Stacking Configurations Research Articles

Stacking engineering induced Z-scheme MoSSe/WSSe heterostructure for photocatalytic water splitting.

Stacking engineering is a popular method to tune the performance of two-dimensional materials for advanced applications. In this work, Jansu MoSSe and WSSe monolayers are constructed as a van der Waals (vdWs) heterostructure by different stacking configurations. Using first-principle calculations, all the relaxed stacking configurations of the MoSSe/WSSe heterostructure present semiconductor properties while the direct type-II band structure can be obtained. Importantly, the Z-scheme charge transfer mode also can be addressed by band alignment, which shows the MoSSe/WSSe heterostructure is an efficient potential photocatalyst for water splitting. In addition, the built-in electric field of the MoSSe/WSSe vdWs heterostructure can be enhanced by the S-Se interface due to further asymmetric structures, which also results in considerable charge transfer comparing with the MoSSe/WSSe vdWs heterostructure built by the S-S interface. Furthermore, the excellent optical performances of the MoSSe/WSSe heterostructure with different stacking configurations are obtained. Our results provide a theoretical guidance for the design and control of the two-dimensional heterostructure as photocatalysts through structural stacking.

A twist for tunable electronic and thermal transport properties of nanodevices.

Twisted graphene-layered materials with nonzero interlayer twist angles (θ) have recently become appealing, as they exhibit a range of attractive physical properties, which include a Mott insulating phase and superconductivity. In this study, we consider nanodevices constructed from zigzag graphene nanoribbons with a top rectangular benzenoid [6,3]-flake. Using density functional theory and a non-equilibrium Green's function approach, we explore how the electronic and thermal transport properties in such nanodevices can be tuned through a twist of the top flake by an angle 0° ≤ θ ≤ 8.8° for different stacking configurations. We found a strong dependency of the electronic structure on the stacking type, as well as on the twisting regime, specifically in AA-stacking devices. Electron and hole van Hove singularities (vHSs), which originate, respectively, from the flatness of the top of the valence band for the minor-spin component and the bottom of the conduction band for the major-spin component, are found very close to the Fermi level in the density of states and electronic transmission spectra of AA-stacking devices with a twist angle of 1.1°. We establish that these vHSs in AA-1.1° devices are stable at higher temperatures and, with the increased number of available states, lead to larger values of electron thermal conductivity and finally total thermal conductivity in AA-1.1°. Our work highlights the essential role of twisting and stacking for the fabrication of nanoscale charge and heat switches and spurs future studies of twisted layered structures.

Single Molecular Semi-Sliding Ferroelectricity/Multiferroicity.

In recent years, the unique mechanism of sliding ferroelectricity with ultralow switching barriers has been experimentally verified in a series of 2-dimensional (2D) materials. However, its practical applications are hindered by the low polarizations, the challenges in synthesis of ferroelectric phases limited in specific stacking configurations, and the low density for data storage since the switching process involves large-area simultaneous sliding of a whole layer. Herein, through first-principles calculations, we propose a type of semi-sliding ferroelectricity in the single metal porphyrin molecule intercalated in 2D bilayers. An enhanced vertical polarization can be formed independent on stacking configurations and switched via sliding of the molecule accompanied by the vertical displacements of its metal ion anchored from the upper layer to the lower layer. Such semi-sliding ferroelectricity enables each molecule to store 1 bit data independently, and the density for data storage can be greatly enhanced. When the bilayer exhibits intralayer ferromagnetism and interlayer antiferromagnetic coupling, a considerable difference in Curie temperature between 2 layers and a switchable net magnetization can be formed due to the vertical polarization. At a certain range of temperature, the exchange of paramagnetic-ferromagnetic phases between 2 layers is accompanied by ferroelectric switching, leading to a hitherto unreported type of multiferroic coupling that is long-sought for efficient "magnetic reading + electric writing".

Exploring the versatility of MoSe2/WS2 heterostructures.

Two-dimensional materials and their combined heterostructures have paved the way for numerous next-generation electronic and optoelectronic applications. Herein, we performed first principles calculations to computationally design the MoSe2/WS2 heterostructure and consider its geometric structure, electronic properties and contact behavior, as well as the effects of the electric fields and strain. Our results show that the MoSe2/WS2 heterostructure is energetically, thermodynamically and mechanically stable. Depending on the stacking configurations, the MoSe2/WS2 heterostructure could form type-I or type-II band alignment. The versatility in contact behavior makes the MoSe2/WS2 heterostructure attractive in electronics and optoelectronics. The combination of the MoSe2/WS2 heterostructure also leads to an enhancement in the adsorption efficiency and the carrier mobility compared with the constituent components. More interestingly, our findings demonstrate that the electric field can induce the transition between type-I and type-II band alignments, as evident by the experimental measurement [J. Kistner-Morris, A. Shi, E. Liu, T. Arp, F. Farahmand, T. Taniguchi, K. Watanabe, V. Aji, C. H. Lui and N. Gabor, Nat. Commun., 2024, 15, 4075]. Additionally, we also find that strain can also induce the transition between type-I and type-II band alignments and lead to the transition from semiconductor to metal in the MoSe2/WS2 heterostructure. Our findings prove that the MoSe2/WS2 heterostructure holds significant potential for developing next-generation electronics.

Molecular dynamics simulations of aggregation and viscosity properties of model asphaltene molecules containing a polycyclic hydrocarbon nucleus with toluene additive under shear interactions.

Reducing the viscosity of heavy oil is beneficial to the process of oil recovery, so it is of great significance to explore the influence of different factors on the viscosity of heavy oil. In this study, molecular dynamics (MD) simulations were carried out to study the viscosity properties of 15 structurally homologous model polycyclic molecules under shear conditions and with a toluene additive with different concentrations. Over 50 sets of simulation systems were constructed and simulated in this work. The molecular structure effect including the phenyl ring arrangements, alkyl side chain decorations, and heteroatoms, as well as the solvent effect such as the concentration of the toluene additive was comprehensively studied. It was found that under the shear conditions, the more branched the benzene ring in the polycyclic hydrocarbon nucleus, the greater the molecular steric hindrance generated, resulting in higher viscosity compared to O-shaped polycyclic hydrocarbon nucleus molecules. The introduction of alkyl side chains and heteroatoms leads to increased intermolecular interactions and more face-to-face stacking configurations, resulting in an increase in viscosity. However, in comparison, the heteroatoms effect is more pronounced in intermolecular interactions and increases in viscosity. Molecular trajectory analysis further indicates the molecular aggregates undergo continuous fracture and recombination under shear interaction, which is related to the trend of changes in viscosity properties. The current research provides new atomic-level insights into the molecular motion of heavy oil components under shear interaction in the presence of a toluene additive.

Controllable electronic properties, contact barriers and contact types in a TaSe2/WSe2 metal-semiconductor heterostructure.

Two-dimensional (2D) metallic TaSe2 and semiconducting WSe2 materials have been successfully fabricated in experiments and are considered as promising contact and channel materials, respectively, for the design of next-generation electronic devices. Herein, we design a metal-semiconductor (M-S) heterostructure combining metallic TaSe2 and semiconducting WSe2 materials and investigate the atomic structure, electronic properties and controllable contact types of the combined TaSe2/WSe2 M-S heterostructure using first-principles calculations. Our results reveal that the TaSe2/WSe2 M-S heterostructure can adopt four different stable stacking configurations, all of which exhibit enhanced elastic constants compared to the constituent monolayers. Furthermore, the TaSe2/WSe2 M-S heterostructure exhibits p-type Schottky contact (SC) with Schottky barriers ranging from 0.36 to 0.49 eV, depending on the stacking configurations. The TaSe2/WSe2 M-S heterostructure can be considered as a promising M-S contact for next-generation electronic Schottky devices owing to its small tunneling resistivity of about 2.14 × 10-9 Ω cm2. More interestingly, the TaSe2/WSe2 M-S heterostructure exhibits tunable contact types and contact barriers under the application of an electric field. A negative electric field induces a transition from Schottky contact type to ohmic contact (OC) type. On the other hand, a positive electric field leads to a transformation from p-type SC to n-type SC. Our findings provide valuable insights into the practical applications of the TaSe2/WSe2 M-S heterostructure towards next-generation electronic devices.

Prediction of the two-dimensional ferromagnetic semiconductor Janus 2H-ZrTeI monolayer with large valley and piezoelectric polarizations.

Two-dimensional room-temperature Janus ferrovalley semiconductors with valley polarization and piezoelectric polarization offer new perspectives for designing multifunctional nanodevices. Herein, using first-principles calculations, we predict that the Janus 2H-ZrTeI monolayer is an intrinsic ferromagnetic semiconductor with in-plane magnetic anisotropy and a Curie temperature of 111 K. The Janus ZrTeI monolayer possesses a significant valley polarization of 141 meV due to time-reversal and inversion symmetry breaking. Based on the valley-contrasting Berry curvature, the anomalous valley Hall effect can be observed under an in-plane electric field. Meanwhile, the breaking of the inversion symmetry and mirror symmetry results in large longitudinal and transverse piezoelectric coefficients. By applying biaxial strain, the Janus 2H-ZrTeI monolayer can also be transformed into a Weyl nodal line semimetal. Furthermore, bilayers of ZrTeI with AB and BA stacking configurations allow the coexistence of valley polarization and ferroelectricity, enabling the manipulation of magnetism, ferroelectric polarization, and valley polarization through interlayer sliding. Our work provides a platform for studying valley polarization, piezoelectricity, and multiferroic coupling, which is significant for the application of multifunctional devices.

Stacking Order Engineering of Two-Dimensional Materials and Device Applications.

Stacking orders in 2D van der Waals (vdW) materials dictate the relative sliding (lateral displacement) and twisting (rotation) between atomically thin layers. By altering the stacking order, many new ferroic, strongly correlated and topological orderings emerge with exotic electrical, optical and magnetic properties. Thanks to the weak vdW interlayer bonding, such highly flexible and energy-efficient stacking order engineering has transformed the design of quantum properties in 2D vdW materials, unleashing the potential for miniaturized high-performance device applications in electronics, spintronics, photonics, and surface chemistry. This Review provides a comprehensive overview of stacking order engineering in 2D vdW materials and their device applications, ranging from the typical fabrication and characterization methods to the novel physical properties and the emergent slidetronics and twistronics device prototyping. The main emphasis is on the critical role of stacking orders affecting the interlayer charge transfer, orbital coupling and flat band formation for the design of innovative materials with on-demand quantum properties and surface potentials. By demonstrating a correlation between the stacking configurations and device functionality, we highlight their implications for next-generation electronic, photonic and chemical energy conversion devices. We conclude with our perspective of this exciting field including challenges and opportunities for future stacking order engineering research.

(Invited) Growth of Hexagonal Boron Nitride by MOCVD for Electronic and Photonic Applications

Hexagonal boron nitride (h-BN) is a 2-dimensional (2D) layered insulating material. Thanks to its wide bandgap of ~6 eV and high thermal conductivity, h-BN has been widely utilized as an ideal substrate, gate dielectric material, passivation layer, and atomic tunnelling layer for 2D electronic devices. Recently, it has gained more attention as active material for photonics applications due to its potential for stable quantum emitters in the visible spectral range, as well as deep-ultraviolet emitters and detectors due to its exceptionally high internal quantum efficiency despite its indirect bandgap. However, mechanically exfoliated bulk h-BN and h-BN films grown on catalytic metal substrates by conventional chemical vapor deposition (CVD) systems have been mainly used to study the fundamental properties, lacking in scalability for practical implementation of h-BN.Here, we exploit the scalable approach to grow h-BN on various substrates such as sapphire, Si, and GaN, by using metal-organic chemical vapor deposition (MOCVD). A few-layer h-BN films were successfully grown on those substrates. In particular, we successfully accomplished the conformal growth of few-layer h-BN over an array of Si-based nanotrenches with 45 nm pitch and the aspect ratio of ~ 7:1. Moreover, it was found that at a specific MOCVD growth condition, a very unique h-BN film can be grown on GaN substrates, in which few-layer h-BN film is suspended on GaN nanoneedles. The combination of state-of-the-art microscopic and spectroscopic analyses revealed that the suspended h-BN films exhibit unprecedented deep ultraviolet photoluminescence spectra with local variation in band-edge emission. In addition, the h-BN films show unprecedented atomic stacking configuration, the mechanism of which will be discussed with optical and structural characterizations and theoretical calculations.

Investigating the influence of High-Void content on the impact and Post-Impact properties of Flax/Epoxy composite laminates with different stacking configurations

Defects in composite materials, such as voids, significantly impact their long-term performance and should be carefully considered in the design process of engineering structures. This study investigates the effects of high void content on the impact and post-impact properties of pure Flax/Epoxy (FE) composite laminates. Three main configurations, namely cross-ply (CFE), angle-ply FE (AFE), and quasi-isotropic FE (QFE), are examined using drop-weight impact and three-point bending tests. The results reveal distinct behavior among the configurations. The drop-weight impact test results show that the AFE configuration exhibits 3.5 % and 6.45 % higher impact resistance compared to CFE and QFE, respectively. to the increase of the impact energy to 15 J amplifies the differences to 9.31 % and 19.11 %. Also, post-impact flexion tests demonstrate a significant decline in flax composite resistance by 14 % for CFE, 26 % for QFE, and AFE. Furthermore, the overall impact and flexural properties of the FE composites are not significantly affected by the void content. However, it has a major impact on the damage mechanism that is ispected visually and through X-ray tomography, emphasizing the importance of considering the void content in the design and analysis of such flax composites. The proposed numerical model to predict the onset of damage and damage evolution in these composite materials under low velocity impact show a good greement with the experimental results.

Bandgap engineering and tuning of optoelectronic properties of 2D NbSe2/MoS2 heterostructure using first principle computations

This study performed first-principles calculations based on density functional theory to study the interlayer electronic and optical properties of NbSe2/MoS2 heterostructures. Bandgap in 2H-MoS2 is often quite large typically around 1.8 eV, showing slow response time and low photoresponsivity (R); however, a slight bandgap variation can improve the properties of semiconducting and conducting heterostructures. Different stacking configurations of the interlayer van der Waals interaction were precisely investigated. Due to their unique properties, atomically thin NbSe2/MoS2 based heterostructures hold great potential for future electronic and optoelectronic devices. LDA, GGA, GGA with SOC, and HSE06 are used to study the monolayers of MoS2, NbSe2, and their T and H stacking structures. Our results demonstrate that the metallic NbSe2 effect on the semi-metallic MoS2 reduces the band gap of MoS2 up to 140 meV. Moreover, these heterostructures exhibit outstanding absorption properties from visible to ultraviolet regions, which makes them ideal candidates for optoelectronic applications, particularly in photodetectors.

Enhanced electron–phonon coupling by delocalizing phonon states for desirable interlayer transfer of excited charges in MoSSe/WS2 heterobilayer

Regulating the interlayer transfer of excited charges is challenging but crucial for high-efficiency photoelectric conversion devices based on semiconductor heterojunction. In this work, the interlayer transfer and recombination of excited charges are investigated for the heterobilayers based on monolayer MoSSe and WS2 by combining density functional theory calculation with nonadiabatic molecular dynamics simulation. Our results reveal that the heterobilayers possess type-II band alignments and the interface engineering from S–Se to S–S stacking configuration reverses the spatial distribution of valence and conduction bands from MoSSe and WS2 to WS2 and MoSSe layers, respectively, which produces interlayer transfer of excited charges in opposite direction. The interface engineering also causes the delocalization of out-of-plane phonon states from the WS2 layer to both WS2 and MoSSe layers. This delocalized character in S–S configuration facilitates the simultaneous coupling of out-of-plane phonon states with the localized donor and acceptor electronic states, accelerates the motion of interface atoms, and reduces the band energy differences, which synergistically promote interlayer transfer of excited charges. As a result, the interlayer transfer of excited charges in S–S configuration is faster than that in S–Se configuration. Our investigation demonstrates that delocalizing phonon states through interface engineering can regulate electron–phonon coupling and interlayer transfer of excited charges.

Janus Zn-IV-VI: Robust Photocatalysts with Enhanced Built-In Electric Fields and Strain-Regulation Capability for Water Splitting.

The use of 2D materials to produce hydrogen (H2 ) fuel via photocatalytic water splitting has been intensively studied. However, the simultaneous fulfillment of the three essential requirements-high photon utilization, rapid carrier transfer, and low-barrier redox reactions-for wide-pH-range production of H2 still poses a significant challenge with noadditional modulation. By employing the first-principles calculations, it has been observed that the Janus ZnXY2 structures (X = Si/Ge/Sn, Y = S/Se/Te) exhibit significantly enhanced built-in electric fields (0.20-0.36eVÅ-1 ), which address the limitations intrinsically. Compared to conventional Janus membranes, the ductile ZnSnSe2 and ZnSnTe2 monolayers have stronger regulation of electric fields, resulting in improved electron mobility and excitonic nature (Ebinding = 0.50/0.35eV). Both monolayers exhibit lower energy barriers of hydrogen evolution reaction (HER, 0.98/0.86eV, pH = 7) and resistance to photocorrosion across pH 0-7. Furthermore, the 1% tensile strain can further boost visible light utilization and intermediate absorption. The optimal AC-type bilayer stacking configuration is conducive to enhancing electric fields for photocatalysis. Overall, Janus ZnXY2 membranes overcome the major challenges faced by conventional 2D photocatalysts via intrinsic polarization and external amelioration, enabling efficient and controllable photocatalysis without the need for doping or heterojunctions.

Mesoscopic Stacking Reconfigurations in Stacked van der Waals Film.

Mesoscopic-scale stacking reconfigurations are investigated when van der Waals (vdW)films are stacked. A method to visualize complicated stacking structures and mechanical distortions simultaneously in stacked atom-thick films using Raman spectroscopy is developed. In the rigid limit, it is found that the distortions originate from the transfer process, which can be understood through thin film mechanics with a large elastic property mismatch. In contrast, with atomic corrugations, the in-plane strain fields are more closely correlated with the stacking configuration, highlighting the impact of atomic reconstructions on the mesoscopic scale. It is discovered that the grain boundaries do not have a significant effect while the cracks are causing inhomogeneous strain in stacked polycrystalline films. This result contributes to understanding the local variation of emerging properties from moiré structures and advancing the reliability of stacked vdW material fabrication.

Effects of π-π Stacking on Shale Gas Adsorption and Transport in Nanopores.

The π-π interaction is a prevalent driving force in the formation of various organic porous media, including the shale matrix. The configuration of π-π stacking in the shale matrix significantly influences the properties of shale gas and plays a crucial role in understanding and exploiting gas resources. In this research, we investigate the impact of different π-π stacking configurations on the adsorption and transport of shale gas within the nanopores of the shale matrix. To achieve this, we construct kerogen nanopores using π-π stacked columns with varying stacking configurations, such as offset/parallel stacking types and different orientations of the stacked columns. Through molecular dynamics simulations, we examined the adsorption and transport of methane within these nanopores. Our findings reveal that methane exhibits stronger adsorption in smoother nanopores, with this adsorption remaining unaffected by the nanoflow. We observe a heterogeneous distribution of the 2D adsorption free energy, which correlates with the specific π-π stacking configurations. Additionally, we introduce the concept of "directional roughness" to describe the surface characteristics, finding that the nanoflow flux increases as the roughness decreases. This research contributes to the understanding of shale gas behavior in the shale matrix and provides insights into nanoflow properties in other porous materials containing π-π stackings.

Electronic Properties and Interlayer Interactions in Antimony Oxide Homo‐ and Heterobilayers

Antimony shows promise as a 2D mono‐elemental crystal, referred to as antimonene. When exposed to ambient conditions, antimonene layers react with oxygen, forming new crystal structures, leading to significant changes in electronic properties. These changes are influenced by the degree of oxidation. Utilizing density‐functional theory calculations, stable configurations of bilayer antimony oxide and their corresponding electronic properties are studied. Additionally, different stacking arrangements and their effects on the physical properties of the materials are investigated. Furthermore, the analysis encompasses strain‐free heterobilayers containing both pristine and oxidized antimonene layers, aiming to understand the interplay between these materials and their collective impact on the bilayer properties. In the results, insight is provided into how the properties of antimony‐based bilayer structures can be modified by adjusting stoichiometry and stacking configurations.

Designing Layered 2D Skyrmion Lattices in Moiré Magnetic Heterostructures

AbstractSkyrmions are promising for the next generation of spintronic and magnonic devices, but their zero‐field stability and controlled nucleation through chiral interactions remain challenging. In this theoretical study, the potential of moiré magnetic heterostructures to generate ordered skyrmion lattices from the stacking‐dependent magnetism in 2D magnets is explored. Heterostructures formed by twisting ultrathin CrBr3 films on top of CrI3 substrates are considered, assuming a moderate interfacial Dzyaloshinskii–Moriya interaction. At large moiré periodicity and appropriate substrate thickness, a moiré skyrmion lattice emerges in the interfacial CrBr3 layer due to the weaker exchange interactions in CrBr3 compared to CrI3. This lattice is then projected to the remaining layers of the CrBr3 film via chiral interlayer exchange fields. By varying the pristine stacking configurations within the ultrathin CrBr3 film, layered ferromagnetic and antiferromagnetic skyrmion lattices without the need for a permanent magnetic field are realized. These findings suggest the possibility of creating ordered skyrmion lattices in moiré magnetic heterostructures, enabling further exploration of their fundamental properties and technological relevance.

Robust Type‐II Band Alignment and Stacking‐Controlling Second Harmonic Generation in GaN/ZnO vdW Heterostructure

AbstractMost traditional 2D materials have small bandgaps, resulting in low laser damage thresholds and limiting their applications in the ultraviolet region. Recently experimentally synthesized 2D GaN and ZnO can be such candidates due to their wide bandgaps, high charge mobilities, and optical transparency. Here, the van der Waals heterostructure GaN/ZnO is predicted that can exhibit both wide bandgap and strong second harmonic generation (SHG) response by compelling simulations. The results show the heterostructure always exhibits type‐II band alignment under all probable stacking configurations. The out‐of‐plane SHG coefficients are up to 90 pm V−1 at 400 nm, comparable to those of MoS2 and MoSe2 and higher than most 3D crystals. Interestingly, the positions are enhanced with localized, symmetric, and stacking‐dependent features in the Brillouin zone. This peculiar momentum space behavior is originated from the relative strength of two distinct mechanisms contributing to the second‐order nonlinear optical (NLO) response, that is, a purely interband transition part and a mixed interband‐intraband contribution. Thus, this study proposes that GaN/ZnO heterostructure may be an efficient and high laser damage thresholds (LDTs) NLO material and an interesting platform for studying NLO optical properties.

Addressing the effect of stacking faults in X-ray diffractograms of graphite through atom-scale simulations

Determining the average contribution and actual distribution of rhombohedral stacking sequences within the average graphitic crystallite remained unsolved. To address this issue, we used a bottom-up approach to simulate X-ray diffractograms of graphite crystallites up to one million atoms in various graphene stacking configurations to find out how to match experimental data. The 100–101 2θ range was highly sensitive to the presence of C layers and can be used to accurately characterize the stacking disorder. On the opposite, the 110–112 2θ range was not sensitive to stacking disorder and thus can be taken as a reference to obtain the average in-plane size La of the crystallites, faulted or not. We used the principle of the L'c parameter, introduced in a former work, which corresponds to the height of the coherent sub-domains within the average crystallite obtainable through the shape of the hkl peaks involving both in-plane and out-of-plane directions. Three types of defects within a Bernal sequence were analyzed, which do not affect the peaks the same way: (i) a substitution of A or B by C, (ii) an insertion of C leading to destructive interferences, and (iii) a so-called "block shifting". It is thus possible to go further in the interpretation of X-Ray diffraction. Finally, we discussed how the overall crystallite size Lc can be obtained from all the 00l peaks.

Low‐velocity impact response and post‐impact assessment of self‐healing composites with different stacking configurations of core–shell nanofibers

AbstractThis work investigates the low‐velocity impact (LVI) and self‐healing behavior of carbon fiber composite laminates interlaced with electrospun polyacrylonitrile core–shell nanofibers (PAN@CFRP). The main goal is to investigate the influence of different stacking configurations of core–shell nanofibers on the impact resistance and self‐healing properties of composite laminates. To achieve the purpose, three different stacking configurations were designed and tested alongside virgin specimens. The damage mechanism and self‐healing of laminates following LVI were determined using ultrasonic C‐scan and cross‐sectional microscopy examinations. At an impact energy of 14.1 J, the flexural strength of the post‐healing PAN‐3@CFRP specimen reached 95.0% of the initial value, whereas at an impact energy of 21.8 J, severe impact damage was observed in the laminates with different configurations. Among the laminates, the PAN‐1@CFRP specimen had the highest flexural strength after healing, which reached 80.1% of its pre‐impact strength. As observed, the impact resistance and self‐healing capacity of composites could be significantly enhanced by optimizing the distribution configuration of core–shell nanofibers for various impact energies.Highlights The introduction of electrospun core–shell nanofibers has not significantly compromised the mechanical properties of the composites, but rather enhanced their toughness. The addition of core–shell nanofibers significantly enhances the impact resistance of the composites and imparts excellent self‐healing properties to the material. The flexural strength of impact‐damaged specimens with different stacking configurations can be restored up to 95% of the undamaged specimen after repair treatment. Significantly improved impact resistance and self‐healing ability of laminates by optimizing the distribution configuration of core–shell nanofibers between composite layers.