Vacancy Defects Research Articles

Strong Metal‐Support Interaction between Pt and TiO2 over High‐temperature CO2 Hydrogenation

The catalytic activities and stability of oxide‐supported metal catalysts are significantly affected by metal‐support interactions (MSI) between oxidic supports and supported metals. The surface properties of the support, such as its phase and defects, are crucial in MSI, including both the strong metal‐support interaction (SMSI) and electronic metal‐support interaction (EMSI). In this study, modulation of SMSI was achieved on rutile‐supported Pt nanoparticles (NP) over high‐temperature CO2 hydrogenation. The encapsulation of Pt NP surfaces with TiO2−x overlayers is precisely controlled by the defects. It is found that oxygen vacancy defects significantly enhance the catalytic stability of Pt/rutile under high‐temperature reverse water‐gas shift (RWGS) reaction by inhibiting the occurrence of SMSI. Pt/rutile with oxygen vacancies achieves a 301 molCO×gM‐1×h‐1 space time yield and considerably catalytic stability (decreased by 8%) at 800 °C over 100 h time‐on‐stream. Density functional theory (DFT) calculations suggest that the adsorption capacity of Pt NP on the rutile overlayer can be reduced by increasing electron density. Experimental results combined with DFT calculations show that electron transfer from Pt NP to rutile is reduced by the oxygen vacancy defects on Pt/R, preserving the metallic nature of Pt species during CO2 hydrogenation, thereby preventing the formation of SMSI.

Visible Light Driven Defect Mediated Photocatalytic Activity of Spray Pyrolyzed Ga and Al Doped ZnO Thin Film Electrodes

AbstractGa and Al doped ZnO thin film electrodes are spray deposited and explored for photocatalytic deterioration of methylene blue dye. X‐ray diffraction unveils both films to have highly textured growth along the (002) plane. The surface morphology is found to have near spherical and distorted rectangular particles for Ga and Al dopants, respectively. Photoluminescence emission study reveals that both films have visible light emissions in the violet, blue, and green regions due to oxygen vacancy defects. The deposited films exhibit a reasonably higher transmittance of 89 and 77 % with mobility of 30.5 and 29.6 cm2/Vs for Ga and Al doped ZnO, respectively. Cyclic test and photo‐corrosion studies performed for selected samples were indicating significant stability. Based on these findings the electrodes are explored for the photocatalytic degradation of methylene blue dye and are found to have significant efficiency upon LED and sunlight irradiation.

Electronic Structure Engineering of Single-Atom Tungsten on Vacancy-enriched V3S4 Nanosheets for Efficient Hydrogen Evolution.

Constructing single-atom catalysts (SACs) and optimizing the electronic structure between metal atoms and support interactions is deemed one of the most effective strategies for boosting the catalytic kinetics of the hydrogen evolution reaction (HER). Herein, a sulfur vacancy defect trapping strategy is developed to anchor tungsten single atoms onto ultrathin V3S4 nanosheets with a high loading of 25.1wt.%. The obtained W-V3S4 catalyst exhibits a low overpotential of 54mV at 10mA cm-2 and excellent long-term stability in alkaline electrolytes. Density functional theory calculations reveal that the in situ anchoring of W single atoms triggers the delocalization and redistribution of electron density, which effectively accelerates water dissociation and facilitates hydrogen adsorption/desorption, thus enhancing HER activity. This work provides valuable insights into understanding highly active single-atom catalysts for large-scale hydrogen production.

Threefold Impact on Reaction Coordinate Mapping of Zirconium Based Tri‐Chalcogenide Pseudo‐Monolayers as Emerging Ultrathin Catalysts for Water Splitting

AbstractThe continuous quest of finding optimum catalysts for photo‐electrocatalytic (PEC) water splitting has been revolving around 2D ultrathin materials because of the fact of exploiting both the surface area. In this work, a threefold impact is envisaged route to enhance the activity both in terms of hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in the emerging Zirconium Tri‐sulfides (ZrS3) based pseudo‐monolayers. Due to the unique and distinct electronic properties of the tri‐chalcogenide systems as compared to the di‐chalcogenide counterpart of Zirconium, one could afford to explore the implications of not only single‐atom functionalization and vacancy defect, but also the external strain to expedite the bifunctional catalytic activity in this promising material. Rigorous electronic structure calculations have been performed for the mentioned threefold effect on not only the band‐edge alignment, but going beyond to it by further constructing the reaction coordinate mapping corresponding to HER and OER mechanism. The repercussion of external strain in addition to the single atom functionalization and vacancy defect on the adsorption free energies of the prime intermediates of HER and OER reaction has been further correlated with the work function variation in this pseudo‐monolayer system.

Effect of Vacancy Defects on the Electronic Structure and Optical Properties of Bi4O5Br2: First-Principles Calculations

First-principles calculations based on density functional theory are employed to investigate the impact of vacancy defects on the optoelectronic properties of Bi4O5Br2. The results indicate that vacancy defects induce minimal lattice distortion in Bi4O5Br2 without compromising its structural stability. Oxygen or bromine vacancies are more likely to occur than bismuth vacancies. The introduction of a bismuth vacancy leads to n-type semiconductor behavior in the Bi4O5Br2 system, while the creation of an oxygen vacancy reduces the bandgap and enhances the light absorption capacity. Bi4O5Br2 with three coordinated oxygen vacancies exhibits a higher effective electron–hole pair mass ratio, which is advantageous for the efficient separation of electron–hole pairs. Bi4O5Br2 with three coordinated oxygen vacancies exhibits enhanced absorption and reflection coefficients in the visible-light region compared to other systems, indicating that oxygen vacancy defects significantly promote visible-light absorption and electron–hole separation. This research provides new theoretical insights for understanding and optimizing the performance of photocatalysts based on Bi4O5Br2.

Spatially Precise Light-Activated Dedoping in Wafer-Scale MoS2 Films.

2D materials, particularly transition metal dichalcogenides (TMDCs), have shown great potential for microelectronics and optoelectronics. However, a major challenge in commercializing these materials is the inability to control their dopingat a wafer scale with high spatial fidelity. Interface chemistry is used with the underlying substrate oxide and concomitant exposure to visible light in ambient conditions for photo-dedoping wafer scale MoS2. It is hypothesized that the oxide layer traps photoexcited holes, leaving behind long-lived electrons that become available for surface reactions with ambient air at sulfur vacancies (defect sites) resulting in dedoping. Additionally, high fidelity spatial control is showcased over the dedoping process, by laser writing, and fine control achieved over the degree of doping by modulating the illumination time and power density. This localized change in MoS2 doping density is very stable (at least 7 days) and robust to processing conditions like high temperature and vacuum. The scalability and ease of implementation of this approach can address one of the major issues preventing the "Lab to Fab" transition of 2D materials and facilitate its seamless integration for commercial applications in multi-logic devices, inverters, and other optoelectronic devices.

Realizing Ultrahigh Conversion Efficiency of ≈9.0% in YbCd2Sb2/Mg3Sb2 Zintl Module for Thermoelectric Power Generation.

Recently, YbCd2Sb2-based Zintl compounds have been widely investigated owing to their extraordinary thermoelectric (TE) performance. However, its p orbitals of anions that determined the valence band structure are split due to crystal field splitting that provides a good platform for band manipulation by doping/alloying and, more importantly, the YbCd2Sb2-based device has yet to be reported. In this work, single-phase YbCd1.5Zn0.5Sb2 is successfully obtained through precise chemical composition control. Then, YbMg2Sb2-alloying increases the cationic vacancy defect formation energy and further optimizes carrier concentration. Moreover, the band structure of YbCd1.5Zn0.5Sb2 is subtly manipulated, and the underlying mechanism is experimentally explored. Combined with the reduced lattice thermal conductivity, a high peak ZT value of ∼1.43 at 700K is obtained for YbCd1.425Zn0.475Mg0.1Sb2. Subsequently, choosing Fe90Sb10 as the diffusion barrier layer and adopting the transient liquid phase bonding technique, for the first time, it is demonstrated that YbCd2Sb2/Mg3(Sb, Bi)2 TE module with an ultrahigh conversion efficiency of ≈9.0% at a heat difference of 430K. More importantly, this module displays good thermal stability. This work paves the way for YbCd2Sb2 materials and devices in mid-temperature heat recovery.

High Temperature-Insensitive Electrostrain Obtained in (K, Na)NbO3-Based Lead-Free Piezoceramics.

Over the last decades, notable progress is achieved in (K, Na)NbO3 (KNN)-based lead-free piezoceramics. However, more studies are conducted to increase its piezoelectric charge coefficient (d33). For actuator applications, piezoceramics need high electric-field induced strain under low electric fields while maintaining exceptional temperature stability across a wide temperature range. In this study, this work developes Li/Sb-codoped KNN (LKNNS) ceramics with high electrostrain by defect engineering and domain engineering. A remarkable strain of 0.43%, along with a giant d33* value of 2177 pm V-1, is attained in the LKNNS ceramic at 20 kV cm-1. The ceramic exhibits a minimal performance decrease of less than 15% over a temperature range from room temperature to 150 °C. The exceptional strain is attributed to the presence of A-site vacancy-oxygen vacancy ( ) defect dipoles and the increase in nano-domains. The hierarchical domain configuration and defect dipoles impede the switched domains from reverting to their original state as temperature increases, furthermore, the elongated dipole moments of caused by rising temperatures compensate for strain reduction results in exceptional temperature stability. This study provides a model for designing piezoelectric materials with exceptional overall performance under low electric fields and across a wide temperature range.

Nanostructured defects-rich black-ZnO/biowaste-derived carbon composites for efficient visible light-driven hydrogen generation: A study on the role of C–Zn@C–O–Zn interface

The use of a highly efficient and noble-metal-free cocatalyst, which is being pursued to create hydrogen (H2) via photocatalysis, has been the subject of many studies. In this work, a unique ultrasonication-assisted laser beam irradiation process is employed to synthesize a new carbon material generated from pineapple peel biowaste (ppC) and mix it with oxygen-deficient black zinc oxide (b-ZnOvac) nanoparticles. In the ppCx@b-ZnOvac nanostructures, the XPS analysis verified the presence of surface oxygen (O2) defects and vacancies as well as chemical interactions between carbon and zinc via carbon-zinc (C–Zn) and carbon-oxygen-zinc (C–O–Zn) connection interfaces. Following optimization, the visible light active photocatalytic H2 production rate of the ppC10@b-ZnOvac nanostructures reached 215.92 μmol h−1 g−1, which was the highest. The positive synergistic interaction between b-ZnOvac and ppC is responsible for the significant increase in the rate of H2 generation. Furthermore, the significant chemical bond between ppC and b-ZnOvac via the C–Zn/C–O–Zn interface, as well as the development of surface O2 vacancy defects in b-ZnOvac, improve the efficient transfer of energetic electrons and make visible active photocatalytic H2 production from methanol in the ppCx@b-ZnOvac nanostructures easier. Our work presents a new strategy for chemically generating affordable carbon materials through the use of metal oxide-based photocatalysts with surface O2 vacancy defects and bio-waste. Applications such as water splitting, energy production, and environmental remediation show promise for these advanced materials for large-scale field applications.

Rod‐Like Microcrystal Scintillators Based on Organic–Inorganic Hybrid Copper Halides for X‐Ray Imaging

AbstractCopper‐based organic–inorganic hybrid halides (OIHHs) have garnered significant interest in X‐ray imaging due to their flexible structural adjustability, efficient light emission, strong X‐ray absorption, etc. Herein, four copper‐based OIHH crystals composed of the same organic ligands (isopropyl triphenylphosphonium cations, IPP+) and inorganic parts (Cu2I42−) are synthesized by varying the ratios of raw materials and types of reaction solvents. Although these crystals share identical structures, they exhibit different luminescent behaviors (blue, green, white, and yellow) attributed to vacancy defects originating from CuI. Notably, the novel copper‐based OIHH (CP2) with green emission shows the best luminescence efficiency (99.54%) and excellent scintillation performance (50675 photons MeV−1). The traditional technology of scintillation screens mixing scintillator powders and polymers often results in light scattering due to powder aggregation and inhomogeneity. To address this challenge, the dispersant polyvinyl pyrrolidone is introduced to prepare uniform rod‐like microcrystals of CP2. The scintillation screen based on CP2 microcrystals achieves a high spatial resolution of 16–18 lp mm−1, surpassing the resolution of most copper‐based OIHH scintillators. Furthermore, it is imaging capabilities are validated using a commercial X‐ray flat panel detector, demonstrating imaging performance comparable to that of commercial scintillators.

Microstructure regulation of WxV1-xO2(B) nanorods with improved electrochemical properties

VO2(B) is regarded as a highly promising cathode material for secondary batteries due to its outstanding theoretical specific capacity and unique expansion tunnel structure, which facilitates reversible insertion and extraction of metal ions. Nonetheless, inherent structural instability, suboptimal ion/electron transport, and constrained capacity resulting from low redox potentials pose challenges to its wider adoption. Hence, in this paper, we proposed a strategy for synthesizing gradient concentration-doped WxV1-xO2(B) nanorods via a one-step hydrothermal method to solve the above problems. The experimental results demonstrated that as the W ion content increased, all fabricated WxV1-xO2(B) nanorods exhibited a monoclinic crystal phase along with noticeable lattice distortion. The positron annihilation lifetime spectra indicated that vacancy clusters were the predominant defect types in WxV1-xO2(B) nanorods. The synergistic effects of grain sizes and vacancy defects contributed to the superior electrochemical performance observed in the W0.01V0.99O2(B) sample. The capacitor retention reached 88.76 % at 0.10 A/g after 1000 charge/discharge cycles. These results had provided experimental foundation for improving electrochemical properties of WxV1-xO2(B) in metal ion secondary batteries.

Structural Stability of Vacancy and Substitutional Defects in g-GaN: A First-Principles Study

Herein, the first-principles calculations of defected monolayer graphene-like gallium nitride (g-GaN) were elucidated. The optimized geometric revealed that the nearest-neighbor distances of N-N (between N atoms) and Ga-Ga (between Ga atoms) were narrowing in most configurations. Interestingly, the VGa has a similar atomic symmetry as the pure g-GaN, which is D3h. Most defected configurations are degraded into C2V symmetries, while the Stone-Wales configuration has the lowest symmetry of CS. The formation energies of V­­Na systems are lower, which implies better energetic stability. For the divacancies, the VGa system is more stable than the V­­Na system. Moreover, the Stone-Wales configuration is energetically more stable than the interchange configuration. Furthermore, the reaction coordinates represent the geometric evolution of each defected system. The result revealed that the N-atoms are consistent with moving outward while the Ga-atoms move inward only for monovacancies and divacancies configurations. In contrast, the N-atoms move inward while the Ga-atoms move outward for substitutions, interchanges, and Stone-Wales configurations. We believe that this finding will be beneficial as the groundwork for future 2D g-GaN-based semiconductor devices. HIGHLIGHTS The V­­Na defective system is more stable than the VGa system in monovacancies and substitutions. The VGaGa defective system is more stable than the V­­Na system in divacancies. The Stone-Wales system is a stable configuration with a Cs symmetry. GRAPHICAL ABSTRACT

Synergistic enhancement in hydrodynamic cavitation combined with peroxymonosulfate fenton-like process for bpa degradation: New insights into the role of cavitation bubbles in regulation reaction pathway

The combination of hydrodynamic cavitation (HC) and Fenton-like oxidation technology can dramatically enhance the pollutant removal capacity, however, the synergistic effect of cavitation and catalysts on reactive oxygen species (ROS) generation remained enigmatic. In this study, we established a combined system based on HC and Ce-MnFe2O4 activated peroxymonosulfate (PMS) for BPA removal, and attentions were paid on the role of cavitation bubbles. The results show that the combination of HC in Ce-MnFe2O4 activated PMS could mediate the degradation of BPA from the non-radical pathway dominated by 1O2 to •O2− dominated radical pathway. Both controlled experiments and theoretical calculations revealed that the cavitation bubbles with different sizes play the dominant role in ROS generation. The microjets produced by the collapse of cavitation bubbles could create a large number of oxygen vacancy defects on Ce-MnFe2O4 surface, which modify the activation barrier of PMS and facilitate the generation of •O2− thermodynamically. The stable existing cavitation bubbles with the size of 100∼400 nm could create considerable gas-liquid interface. The molecular dynamics simulations show that the nano bubbles can concentrate the BPA and increase the probability of contacts between BPA and Ce-MnFe2O4, hence effectively solve the issues of short lifetime of •O2− radicals and limited mass transfer distance to strengthen the reaction. In addition, the PMS/Ce-MnFe2O4/HC system not only achieves the satisfied COD (95 %) and TOC (65 %) removal efficiency but also enabled the BPA-contaminated water with a low energy cost of 0.065 kWh·m−3 and oxidant cost, highlighting the application potential of the HC technology for contaminated water.

Suppressing vacancies and crystal water of sodium manganese iron-based Prussian blue analogue by potassium doping for advanced sodium-ion batteries

Sodium manganese iron-based Prussian blue analogue (MnFe-PBAs) is regarded as potential cathode material for sodium-ion batteries due to its simple synthesis process, low production cost, and high theoretical capacity. Unfortunately, electrochemical performances of MnFe-PBAs are inevitably hindered owing to the crystal vacancies and crystal water produced from aqueous co-precipitation process. Herein, highly crystallized cubic potassium-doped sodium manganese iron-based Prussian blue analogue is synthesized by a modified co-precipitation method. By introducing a larger ionic radius potassium (K) to substitute the part of Na in the MnFe-PBAs, a coexistence composite of sodium and potassium phases is obtained with less crystal water and fewer vacancies compared with pure sodium phase compound, resulting that potassium-doped sodium manganese iron-based Prussian blue analogue (Na1.08K0.74Mn[Fe(CN)6]0.86⋅□0.14⋅1·.86H2O, NaKMHCF) can deliver high discharge specific capacity (129.3 mAh/g at 10 mA g−1), excellent rate performance (82.3 mAh/g at 1500 mA g−1) as well as high cycling stability (77.0 % capacity retention at 500 mA g−1 after the 500th cycle). Besides, the full cell, based on NaKMHCF as cathode material and sodium titanium phosphate (NTP) as anode material, confirms its potential as high-performance cathode material for SIBs.

Non-volatile and Secure Optical Storage Medium with Multilevel Information Encryption.

Non-volatile photomemory based on photomodulated luminescent materials offers unique advantages over voltage-driven memory, including low residual crosstalk and high storage speed. However, conventional materials have thus far been volatile and insecure for data storage because of low trap depth and single-level storage channels. Therefore, the development of a novel non-volatile multilevel storage medium for data encryption remains a challenge. Herein, a robust, non-volatile, multilevel optical storage medium is reported, based on a photomodulated Ba3MgSi2O8:Eu3+, which combined the merits of light-induced valence (Eu3+ → Eu2+) and photochromic phenomena using optical stimulation effects, accompanied by larger luminescent and color contrasts (>90%). These two unique features provided dual-level storage channels in a single host, significantly improving the data storage security. Notably, dual-level optical signals could be written and erased simultaneously by alternating 265 and 365 nm light stimuli. Theoretical calculations indicated that robust color centers induced by intrinsic interstitial Mg and vacancy defects with suitable trap depths enable excellent reversibility and long-term storage capability. By relying on different luminescent readout mechanisms, the encrypted dual-level information can be accurately decrypted by separately probing the Eu2+ and Eu3+ signals, thus ensuring information security. This study proposes a novel approach for constructing multilevel information storage channels for information security.

Hybrid Density Functional Study on the p-Type Conductivity Mechanism in Intrinsic Point Defects and Group V Element-Doped 2D β-TeO2.

The newly discovered two-dimensional (2D) β-TeO2 possesses extraordinarily high p-type carrier mobility and demonstrates immense potential in the electronics field. However, current research on its p-type conductivity mechanisms and the modifications of element doping remains relatively insufficient. In this study, the intrinsic point defects and extrinsic element doping in monolayer β-TeO2 are comprehensively analyzed to probe the potential sources of the intrinsic p-type conductivity and the extrinsic p-type doping possibility in 2D β-TeO2 through hybrid density functional calculations. Our results reveal that the vacancy defects with low formation energies have deep transition levels and thus cannot be used as sources of unintentional p-type conductivity in 2D β-TeO2. The investigations and discussions via Group V element doping modifications in 2D β-TeO2 indicate that bismuth (Bi) doping can easily and significantly enhance the p-type conductivity of 2D β-TeO2 under the presence of O-rich, which can be achieved experimentally. Furthermore, Bi doping can significantly increase carrier mobility without seriously affecting the electronic structure. The finding shows that the Bi element is an ideal dopant candidate for a p-type modification in 2D β-TeO2. Our calculations pave an alternative strategy to achieve the realization of superior p-type conductivity in 2D β-TeO2.

Engineering Dual Carbon and Nitrogen Vacancies in g-C3N4 for Enhanced Photodegradation of Tetracycline Hydrochloride.

Ultrathin g-C3N4 nanosheets with specific nitrogen vacancies and combined carbon and nitrogen dual vacancies were created by annealing g-C3N4 under different atmospheric conditions. The nanosheets with dual vacancies showed significant improvements in the photodegradation of tetracycline hydrochloride (TC-HCl) compared with both the pristine g-C3N4 and its nitrogen-deficient version. Various techniques, such as Raman spectroscopy, electron spin resonance (ESR), X-ray photoelectron spectroscopy, wavelength-dependent studies, electrochemical methods, and photoluminescence measurements, were used to identify vacancy defects, revealing that performance enhancement was particularly notable under visible light. Density functional theory calculations indicated that dual vacancies introduced a shallow defect state above the valence band, enhancing visible light absorption and reducing electron-hole pair recombination. Conversely, nitrogen vacancies alone formed a deep defect state, which extended light absorption but potentially trapped photoelectrons, limiting their contribution to photoreactions. Radical-scavenging experiments and ESR spin-trap spectra identified the superoxide radical (·O2-) as the primary reactive oxygen species responsible for TC-HCl degradation. A comprehensive degradation pathway for TC-HCl was proposed using liquid chromatography-mass spectrometry data. This research highlights a strategic approach to boost TC-HCl photodegradation by engineering the vacancies in g-C3N4.

Synergistic Tuning of Heterovalent States and Oxygen-Vacancy Defect Engineering in Hydrophilic W-Doped Sb2OS2 for Enhanced Nitrogen Photoreduction to Ammonia.

Nitrogen fixation reaction via photocatalysis offers a green and promising strategy for renewable NH3 synthesis, and catalysts with high-efficiency photocatalytic properties are essential to the process. Herein, we demonstrate a W-doped Sb2OS2 bimetal oxysulfide catalyst (labeled as SbWOS) with abundant oxygen vacancies, heterovalent metal states, and hydrophilic surfaces for nitrogen photoreduction to ammonia. The SbWOS-3 with suitable W-doping exhibited excellent nitrogen fixation activity of 408.08 μmol·g-1·h-1 and an apparent quantum efficiency (AQE) of 1.88% at 420 nm and a solar-to-ammonia (STA) conversion efficiency of 0.082% in pure water under AM1.5G light irradiation. The W-doping not only transforms hydrophobic Sb2OS2 into a hydrophilic catalyst, making it easier for H2O molecules adsorbed on the SbWOS surface and catalyzed into protons, but also endows the SbWOS catalyst with rich oxygen vacancies, acting as the active sites for trapping and activating the N2 molecule, and for trapping and activating H2O to produce the protons for the N2 photocatalytic reduction reaction. The hydrazine drives the SbWOS catalyst with the heterovalent metal states, which acts as the photogenerate electrons quickly hopping between W5+ and W6+ to transfer for the N2 reduction reaction. This study provides a feasible scheme for applying oxygen vacancy defects, heterovalent metal states, and surface hydrophobic-to-hydrophilic wetting engineering in bimetal oxysulfide for N2 photoreduction to ammonia.

The breakthrough of oxide pathway mechanism in stability and scaling relationship for water oxidation

Abstract An in-depth understanding of electrocatalytic mechanisms is essential for advancing electrocatalysts for the oxygen evolution reaction (OER). The emerging oxide pathway mechanism (OPM) streamlines direct O–O radical coupling, circumventing the formation of oxygen vacancy defects characteristic of the lattice oxygen mechanism (LOM) and bypassing additional reaction intermediates (*OOH) inherent to the adsorbate evolution mechanism (AEM). With only *O and *OH as intermediates, OPM-driven electrocatalysts stand out for their ability to disrupt traditional scaling relationships while ensuring stability. This review compiles the latest significant advances in OPM-based electrocatalysis, detailing design principles, synthetic methods, and sophisticated techniques to identify active sites and pathways. We conclude with prospective challenges and opportunities for OPM-driven electrocatalysts, aiming to advance the field into a new era by overcoming traditional constraints.

Strained van der Waals Metallic Magnet for Photomagnetic Modulation and Spin Photodiode Application

AbstractAll‐optical magnetization reversal provides a low‐power approach for investigating spin state manipulation in 2D magnets. However, the ambient observation of photomagnetic coupling presents significant challenges due to the low Curie temperatures exhibited by most 2D magnets. Herein, a mixed‐dimensional heterostructure comprising a surface‐oxidized Fe3GeTe2 nanosheet with enhanced magnetic properties and individual semiconducting ZnO nanorod is proposed to explore proximity photomagnetic modulation and spin‐enhanced photodetection behaviors. The surface curvature of ZnO nanorod induces pronounced strains for Fe3GeTe2 nanosheet, leading to its anomalous Raman polarization and spin ordering at room temperature. Strain‐activated itinerant spin electrons are immobilized on the O‐2p orbitals of adjacent ZnO, thereby facilitating the optical demagnetization process in Fe3GeTe2 without aid of magnetic field. First‐principles calculations together with in situ characterization experiments further confirm that the primary charge transfer channel involves coupling between Fe3+ and oxygen vacancy defects anchored at heterointerfaces. The rapid establishment of magnetization by illumination in ZnO nanorod contributes to spin‐tunneling‐enhanced photocurrent, device response dynamics, polarization detection and ultraviolet imaging capability. These findings offer valuable insights to optimize the optoelectronic properties of conventional semiconductors and advance complex dimensional spin‐optoelectronic devices.