- 标题
- 摘要
- 关键词
- 实验方案
- 产品
-
Atomistic modeling of resistivity evolution of copper nanoparticle in intense pulsed light sintering process
摘要： In this work, the intense pulsed light (IPL) sintering process of copper nanoparticle ink is simulated using molecular dynamics (MD) method. First, the neck size growth between the two copper nanoparticles during the IPL sintering process is computed. The resultant electrical resistivity is then calculated by substituting the neck size into the Reimann-Weber formula. Overall, a rapid decrease of electric resistivity is observed in the beginning of the sintering, which is caused by quick neck size growth, followed by a gradually decrease of resistivity. In addition, the correlation of the simulated temperature dependent resistivity is similar to that of the experimentally measured resistivity. The MD model is an effective tool for designers to optimize the IPL sintering process.
关键词： Molecular dynamics,Nanoparticle,Electrical resistivity,Intense pulsed light,Copper
更新于2025-09-23 15:23:52
-
Treatment of disorder effects in X-ray absorption spectra beyond the conventional approach
摘要： The contribution of static and thermal disorder is one of the largest challenges for the accurate determination of the atomic structure from the extended X-ray absorption fine structure (EXAFS). Although there are a number of generally accepted approaches to solve this problem, which are widely used in the EXAFS data analysis, they often provide less accurate results when applied to outer coordination shells around the absorbing atom. In this case, the advanced techniques based on the molecular dynamics and reverse Monte Carlo simulations are known to be more appropriate: their strengths and weaknesses are reviewed here.
关键词： Reverse Monte Carlo,Extended X-ray absorption fine structure (EXAFS),Molecular dynamics,Static and thermal disorder,X-ray absorption spectroscopy
更新于2025-09-23 15:23:52
-
Femtosecond Electron Dynamics in Graphene Nanoribbons - A Nonequilibrium Green Functions Approach Within an Extended Hubbard Model
摘要： A new approach to study the correlated femtosecond electron dynamics in finite graphene clusters, such as nanoribbons, is presented here. The systems are described by an extended Hubbard model that takes into account the overlap of adjacent orbitals and hopping between up to third-nearest neighbors. The model is solved by the nonequilibrium Green functions approach combined with different self-energy approximations, including the second-Born and GW self-energy, to take into account electronic correlations. The description allows us to predict the correlated nonequilibrium dynamics of excited graphene nanostructures of arbitrary geometry containing up to 100 carbon atoms for up to 25 fs.
关键词： correlated dynamics,nonequilibrium Green functions,Hubbard model,graphene nanoribbons
更新于2025-09-23 15:23:52
-
Artifacts in Transient Absorption Measurements of Perovskite Films Induced by Transient Reflection from Morphological Microstructures
摘要： Organolead halide perovskites MAPbX3 (MA = CH3NH3+; X = Cl?, Br?, I?) have attracted broad tremendous interest in the past 10 years for applications in solar cells and light-emitting devices. In evaluating the quality of the perovskite materials, spectroscopic characterizations such as static and time-resolved absorption and photoluminescence measurements are essential to examine their photophysical properties. A recent report found that the correct measurement of static absorption spectra of MAPbX3 films is indeed difficult due to the strong light scattering caused by their poor surface coverage or complex microstructures. These morphological complexities seem to be inevitable in thin-film fabrication and should not only affect the steady-state spectroscopic measurements but also can significantly impact the time-resolved spectroscopic characterizations, whose results are crucial for understanding photoinduced carrier dynamics in the examined materials. Photoexcited states in semiconductor materials induce changes in the real and imaginary parts of the dielectric function. This leads to changes in absorption (imaginary part) and reflectivity (real part), which can be substantial for materials with significant values of refractive index such as lead halide perovskites. Transient absorption (TA) spectroscopy is a typical technique that has been broadly used to probe photoexcited state dynamics in perovskites and other semiconductor materials. In TA measurements, a pump laser pulse is used to excite the perovskite films, and the induced absorption changes (ΔA) are recorded as a function of both wavelength and time. With the transmitted light as the probe (Figure 1a), the TA signal (ΔA) is mainly decided by the ratio of the intensity of transmitted probe light with and without pump excitation (see eq S1 in the SI), assuming that the loss of transmitted probe light completely results from the sample absorption. On the basis of the same experimental setup, transient reflection (TR) measurements can also be carried out by using the reflected probe light as detection signal (Figure 1b). The TR signal (ΔR/R) can also be determined by the ratio of the intensity of reflected probe light with and without pump excitation (see eq S4 in the SI). Unlike the TA measurements that mainly probe the bulk property of samples, the TR signal mainly detects the photoinduced reflection variations due to the refractive index change at the sample surface. Therefore, the TR spectrum and kinetics can be significantly different from those of TA even in the same sample. For example, previous TA and TR measurements have found dramatically faster carrier recombination kinetics on the surface than in the bulk of MAPbX3 perovskite films or single crystals because of the presence of more surface defects. There is an abnormal case in the regular TA measurements particularly when performed on the films with large and heterogeneous microstructures (e.g., films with poor coverage, large grains, and pinholes) because the loss of transmitted probe light in their TA measurements likely results not only from the sample absorption but also from the reflection of the film surface or the boundary of microstructures in samples. In this case, the measured transient spectrum, though collected in the transmittance mode as in TA, can contain contributions from both TA and TR signals (see Figure 1c and eq S6 in the SI). This could lead to distorted TA spectra and thus inaccurate analysis of photoinduced kinetics. A solution-processed organic or inorganic halide perovskite thin film is a typical material whose morphological microstructures were found to have significant impact on device performance. Although the photoinduced carrier dynamics in perovskite films has been extensively studied using TA spectroscopy, the possible artifacts in TA results induced by TR signal originating from the photoinduced reflectivity variation of film surfaces and microstructures have been overlooked. Herein, in order to clarify the influence of TR signal in the regular TA measurements, we performed a careful transient spectroscopic analysis on a series of MAPbBr3 perovskite films with different microstructure morphology. Meanwhile, TR measurements on MAPbBr3 single crystals (SCs) were carried out for comparison. We confirmed that the TA spectra measured in MAPbBr3 perovskite films with large and heterogeneous microstructures do comprise non-negligible TR signals from the photoinduced reflection of microstructures, with the weight of contribution increased from ～20 to ～100% as the size of the microstructure increased from <200 nm to 1?2 μm. The presence of TR signal leads to an “artifact” feature in the TA spectra and faster observed kinetics owing to the faster surface carrier recombination, which will thus mislead the analysis of bulk carrier dynamics. We also provided a method to reduce the TR signal in actual TA measurements by adding solvent with its refractive index close to the samples, by which the TR distortion can be suppressed to some extent.
关键词： artifacts,transient reflection,transient absorption,carrier dynamics,perovskite films,microstructures
更新于2025-09-23 15:23:52
-
Topology and polarity of dislocation cores dictate the mechanical strength of monolayer MoS2
摘要： In contrast to homoelemental graphene showing common dislocation dipole with pentagon-heptagon (5|7) core, heteroelemental MoS2 is observed to contain diverse dislocation cores that tune the chemical and physical properties. Yet, how the inevitable dislocation cores in MoS2 affect the mechanical behaviours remains virtually unexplored. Herein, we report direct atomistic simulations of mechanical characteristics of isolated dislocation-embedded MoS2 monolayers under tensile load. All isolated dislocation cores in MoS2 monolayer rise polar stress-concentration, while those with larger Burgers vector are less energetically-favorable configurations but show local wrinkling behaviour. It is revealed that the intrinsic tensile strength of MoS2 is dictated by topology and polarity of dislocation cores. There is a strong inverse correlation between the maximum residual stresses induced by the dislocation cores and the strength of MoS2 monolayers. Mechanical failure initiates from the bond at dislocation polygon on which side there is a missing atomic chain. Armchair-oriented 4|8 dislocation exhibits sole brittle failure, however, dual brittle/ductile fractures occur in zigzag-oriented dislocations; Mo-S-Mo angle-oriented crack is brittle, while the S-Mo-S angle-oriented crack becomes ductile. Our findings shed sights on mechanical design of heteroelemental 2D materials via dislocation engineering for practical application.
关键词： Mechanical strength,Fracture characteristics,Monolayer MoS2,Molecular dynamics simulations,Dislocation cores
更新于2025-09-23 15:23:52
-
Investigation of the graphene thermal motion by rainbow scattering
摘要： The thermal motion of graphene atoms was investigated using angular distributions of transmitted protons. The static proton-graphene interaction potential was constructed applying the Doyle-Turner’s expression for the proton-carbon interaction potential. The effects of atom thermal motion were incorporated by averaging the static proton-graphene interaction potential over the distribution of atom displacements. The covariance matrix of graphene displacements was modeled according to the Debye theory, and calculated using Molecular Dynamics approach. Proton trajectories were used for construction of angular yields. We have found that there are lines, called rainbows, along which the angular yield is very large. Their evolution in respect to different sample orientation was examined in detail. Further we found that atom thermal motion has negligible influence on rainbows generated by protons experiencing distant collisions with the carbon atoms forming the graphene hexagon. On the other hand, rainbows generated by protons experiencing close collisions with the carbon atoms can be modeled by ellipses whose parameters are very sensitive to the structure of the covariance matrix. Numerical procedure was developed for extraction of the covariance matrix from the corresponding rainbow patterns in the general case, when atoms perform fully anisotropic and correlated motion.
关键词： thermal motion,graphene nanoribbon,molecular dynamics,graphene,rainbow scattering
更新于2025-09-23 15:23:52
-
Analysis of trajectory similarity and configuration similarity in on-the-fly surface-hopping simulation on multi-channel nonadiabatic photoisomerization dynamics
摘要： We propose an “automatic” approach to analyze the results of the on-the-fly trajectory surface hopping simulation on the multi-channel nonadiabatic photoisomerization dynamics by considering the trajectory similarity and the configuration similarity. We choose a representative system phytochromobilin (PΦB) chromophore model to illustrate the analysis protocol. After a large number of trajectories are obtained, it is possible to define the similarity of different trajectories by the Fréchet distance and to employ the trajectory clustering analysis to divide all trajectories into several clusters. Each cluster in principle represents a photoinduced isomerization reaction channel. This idea provides an effective approach to understand the branching ratio of the multi-channel photoisomerization dynamics. For each cluster, the dimensionality reduction is employed to understand the configuration similarity in the trajectory propagation, which provides the understanding of the major geometry evolution features in each reaction channel. The results show that this analysis protocol not only assigns all trajectories into different photoisomerization reaction channels but also extracts the major molecular motion without the requirement of the pre-known knowledge of the active photoisomerization site. As a side product of this analysis tool, it is also easy to find the so-called “typical” or “representative” trajectory for each reaction channel.
关键词： trajectory similarity,multi-channel nonadiabatic photoisomerization dynamics,Fréchet distance,dimensionality reduction,phytochromobilin chromophore,on-the-fly surface-hopping simulation,configuration similarity,clustering analysis
更新于2025-09-23 15:23:52
-
Resonance enhanced multiphoton ionisation (REMPI) detection of Cl( <sup>2</sup> P <sub/>j</sub> ) atom in the photodissociation of halogenated pyrimidines at 235 nm: role of triplet states
摘要： The dynamics of chlorine atom (2Pj) formation in the photodissociation process of halogen substituted pyrimidines, namely, 2,4,6-trichloropyrimidine and 5-chloro-2,4,6-trifluoropyrimidine have been studied around 235 nm using Resonance Enhanced Multiphoton Ionisation Time-of-Flight Mass Spectrometry technique. For the chlorine atom dissociation channel, we have determined the translational energy distribution, the recoil anisotropy parameter, β, and the spin–orbit branching ratio. In both the molecules, the TOF profiles for Cl (2P3/2) and Cl* (2P1/2) are found to be independent of laser polarisation suggesting a zero value for β, within the experimental uncertainties. For 2,4,6-trichloropyrimidine, the average translational energies for Cl and Cl* elimination channels are determined to be 6.0 ± 1.2 and 7.0 ± 1.5 kcal/mol, respectively. Similarly, for 5-chloro-2,4,6-trifluoropyrimidine, the average translational energies for Cl and Cl* elimination channels are determined to be 6.5 ± 1.2 and 7.9 ± 1.6 kcal/mol, respectively. Computational calculations are performed to generate the potential energy curves along the dissociating C-Cl bond using equation of motion coupled cluster with single and double excitations (EOM-CCSD) method. Computational studies suggest the role of triplet states in the photodissociation process forming the Cl atom.
关键词： REMPI-TOF,halogenated pyrimidines,translational energy,spin-orbit ratio,Photodissociation dynamics
更新于2025-09-23 15:23:52
-
Calcination-free synthesis of high strength self-cleaning anti-reflective MgF2-TiO2 coating
摘要： In order to understand the nonlinear dynamic behavior of a planar mechanism with clearance, the nonlinear dynamic model of the 2-DOF nine-bar mechanism with a revolute clearance is proposed; the dynamic response, phase diagrams, Poincar′e portraits, and largest Lyapunov exponents (LLEs) of mechanism are investigated. The nonlinear dynamic model of 2-DOF nine-bar mechanism containing a revolute clearance is established by using the Lagrange equation. Dynamic response of the slider’s kinematics characteristic, contact force, driving torque, shaft center trajectory, and the penetration depth for 2-DOF nine-bar mechanism are all analyzed. Chaos phenomenon existed in the mechanism has been identi?ed by using the phase diagrams, the Poincar′e portraits, and LLEs. The e?ects of the di?erent clearance sizes, di?erent friction coe?cients, and di?erent driving speeds on dynamic behavior are studied. Bifurcation diagrams with changing clearance value, friction coe?cient, and driving speed are drawn. The research could provide important technical support and theoretical basis for the further study of the nonlinear dynamics of planar mechanism.
关键词： Lyapunov exponent,nonlinear dynamics,chaos,clearance joint,bifurcation
更新于2025-09-23 15:23:52
-
Nuclear spin dynamics in [001] AlAs quantum well in the regime of integer and fractional quantum Hall effect
摘要： Relaxation of nuclear spins located in the vicinity of 2D electron system confined in a 16 nm [001] AlAs/AlGaAs quantum well was studied with the aid of electron spin resonance (ESR) in the regime of integer and fractional quantum Hall effect. Nuclear spin-lattice relaxation time τ was measured from the time decay of the Overhauser shift near different filling factors of the electron system. The resultant dependence of τ on filling factor turned out to be nontrivial. At the temperature 1.5 K τ reached its maximal value at the exact filling ν = 1 and decreased when ν was altered, yet this maximum vanished when the system was cooled down to 0.5 K. The fractional quantum Hall effect state at the filling of 2/3 was formed at the temperature of 0.5 K, and the development of this state was accompanied by the slowing of the nuclear spin relaxation. This observation suggests the enhancement of energy gap in the spin excitation spectrum of two-dimensional electrons at 2/3 state.
关键词： quantum wells,quantum Hall effect,spin dynamics,electron paramagnetic resonance
更新于2025-09-23 15:23:52