.4, corresponding to the coupling strength of 0.42 eV +/- 40 meV and 0.21 eV +/- 30 meV, for zone center and boundar…
Femtosecond core-level transient absorption spectroscopy is utilized to investigate photoinduced dynamics of the charge density wave in 1T-TiSe2 at the Ti M2,3 edge (30-50 eV). Photoexcited carriers and phonons are found to primarily induce spectral red-shifts of core-level excitations, and a carrier relaxation time and phonon heating time of approximately 360 fs and 1.0 ps are extracted, respectively. Pronounced oscillations in delay-dependent absorption spectra are assigned to coherent excitations of the optical $A_{1g}$ phonon (6.0 THz) and the $A_{1g}^*$ charge density wave amplitude mode …
Ultrafast excitation of Bloch plasmon polaritons in hyperbolic metamaterials with an extreme ultra-violet transient grating
Umeå University（于默奥大学）；Elettra Sincrotrone Trieste（的里雅斯特同步辐射中心）；CIC nanoGUNE BRTA（nanoGUNE研究中心）；Ikerbasque, Basque Foundation for Science（伊卡巴斯克，巴斯克科学基金会）；Università degli Studi di Modena e Reggio Emilia（摩德纳和雷焦艾米利亚大学）；Wallenberg Initiative Materials Science for Sustainability（瓦伦堡可持续材料科学倡议）
Intense ultrafast laser excitation can produce transient states of condensed matter that would otherwise be inaccessible. At high excitation level, the interatomic forces can be altered resulting in an unusual lattice dynamics. Here we report the study of coherent lattice dynamics in Bi made for various excitation levels at helium temperature. We demonstrate that under certain conditions the fully symmetric phonons of large amplitude exhibit anomalous decay and phase rigidity, both of which possibly signaling the attainment of transient supersolid state.
X-ray reflectivity (XRR) measurements of femtosecond laser-induced transient gratings are applied to demonstrate the spatio-temporal coherent control of thermally induced surface deformations on ultrafast timescales. Using gracing incidence X-ray diffraction we unambiguously measure the amplitude of transient surface deformations with sub-Å resolution. Understanding the dynamics of femtosecond TG excitations in terms of superposition of acoustic and thermal gratings makes it possible to develop new ways of coherent control in X-ray diffraction experiments. Being the dominant source of TG signa…
In this work we compare Monte Carlo (MC) simulations of electron transport properties with reflection electron energy loss measurements in diamond and graphite films. We assess the impact of different approximations of the dielectric response on the observables of interest for the characterization of carbon-based materials. We calculate the frequency-dependent dielectric response and energy loss function of these materials in two ways: a full ab initio approach, in which we carry out time-dependent density functional simulations in linear response for different momentum transfers, and a semi-c…
Current advances in ultrafast electron microscopy make it possible to combine optical pumping of a nanostructure and electron beam probing with subångstrom and femtosecond spatiotemporal resolution. We present a theory predicting that this technique can reveal a rich out-of-equilibrium dynamics of plasmon excitations in graphene and graphite samples. In a disruptive departure from the traditional probing of nanoscale excitations based on the identification of spectral features in the transmitted electrons, we show that measurement of angle-resolved, energy-integrated inelastic electron scatter…
We employed femtosecond time- and angle-resolved photoelectron spectroscopy to analyze the response of the electronic structure of the 122 Fe-pnictide parent compounds Ba/EuFe_2As_2 and optimally doped BaFe_{1.85}Co_{0.15}As_2 near the Γpoint to femtosecond optical excitation. We identify pronounced changes of the electron population within several 100 meV above and below the Fermi level, which we explain as combination of (i) coherent lattice vibrations, (ii) a hot electron and hole distribution, and (iii) transient modifications of the chemical potential. The response of the three different …
We present a finite-temperature density functional theory investigation of the nonequilibrium transient electronic structure of warm dense Li, Al, Cu, and Au created by laser excitation. Photons excite electrons either from the inner shell orbitals or from the valence bands according to the photon energy, and give rise to isochoric heating of the sample. Localized states related to the 3d orbital are observed for Cu when the hole lies in the inner shell 3s orbital. The electrical conductivity for these materials at nonequilibrium states is calculated using the Kubo-Greenwood formula. The chang…
We have performed time-resolved resonant x-ray scattering studies in the Lanthanide metal Dy to reveal the dynamic response of the helical order exchange coupling to injection of unpolarized spins. The observed spin dynamics are significantly slower than that exhibited by the ferromagnetic phase in Lanthanide metals and are strongly dependent on temperature and excitation fluence. This unique behavior results from transient changes in the shape of the conduction electron Fermi surface and subsequent scattering events that transfer the excitation to the core spin.
In this paper we study the excitation spectrum of single- and multi-layer graphene beyond the Dirac cone approximation. The dynamical polarizability of graphene is computed using a full $π$-band tight-binding model, considering the possibility of inter-layer hopping in the calculation. The effect of electron-electron interaction is considered within the random phase approximation. We further discuss the effect of disorder in the spectrum, which leads to a smearing of the absorption peaks. Our results show a redshift of the $π$-plasmon dispersion of single-layer graphene with respect to graphit…
A central prospect of antiferromagnetic spintronics is to exploit magnetic properties that are unavailable with ferromagnets. However, this poses the challenge of accessing such properties for readout and control. To this end, light-induced manipulation of the transient ground state, e.g. by changing the magnetic anisotropy potential, opens promising pathways towards ultrafast deterministic control of antiferromagnetism. Here, we use this approach to trigger a $\it{coherent}$ rotation of the entire long-range antiferromagnetic spin arrangement about a crystalline axis in $GdRh_2Si_2$ and demon…
Single-pulse strain-induced precessional dynamics of magnetization in Co-doped iron garnet
HFML-FELIX；Radboud University, Institute for Molecules and Materials（拉德堡德大学分子与材料研究所）；Russian Quantum Center, Skolkovo Innovation Center（俄罗斯量子中心斯科尔科沃创新中心）；Faculty of Physics, Lomonosov Moscow State University（莫斯科国立大学物理系）；Faculty of Physics, University of Bialytsok（比亚韦斯托克大学物理系）
The nature of the low-lying electronic states in carotenoids has been debated for decades. We use excitation-dependent transient absorption spectroscopy and comparison with published results on \b{eta}-carotene to demonstrate that the so-called S* feature in astaxanthin, echinenone and spheroidenone spectra is due to an impurity in the sample. Excitation at the absorption band-edge results in a transient absorption spectrum dominated by the pure S1 photo-induced absorption, with no contribution from impurities (S*). We find that this S1 absorption resembles the triplet excited-state absorption…
Optical-domain Transient Grating (TG) spectroscopy is a versatile background-free four-wave-mixing technique used to probe vibrational, magnetic and electronic degrees of freedom in the time domain. The newly developed coherent X-ray Free Electron Laser sources allow its extension to the X-ray regime. Xrays offer multiple advantages for TG: their large penetration depth allows probing the bulk properties of materials, their element-specificity can address core-excited states, and their short wavelengths create excitation gratings with unprecedented momentum transfer and spatial resolution. We …
The coherent optical response from 140~nm and 65~nm thick ZnO epitaxial layers is studied using transient four-wave-mixing spectroscopy with picosecond temporal resolution. Resonant excitation of neutral donor-bound excitons results in two-pulse and three-pulse photon echoes. For the donor-bound A exciton (D$^0$X$_\text{A}$) at temperature of 1.8~K we evaluate optical coherence times $T_2=33-50$~ps corresponding to homogeneous linewidths of $13-19~μ$eV, about two orders of magnitude smaller as compared with the inhomogeneous broadening of the optical transitions. The coherent dynamics is deter…
