Electronic orderings of charges, orbitals and spins are observed in many strongly correlated electron materials, and revealing their dynamics is a critical step toward understanding the underlying physics of important emergent phenomena. Here we use
time-resolved resonant soft x-ray scattering spectroscopy to probe the dynamics of antiferromagnetic spin ordering in the manganite Pr$_{0.7}$Ca$_{0.3}$MnO$_3$ following ultrafast photo-exitation. Our studies reveal a glass-like recovery of the spin ordering and a crossover in the dimensionality of the restoring interaction from quasi-1D at low pump fluence to 3D at high pump fluence. This behavior arises from the metastable state created by photo-excitation, a state characterized by spin disordered metallic droplets within the larger charge- and spin-ordered insulating domains. Comparison with time-resolved resistivity measurements suggests that the collapse of spin ordering is correlated with the insulator-to-metal transition, but the recovery of the insulating phase does not depend on the re-establishment of the spin ordering.
We present resonant soft X-ray scattering (RSXS) results from small band width manganites (Pr,Ca)MnO$_3$, which show that the CE-type spin ordering (SO) at the phase boundary is stabilized only below the canted antiferromagnetic transition temperatur
e and enhanced by ferromagnetism in the macroscopically insulating state (FM-I). Our results reveal the fragility of the CE-type ordering that underpins the colossal magnetoresistance (CMR) effect in this system, as well as an unexpected cooperative interplay between FM-I and CE-type SO which is in contrast to the competitive interplay between the ferromagnetic metallic (FM-M) state and CE-type ordering.
By performing angle-resolved photoemission spectroscopy of the bilayer colossal magnetoresistive (CMR) manganite, $La_{2-2x}Sr_{1+2x}Mn_{2}O_{7}$, we provide the complete mapping of the Fermi level spectral weight topology. Clear and unambiguous bila
yer splitting of the in-plane 3d$_{x^2-y^2}$ band, mapped throughout the Brillouin zone, and the full mapping of the 3d$_{3z^2-r^2}$ band are reported. Peculiar doping and temperature dependencies of these bands imply that as transition from the ferromagnetic metallic phase approaches, either as a function of doping or temperature, coherence along the c-axis between planes within the bilayer is lost, resulting in reduced interplane coupling. These results suggest that interplane coupling plays a large role in the CMR transition.
We study the stability of various kinds of graphene samples under soft X-ray irradiation. Our results show that in single layer exfoliated graphene (a closer analogue to two dimensional material), the in-plane carbon-carbon bonds are unstable under X
-ray irradiation, resulting in nanocrystalline structures. As the interaction along the third dimension increases by increasing the number of graphene layers or through the interaction with the substrate (epitaxial graphene), the effect of X-ray irradiation decreases and eventually becomes negligible for graphite and epitaxial graphene. Our results demonstrate the importance of the interaction along the third dimension in stabilizing the long range in-plane carbon-carbon bonding, and suggest the possibility of using X-ray to pattern graphene nanostructures in exfoliated graphene.
The capability to control the type and amount of charge carriers in a material and, in the extreme case, the transition from metal to insulator is one of the key challenges of modern electronics. By employing angle resolved photoemission spectroscopy
(ARPES) we find that a reversible metal to insulator transition and a fine tuning of the charge carriers from electrons to holes can be achieved in epitaxial bilayer and single layer graphene by molecular doping. The effects of electron screening and disorder are also discussed. These results demonstrate that epitaxial graphene is suitable for electronics applications, as well as provide new opportunities for studying the hole doping regime of the Dirac cone in graphene.
The interplay of electron-phonon (el-ph) and electron-electron (el-el) interactions in epitaxial graphene is studied by directly probing its electronic structure. We found a strong coupling of electrons to the soft part of the A1g phonon evident by a
kink at 150+/-15 meV, while the coupling of electrons to another expected phonon E2g at 195 meV can only be barely detected. The possible role of the el-el interaction to account for the enhanced coupling of electrons to the A1g phonon, and the contribution of el-ph interaction to the linear imaginary part of the self energy at high binding energy are also discussed. Our results reveal the dominant role of the A1g phonon in the el-ph interaction in graphene, and highlight the important interplay of el-el and el-ph interactions in the self energy of graphene.
The pi bands of epitaxially grown graphene are studied by using high resolution angle resolved photoemission spectroscopy. Clear deviations from the conical dispersion expected for massless Dirac fermions and an anomalous increase of the scattering r
ate are observed in the vicinity of the Dirac point energy. Possible explanations for such anomalies are discussed in terms of many-body interactions and the opening of a gap. We present detailed experimental evidences in support of the gap scenario. This finding reveals a fundamental intrinsic property of epitaxial graphene and demonstrates the possibility of engineering the band gap in epitaxial graphene.
We studied the effect of quantum confinement on the size of the band gap in single layer epitaxial graphene. Samples with different graphene terrace sizes are studied by using low energy electron microscopy (LEEM) and angle-resolved photoemission spe
ctroscopy (ARPES). The direct correlation between the terrace size extracted from LEEM and the gap size extracted from ARPES shows that quantum confinement alone cannot account for the large gap observed in epitaxial graphene samples.
Graphene has shown great application potentials as the host material for next generation electronic devices. However, despite its intriguing properties, one of the biggest hurdles for graphene to be useful as an electronic material is its lacking of
an energy gap in the electronic spectra. This, for example, prevents the use of graphene in making transistors. Although several proposals have been made to open a gap in graphenes electronic spectra, they all require complex engineering of the graphene layer. Here we show that when graphene is epitaxially grown on the SiC substrate, a gap of ~ 0.26 is produced. This gap decreases as the sample thickness increases and eventually approaches zero when the number of layers exceeds four. We propose that the origin of this gap is the breaking of sublattice symmetry owing to the graphene-substrate interaction. We believe our results highlight a promising direction for band gap engineering of graphene.
