Theoretical Determination of the Electronic Structures and Energy-Level Splitting for Pr3+-Doped Y2SiO5 Crystals.

Trivalent praseodymium (Pr3+)-doped yttrium silicate (Y2SiO5) crystals have been widely used in various phosphors owing to their excellent luminescence characteristics. Although a series of studies have been carried out on its application prospects, the electronic structures and energy-transfer mechanisms of Pr3+-doped Y2SiO5 (Y2SiO5:Pr) remain an exploratory topic. Herein, the crystal structure analysis by the particle swarm optimization structure search method is used to study the structural evolution of Y2SiO5:Pr. Two novel structures with local [PrO7]-11 and [PrO6]-9 [Y2SiO5:Pr (I) and Y2SiO5:Pr (II)] are successfully identified. The impurity Pr3+ ions occupy the Y3+ sites and successfully integrate into the Y2SiO5 host crystal with a Pr3+ concentration of 6.25%. The calculated electronic band structures show that the doping of Pr3+ induces a reduction in band gaps for the host Y2SiO5 crystal. The conduction bands near the Fermi level are completely composed of f states. For the atomic energies of Pr3+ in Y2SiO5, the Stark levels and transitions are properly simulated based on a new set of crystal field parameters (CFPs) at the C1 site symmetry. A satisfactory r.m.s. dev. of 15.57 cm-1 with 9 free ion parameters (plus 27 fixed CFPs as obtained from ab initio calculation) fitted to the 33 observed levels is obtained for the first time. The plentiful energy-level transition lines, from the visible light to the near-infrared region, are deciphered for Pr3+ in Y2SiO5. Blue 3P0 → 3H4 at 465 nm is calculated to be a strong emission line, and it might be an ideal channel for laser actions. These results could not only provide important insights into the rare-earth-doped crystals but also lay the foundation for future research studies of designing the new laser materials.

Heterojunction of MXenes and MN4-graphene: Machine learning to accelerate the design of bifunctional oxygen electrocatalysts.

Oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are essential for the development of excellent bifunctional electrocatalysts, which are key functions in clean energy production. The emphasis of this study lies in the rapid design and investigation of 153 MN4-graphene (Gra)/ MXene (M2NO) electrocatalysts for ORR/OER catalytic activity using machine learning (ML) and density functional theory (DFT). The DFT results indicated that CoN4-Gra/Ti2NO had both good ORR (0.37 V) and OER (0.30 V) overpotentials, while TiN4-Gra/M2NO and MN4-Gra/Cr2NO had high overpotentials. Our research further indicated orbital spin polarization and d-band centers far from the Fermi energy level, affecting the adsorption energy of oxygen-containing intermediates and thus reducing the catalytic activity. The ML results showed that the gradient boosting regression (GBR) model successfully predicted the overpotentials of the monofunctional catalysts RhN4-Gra/Ti2NO (ORR, 0.39 V) and RuN4-Gra/W2NO (OER, 0.45 V) as well as the overpotentials of the bifunctional catalyst RuN4-Gra/W2NO (ORR, 0.39 V; OER, 0.45 V). The symbolic regression (SR) algorithm was used to construct the overpotential descriptors without environmental variable features to accelerate the catalyst screening and shorten the trial-and-error costs from the source, providing a reliable theoretical basis for the experimental synthesis of MXene heterostructures.

Prediction of a two-dimensional high Curie temperature Weyl nodal line kagome semimetal.

Kagome lattices may have numerous exotic physical properties, such as stable ferromagnetism and topological states. Herein, combining the particle swarm structure search method with first-principles calculations, we identify a two-dimensional (2D) kagome Mo2Se3 crystal structure with space group P6/mmm. The results show that 2D kagome Mo2Se3 is a 100% spin-polarized topological nodal line semimetal and exhibits excellent ambient stability. The band crossing points form two nodal loops around the high-symmetry points Γ and K. On the other hand, Mo2Se3 shows intrinsic ferromagnetism with a large magnetic moment of 3.05 µB per Mo atom and magnetic anisotropy energy (MAE) of 4.78 meV. Monte Carlo simulations estimate that Mo2Se3 possesses a high Curie temperature of about 673 K. In addition, its ferromagnetic ground state can be well preserved under external strain, and the MAE can be improved by increasing the strain. More importantly, the position of each nodal line can be adjusted to the Fermi level through hole doping. This multifunctional 2D magnetic material that combines spin and topology has great potential in the field of nanoscale spintronic devices.

Electric Field-Controlled Magneto-Optical Kerr Effect in A-Type Antiferromagnetic Fe2CX2 (X = F, Cl) and Its Janus Monolayer.

The magneto-optical Kerr effect (MOKE) is a powerful probe of magnetism and has recently gained new attention in antiferromagnetic (AFM) materials. Through extensive first-principles calculations and group theory analysis, we have identified Fe2CX2 (X = F, Cl) and Janus Fe2CFCl monolayers as ideal A-type collinear AFM materials with high magnetic anisotropy and Néel temperatures. By applying a vertical external electrical field (Ef) of 0.2 V/Å, the MOKE is activated for Fe2CF2 and Fe2CCl2 monolayers without changing their magnetic ground state, and the maximum Kerr rotation angles are 0.13 and 0.08°, respectively. Due to the out-of-plane spontaneous polarization, the intrinsic and nonvolatile MOKE is found in the Janus Fe2CFCl monolayer and the maximal Kerr rotation angle without external electronic field is 0.25°. Moreover, the intrinsic built-in electronic field also gives origin to more robust A-type AFM ordering and reversible Kerr angle against external Ef. Our study suggests that Ef is an effective tool for controlling MOKE in two-dimensional (2D) AFM materials. This research opens the possibility of related studies and applications in AFM spintronics.

Excellent 5f-electron magnet of actinide atom decorated gh-C3N4 monolayer.

Atomic functionality of two-dimensional (2D) materials, typically with a controllable doping route for offering regular atomic arrangement as well as excellent magnetism, is crucial for both fundamental studies and spintronic applications. Here, the adsorptions of the 5f-electron actinide series (An = Ac-Am) on porous graphene-like carbon-nitride (gh-C3N4) layers are explored to determine their structural stabilities, electronic nature and magnetic properties using the combination of density functional theory (DFT) calculations, ab initio molecular dynamics (AIMD), Monte Carlo (MC) simulations and chemical bonding analyses. Our investigations reveal that each An atom can be individually adsorbed at the vacancy site of gh-C3N4 sheet with high energetic, thermal and dynamical stabilities, which are rooted in the major interactions of ionic An-N bonding as well as the minor interactions of covalent bonding of An-5f6d states with N-2s2p states. The delocalization of a very few 5f electrons is dependent on whether they occupy the suborbitals that are matching and conducive to hybridize with the ligand orbitals forming the 5f-2s2p covalent bonds. We propose that the Ruderman-Kittel-Kasuya-Yosida (RKKY) mechanism plays a determining role for the inter-atomic 5f-5f magnetic exchange via the 6d electrons as the conduction electrons. Large magnetic moment and magnetic anisotropy energy (MAE) from the localized 5f electrons, together with the metallic characteristics owing to the delocalized 6d electrons, render these An-based 2D materials excellent metallic magnets, especially for the U@gh-C3N4 system with the modest magnetic moment of 0.6 µB, large MAE of 53 meV and high Curie temperature (TC) of 538 K.

Study of electronic and optical properties of CdI2 modulated by electric field: a first-principles study.

We found that an out-of-plane vertical electric field of 1.0 V/Ang helps to maintain the thermodynamic and kinetic stability of monolayer CdI2.The results indicated that the electric field modulates monolayer CdI2 to produce the Mexican-hat electronic state and the giant Stark effect of the vertical electric field on monolayer CdI2 originates from electric field lifting its conduction band. The results based on HSE06 + SOC calculations show that electric field induces strong spin polarization, leading to significant energy level splitting and spin flipping in the valence band. Based on GW0 + BSE, the electric field broadens effective optical response range of monolayer CdI2, the new peak in the optical absorption spectrum under electric field indicates that electric field helps to diminish excitonic effect of monolayer CdI2.

Photoluminescence and energy transfer mechanisms of Tm3+ doped Y2O3 laser crystals: experimental and theoretical insights.

Rare-earth thulium (Tm3+) doped yttrium oxide (Y2O3) host single crystals are promising "eye-safe" laser materials. However, the mechanisms of photoluminescence and energy transfer in Tm3+ doped Y2O3 crystals are not yet understood at the fundamental level. Here, we synthetize a series of Y2O3:Tm3+ samples by the sol-gel method. Our experimental results show that the most intensive absorption line of the 3H6 → 1D2 transition occurs at 358 nm, and the strongest emission line of the 1D2 → 3F4 transition is located at 453 nm, which are in good agreement with the calculations of 363 nm and 458 nm, respectively. By using the CALYPSO structural search method, the ground state structure of Y2O3:Tm3+ with P2 space group symmetry is uncovered. The complete energy levels, including free-ion LS terms and crystal-field LSJ multiplet manifolds, of Y2O3:Tm3+ are obtained based on our developed WEPMD method. The present findings show that our WEPMD method can be used in experiments to elucidate the underlying mechanisms of photoluminescence and energy transfer in Tm3+ doped Y2O3 crystals, which offer insights for further understanding of other rare-earth doped laser materials.

Thermoelectric response of single quintuple layer sodium copper chalcogenides persisting at high temperature.

The thermoelectric transport properties of two-dimensional (2D) layered NaCuX (X = S, Se) are investigated by employing first-principles based Boltzmann transport theory. Single quintuple NaCuX layers have a relatively large Seebeck coefficient (S), electrical conductivity (σ) and hence power factor (PF = S2σ) for a p-type heavy doped region due to the valence band degeneracy. The largely reduced σ by dominant polar scattering leads to a PF up to 0.27 and 0.84 mW m-1 K-2 at 1200 K for p-type NaCuS and NaCuSe monolayers, respectively. The high polarizability of the Cu-X bonds in the CuX4 tetrahedra leads to anharmonic phonon behavior which produces an intrinsic lattice thermal conductivity (κl) as low as 1.03 and 0.75 W m-1 K-1 at 300 K for NaCuS and NaCuSe, respectively. The predicted figure of merit (zT) increases monotonically from around 0.25 at 300 K to 2.01 at 1200 K at an optimal carrier density of around 1 × 1013 cm-2 for p-type NaCuSe and from around 0.09 at 300 K to 1.15 at 1200 K at an optimal carrier density of around 1 × 1014 cm-2 for p-type NaCuS. These findings indicate that the NaCuS, especially NaCuSe, monolayers are promising 2D thermoelectric materials persisting at high temperature.

High thermoelectric performance of two-dimensional layered AB2Te4 (A = Sn, Pb; B = Sb, Bi) ternary compounds.

The thermoelectric properties of two-dimensional layered ternary compounds AB2Te4, in which A (Sn, Pb) and B(Sb, Bi) are group-IV and group-V cations, respectively, were investigated by using first-principles based transport theory. These septuple-atom-layer monolayers have wider band gaps with respect to their bulks, which extend their operating temperature and inhibit the bipolar carrier conduction and thermal conductivity, and more importantly, their energy bands exhibit multiple valence band convergence to a narrow energy range near the Brillouin zone center, which induces an optimal p-type power factor up to 10.94-32.11 W m-1 K-2 at room temperature. Moreover, these monolayers contain heavy atomic masses and high polarizability of some chemical bonds, leading to small group velocities of phonons and anharmonic phonon behavior that produce an intrinsic lattice thermal conductivity as low as 0.79-3.13 W m-1 K-1 at room temperature. Thus, these monolayers act as p-type thermoelectric materials with thermoelectric figure of merit of up to 2.6-5.5 for SnSb2Te4, 0.7-2.2 for PbSb2Te4, and 1.6-4.2 for PbBi2Te4 in the temperature range of 300 to 750 K, and 4.5-5.9 for SnBi2Te4 in the temperature range of 300 to 450 K.

Electronic structure, magnetoresistance and spin filtering in graphene|2 monolayer-CrI33|graphene van der Waals magnetic tunnel junctions.

In the pursuit of designing van der Waals magnetic tunneling junctions (vdW-MTJs) with two-dimensional (2D) intrinsic magnets, as well as to quantitatively reveal the microscopic nature governing the vertical tunneling pathways beyond the phenomenological descriptions on CrI3-based vdW-MTJs, we investigate the structural configuration, electronic structure and spin-polarized quantum transport of graphene|2 monolayer(2ML)-CrI3|graphene heterostructure with Ag(111) layers as the electrode, using density functional theory (DFT) and its combination of non-equilibrium Green's function (DFT-NEGF) methods. The in-plane lattice of CrI3 layers is found to be stretched when placed on the graphene (Gr) layer, and the layer-stacking does not show any site selectivity. The charge transfer between CrI3 and Gr layers make the CrI3 layer lightly electron-doped, and the Gr layer hole-doped. Excitingly, the inter-layer hybridization between graphene and CrI3 layers render the CrI3 layer metallic in the majority spin channel, giving rise to an insulator-to-half-metal transition. Due to the metallic/insulator characteristics of the spin-majority/minority channel of the 2ML-CrI3 barrier in vdW-MTJs, Gr|2ML-CrI3|Gr heterostructures exhibit an almost perfect spin filtering effect (SFE) near the zero bias in parallel magnetization, a giant tunneling magnetoresistance (TMR) ratio up to 2 × 104%, and remarkable negative differential resistance (NDR). Our results not only give an explanation for the observed giant TMR in CrI3-based MTJs but also show the direct implications of 2D magnets in vdW-heterostructures.

A two-dimensional PtS2/BN heterostructure as an S-scheme photocatalyst with enhanced activity for overall water splitting.

Photocatalytic hydrogen production from water is a sustainable solution to the environmental pollution and energy crises. Encouraged by the successful synthesis of PtS2 and BN nanosheets and their suitable band edges, we have designed a PtS2/BN bilayer heterojunction and investigated its electronic and optical properties for the first time based on hybrid DFT calculations. In this system, the built-in electric field and band edge bending can retain useful electrons on the conduction band of BN and holes on the valence band of PtS2, which endow this system with a stronger redox ability. Meanwhile, this electric field can efficiently separate photoinduced electron-hole pairs and improve the photocatalytic efficiency. Compared with BN and PtS2 single layers, the PtS2/BN heterojunction with its smaller bandgap can make better use of visible and infrared light. Additionally, we have studied the effect of applied strain on the electronic and optical properties. This work aims to provide a method for constructing high-efficiency BN-based photocatalysts and illuminating the electron migration mechanism in step-scheme (S-scheme) heterostructures. We have found that the PtS2/BN bilayer heterojunction is a promising S-scheme photocatalyst for overall water decomposition.

Intrinsic spin, valley and piezoelectric polarizations in room-temperature ferrovalley Janus TiXY (XY = SCl and SeBr) monolayers.

Two-dimensional room-temperature Janus ferrovalley semiconductors with large spin, valley and piezoelectric polarizations provide fertile platforms for designing multifunctional nanodevices. Little research has been reported to date on such materials. Here, using first-principles calculations, we predict two dynamically stable Janus titanium chalcohalide (TiSCl and TiSeBr) monolayers, which are excellent piezoelectric ferrovalley semiconductors with in-plane magnetization and high magnetic transition temperatures (738 and 884 K). When an extrinsic magnetic field is used to force the magnetization along the out-of-plane direction, a large valley polarization (64 and 146 meV) can be generated in the highest valence band with a large spin-orbit coupling by the breaking of time-reversal and space-inversion symmetry, which can be further clarified by a two-band k·p model. This robust valley-contrasting physics characterized by the valley-dependent Berry curvature leads to the anomalous valley Hall effect. It can be observed by suitable hole doping or light irradiation under an in-plane electric field. Besides, we find that the missing mirror symmetry results in giant out-of-plane piezoelectric polarization (2.05 and 2.04 pm V-1). These outstanding properties give the Janus TiSCl and TiSeBr monolayers potential for a wide variety of applications in nanoelectronics, spintronics, valleytronics, piezoelectrics and other demanding areas.

Above-room Curie temperature and barrier-layer-dependent tunneling magnetoresistance in 1T-CrO2 monolayer based magnetic tunnel junctions.

van der Waals (vdW) heterostructures based on two-dimensional (2D) ferromagnetic materials hold great potential applications in spintronics. Using the density functional theory (DFT) method and first-principles quantum transport simulation, we studied the structures, magnetic properties and spin-resolved transport of 1T-CrO2 monolayer (ML) based vdW magnetic tunnel junctions (MTJs). Owing to a high Curie temperature (TC) of 392 K and a moderate magnetic anisotropy energy (MAE) of 94 µeV of the ferromagnetic 1T-CrO2 monolayer, Cu(111)|CrO2|nML-Gr|CrO2|Cu(111) MTJs were built. Our results reveal that their tunneling magnetoresistance (TMR) ratios are dependent on the number of Gr barrier layers within a working bias voltage of 1 V. For the thin barrier layers (n = 1-2), the maintained TMR ratios can reach a giant value of about 1 × 104%, while there appears a decreasing trend with the increasing bias voltage for thick Gr layers (n = 3-5). The barrier-layer-dependent phenomenon is attributed to the decreasing transmission magnitude with increasing bias voltage in a parallel configuration (PC), which is as small as that in an anti-parallel configuration (APC) eventually. Our results would provide some guidance for future experimental fabrications of these 2D materials based MTJs.

A Hybrid Functional Study on Perovskite-Based Compounds CsPb1-αZnαI3-ßXß (X = Cl or Br).

Inorganic perovskites have attracted a great deal of attention because of their stability. Unfortunately, a weak optical response and the toxicity of lead are hampering their development. Motivated by these facts, we focus herein on the perovskite-based doped series CsPb1-αZnαI3-ßXß (X = Cl or Br). The geometric structures and the electronic and optical properties of CsPb1-αZnαI3-ßXß (X = Cl or Br) are investigated systematically by hybrid functional theory. Analysis of the electronic properties indicates that Zn/Cl/Br mono-doping and co-doping efficiently tune bandgaps. Moreover, we find that the ability to obtain electrons for CsPb0.625Zn0.375I2Cl is superior to the abilities of the others, which implies a stronger electron transition. In addition, CsPb0.625Zn0.375I2Cl and CsPb0.625Zn0.375I2Br show stronger visible-light responses in the range of 467-780 nm. Both CsPb0.625Zn0.375I2Cl and CsPb0.625Zn0.375I2Br are hence good choices for photovoltaic applications. Furthermore, the physically accessible region is also explored herein. These findings shed new light on the design of highly efficient and low-lead perovskite-based optoelectronic materials.

Dual-Metal Active Sites Mediated by p-Block Elements: Knowledge-Driven Design of Oxygen Reduction Reaction Catalysts.

In this study, the oxygen reduction reaction (ORR) process of dual-metal active site catalysts (FeMN6-Gra, M = Mn, Ni, Co, or Cu) mediated by p-block elements was investigated using density functional theory calculations. The obtained results demonstrate that, in most cases, the B-doped FeMN6-Gra (M = Mn, Ni, Co, or Cu) catalysts exhibit higher catalytic performance than their undoped counterparts. Among the investigated catalysts, FeNiN6-Gra doping by B modulates the adsorption strength of the metal center on the oxygen-containing intermediates, showing the largest increase in the onset potential (from 0.66 to 0.94 V). Importantly, we found a new law that B-doping affects the total charge of the metal adsorption site and the four surrounding N atoms and that there is a linear relationship between the total charge and the Gibbs free energy. Transition state analysis shows that the energy barrier of the thermodynamic rate-determining step (*OH hydrogenation to H2O) in the FeNiN6B1-Gra-catalyzed ORR process is 0.17 eV, which is smaller than that of the FeNiN6-Gra-catalyzed process (0.28 eV). Overall, the results demonstrate that B-doping can improve the activity of FeMN6-Gra catalysts and provide a new method for the future development of efficient electrocatalysts.

Rational design of M-N4-Gr/V2C heterostructures as highly active ORR catalysts: a density functional theory study.

Inspired by the composites of N-doped graphene and transition metal-based materials as well as MXene-based materials, heterostructures (M-N4-Gr/V2C) of eight different transition metals (M = Ti, Cr, Mn, Fe, Co, Ni, Cu, and Zn) doped with nitrogen-coordinated graphene and V2C as potential catalysts for the oxygen reduction reaction (ORR) using density functional theory (DFT) were designed and are described herein. The calculations showed that the heterostructure catalysts (except for Zn-N4-Gr/V2C) were thermodynamically stable. Ni-N4-Gr/V2C and Co-N4-Gr/V2C showed higher activities towards the ORR, with overpotentials as low as 0.32 and 0.45 V, respectively. Excellent catalytic performance results were observed from the change in electronic structure caused by the strong interaction between V2C and the graphene layers as well as the synergistic effect between the MN4 groups and the graphene layers. This study further provides insights into the practical application of ORR catalysts for MXene systems through the modulation of the electronic structure of two-dimensional materials.

Hourglass Weyl and Dirac nodal line phonons, and drumhead-like and torus phonon surface states in orthorhombic-type KCuS.

In parallel to electronic systems, the concept of topology has been extended to phonons, which has led to the birth of topological phonons. In this Communication, based on symmetry analysis and first-principles calculations, we propose that hourglass Weyl nodal line (HWNL) phonons and Dirac nodal line (DNL) phonons coexist in the phonon dispersion of a single material, KCuS, with a Pnma-type structure. The HWNLs and DNLs are relatively flat in frequency and well separated from other phonon bands. The drumhead-like phonon surface state and the torus phonon surface state appear at the [001] and [100] surfaces, respectively. The reason for this phenomenon is explained based on the Zak phase calculations. The DNL and HWNL phonons are symmetry-related and these phonons can also be observed in other realistic materials, such as BaSi2, TiB and ZrSi, with a Pnma-type structure. Our Communication, for the first time, proves that phononic nodal lines with different types of degeneracies and different types of phonon surface states can be achieved in one single material. Thus, KCuS with a Pnma-type structure can be viewed as a good platform to investigate the entanglement between HWNL phonons and DNL phonons and to realize the drumhead-like and torus phonon surface states.

Monolayer gadolinium halides, GdX2 (X = F, Cl, Br): intrinsic ferrovalley materials with spontaneous spin and valley polarizations.

Two-dimensional (2D) intrinsic ferrovalley semiconductors provide unprecedented opportunities to investigate valley physics as well as providing promising device applications due to their exceptional combination of spontaneous spin and valley polarizations. Here, we have predicted from first-principles calculations and Monte Carlo simulations that monolayers (MLs) GdX2 are such extremely rare excellent materials. Apart from their robust stabilities energetically, dynamically, thermally, and mechanically, these 2D materials are found to be semiconducting intrinsic ferromagnets where the magnetic coupling is ascribed to 5d-electron-mediated 4f-4f exchange interactions. Moreover, MLs GdX2 (X = F, Cl, Br) not only exhibit significant magnetic anisotropy energy of 351, 268, and 30 µeV per Gd, but also have a high Curie temperature of 300, 245, and 225 K, respectively. In particular, spontaneous valley polarization in three systems occurs due to the cooperative interplay between the spin-orbit coupling and magnetic exchange interactions, whose magnitude is as sizable as 55, 38, and 82 meV for MLs GdF2, GdCl2, and GdBr2, respectively. Under the action of an in-plane longitudinal electrical field, the valley-contrasting Berry curvatures arising from the broken space-inversion and time-reversal symmetries in MLs GdX2 could yield opposite transverse velocities of the carriers, giving rise to the occurrence of a spin-polarized anomalous valley Hall effect. Overall, these findings render 2D GdX2 a class of promising candidate materials for experimental studies and practical spintronics and valleytronics applications.

Two-dimensional CdS/SnS2 heterostructure: a highly efficient direct Z-scheme water splitting photocatalyst.

A desired water splitting photocatalyst should not only possess a suitable bandgap and band edge position, but also host the spontaneous progress for overall water splitting without the aid of any sacrificial agents. In this work, we propose a two-dimensional CdS/SnS2 heterostructure (CSHS) as a possible water splitting photocatalyst by first-principles calculations. The CSHS enhances the absorption of visible and infrared light, and the type-II band alignment guarantees the spatial separation of the photoinduced carriers. The induced built-in electric field across the CSHS interface efficiently separates the photoexcited carriers and extends their carrier lifetimes. All these properties make the CSHS a direct Z-scheme system with the hydrogen and oxygen evolution reactions occurring, respectively, at the CdS and SnS2 layers. More encouragingly, the introduction of a S-vacancy into SnS2 could effectively lower the overpotential of the oxygen evolution reaction, thus ensuring the overall water redox reaction to be achieved spontaneously under light irradiation. Our findings suggest that the CSHS is a promising water splitting photocatalyst.

Study of photogenerated exciton dissociation in transition metal dichalcogenide van der Waals heterojunction A2-MWS4: a first-principles study.

In order to explore the photocatalytic hydrogen production efficiency of the MoS2/WSe2 heterostructure (A2-MWS4) as a photocatalyst, it is highly desirable to study the photogenerated exciton dissociation related to photocatalysis. The electronic properties, optical absorption, and lattice dynamic properties of A2-MWS4 were investigated using a first-principles approach. The results show that the type II energy band alignment of A2-MWS4 facilitates the dissociation of photogenerated excitons (electrons and holes). The highly localized d-state electrons of A2-MWS4 induce the formation of internal potentials that promote the dissociation of photogenerated excitons. The hot carrier diffuses its extra energy into the lattice by scattering with phonons and forms a hot spot in the lattice while releasing phonons, which are dragged away from the hot spot by Ridley decay to promote exciton dissociation. These findings could provide insights for research studies on photochemical reactions and photovoltaic devices.