- 标题
- 摘要
- 关键词
- 实验方案
- 产品
-
Third-Order Unitary Coupled Cluster (UCC3) for Excited Electronic States: Efficient Implementation and Benchmarking
摘要： The efficient implementation of the third-order unitary coupled-cluster scheme (UCC3) for the calculation of excited electronic states is reported. The UCC3 scheme and its second-order UCC2 variant have been benchmarked and compared to Jacquemin’s recently introduced as well as Thiel’s well-established benchmark sets for excitation energies and oscillator strengths. For the latter, the calculation of 134 excited singlet and 71 excited triplet states of 28 small to medium-sized organic molecules has revealed that UCC2 exhibits a mean error and standard deviation of 0.36 ± 0.41 eV for singlet states and 0.22 ± 0.21 eV for triplet states, whereas UCC3 revealed an accuracy of 0.06 ± 0.27 eV for singlet and ?0.22 ± 0.15 eV for triplet states. Additionally, the oscillator strengths obtained with effective transition moments correct through second order in perturbation theory are in very good agreement with literature data.
关键词： perturbation theory,unitary coupled-cluster,oscillator strengths,excited electronic states,benchmarking
更新于2025-09-23 15:21:01
-
Inactivation of Bacteria during Stimulation of Sensitizers with High-Power Nanosecond Laser Pulses
摘要： The results of a study of photoinactivation of bacteria during stimulation of sensitizers with nanosecond laser pulses with a power density within 1–30 MW/cm2 are presented. The irreversible damage to living cells by shock waves developed during the formation and collapse of vapor bubbles in locally heated microregions of the medium is discussed. The local heating of the medium occurred due to heat release during nonradiative relaxation of high electronic states of sensitizer molecules.
关键词： local heating,highly excited electronic states of molecules,photoinactivation of bacteria,acoustic waves
更新于2025-09-16 10:30:52
-
Broadening of van Hove Singularities Measured by Photoemission Spectroscopy of Single and Mixed Chirality Single-Walled Carbon Nanotubes
摘要： The occupied valence electronic states of single walled carbon nanotubes (SWCNTs) are responsible for their optoelectronic properties and are unique for each SWCNT chirality. Photoemission spectroscopy (PES) is one of the few methods capable of directly measuring the electron density in the valence states of materials but there are only few reports which have observed the valence states of SWCNTs and no examples for single-chirality SWCNTs. Here we prepare single and mixed chirality SWCNT films and characterise their valence states using PES. Chirality pure SWCNTs were isolated using both gel permeation chromatography and ssDNA facilitated aqueous two phase extraction from starting materials consisting of mixed chirality species. Chirality separation and purity was confirmed with UV-Vis-nIR absorption spectroscopy. SWCNT films were prepared for the single chirality species (10,3), (7,6), (7,3), (6,5), (8,3), (9,1) along with SWCNT chirality mixture of metallic and semiconducting SWCNTs, and as-synthesised mixtures possessing a range of SWCNT diameter. PES using synchrotron radiation was completed for all samples with survey and C 1s core level spectra obtained to confirm SWCNT coverage, defect level and purity. Valence band PES was obtained to characterise the valence electronic states and showed significant broadening of the signal, in comparison to calculated density of states, which could not be accounted for by instrument resolution. An inverse diameter dependence of the broadening was observed with greater broadening for smaller diameter SWCNTs. The broadening is hypothesised to be related to the photohole lifetime which was found to be significantly longer for wide diameter SWCNTs. The diameter dependence of the broadening and photohole lifetimes is discussed in terms of both Tomonaga-Luttinger and Landau theory of Fermi liquids.
关键词： chirality,valence electronic states,single-walled carbon nanotubes,van Hove singularities,photoemission spectroscopy
更新于2025-09-16 10:30:52
-
Local valence electronic states of silicon (sub)oxides on HfO2/Si-(sub)oxide/Si(110) and HfSi2/Si-(sub)oxide/Si(110) Islands
摘要： The effect on the local valence electronic states of Sin+ suboxide components (n = 2, 3, and 4) of hafnium deposited on a low-index Si(110) substrate is investigated by Si-L23VV Auger electron Sin+-2p photoelectron coincidence spectroscopy (Si-L23VV-Sin+-2p APECS), and the chemical states and stabilities are discussed. Hafnium-covered Si(110) is immediately oxidized to HfO2 and SiO2 because hafnium serves as an effective catalyst for Si oxidation. Therefore, a HfO2/Sin+-(sub)oxide/Si(110) [HfO2/Sin+/Si(110)] structure is easily formed (n = 1, 2, 3, and 4). Oxygen diffusion from HfO2 layers toward the Si(110) substrate is promoted by annealing at 923 K. Oxygen atom desorption from the HfO2/Sin+/Si(110) surface occurs after annealing at 1073 K, and HfSi2 islands (i-HfSi2) are formed with a partly exposed Si(110)-16 × 2 double domain (DD) surface. i-HfSi2 shows low reactivity toward O2 molecules, whereas the exposed Si(110)-16 × 2 DD surface is immediately oxidized. Here, a i-HfSi2/Sin+-(sub)oxide/Si(110) structure is formed. Furthermore, we measure the Si-L23VV-Sin+-2p APECS spectra of Sin+ in the HfO2/Sin+/Si(110) and the i-HfSi2/Sin+/Si(110) structures (n = 2, 3, and 4) to evaluate the local valence electronic states of the Sin+ (sub)oxide components. The binding energy at the valence band maximum (BEVBM) of Sin+ in the i-HfSi2/Sin+/Si(110) structure is lower than 1.5 ± 0.7 eV as compared to that in the HfO2/Sin+/Si(110) structure (n = 2, 3, and 4). The local valence electric states of the nearest neighbors and the second neighbors through oxygen of Sin+ are determined to affect those of the Sin+ atom (n = 2, 3, and 4). The Sin+ atoms in the i-HfSi2/Sin+/Si(110) structure can directly bond to hafnium atoms as the nearest neighbors and most commonly have Sim+ atoms in lower ionic valence states as second neighbors (m < 4), whereas the Sin+ atoms in the HfO2/Sin+/Si(110) structure cannot form this bond. In addition, the existence of Hf silicide and Si in lower ionic valence states can reduce the band gap of the HfO2/Si(110) structure.
关键词： High-dielectric-constant material,X-ray photoelectron spectroscopy,Local valence electronic states at surface and interface,Synchrotron radiation,Auger photoelectron coincidence spectroscopy,Metal-insulator-semiconductor structure
更新于2025-09-11 14:15:04
-
AgI-BiOI-graphene composite photocatalysts with enhanced interfacial charge transfer and photocatalytic H2 production activity
摘要： BiOI-based photocatalysts were proved to exhibit photocatalytic H2 production activity. AgI-BiOI-graphene showed better H2 production activity than BiOI and BiOI-graphene. The surface chemistry, electronic property, phase structure, morphology, optical property and photocatalytic performance of these photocatalysts were studied. The interfacial electronic states of the photocatalysts were investigated through their C K-edge near-edge X-ray-absorption fine-structure (NEXAFS) spectra. Based on the in situ NEXAFS spectra measured with and without illumination, a mechanism about the transport of photoelectron from AgI to graphene through BiOI is proposed for the photocatalytic H2 production process. The incorporation of graphene restricted the three-dimensional self-assembly of BiOI nanocrystals and led to the formation of less extensively crystallized BiOI domains through a confined-space effect. Addition of AgNO3 precursor altered the crystal structure of BiOI from flower-like to horizontally stacked flat plates. The results of NEXAFS spectra, photoluminescence spectra and photocurrent tests reveal that the improved photocatalytic activity of the AgI-BiOI-graphene photocatalyst is attributable to the interfacial interaction among AgI, BiOI and graphene, which enhanced the separation of photogenerated electrons to generate H2. AgI-BiOI-graphene photocatalyst was a stable photocatalyst for the production of H2. After three cycles, 86 % activity of recycled photocatalysts was retained.
关键词： X-ray absorption spectra,Near edge X-ray absorption fine structure,Interfacial electronic states,Photocatalytic H2 production,BiOI
更新于2025-09-10 09:29:36
-
Nanolayer Research || Nanolayer Analysis by Photoelectron Spectroscopy
摘要： Photoelectron spectroscopy (PES), or photoemission spectroscopy, is one of the most important and useful techniques for investigating electronic and chemical states in solids, especially in nanolayers because of its high-energy resolution and surface sensitivity [1–5]. The physics behind PES is an application of the photoelectric effect. Through photoelectric ionization by irradiating samples with X-rays, vacuum ultraviolet (VUV) or ultraviolet (UV) light, the energies of the emitted photoelectrons are characteristic of their original electronic and chemical states. Therefore PES is one of the most sensitive and accurate techniques for measuring the energies and shapes of electronic states and molecular orbitals. X-ray photoelectron spectroscopy (XPS) was developed by Kai Siegbahn in 1957 and is used to study the energy levels of atomic core electrons, mainly in solids. Siegbahn referred to the technique as electron spectroscopy for chemical analysis (ESCA), since chemical structure can be determined by analyzing the core levels with small chemical shifts depending on the chemical environment of the atom. Siegbahn was awarded the Nobel Prize in Physics in 1981.
关键词： PES,Kai Siegbahn,ESCA,XPS,Photoelectron spectroscopy,photoelectric effect,electronic states,nanolayers,chemical states
更新于2025-09-09 09:28:46
-
Evidence of Pure Spin-Current Generated by Spin Pumping in Interface Localized States in Hybrid Metal-Silicon-Metal Vertical Structures
摘要： Due to the difficulty to grow high quality semiconductors on ferromagnetic metals, the study of spin diffusion transport in Si was only limited to lateral geometry devices. In this work, by using ultra-high vacuum wafer-bonding technique, we have successfully fabricated metal-semiconductor-metal CoFeB/MgO/Si/Pt vertical structures. We hereby demonstrate pure spin-current injection and transport in the perpendicular current flow geometry over a distance larger than 2μm in n-type Si at room temperature. In those experiments, a pure propagating spin-current is generated via ferromagnetic resonance spin-pumping and converted into a measurable voltage by using the inverse spin-Hall effect occurring in the top Pt layer. A systematic study by varying both Si and MgO thicknesses reveals the important role played by the localized states at the MgO/Si interface for the spin-current generation. Proximity effects involving indirect exchange interactions between the ferromagnet and the MgO/Si interface states appears to be a prerequisite to establish the necessary out-of-equilibrium spin-population in Si under the spin-pumping action.
关键词： localized electronic states,wafer-bonding,inverse spin Hall effect,spin-current,spin pumping
更新于2025-09-09 09:28:46
-
Tunnel spectroscopy of localised electronic states in hexagonal boron nitride
摘要： Hexagonal boron nitride is a large band gap layered crystal, frequently incorporated in van der Waals heterostructures as an insulating or tunnel barrier. Localised states with energies within its band gap can emit visible light, relevant to applications in nanophotonics and quantum information processing. However, they also give rise to conducting channels, which can induce electrical breakdown when a large voltage is applied. Here we use gated tunnel transistors to study resonant electron tunnelling through the localised states in few atomic-layer boron nitride barriers sandwiched between two monolayer graphene electrodes. The measurements are used to determine the energy, linewidth, tunnelling transmission probability, and depth within the barrier of more than 50 distinct localised states. A three-step process of electron percolation through two spatially separated localised states is also investigated.
关键词： quantum information processing,hexagonal boron nitride,tunnel spectroscopy,localised electronic states,graphene
更新于2025-09-04 15:30:14