Valence Electrons Research Articles

Applicability of the Zintl Concept to Understanding the Crystal Chemistry of Lithium-Rich Germanides and Stannides.

With this contribution, we take a new, critical look at the structures of the binary phases Li5Ge2 and Li5Sn2. Both are isostructural (centrosymmetric space group R3̅m, no. 166), and in their structures, all germanium (tin) atoms are dimerized. Application of the valence rules will require the allocation of six additional valence electrons per [Ge2] or [Sn2] unit considering single covalent bonds, akin to those in the dihalogen molecules. Alternatively, four additional valence electrons per [Ge2] or [Sn2] anion will be needed if homoatomic double bonds exist, in an analogy with dioxygen. Therefore, five lithium atoms in one formula unit cannot provide the exact number of electrons, leaving open questions as to what is the nature of the chemical bonding within these moieties. Additionally, by means of single-crystal X-ray diffraction, synchrotron powder X-ray diffraction, and neutron powder diffraction, we established that the Li and Sn atoms in Li5Sn2 are partially disordered, i.e., the actual chemical formula of this compound is Li5-xSn2+x (0 < x < 0.1). The convoluted atomic bonding in the case where tin atoms partially displace lithium atoms results in the formation of larger covalently bonded fragments. Our first-principle calculations suggest that such disorder leads to electron doping. Contrary to that, both experimental and computational findings indicate that in the Li5Ge2 structure, the [Ge2] dimers are slightly oxidized, i.e., hole-doped, as a result of approximately 30% vacancies on a Li site, i.e., the actual chemical formula of this compound is Li5-xGe2 (x ≈ 0.3).

The eutectic compositional space in Al-Cr-Fe-Ni system utilizing the high-throughput Calphad approach

Eutectic High-Entropy Alloys (EHEAs) show promise in balancing strength and ductility, along with excellent castability and chemical homogeneity. However, identifying optimal eutectic compositions in HEAs has been a persistent challenge, primarily due to the lacuna of multi-component phase diagrams. In addressing this challenge, the eutectic compositional space in Al-Cr-Fe-Ni is unveiled for the first time as a case study using the High-Throughput Calphad methodology. By integrating the Python application programming interface into Thermo-Calc, Latin Hypercube Sampling generated 100,000 compositions examined for eutectic formation based on thermodynamic parameters. This analysis revealed the significant correlation of valence electron concentration, enthalpy of mixing, and atomic size difference on eutectic formation. Moreover, the predictions of the proposed design methodology were compared with reported eutectic compositions, exhibiting excellent agreement. Further, a novel dual-phase eutectic alloy featuring an FCC+B2 combination predicted through the proposed design framework has been successfully cast, providing further experimental validation.

Engineering the Activity and Stability of the Zn-MOF Catalyst via the Interaction of Doped Zr with Zn.

Metallic atoms within metal-organic framework (MOF) materials exhibit a distinctive and adaptable coordination structure. The three-dimensional (3D) pore configuration of MOFs enables the complete exposure of metal active sites, rendering them prevalent in various catalytic reactions. In this study, zinc (Zn) atoms within Zn-based MOF materials, characterized by an abundance of valence electrons, are utilized for the transesterification of dimethyl carbonate (DMC). Additionally, the introduction of zirconium (Zr) effectively addresses the susceptibility of the MOFs' crystal structure to dissolution in organic solvents. The formulated catalyst, Zn-10%Zr-MOF(300), demonstrates remarkable catalytic performance with 91.5% DMC selectivity, 61.9% propylene carbonate (PC) conversion, and 56.6% DMC yield. Impressively, the catalyst maintains its high performance over five cycles. Results indicate that Zr interacts with Zn, forming new coordination bonds and enhancing the catalyst crystal structure stability. Moreover, electron transfer intensifies the alkalinity of the active Zn atoms, enhancing the overall catalyst performance. This research informs the development of transesterification heterogeneous catalysts and broadens the application scope of MOF catalysts.

Phase stability and elastic properties of NbMoTaWMx (M = Al, V, Zr, Tc, Re and Ir) RHEAs: A first-principles assessment

Using the exact muffin-tin orbital (EMTO) method in combination with the coherent potential approximation (CPA), we studied the influence of alloying elements Al, V, Zr, Tc, Re and Ir on the phase stability, lattice parameters, densities, and elastic properties of NbMoTaWMx (M = Al, V, Zr, Tc, Re, Ir; 0 ≤ x ≤ 1.0) refractory high entropy alloys. The predicted lattice parameter and elastic parameters agree with the available experimental and theoretical data. We calculated the atomic size difference (δ), the valence electron concentration (VEC) and the total energy of face-centered cubic (fcc), body-centered cubic (bcc) and hexagonal closed-pack (hcp) structures. We found that all studied NbMoTaWMx (M = Al, V, Zr, Tc, Re, Ir; 0 ≤ x ≤ 1.0) systems have the bcc structure. We showed that Al and Ir decrease the stability of the bcc structure and Zr significantly enlarges the lattice parameter of the host. Vanadium increases the ductility of NbMoTaW system. On the other hand, Al and Ir have strongly non-linear effect on the ductility, with clear minimum at x = 0.55. The present results provide consistent theoretical data and call for experimental investigation for these alloys.

Modulating Valence Electrons and Na Occupancy in Layered Cathodes for High-Performance Na-Ion Batteries.

Na-ion batteries (NIBs) hold promise as a leading option for large-scale energy storage. However, their development faces challenges due to the lack of high-performance cathode materials. P2-type layered oxides are seen as potential cathode materials for NIBs due to higher structure stability, yet their commercialization is hindered by limited capacity and subpar phase transitions during Na extraction and insertion at high voltages. In this study, we introduce a new P2-type cathode material, Na0.76Ni0.23Li0.1Ti0.02Mn0.65O1.998F0.02 (NLTMOF), synthesized with ternary Li/Ti/F substitution. This modification of ternary Li/Ti/F substitution significantly tailors the electronic structures, increasing the number of valence electrons near the Fermi energy level. This facilitates the electronic conductivity and their involvement in charge compensation, thereby enhancing reversible capacity. Additionally, ternary doping synergistically adjusts the Na occupancy at the Na layer for favorable Na extraction without P2-O2 phase transitions even under a high voltage of 4.4 V, boosting cycling stability. As a result, NLTMOF demonstrates a reversible capacity of 110.0 and 132.2 mAh g-1 at 2-4.2 and 2-4.4 V, respectively, and maintains greatly enhanced cycling stability over long cycles. This study sheds light on the design of transition metal oxides for advanced cathode materials through the modulation of electronic structure and Na occupancy in cathode materials, thus promoting the development of NIBs.

Field-assisted sintering of high-entropy alloy-reinforced aluminium matrix composites: phase identification and microstructural properties

AbstractThis study investigates the design, phase identification, and microstructural properties of high-entropy alloy (HEA)-reinforced aluminium (Al) matrix composites. Thermophysical expressions for HEAs were employed during the design phase of the HEA; both theoretical frameworks and experimental analyses were used to anticipate stable phases while a field-assisted sintering technique was employed to consolidate the samples. Calculation of phase diagram (CALPHAD) predictions for the phases present in the HEA align with valence electron concentration (VEC) calculations as both predicted the presence of BCC and FCC phases. The microhardness results reveal a substantial increase in the hardness value of the composites as compared to the pure Al, such that as low as 5 wt% HEA addition resulted in over a 100% improvement, while the densification of the composites was found to decrease with an increase in the wt% of HEA. SEM micrographs and XRD analyses show fair dispersion, bonding, and phase integration in the HEA-reinforced composites.

Sparse-Stochastic Fragmented Exchange for Large-Scale Hybrid Time-Dependent Density Functional Theory Calculations.

We extend our recently developed sparse-stochastic fragmented exchange formalism for ground-state near-gap hybrid DFT to calculate absorption spectra within linear-response time-dependent generalized Kohn-Sham DFT (LR-GKS-TDDFT) for systems consisting of thousands of valence electrons within a grid-based/plane-wave representation. A mixed deterministic/fragmented-stochastic compression of the exchange kernel, here using long-range explicit exchange functionals, provides an efficient method for accurate optical spectra. Both real-time propagation as well as frequency-resolved Casida-equation-type approaches for spectra are presented, and the method is applied to large molecular dyes.

Unravelling the Role of the BCC-B2 Transition and V Occupancies in the Contradictory Magnetism-Ductility Relationship of FeCoV Alloys

The contradictory relationship between magnetism and ductility restricts further applications of FeCoV alloys in high-performance electrical machines. The role of the BCC-B2 transition, accompanied by vanadium (V) site occupancies, in magnetic moments and ductility has been explored using first-principles calculations. The variations in magnetism and ductility of FeCoV alloys are attributed to the coupling of the BCC-B2 transition and V occupancies. When V replaces Fe atoms in the equiatomic B2-FeCo alloy, the superior magnetism observed in B2-Fe50-cCo50Vc alloys is a consequence of the enhanced local magnetic moment of Fe and the ferrimagnetic-ferromagnetic transition in the magnetic state. Moreover, due to the preferential V occupancy in the B2 phase, the B2-Fe46Co50V4 alloy exhibits comparable ductility to the BCC-Fe50Co46V4 alloy. The results indicate that the increased brittleness in the B2 phase arises from the raised Peierls stress and the enhanced covalent component in interatomic bonding, which is caused by the strong hybridization between Fe and Co atoms. Pearson correlation analysis illustrates that valence electron concentration (VEC) and V content are significant factors in the contradictory relationship between magnetization and ductility. The theoretical results demonstrate that tuning the V content and atomic occupancies is helpful to achieve a trade-off between magnetization and ductility in B2-FeCoV alloys.

Calculation of spontaneous radiation during channeling of relativistic positrons in non-chiral nanotubes using a quadratic approximation

The work investigates the conditions for the possibility of using the quadratic approximation U(ρ) = αρ2 for the interaction potentials of channeled positrons with the inner walls of non-chiral carbon nanotubes of types (n, 0) and (n, n). In particular, (8, 0), (10, 0), (12, 0) and (8, 8), (10, 10), (12, 12) nanotubes were selected. In this case, when calculating the single-particle potential of the carbon atom, only the contribution of valence electrons was taken into account. As a result of this approximation, the parameters α were determined for all the nanotubes studied. Using wave functions and the corresponding quantum levels of transverse energy obtained by solving the Schrödinger equation, the probabilities of occupation of these levels were calculated for positron beams with zero angular dispersion moving along the axes of nanotubes. Based on this information, values of the longitudinal energy of positrons for which the quadratic approximation is applicable were determined for all the studied nanotubes. Spectral distributions of spontaneous radiation were calculated in the dipole approximation for non-dispersive relativistic positron beams, both within the framework of quantum-mechanical and classical approaches.

The Effect of Ligand Field on Enhanced Electrocatalytic Performance of NO Reduction Under Applied Potential

We employed density functional theory to investigate Co-N4/Gra single-atom catalysts, focusing on the modification of axial ligand (X=-F, -CN and -C3H4N2) and examined the influence of ligand field and electric potential on eNORR. Our results demonstrate that Co-N4[X]/Gra exhibit favorable thermodynamic adsorption (ΔG *NO < 0) and remarkable activation activity toward NO molecules. Co-N4/Gra demonstrates a limiting potential of −0.13 V with the potential-determining step (PDS) of *NH3 → * + NH3(g). Notably, under the introduction of ligands, Co-N4[F]/Gra achieves the most favorable overpotential of −0.07 V, superior to most of NORR electrocatalysts, and meanwhile shows an exceptional selectivity of 99.99% for eNORR compared to competitive hydrogen evolution reaction. Under the solvent environment, Co-N4/Gra features the triggering potentials of −0.33 V for a pH of 1, −0.71 V for a pH of 7, and −1.10 V vs RHE for a pH of 13, respectively. Additionally, the potential reduces the desorption energy and adsorption energy of NH3, facilitating the accessibility of the NH3 desorption step (PDS) and promoting NO reduction. Thus, under realistic conditions, the Co ion’s active site displays variable valence electrons and forms a dynamic interplay with the ligand field effect, rendering a crucial effect on the adsorption of reaction species during the eNORR.

Tuning the electronic and magnetic properties of MoS2 bilayers by transition-metal intercalation

Two dimensional (2D) transition-metal dichalcogenides and their heterostructures are important materials for future electronic device applications. By using the first-principles calculations we investigate how the electronic and magnetic properties of MoS2 bilayer is modified by intercalating transition-metals (Fe, Co, and Ni). The Fe-intercalated MoS2 bilayer is found to be a non-magnetic gapless semimetal. Without spin–orbit coupling it has the Dirac state on the Γ-M line in k space at the Fermi level. The spin degeneracy of the Dirac state is removed by spin–orbit coupling. However, the bottom of the conduction band and the top of the valence band are in contact with the Fermi level making the system a non-magnetic gapless semimetal. The Dirac state is also observed in both Co-intercalated and Ni-intercalated MoS2 bilayers because they have the same symmetry in crystal structure as the Fe-intercalated MoS2 bilayer. The difference in the number of valence electrons in the intercalated atoms drastically change the electronic and magnetic properties. The Co-intercalated MoS2 bilayer is a ferromagnetic metal, where the Dirac state is below the Fermi level. The Ni-intercalated MoS2 bilayer is a non-magnetic narrow gap semiconductor, where the Dirac state is far below the Fermi level. The results revealed the electronic and magnetic properties of the transition-metal-intercalated MoS2 bilayers and will be useful for designing a variety of 2D materials.

Nature of C-C coupling and strategy of tuning the catalytic activity of Cu-N-C catalysts for electro-reduction of CO2 to ethanol

With high atomic utilization and remarkable catalytic activity, Cu-N-C type catalysts display great potential for electro-catalysis in CO2 reduction. However, the relationship between the active moiety and catalytic activity of generating high-value C2 products is still unclear, and the explicit screening criteria is scarcity. Herein, based on the first-principle simulation, the structure-performance relationship on Cu-N-C type catalysts has been investigated by modulating the CO2 reduction process as the number of Cu atom (Cu1, Cu2, Cu3) and the ligand environment (B, C, N, O, P, S) changed. We find the adsorption strength of intermediate *CO strongly affect the possibility of C-C coupling, which can be determined by Bader charge on Cu atom, mainly depending on the number of loaded atomic Cu on Cu-N-C catalysts. Furthermore, the Bader charge can be refined by adjusting the coordination atom of Cu, thus optimizing catalytic activity for the CO2 to ethanol. The moderate Bader charge value, between +0.35 and +0.45, enables the catalyst to behave as a potentially excellent activity with low limiting potential for generating ethanol. More importantly, an intrinsic descriptor, composed of the radius, electronegativity, and number of valence electrons of coordination atoms (φ=∑χ∑r⁎∑np), was established to characterize the catalytic activity of Cu-N(X)-C catalysts for producing ethanol. Two excellent catalysts, Cu3-N2O2 (-0.51V) and Cu3-N3S (-0.64V), are screened out for the CO2RR to generate ethanol. This work discloses theoretical basis for catalytic selectivity of C2 products on Cu-N-C catalysts and provides a regulating and screening principle for high performance catalysts to ethanol.

The interfacial electric field enhanced piezo-catalytic performance of Bi2S3/Ni/CN composites for peroxymonosulfate activation advanced oxidation processes (AOP) systems

The interfacial electric field of Bi2S3/Ni/CN composites has been found to enhance the piezo-catalytic performance in peroxymonosulfate activation for advanced oxidation processes (AOP) systems. This novel research field aims to strengthen AOP systems for pollutant control and degradation through the utilization of the piezo-catalysis. In this particular study, a hammer coral-like Bi2S3/Ni/CN composite with interfacial electric field was synthesized by incorporating bismuth sulfide into the Ni/CN matrix. The efficient separation of piezoelectric carriers and charge transfer between nickel and bismuth in the resulting Bi2S3/Ni/CN composite facilitate a synergistic effect in the activation of peroxymonosulfate (PMS). It has been observed that, when subjected to ultrasound, this composite can achieve a degradation rate exceeding 90% within a minute towards Rh B as a model dye. Notably, the degradation process is primarily driven by piezoelectric hole and mono-linear oxygen non-free radicals. Additionally, the interfacial electric field facilitates valence electron transfer and ultimately enhancing reaction efficiency. Experimental results further demonstrate that the removal efficiency of organic pollutants can surpass 98% within a pH range of 1–9 over a duration of 3 min, demonstrating wide pH response range and high catalytic activities.

Magnetic transition of 1D ferromagnetic catalysts during the NO electroreduction

Exploration of magnetic phase transitions during electrochemical processes is of great importance for rational design of supported magnetic-metal electrocatalysts. Herein, we systematically investigated the magnetic transition between ferromagnetism (FM) and anti-ferromagnetism (AFM) in one-dimensional ferromagnetic Co chain supported on graphene (Co4N8-gra) during NO electroreduction (NORR) process, focusing on the impact of potential and acidity on the catalytic property and magnetic transition. A combination of catalytic kinetics calculations and microkinetic simulations reveals that the Co4N8-gra exhibits excellent NH3 selectivity and thermal stability. In the implicit solvent model, the general reaction follows optimal pathway: * + NO(g) → *NO → *HNO → *H2NO → *H2NOH → *NH2 → *NH3 → * + NH3, with the potential-determining step (PDS) identified as *NO → *HNO. In acidic solvent, the magnetic transitions follow the pathway (FM → AFM2 → AFM2 → AFM2 → AFM1 → AFM1 → AFM1 → FM) under an applied potential of −0.20 V/RHE. In neutral solvent, the magnetic transitions occur according to this pathway (FM → AFM2 → AFM2 → FM → AFM1 → AFM1 → AFM1 → FM) under an applied potential of −0.14 V/RHE. In an alkaline solvent, the magnetic transitions proceed along this sequence (FM → AFM1 → AFM2 → FM → AFM1 → AFM1 → AFM1 → FM) under an ultralow potential of −0.08 V/RHE. Essentially, the improvement of catalytic property is attributed to the synergistic influence of external potential and magnetic-state transition on the adsorption of reaction species (e.g., NO and NH3). Magnetic transitions are closely associated with ligand field effect of metal site with variable valence electron induced by applied potential. In general, this study provides valuable insights for the controllable design of magnetic metal catalysts.

Regulation of chemical microenvironment to overcome strength-ductility trade-off in FeCrVTiSix high-entropy alloys coating

Developing metallic materials with both high strength and ductility is an enormous challenge in the field of materials science and engineering due to commonly known “strength-ductility trade-off”. In this work, we proposed a regulation strategy of the chemical microenvironment through changing valence electron concentration (VEC) to achieve simultaneous improvement of the strength and ductility of metallic materials. Taking FeCrVTiSix system as a proof-of-concept model, we first predicted the influence of Si on the chemical microenvironment through density functional theory calculations. These calculations unveiled that Si atoms effectively modify the bonding state among alloy elements, resulting in an enhancement of the strength within the FeCrVTi alloy system while maintaining its ductility. Building upon this insight, we successfully synthesized FeCrVTiSix alloys coating using laser cladding techniques. Subsequent tests, including nanoindentation, Vickers hardness, and tensile assessments, unequivocally demonstrated that the introduction of Si significantly increases the strength of the alloy while maintaining its ductility. Si atoms play a pivotal role in modulating the slip behavior of high-entropy alloys (HEAs) by reshaping the chemical microenvironment, thus enabling the elevation of strength in HEAs while preserving ductility. This work provides a novel approach for designing HEAs that effectively circumvent the “strength-ductility trade-off”, potentially broadening the horizons of engineering applications for HEAs coating.

Excellent specific strength-ductility synergy in novel complex concentrated alloy after suction casting

Lightweight alloys are known to improve the fuel efficiency of the structural components due to high strength-to-weight ratio, however, they lack formability at room temperature. This major limitation of poor formability is most of the time overcome by post-fabrication processing and treatments thereby increasing their cost exponentially. We present a novel Ti50V16Zr16Nb10Al5Mo3 (all in at. %) complex concentrated alloy (Ti-CCA) designed based on the combination of valence electron concentration theory and the high entropy approach. The optimal selection of constituent elements has led to a density of 5.63 gm/cc for Ti-CCA after suction casting (SC). SC Ti-CCA displayed exceptional room temperature strength (UTS ∼ 1.25 GPa) and ductility (ε ∼ 35 %) with a yield strength (YS) of ∼ 1.1 GPa (Specific YS = 191 MPa/gm/cc) without any post-processing treatments. The exceptional YS in Ti-CCA is attributed to hetero grain size microstructure, whereas enormous strength-ductility synergy is due to the concurrent occurrence of slip and deformation band formation in the early stages of deformation followed by prolonged necking event due to delayed void nucleation and growth. The proposed philosophy of Ti-CCA design overcomes the conventional notion of strength-ductility trade-off in such alloy systems by retaining their inherent characteristics.

Phase stability and mechanical properties of the six-principal element TiVNbCrCoNi alloys

This study designed a series of six-principal element TiVNbCrCoNi alloys according to the maximum entropy principle under the constraint of valence electron concentration (VEC). The phase stability and mechanical properties were investigated. It was showed that at VEC levels below 5.2, the body-centered cubic (BCC)-structured solid-solution phase remained stable at room temperature. As VEC exceeded 8.0, the face-centered cubic (FCC)-structured solid-solution phase stabilized. In the VEC range of 5.2–8.0, (Co, Ni)Ti and Ni3Nb intermetallic compounds formed combining with the solid-solution phases. Both yield strength and ductility increased with increase of VEC in the BCC-structured solid-solution alloys. The phase stability was elucidated through First-principle and thermodynamic calculations, while the evolution of mechanical properties of solid-solution alloys was evaluated in terms of multiple parameters. The thermodynamic calculation achieved satisfactory accuracy after being adjusted to utilize atomic bond enthalpy instead of atomic electronegativity difference.

STUDY ON MAGNETIC PROPERTIES OF FeCoPSiBCu AMORPHOUS ALLOY BY EMPIRICAL ELECTRON THEORY

In this study, a new evaluation method was investigated for the magnetic properties of the amorphous alloys by comparing the experimental results with the theoretical calculations. First, The (Fe[Formula: see text]Co6P[Formula: see text]Si[Formula: see text]B[Formula: see text])[Formula: see text]Cux ([Formula: see text]–0.5) amorphous ribbons were prepared by melt spinning method. Then, the magnetic properties of the prepared amorphous alloys were measured as 165.86–147.04[Formula: see text]emu/g, respectively. On the other side, we analyzed the valence electron structure and obtained the magnetizations as 159.92–158.77[Formula: see text]emu/g by calculating the magnetic moments of unit cells based on empirical electron theory (EET) of solids and molecules. Through comparing the magnetic properties of the calculations with the measurements, we found that the differences between the calculations and the measurements are less than 12% for all samples, meeting the first approximation requirement. Moreover, with the addition of Cu, the change trends both in the calculated and measured magnetic properties are also consistent. These results prove that it is feasible to calculate the magnetic property of the amorphous alloy from the valence electron level using EET, which provides a new method to investigate the soft magnetic property of the amorphous alloy instead of the real measurement.

Hardness of single phase high entropy carbide ceramics with different compositions

Five high entropy carbide ceramics, (Hf0.2,Nb0.2,Ta0.2,Ti0.2,Zr0.2)C, (Cr0.2,Hf0.2,Ta0.2,Ti0.2,Zr0.2)C, (Hf0.2,Mo0.2,Ta0.2,Ti0.2,Zr0.2)C, (Hf0.2,Ta0.2,Ti0.2,W0.2,Zr0.2)C, and (Hf0.2,Mo0.2,Ti0.2,W0.2,Zr0.2)C, were synthesized by carbothermal reduction of oxides and direct current sintering. The five high entropy carbide ceramics were determined to be nominally phase-pure with relative densities of more than 98.9% and mean grain sizes of less than 5 μm. Average Vickers hardness values ranged from 19.2 ± 0.4 GPa for (Hf0.2,Nb0.2,Ta0.2,Ti0.2,Zr0.2)C at a load of 2 kgf to 43.5 ± 0.4 GPa for (Hf0.2,Mo0.2,Ti0.2,W0.2,Zr0.2)C at a load of 0.05 kgf. Hardness generally increased with increasing the valence electron concentration and strain as measured by the Williamson–Hall analysis. However, neither correlation was conclusive enough to be a clear indicator of hardness. Instead, it was determined that a combination of effects that includes the valence electron concentration, lattice strain, and grain size all contribute to the hardness of high entropy carbide ceramics.

Promoting the optoelectronic and nonlinear optics properties of MoS2 nanosheets via metal Al anchoring

Molybdenum disulfide (MoS2) has attracted much attention in the field of optoelectronic materials due to its stability and adjustable bandgap structure. However, improving the optoelectronic properties of MoS2 is still a challenging research. Herein, Al doped MoS2 (AMS) films were prepared by a simple single-step magnetron sputtering method. The bonding modes of Al implantation and auxiliary MoS2 were investigated by adjusting metal Al anchoring. The successful synthesis of AMS films was confirmed by the analysis of X-ray diffraction and X-ray photoelectron spectroscopy measurements to investigate the diffraction peaks of Al and Al2S3 and the valence electron structures of Al3+. Compared to MoS2, the A1g Raman peaks of AMS films are slightly blue-shifted, and the peak positions of both Mo3d and S2p are slightly shifted towards higher binding energies. This is attributed to the surface plasmon resonance effect produced by Al doping resulting in a large amount of electron transfer to the conduction band (CB) of MoS2. In addition, the density functional theory calculations reveal that Al doping of MoS2 results in a higher concentration of electrons in CB of MoS2, the band gap of MoS2 can be adjusted by changing the doping concentration of Al. The Z-scan results illustrated that MoS2 was converted from saturable absorption to reverse saturable absorption (RSA) by adjusting the sputtering power of Al. This is attributed to the fact that Al doping increases the electron concentration in the CB of MoS2, which promotes the RSA of the excited states and doping energy levels of AMS films. The values of the nonlinear absorption coefficients of AMS films are 2–5 times higher than those of MoS2, which significantly improves the nonlinear absorption performance of MoS2. The carrier relaxation process and kinetic mechanism of AMS films were investigated by transient absorption spectroscopy, moderate doping of Al can effectively improve the carrier lifetime. This implies that AMS films have good optoelectronic properties and have a wide application potential in optoelectronic devices.