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We examined the field emission properties of lithium(Li)/oxygen(O)-co-terminated diamond (001) surface [C(001)-LiO] through real-time electron dynamics simulation under an applied field. The current emitted from this surface was found to be more than four-fold that emitted by an H-terminated (001) surface, the latter being a typical negative electron affinity system. This high performance is attributed to the Li layer, which bends the potential wall of O-induced electron pockets down in the direction of vacuum, thus facilitating electron emission. Detailed analysis of the emitted electrons and the profile of the self-consistent potential elucidated that the role of O atoms changes from an electron barrier on OH-terminated diamond surfaces to an outlet for electron emission on C(001)-LiO. [ABSTRACT FROM AUTHOR]

The coherence of electron dynamics in medium-sized molecules was examined by real-time time-dependent density functional theory calculations coupled with molecular dynamics. We observed laser-pulse-induced oscillation of the dipole and an increase in the potential energy of the molecules studied (benzene, naphthalene, and anthracene). Moreover, the second laser pulse with an antiphase optical field oscillation suppressed the dipole oscillation by interference and reduced the potential energy of the molecules. This interference was not observed in a simulation that freezes ion motion. Thus, the photoinduced coherent beat was maintained for a finite time in large molecules, and here, we discuss the effects of the molecular size and the influence of temperature on the coherence preservation. [ABSTRACT FROM AUTHOR]

We propose a transient interlayer compression in two-dimensional compound materials by using an intense IR laser resonant with the out-of-plane optical phonon mode (A2u mode). As a test case, we studied bilayer hexagonal boron nitride (h-BN), which is one of the compound layered materials. Excited state molecular dynamics calculations using time-dependent density functional theory show an 11.3% transient interlayer contraction of h-BN due to an interlayer dipole-dipole attraction of the laser-pumped A2u mode. These results are applicable to other layered compound materials. Such layered materials are a good material for nanospace chemistry, e.g., intercalating molecules and acting with them, and IR irradiation to contract the interlayer distance could provide a new route for chemical reactions under pressure. The duration of the contraction is at least 1 ps in the current simulation, which is observable by high-speed electron-beam diffraction measurements. [ABSTRACT FROM AUTHOR]

Nitrogen-vacancy (NV) centers in diamond have attracted a great deal of attention because of their possible use in information processing and electromagnetic sensing technologies. We examined the atomistic generation mechanism for the NV defect aligned in the [111] direction of C(111) substrates. We found that N is incorporated in the C bilayers during the lateral growth arising from a sequence of kink propagation along the step edge down to [112]. As a result, the atomic configuration with the N-atom lone-pair pointing in the [111] direction is formed, which causes preferential alignment of NVs. Our model is consistent with recent experimental data for perfect NV alignment in C(111) substrates. [ABSTRACT FROM AUTHOR]

Nitrogen-vacancy (NV) centers in diamond have attracted a great deal of attention because of their possible use in information processing and electromagnetic sensing technologies. We examined the atomistic generation mechanism for the NV defect aligned in the [111] direction of C(111) substrates. We found that N is incorporated in the C bilayers during the lateral growth arising from a sequence of kink propagation along the step edge down to [112]. As a result, the atomic configuration with the N-atom lone-pair pointing in the [111] direction is formed, which causes preferential alignment of NVs. Our model is consistent with recent experimental data for perfect NV alignment in C(111) substrates. [ABSTRACT FROM AUTHOR]

We demonstrate through extensive first-principles time-dependent density functional calculations that attractive van der Waals interaction between closed-shell atoms can be enhanced by light with constant spatial intensity. We illustrate this general phenomenon for a He dimer as a prototypical case of complex van der Waals interactions and show that when excited by light with a frequency close to the 1s → 2p He-atomic transition, an attractive force larger than 7 pN is produced. This force gain is manifested as a larger acceleration of He-He contraction under an optical field. The concerted dynamical motions of the He atoms together with polarity switching of the chargeinduced dipole cause the contraction of the dimer. These findings are relevant for the photo-induced control of weakly bonded molecular species, either in gas phase or in solution. [ABSTRACT FROM AUTHOR]

Tin-vacancy (Sn-V) color centers were created in diamond via ion implantation and subsequent high-temperature annealing up to 2100°C at 7.7 GPa. The first-principles calculation suggested that a large atom of tin can be incorporated into a diamond lattice with a split-vacancy configuration, in which a tin atom sits on an interstitial site with two neighboring vacancies. The Sn-V center showed a sharp zero phonon line at 619 nm at room temperature. This line split into four peaks at cryogenic temperatures, with a larger ground state splitting (~850 GHz) than that of color centers based on other group-IV elements, i.e., silicon-vacancy (Si-V) and germanium-vacancy (Ge-V) centers. The excited state lifetime was estimated, via Hanbury Brown-Twiss interferometry measurements on single Sn-V quantum emitters, to be ~5 ns. The order of the experimentally obtained optical transition energies, compared with those of Si-V and Ge-V centers, was in good agreement with the theoretical calculations. [ABSTRACT FROM AUTHOR]

We use time-dependent density functional theory to study laser-pulse induced decomposition of H2O molecules above the two-dimensional (2D) materials graphene, hexagonal boron nitride, and graphitic carbon nitride. We examine femtosecond-laser pulses with a full width at half maximum of 10 or 20 fs for laser-field intensity and wavelengths of 800 or 400 nm by varying the intensity of the laser field from 5 to 9 V/Å, with the corresponding range of fluence per pulse up to 10.7J/cm². For a H2O molecule above the graphitic sheets, the threshold for laser-field H2O decomposition is reduced by more than 20% compared with that of an isolated H2O molecule. We also show that hole doping enhances the water adsorption energy above graphene. The present results indicate that the graphitic materials should support laser-induced chemistry and that other 2D materials that can enhance laser-induced H2O decomposition should be investigated. [ABSTRACT FROM AUTHOR]

We have used first-principles simulations based on time-dependent density functional theory to show that short laser pulses can trigger preferential hydrogen desorption from the upper or lower side of suspended graphane (H-terminated graphene). This control is achieved by using intense ultrashort p-polarized laser pulses (~2 fs) with an asymmetric time envelope. The dynamical Stark effect induced by the pulse creates an asymmetric charge distribution and force field on the H ions, even at low laser fluence. At finite temperatures the carbon-hydrogen stretching softens, favoring H desorption from one side. This transient geometry can be modified by halogen functionalization, which results in a two-dimensional dipolar structure. [ABSTRACT FROM AUTHOR]

Recently, single-layer group III monochalcogenides have attracted both theoretical and experimental interest at their potential applications in photonic devices, electronic devices, and solar energy conversion. Excited by this, we theoretically design two kinds of highly stable single-layer group IV-V (IV=Si,Ge, and Sn; V=N and P) and group V-IV-III-VI (IV=Si,Ge, and Sn; V=N and P; III=Al,Ga, and In; VI=O and S) compounds with the same structures with single-layer group III monochalcogenides via first-principles simulations. By using accurate hybrid functional and quasiparticle methods, we show the single-layer group IV-V and group V-IV-III-VI are indirect bandgap semiconductors with their bandgaps and band edge positions conforming to the criteria of photocatalysts for water splitting. By applying a biaxial strain on single-layer group IV-V, single-layer group IV nitrides show a potential on mechanical sensors due to their bandgaps showing an almost linear response for strain. Furthermore, our calculations show that both single-layer group IV-V and group V-IV-III-VI have absorption from the visible light region to far-ultraviolet region, especially for single-layer SiN-AlO and SnN-InO, which have strong absorption in the visible light region, resulting in excellent potential for solar energy conversion and visible light photocatalytic water splitting. Our research provides valuable insight for finding more potential functional two-dimensional semiconductors applied in optoelectronics, solar energy conversion, and photocatalytic water splitting. [ABSTRACT FROM AUTHOR]

Recently, the two-dimensional (2D) semiconductors arsenene and antimonene, with band gaps larger than 2.0 eV, have attracted tremendous interest, especially for potential applications in optoelectronic devices with a photoresponse in the blue and UV range. Motivated by this exciting discovery, types of highly stable wide-band-gap 2D nitride semiconductors were theoretically designed. We propose single-layer 1T-XN2 (X=S, Se, and Te) via first-principles simulations. We compute 1T-XN2 (X=S, Se, and Te) with indirect band gaps of 2.825, 2.351, and 2.336 eV, respectively. By applying biaxial strain, they are able to induce the transition from a wide-band-gap semiconductor to a metal, and the range of absorption spectra of 1T-XN2 (X=S, Se, and Te) obviously extend from the ultraviolet region to the blue-purple light region. With an underlying graphene, we find that 1T-XN2 can completely shield the light absorption of graphene in the range of 1-1.6 eV. Our research paves the way for optoelectronic devices working under blue or UV light, and mechanical sensors based on these 2D crystals. [ABSTRACT FROM AUTHOR]

Compared with conventional metal plasmonic materials, surface plasmons in graphene are advantageous in terms of higher confinement, relative low loss, flexible featuring, and good tunability. However, the working frequencies of the pristine graphene (undoped graphene) surface plasmons are located in the terahertz and infrared regions, which limit their applications. Here we show high-frequency plasmons in nitrogen (N)-doped graphene nanostructures investigated by time-dependent density functional theory. We found the optical absorption strength of systems containing two layers to be more than twofold stronger than that of systems with monolayers. The optical absorption strength increases as the interlayer distance increases, and the absorption spectra are red-shifted for impulse excitations polarized in the armchair edge direction (x axis). For microstructures of more than two layers, the optical absorption strength increases as number of layers of the N-doped graphene nanostructures increases. In addition, when the number of layers becomes elevated at low-energy resonances, the absorption spectra are seen to blue-shift. The plasmon energy resonance points are located in the visible and ultraviolet regions. The N-doped graphene provides an effective strategy for nanoscale plasmon devices in the visible and ultraviolet regions, despite their weaker absorption intensities when compared with the pristine graphene. [ABSTRACT FROM AUTHOR]