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The hot carriers generated by plasmon damping hold significant potential for photoelectric conversion and photocatalysis. Despite numerous experiments and theoretical analyses, the precise role of plasmonic hot carriers in such dynamical processes has not been well understood. Here we present a theory of plasmonic photocatalysis based on the microscopic model of electron-vibrational coupling and the vibrational heating mechanism. The nonthermal hot carrier distribution was derived and treated on equal footing with the thermal Fermi-Dirac distribution. The inelastic rates of vibrational excitations were calculated including the effect of multiple electronic transitions. As an example of application, the O$_2$ dissociation on silver nanoparticles was explored with focus on the temperature- and light-intensity dependences. The dissociation rate evolves from a linear regime into a superlinear regime due to the onset of vibrational heating induced by hot carriers. In the nonlinear regime, nonthermal hot carriers greatly promote molecular dissociation. Our findings provide insight into plasmonic photocatalysis, and paves the way for harnessing light energies in the nonthermal regime.

Intervalley scattering involves microscopic processes that electrons are scattered by atomic-scale defects on nanometer length scales. Although central to our understanding of electronic properties of materials, direct characterization and manipulation of range and strength of the intervalley scattering induced by an individual atomic defect have so far been elusive. Using scanning tunneling microscope, we visualized and controlled intervalley scattering from an individual monovacancy in graphene. By directly imaging the affected range of intervalley scattering of the monovacancy, we demonstrated that it is inversely proportional to the energy, i.e., it is proportional to the wavelength of massless Dirac Fermions. A giant electron-hole asymmetry of the intervalley scattering is observed because that the monovacancy is charged. By further charging the monovacancy, the bended electronic potential around the monovacancy softened the scattering potential, which, consequently, suppressed the intervalley scattering of the monovacancy., Comment: 18 pages, 4 figures

Plasmon opens up the possibility to efficiently couple light and matter at sub-wavelength scales. In general, the plasmon frequency is dependent of carrier density. This dependency, however, renders fundamentally a weak plasmon intensity at low frequency, especially for Dirac plasmon (DP) widely studied in graphene. Here we demonstrate a new type of DP, excited by a Dirac nodal-surface state, which exhibits an anomalously density-independent frequency. Remarkably, we predict realization of anomalous DP (ADP) in 1D topological electrides, such as Ba3CrN3 and Sr3CrN3, by first-principles calculations. The ADPs in both systems have a density-independent frequency and high intensity, and their frequency can be tuned from terahertz to mid-infrared by changing the excitation direction. Furthermore, the intrinsic weak electron-phonon coupling of anionic electrons in electrides affords an added advantage of ultra-low phonon-assisted damping and hence a long lifetime of the ADPs. Our work paves the way to developing novel plasmonic and optoelectronic devices by combining topological physics with electride materials.

Removing a single-carbon vacancy introduces (quasi-)localized states for both and electrons in graphene. Interactions between the localized dangling bond and quasilocalized electrons of a single-carbon vacancy in graphene are predicted to control its magnetism. However, experimentally confirming this prediction through manipulating the interactions between the and electrons remains an outstanding challenge. Here we report the manipulation of magnetism of individual single-carbon vacancy in graphene by using a scanning tunnelling microscopy (STM) tip. Our spin-polarized STM measurements, complemented by density functional theory calculations, indicate that interactions between the localized and quasilocalized electrons could split the electrons into two states with opposite spins even when they are well above the Fermi level. Via the STM tip, we successfully manipulate both the magnitude and direction of magnetic moment of the electrons with respect to that of the electrons. Three different magnetic states of the single-carbon vacancy, exhibiting magnetic moments of about 1.6, 0.5, and 0 respectively, are realized in our experiment., Comment: 4 figures

The past decade has witnessed numerous discoveries of two-dimensional (2D) semimetals and insulators, whereas 2D metals are rarely identified. Borophene, a monolayer boron sheet, has recently emerged as a perfect 2D metal with unique structure and electronic properties. Here we study collective excitations in borophene, which exhibit two major plasmon modes with low damping rates extending from infrared to ultraviolet regime. The anisotropic 1D plasmon originates from electronic excitations of tilted Dirac cones in borophene, analogous to that in heavily doped Dirac semimetals. These features make borophene promising to realize directional polariton transportation and broadband optical communications for next-generation optoelectronic devices.

An atomistic insight into potential barrier formation and band bending at the interface between a metal and an n-type semiconductor is achieved by ab initio simulations and model analysis of a prototype Schottky diode, i.e., niobium doped rutile titania in contact with gold (Au/Nb:TiO$_2$). The local Schottky barrier height is found to vary between 0 and 1.26 eV depending on the position of the dopant. The band bending is caused by a dopant induced dipole field between the interface and the dopant site, whereas the pristine Au/TiO$_2$ interface does not show any band bending. These findings open the possibility for atomic scale optimization of the Schottky barrier and light harvesting in metal-semiconductor nanostructures.