Analysis of the injection layer of PTCDA in OLEDs using x-ray photoemission spectroscopy and atomic force microscopy

Through the investigation of the sample surface and interface of 3, 4, 9, 10-perylenetetracarboxylic dianhydride （PTCDA）/indium-tin-oxide （ITO） thin films using atomic force microscopy, it has been found that the surface is complanate, the growth is uniform and the defects cover basically the surface of ITO. Furthermore, the number of pinholes is small. The analysis of the sample surface and interface further verifies this result by using x-ray photoemission spectroscopy. At the same time, PTCDA is found to have the ability of restraining the diffusion of chemical constituents from ITO to the hole transport layer, which is beneficial to the improvement of the performance and the useful lifetime of the organic light emitting diodes （OLEDs）.

X-ray Photoemission Spectroscopy Studies of the Semiconducting Molybdenum Purple Bronze Bi_(0.2)MoO_3

The electronic structure of the quasi-two-dimensional （2D） semiconducting molybdenum purple bronze Bio.2MoO3 was presented by X-ray photoemission spectroscopy. The valence band of Bio.2MoO3 is made up of Opπ nonbonding level, π and a bonding bands. The peak at 1.5 eV and the shoulder at 0.5 eV in the forbidden band may be formed from the non-bonding dxy orbitals of some Mo atoms. The O1s core-level spectrum demonstrates the presence of two inequivalent bonds of oxygen ions in Bio.2MoO3. Bi4f core-level spectrum shows two bonding characters of Bi atoms in bismuth molybdenum single crystal. Mo3d core-level spectrum confirms two kinds of valence states of Molybdenum （Mo^＋5 and Mo^＋6）. Ar^＋ ion irradiation induces more significant distortion of MoO6 octahedra.

Negligible normal fluid in superconducting state of heavily overdoped Bi_(2)Sr_(2)CaCu_(2)O_(8+δ) detected by ultra-low temperature angle-resolved photoemission spectroscopy

In high temperature cuprate superconductors,it was found that the superfluid density decreases with the increase of hole doping.One natural question is whether there exists normal fluid in the superconducting state in the overdoped region.In this paper,we have carried out high-resolution ultra-low temperature laser-based angle-resolved photoemission measurements on a heavily overdoped Bi2212 sample with a T_(c) of 48 K.We find that this heavily overdoped Bi2212 remains in the strong coupling regime with 2Δ_(0)/(k_(B)T_(c))=5.8.The single-particle scattering rate is very small along the nodal direction(~5 meV) and increases as the momentum moves from the nodal to the antinodal regions.A hard superconducting gap opening is observed near the antinodal region with the spectral weight at the Fermi level fully suppressed to zero.The normal fluid is found to be negligibly small in the superconducting state of this heavily overdoped Bi2212.These results provide key information to understand the high T_(c) mechanism in the cuprate superconductors.

In situ infrared, Raman and X-ray spectroscopy for the mechanistic understanding of hydrogen evolution reaction

Hydrogen production by water reduction reactions has received considerable attention because hydrogen is considered a clean-energy carrier,key for a sustainable energy future.Computational methods have been widely used to study the reaction mechanism of the hydrogen evolution reaction(HER),but the calculation results need to be supported by experimental results and direct evidence to confirm the mechanistic insights.In this review,we discuss the fundamental principles of the in situ spectroscopic strategy and a theoretical model for a mechanistic understanding of the HER.In addition,we investigate recent studies by in situ Fourier transform infrared(FTIR),Raman spectroscopy,and X-ray absorption spectroscopy(XAS) and cover new findings that occur at the catalyst-electrolyte interface during HER.These spectroscopic strategies provide practical ways to elucidate catalyst phase,reaction intermediate,catalyst-electrolyte interface,intermediate binding energy,metal valency state,and coordination environment during HER.

A seven-crystal spectrometer for high-energy resolution X-ray spectroscopy at Shanghai Synchrotron Radiation Facility

A Johann-type X-ray spectrometer was successfully developed at the hard X-ray branch(in-vacuum undulator with a 24-mm periodic length)of the energy material beamline(E-line)at the Shanghai Synchrotron Radiation Facility(SSRF).This spectrometer was utilized to implement X-ray emission spectroscopy(XES),high-energy resolution fluorescence-detected X-ray absorption spectroscopy(HERFD-XAS),and resonant inelastic X-ray scattering.Seven spherically bent crystals were positioned on the respective vertical 500-mm-diameter Rowland circles,adopting an area detector to increase the solid angle to 1.75%of 4πsr,facilitating the study of low-concentrate systems under complex reaction conditions.Operated under the atmosphere pressure,the spectrometer covers the energy region from 3.5 to 18 keV,with the Bragg angle ranging from 73°to 86°during vertical scanning.It offers a promised energy resolution of sub-eV(XES)and super-eV(HERFD-XAS).Generally,these comprehensive core-level spectroscopy methods based on hard X-rays at the E-line with an extremely high photon flux can meet the crucial requirements of a green energy strategy.Moreover,they provide substantial support for scientific advances in fundamental research.

Angle-resolved photoemission study of NbGeSb with non-symmorphic symmetry

We investigate the electronic structure of NbGeSb with non-symmorphic symmetry.We employ angle-resolved photoemission spectroscopy(ARPES)to observe and identify the bulk and surface states over the Brillouin zone.By utilizing high-energy photons,we identify the bulk Fermi surface and bulk nodal line along the direction X–R,while the Fermi surface of the surface state is observed by using low-energy photons.We observe the splitting of surface bands away from the high-symmetry point X.The density functional theory calculations on bulk and 1 to 5-layer slab models,as well as spin textures of NbGeSb,verify that the band splitting could be attributed to the Rashba-like spin–orbit coupling caused by space-inversion-symmetry breaking at the surface.These splitted surface bands cross with each other,forming two-dimensional Weyl-like crossings that are protected by mirror symmetry.Our findings provide insights into the two-dimensional topological and symmetry-protected band inversion of surface states.

Optical manipulation of the topological phase in ZrTe_(5) revealed by time-and angle-resolved photoemission

High-resolution time-and angle-resolved photoemission measurements were conducted on the topological insulator ZrTe_(5).With strong femtosecond photoexcitation,a possible ultrafast phase transition from a weak to a strong topological insulating phase was experimentally realized by recovering the energy gap inversion in a time scale that was shorter than 0.15 ps.This photoinduced transient strong topological phase can last longer than 2 ps at the highest excitation fluence studied,and it cannot be attributed to the photoinduced heating of electrons or modification of the conduction band filling.Additionally,the measured unoccupied electronic states are consistent with the first-principles calculation based on experimental crystal lattice constants,which favor a strong topological insulating phase.These findings provide new insights into the longstanding controversy about the strong and weak topological properties in ZrTe_(5),and they suggest that many-body effects including electron–electron interactions must be taken into account to understand the equilibrium weak topological insulating phase in ZrTe_(5).

Theoretical characterization of the adsorption configuration of pyrrole on Si(100)surface by x-ray spectroscopy

The possible configurations of pyrrole absorbed on a Si(100)surface have been investigated by x-ray photoelectron spectroscopy(XPS)and near-edge x-ray absorption fine structure(NEXAFS)spectra.The C-1s XPS and NEXAFS spectra of these adsorption configurations have been calculated by using the density functional theory(DFT)method and fullcore hole(FCH)approximation to investigate the relationship between the adsorption configurations and the spectra.The result shows that the XPS and NEXAFS spectra are structurally dependent on the configurations of pyrrole absorbed on the Si(100)surface.Compared with the XPS,the NEXAFS spectra are relatively sensitive to the adsorption configurations and can accurately identify them.The NEXAFS decomposition spectra produced by non-equivalent carbon atoms have also been calculated and show that the spectral features vary with the diverse types of carbon atoms and their structural environments.

Intrinsic electronic structure and nodeless superconducting gap of YBa_(2)Cu_(3)O_(7)-σ observed by spatially-resolved laser-based angle resolved photoemission spectroscopy

The spatially-resolved laser-based high-resolution angle resolved photoemission spectroscopy(ARPES) measurements have been performed on the optimally-doped YBa_(2)Cu_(3)O_(7)-σ(Y123) superconductor. For the first time, we found the region from the cleaved surface that reveals clear bulk electronic properties. The intrinsic Fermi surface and band structures of Y123 were observed. The Fermi surface-dependent and momentum-dependent superconducting gap was determined which is nodeless and consistent with the d+is gap form.

Flat band in hole-doped transition metal dichalcogenide observed by angle-resolved photoemission spectroscopy

Layered transition metal dichalcogenides(TMDCs)gained widespread attention because of their electron-correlationrelated physics,such as charge density wave(CDW),superconductivity,etc.In this paper,we report the high-resolution angle-resolved photoemission spectroscopy(ARPES)studies on the electronic structure of Ti-doped 1T-Ti_(x)Ta_(1-x)S_(2) with different doping levels.We observe a flat band that originates from the formation of the star of David super-cell at the x=5%sample at the low temperature.With the increasing Ti doping levels,the flat band vanishes in the x=8%sample due to the extra hole carrier.We also find the band shift and variation of the CDW gap caused by the Ti-doping.Meanwhile,the band folding positions and the CDW vector g_(CDW)intact.Our ARPES results suggest that the localized flat band and the correlation effect in the 1T-TMDCs could be tuned by changing the filling factor through the doping electron or hole carriers.The Ti-doped 1T-Ti_(x)Ta_(1-x)S_(2) provides a platform to fine-tune the electronic structure evolution and a new insight into the strongly correlated physics in the TMDC materials.

Exploring battery material failure mechanisms through synchrotron X-ray characterization techniques

Rechargeable battery cycling performance and related safety have been persistent concerns.It is crucial to decipher the capacity fading induced by electrode material failure via a range of techniques.Among these,synchrotron-based X-ray techniques with high flux and brightness play a key role in understanding degradation mechanisms.In this comprehensive review,we summarize recent advancements in degra-dation modes and mechanisms that were revealed by synchrotron X-ray methodologies.Subsequently,an overview of X-ray absorption spectroscopy and X-ray scattering techniques is introduced for charac-terizing failure phenomena at local coordination atomic environment and long-range order crystal struc-ture scale,respectively.At last,we envision the future of exploring material failure mechanism.

Angle-resolved photoemission spectroscopy study on iron-based superconductors

Angle-resolved photoemission spectroscopy （ARPES） has played an important role in determining the band structure and the superconducting gap structure of iron-based superconductors. In this paper, from the ARPES perspective, we briefly review the main results from our group in recent years on the iron-based superconductors and their parent compounds, and depict our current understanding on the antiferromagnetism and superconductivity in these materials.

Investigation of the sodium storage mechanism of iron fluoride hydrate cathodes using X-ray absorption spectroscopy and mossbauer spectroscopy

Elucidation of a reaction mechanism is the most critical aspect for designing electrodes for highperformance secondary batteries.Herein,we investigate the sodium insertion/extraction into an iron fluoride hydrate(FeF_(3)·0.5H_(2)O)electrode for sodium-ion batteries(SIBs).The electrode material is prepared by employing an ionic liquid 1-butyl-3-methylimidazolium-tetrafluoroborate,which serves as a reaction medium and precursor for F^(-)ions.The crystal structure of FeF_(3)·0.5H_(2)O is observed as pyrochlore type with large open 3-D tunnels and a unit cell volume of 1129A^(3).The morphology of FeF_(3)·0.5H_(2)O is spherical shape with a mesoporous structure.The microstructure analysis reveals primary particle size of around 10 nm.The FeF_(3)·0.5H_(2)O cathode exhibits stable discharge capacities of 158,210,and 284 mA h g^(-1) in three different potential ranges of 1.5-4.5,1.2-4.5,and 1.0-4.5 V,respectively at 0.05 C rate.The specific capacities remained stable in over 50 cycles in all three potential ranges,while the rate capability was best in the potential range of 1.5-4.5 V.The electrochemical sodium storage mechanism is studied using X-ray absorption spectroscopy,indicating higher conversion at a more discharged state.Ex-situ M?ssbauer spectroscopy strengthens the results for reversible reduction/oxidation of Fe.These results will be favorable to establish high-performance cathode materials with selective voltage window for SIBs.

Energy-dispersive X-ray Spectroscopy for the Quantitative Analysis of Pyrite Thin Specimens

To explore ways to improve the accuracy of quantitative analysis of samples in the micrometer to nanometer range of magnitudes,we adopted analytical transmission electron microscopy(AEM/EDS)for qualitative and quantitative analysis of pyrite materials.Additionally,the k factor of pyrite is calculated experimentally.To develop an appropriate non-standard quantitative analysis model for pyrite materials,the experimentally calculated k factor is compared with that estimated from the non-standard quantitative analytical model of the instrument software.The experimental findings demonstrate that the EDS attached to a TEM can be employed for precise quantitative analysis of micro-and nanoscale regions of pyrite materials.Furthermore,it serves as a reference for improving the results of the EDS quantitative analysis of other sulfides.

Femtosecond Time-Resolved Spectroscopic Photoemission Electron Microscopy for Probing Ultrafast Carrier Dynamics in Heterojunctions

The fast developing semiconductor industry is pushing to shrink and speed up transistors. This trend requires us to understand carrier dynamics in semiconductor heterojunctions with both high spatial and temporal resolutions. Recently, we have successfully set up a timeresolved photoemission electron microscopy (TR-PEEM), which integrates the spectroscopic technique to measure electron densities at specific energy levels in space. This instrument provides us an unprecedented access to the evolution of electrons in terms of spatial location, time resolution, and energy, representing a new type of 4D spectro-microscopy. Here in this work, we present measurements of semiconductor performance with a time resolution of 184 fs, electron kinetic energy resolution of 150 meV, and spatial resolution of about 150 nm or better. We obtained time-resolved micro-area photoelectron spectra and energy-resolved TR-PEEM images on the Pb island on Si(111). These experimental results suggest that this instrument has the potential to be a powerful tool for investigating the carrier dynamics in various heterojunctions, which will deepen our understanding of semiconductor properties in the submicron/nanometer spatial scales and ultrafast time scales.

Common Electronic Features and Electronic Nematicity in Parent Compounds of Iron-Based Superconductors and FeSe/SrTiO_3 Films Revealed by Angle-Resolved Photoemission Spectroscopy

We report comprehensive angle-resolved photoemission investigations on the electronic structures and nematicity of the parent compounds of the iron-based superconductors including CeFeAsO, BaFe2As2, NaFeAs, FeSe and undoped FeSe/SrTiO3 films with 1, 2 and 20 layers. While the electronic structure near tile Brillouin zone center F varies dramatically among different materials, the electronic structure near the Brillouin zone corners （M points）, as well as their temperature dependence, are rather similar. The electronic structure near the zone corners is dominated by the electronic nematicity that gives rise to a band splitting of the dxz and dyz bands below the nematie transition temperature. A clear relation is observed between the band splitting magnitude arid the onset temperature of nematicity. Our results may shed light on the origin of nematicity, its effect on the electronic structures, and its relation with superconductivity in the iron-based superconductors.

Identification of Topological Surface State in PdTe2 Superconductor by Angle-Resolved Photoemission Spectroscopy

High-resolution angle-resolved photoemission measurements are carried out on transition metal dichalcogenide PdTe2 that is a superconductor with a Tc at 1.7K. Combined with theoretical calculations, we discover for the first time the existence of topologically nontrivial surface state with Dirac cone in PbTe2 superconductor. It is located at the Brillouin zone center and possesses helical spin texture. Distinct from the usual three-dimensional topological insulators where the Dirac cone of the surface state lies at the Fermi level, the Dirac point of the surface state in PdTe2 lies deeply below the Fermi level at - 1.75 eV binding energy and is well separated from the bulk states. The identification of topological surface state in PdTe2 superconductor deeply below the Fermi level provides a unique system to explore new phenomena and properties and opens a door for finding new topological materials in transition metal ehalcogenides.

Core-level spectroscopy of the photodissociation process of BrCN molecule

Fewest-switches surfacing hopping(FSSH) simulations have been performed with the high-level multi-reference electronic structure method to explore the coupled electronic and nuclear dynamics upon photoexcitation of cyanogen bromide(BrCN). The potential energy surfaces(PES) of BrCN are charted as functions of the Jacobi coordinates(R, θ). An indepth examination of the FSSH trajectories reveals the temporal dynamics of the molecule and the population changes of the lowest twelve states during BrCN's photodissociation process, which presents a rich tapestry of dynamical information.Furthermore, the carbon K-edge x-ray absorption spectroscopy(XAS) is calculated with multi-reference inner-shell spectral simulations. The rotation of the CN fragment and the elongation of the C–Br bond are found to be the reason for the peak shifting in the XAS. Our findings offer a nuanced interpretation for inner-shell probe investigations of BrCN, setting the stage for a deeper understanding of the photodissociation process of cyanogen halides molecules.

Molecular structure characterization of middle-high rank coal via^(13)C NMR,XPS,and FTIR spectroscopy

Elemental analysis,nuclear magnetic resonance carbon spectroscopy(^(13)C-NMR),X-ray photoelectron spectroscopy(XPS)and Fourier transform infrared spectroscopy(FTIR)experiments were carried out to determine the existence of aromatic structure,heteroatom structure and fat structure in coal.MS(materials studio)software was used to optimize and construct a 3D molecular structure model of coal.A method for establishing a coal molecular structure model was formed,which was“determination of key structures in coal,construction of planar molecular structure model,and optimization of three-dimensional molecular structure model”.The structural differences were compared and analyzed.The results show that with the increase of coal rank,the dehydrogenation of cycloalkanes in coal is continuously enhanced,and the content of heteroatoms in the aromatic ring decreases.The heteroatoms and branch chains in the coal are reduced,and the structure is more orderly and tight.The stability of the structure is determined by theπ-πinteraction between the aromatic rings in the nonbonding energy EN.Key Stretching Energy The size of EB determines how tight the structure is.The research results provide a method and reference for the study of the molecular structure of medium and high coal ranks.

Detailed electronic structure of three-dimensional Fermi surface and its sensitivity to charge density wave transition in ZrTe3 revealed by high resolution laser-based angle-resolved photoemission spectroscopy

The detailed information of the electronic structure is the key to understanding the nature of charge density wave （CDW） order and its relationship with superconducting order in the microscopic level. In this paper, we present a high resolution laser-based angle-resolved photoemission spectroscopy （ARPES） study on the three-dimensional （3D） hole-like Fermi surface around the Brillouin zone center in a prototypical quasi-one-dimensional CDW and superconducting system ZrTe3. Double Fermi surface sheets are clearly resolved for the 3D hole-like Fermi surface around the zone center. The 3D Fermi surface shows a pronounced shrinking with increasing temperature. In particular, the quasiparticle scattering rate along the 3D Fermi surface experiences an anomaly near the charge density wave transition temperature of ZrTe3 - 63 K）. The signature of electron-phonon coupling is observed with a dispersion kink at -20 meV; the strength of the electron-phonon coupling around the 3D Fermi surface is rather weak. These results indicate that the 3D Fermi surface is also closely connected to the charge-density-wave transition and suggest a more global impact on the entire electronic structure induced by the CDW phase transition in ZrTe3.