A first-principles approach is introduced to calculate electron field emission characteristics of nanostructures, based on the nonequilibrium Green function technique combined with the density functional theory. The method employs atomic-like basis orbitals with large confinement radii and lithium anode to describe the electron density in the vacuum between the nanostructure tip and the anode, so takes the presence of emitted current into account. The simulation results on a capped single-walled carbon nanotube reproduce the experimental trend closely, in particular, the current saturation and the deviation from the Fowler-Nordheim behavior.
We present a novel formulation for calculating the transversal flexoelectric coefficient of nanostructures at finite deformations from first principles. Specifically, we introduce the concept of \emph{radial polarization} to make the coefficient a well-defined quantity for uniform bending deformations. We use the framework to calculate the flexoelectric coefficient for group IV atomic monolayers using density functional theory. We find that graphene's coefficient is significantly larger than previously reported, with a charge transfer mechanism that differs from other members of its group.
Metallic nanostructures (the nanofilms and nanowires) are widely used in electronic devices, and their thermal transport properties are crucial for heat dissipation. However, there are still gaps in understanding thermal transport in metallic nanostructures, especially regarding the size effect and validity of the Wiedemann-Franz law. In this work, we perform mode-by-mode first-principles calculations combining the Boltzmann transport equation to understand thermal transport in metallic nanostructures. We take the gold (Au) and tungsten (W) nanostructures as prototypes. It is found that when t…
The ability to harness light-matter interactions at the few-photon level plays a pivotal role in quantum technologies. Single photons - the most elementary states of light - can be generated on-demand in atomic and solid state emitters. Two-photon states are also key quantum assets, but achieving them in individual emitters is challenging because their generation rate is much slower than competing one-photon processes. We demonstrate that atomically thin plasmonic nanostructures can harness two-photon spontaneous emission, resulting in giant far-field two-photon production, a wealth of resonan…
First-principles calculations of thermal transport in homogeneous materials have reached remarkable predicting power. Modeling deterministically phonon transport in nanostructures, however, poses novel challenges; notably, it entails solving as many algebraic equations as the number of combinations of wave vectors in the discretized Brillouen and polarizations. We show that, within the relaxation time approximation of the Boltzmann transport equation (BTE), this issue is resolved by interpolating the phonon distributions in the vectorial phonon mean free paths (MFP) space. The coupling between…
The effective mass approximation (EMA) could be an efficient method for the computational study of semiconductor nanostructures with sizes too large to be handled by first-principles calculations, but the scheme to accurately and reliably introduce EMA parameters for given nanostructures remains to be devised. Herein, we report on an EMA approach based on first-principles-derived data, which enables accurate predictions of the optoelectronic properties of quantum nanostructures. For the CdS/ZnS core/shell quantum rods, for which we recently reported its experimental synthesis, we first carry o…
Enhanced room temperature ferromagnetism in nanostructured MoS2 flakes by hydrogen post-treatment: Combined experimental and first-principles-based studies
The uniform field assumption used to derive semi-classical cutoff energies of $10U_p$ for electron emission and $3.17U_p$ for high harmonic generation is applicable for ponderomotive amplitudes ($\propto Eλ^2$) much smaller than the field drop-off scale. For large wavelength and high field experiments at nanoscale structures this assumption may break down by predicting energies beyond the true classical energy limits. Here we provide generalized calculations for these cutoff energies by taking into account the spatial field drop-off. The modified cutoff energies vary significantly from the uni…
Thermoelectric power factors of defective scandium nitride nanostructures from first principles
IT4Innovations, VŠB – Technical University of Ostrava（俄斯特拉发理工大学 IT4 创新中心）；Department of Condensed Matter Physics, Faculty of Mathematics and Physics, Charles University（查理大学数学与物理学院凝聚态物理系）
We develop a theory for spontaneous decay of a quantum emitter (QE) situated near metal-dielectric structure supporting localized surface plasmons. If plasmon resonance is tuned close to the QE emission frequency, the emission is enhanced due to energy transfer from the QE to a localized plasmon mode followed by photon emission by plasmonic antenna. The emission rate is determined by intimate interplay between the plasmon coupling to radiation field and the Ohmic losses in metal. Here we develop plasmon Green's function approach that includes plasmon's interaction with radiation to obtain expl…
The plasmon-mediated manipulation of light-matter interaction in two-dimensional atomically transition-metal dichalcogenides (TMDs) critically depends on the design of plasmonic nanostructures to achieve the maximum optical field in TMDs. Here, a metal-isolator-metal Salisbury-type perfect absorber was fabricated to serve as a generator of the localized surface plasmons. The significant photoluminescence (PL) enhancement up to 60-fold was observed experimentally in the monolayer (ML) MoS2 on the top of this gold plasmonic hybrid nanostructures. Furthermore, the PL linear polarization can appro…
We suggest a new spin orientation mechanism for localized electrons: $dynamic~electron~spin~polarization~provided~by~nuclear~spin~fluctuations$. The angular momentum for the electrons is gained from the nuclear spin system via the hyperfine interaction in a weak magnetic field. For this the sample is illuminated by an unpolarized light, which directly polarizes neither the electrons nor the nuclei. We predict, that for the electrons bound in localized excitons 100% spin polarization can be reached in longitudinal magnetic fields of a few millitesla. The proof of principle experiment is perform…
Although the field of 2D materials has democratized materials science by making high quality samples accessible cheaply, due to the atomically thin nature of these systems, an integration with nanostructures is almost always required to obtain a significant optical response. Traditionally, these nanostructures are fabricated via electron beam lithography or focused ion beam milling, which are expensive and large area fabrication can be further time consuming. In order to overcome this problem, we report the integration of 2D semiconductors on a cost-effective and large area fabricated nanocone…
Thermal emission of localized surface phonons (LSPhs) from nanostructures of polaritonic materials is a promising mechanism for tuning the spectrum of near-field thermal radiation. Previous studies have theoretically shown that thermal emission of LSPhs results in narrow-band peaks in the near-field spectra, whose spectral locations can be modulated by changing the dimensions of the nanostructure. However, near-field thermal emission of LSPhs has not been experimentally explored yet. In this study, we measure the spectrum of near-field thermal radiation from arrays of 6H-silicon carbide (6H-Si…
