An Impressive Open-Circuit Voltage of 1.223 V and High Humidity Stability of Perovskite Solar Cells with MgO Buffer Layer Deposited by Low-Temperature Atomic Layer Deposition.

The performance of perovskite solar cells has been continuously improving. However, humidity stability has become a key problem that hinders its promotion in the process of commercialization. A buffer layer deposited by atomic layer deposition is a very helpful method to solve this problem. In this work, MgO film is deposited between Spiro-OMeTAD and electrode by low-temperature atomic layer deposition at 80 °C, which resists the erosion of water vapor, inhibits the migration of electrode metal ions and the decomposition products of perovskite, then finally improves the stability of the device. At the same time, the MgO buffer layer can passivate the defects of porous Spiro, thus enhancing carrier transport efficiency and device performance. The Cs0.05(FAPbI3)0.85(MAPbBr3)0.15 perovskite device with a MgO buffer layer has displayed PCE of 22.74%, also with a high Voc of 1.223 V which is an excellent performance in devices with same perovskite component. Moreover, the device with a MgO buffer layer can maintain 80% of the initial efficiency after 7200 h of storage at 35% relative humidity under room temperature. This is a major achievement for humidity stability in the world, providing more ideas for further improving the stability of perovskite devices.

Strong doping reduction on wafer-scale CVD graphene devices via Al2O3 ALD encapsulation.

We present the electrical characterization of wafer-scale graphene devices fabricated with an industrially-relevant, contact-first integration scheme combined with Al2O3 encapsulation via atomic layer deposition. All the devices show a statistically significant reduction in the Dirac point position, Vcnp, from around + 47V to between -5 and 5 V (on 285 nm SiO2), while maintaining the mobility values. The data and methods presented are relevant for further integration of graphene devices, specifically sensors, at the back-end-of-line of a standard CMOS flow.

Unraveling the Role of the Stoichiometry of Atomic Layer Deposited Nickel Cobalt Oxides on the Oxygen Evolution Reaction.

Nickel cobalt oxides (NCOs) are promising, non-precious oxygen evolution reaction (OER) electrocatalysts. However, the stoichiometry-dependent electrochemical behavior makes it crucial to understand the structure-OER relationship. In this work, NCO thin film model systems are prepared using atomic layer deposition. In-depth film characterization shows the phase transition from Ni-rich rock-salt films to Co-rich spinel films. Electrochemical analysis in 1 m KOH reveals a synergistic effect between Co and Ni with optimal performance for the 30 at.% Co film after 500 CV cycles. Electrochemical activation correlates with film composition, specifically increasing activation is observed for more Ni-rich films as its bulk transitions to the active (oxy)hydroxide phase. In parallel to this transition, the electrochemical surface area (ECSA) increases up to a factor 8. Using an original approach, the changes in ECSA are decoupled from intrinsic OER activity, leading to the conclusion that 70 at.% Co spinel phase NCO films are intrinsically the most active. The studies point to a chemical composition dependent OER mechanism: Co-rich spinel films show instantly high activities, while the more sustainable Ni-rich rock-salt films require extended activation to increase the ECSA and OER performance. The results highlight the added value of working with model systems to disclose structure-performance mechanisms.

Atomic Layer Growth of Rutile TiO2 Films with Ultrahigh Dielectric Constants via Crystal Orientation Engineering.

In general, the electronic and optical properties of oxide films can significantly benefit from highly textured crystallinity. However, oxide films grown by atomic layer deposition (ALD), a powerful technique for the synthesis of high-quality, nanoscale thin films, usually exhibit amorphous or randomly oriented polycrystalline phases. Here, we demonstrate the growth of highly textured rutile phase ALD TiO2 films through rational substrate design. Both a- and c-axis preferentially oriented TiO2 films are obtained by varying the lattice parameters of the initial ALD growth surface. Under optimized conditions, we find that it is possible to deposit high-quality, c-axis preferentially aligned TiO2 films with a bulk dielectric constant approaching 185, rivaling the single crystal limit. These films display a remarkably high dielectric constant of 117 despite thin thickness of 5.2 nm. Moreover, the addition of a single doping sequence of Al2O3 successfully suppresses leakage currents to levels compatible with modern dynamic random access memory cells, all the while maintaining the high bulk dielectric constant of 137. These results clearly highlight the prospect of utilizing crystal orientation engineering in ALD thin films for emerging semiconductor devices.

Enhanced Deposition Selectivity of High-k Dielectrics by Vapor Dosing and Selective Removal of Phosphonic Acid Inhibitors.

Area-selective atomic layer deposition (AS-ALD), which provides a bottom-up nanofabrication method with atomic-scale precision, has attracted a great deal of attention as a means to alleviate the problems associated with conventional top-down patterning. In this study, we report a methodology for achieving selective deposition of high-k dielectrics by surface modification through vapor-phase functionalization of octadecylphosphonic acid (ODPA) inhibitor molecules accompanied by post-surface treatment. A comparative evaluation of deposition selectivity of ZrO2 thin films deposited with the O2 and O3 reactants was performed on SiO2, TiN, and W substrates, and we confirmed that high enough deposition selectivity over 10 nm can be achieved even after 200 cycles of ALD with the O2 reactant. Subsequently, the electrical properties of ZrO2 films deposited with O2 and O3 reactants were investigated with and without post-deposition treatment. We successfully demonstrated that high-quality ZrO2 thin films with high dielectric constants and stable antiferroelectric properties can be produced by subjecting the films to ozone, which can eliminate carbon impurities within the films. We believe that this work provides a new strategy to achieve highly selective deposition for AS-ALD of dielectric on dielectric (DoD) applications toward upcoming bottom-up nanofabrication.

Lead-rivet strategy of growing perovskite nanocrystals for excellent toxicity inhibition and spinning application.

Lead halide perovskite has demonstrated remarkable potential in the wearable field due to its exceptional photoelectric conversion capability. However, its lead toxicity issue has consistently been subject to criticism, significantly impeding its practical application. To address this challenge, an innovative approach called lead-rivet was proposed for the in-situ growth of perovskite crystalline structures. Through the formation of S-Pb bonds, each Pb2+ ion was firmly immobilized on the surface of the silica matrix, enabling in situ growth of perovskite nanocrystals via ion coordination between Cs+ and halide species. The robust S-Pb bonding effectively restricted the mobility of lead ions and stabilized the perovskite structure without relying on surface ligands, thereby not only preventing toxicity leakage but also providing a favorable interface for depositing protective shells. The obtained perovskites exhibit intense and narrow-band fluorescence with full-width at half-maximum less than 23 nm and show excellent stability to high temperature (above 202 °C) and high humidity (water immersion over 27 days), thus making it possible to be used in varies textile technologies including melt spinning and wet spinning. The lead leakage rate of particles is only 4.15 % demonstrating excellent toxicity inhibition performance. The prepared fibers maintained good extensibility and flexibility which could be used for 3D-printing and textiles weaving. Most importantly, the detected Pb2+ leaching was negligible as low as to 0.732 ppb which meet the standard of World Health Organization (WHO) for drinking water (<10 ppb), and the cell survival rate remained 99.196 % for PLA fluorescent filament after 24 h cultivation which showing excellent safety to human body and environment. This study establishes a controllable and highly adaptable synthesis method, thereby providing a promising avenue for the safe utilization of perovskite materials.

Wide process temperature of atomic layer deposition for In2O3thin-film transistors using novel indium precursor (N,N'-di-tert butylacetimidamido)dimethyllindium.

This study introduces a novel heteroleptic indium complex, which incorporates an amidinate ligand, serving as a high-temperature atomic layer deposition (ALD) precursor. The most stable structure was determined using density functional theory and synthesized, demonstrating thermal stability up to 375 °C. We fabricated indium oxide thin-film transistors (In2O3TFTs) prepared with DBADMI precursor using ALD in wide range of window processing temperature of 200 °C, 300 °C, and 350 °C with an ozone (O3) as the source. The growth per cycle of ALD ranged from 0.06 to 0.1 nm cycle-1at different deposition temperatures. X-ray diffraction and transmission electron microscopy were employed to analyze the crystalline structure as it relates to the deposition temperature. At a relatively low deposition temperature of 200 °C, an amorphous morphology was observed, while at 300 °C and 350 °C, crystalline structures were evident. Additionally, x-ray photoelectron spectroscopy analysis was conducted to identify the In-O and OH-related products in the film. The OH-related product was found to be as low as 1% with an increase the deposition temperature. Furthermore, we evaluated In2O3TFTs and observed an increase in field-effect mobility, with minimal change in the threshold voltage (Vth), at 200 °C, 300 °C, and 350 °C. Consequently, the DBADMI precursor, given its stability at highdeposition temperatures, is ideal for producing high-quality films and stable crystalline phases, with wide processing temperature range makeing it suitable for various applications.

High-Performance TiO2/ZrO2/TiO2 Thin Film Capacitor by Plasma-Assisted Atomic Layer Annealing.

Although laminate structures are widely used in electrostatic capacitors, unavoidable heterogeneous interfaces often deteriorate the dielectric properties by impeding film crystallization. In this study, a TiO2/ZrO2/TiO2 (TZT) laminate structure, where upper-TiO2 deposited on the heterogeneous interface was crystallized by plasma-assisted atomic layer annealing (ALA), was investigated. ALA effectively induced the phase transition of the upper-TiO2 from the amorphous or anatase phase to the rutile phase, leading to an increase in the dielectric constant, whereas the ZrO2 blocking interlayer maintained the amorphous phase owing to the extremely localized effect of ALA. Consequently, through the layer-by-layer phase control of ALA, the dielectric constant of the upper-TiO2 was enhanced by 25% by applying ALA, leading to an increase in a capacitance density of 27% of the TZT capacitor, whereas a low leakage current density of ∼10-8 A/cm2 was maintained (at 1 V). In addition, the TZT capacitor on three-dimensional structures (aspect ratio of 5:1) shows a high capacitance density of up to 461 nF/mm2 owing to ALA.

Rational Design of Fe Single Sites Supported on Hierarchical Zeolites via Atomic Layer Deposition for Few-Walled Carbon Nanotube Production.

Metal single-site catalysts have recently played an essential role in catalysis due to their enhanced activity, selectivity, and precise reaction control compared to those of conventional metal cluster catalysts. However, the rational design and catalytic application of metal single-site catalysts are still in the early stages of development. In this contribution, we report the rational design of Fe single sites incorporated in a hierarchical ZSM-5 via atomic layer deposition (ALD). The designer catalysts demonstrated highly dispersed Fe species, predominantly stabilized by oxygen atoms in the zeolite framework at terminal, isolated, and vicinal silanol groups within the micropores and external surfaces of the zeolite. The successful incorporation of highly thermally stable and uniform Fe single sites into hierarchical zeolite through ALD represents a significant advancement in few-walled carbon nanotube production. The inner and outer diameters of produced CNTs are approximately 4.4 ± 2.4 and 8.6 ± 1.8 nm, respectively, notably smaller than those produced via traditional impregnated catalysts. This example emphasizes the concept of rational design of a single Fe site dispersed on a hierarchical ZSM-5 surface, which is anticipated to be a promising catalyst for advancing catalytic applications.

Thiol-Functionalized Adsorbents through Atomic Layer Deposition and Vapor-Phase Silanization for Heavy Metal Ion Removal.

The removal of toxic heavy metal ions from water resources is crucial for environmental protection and public health. In this study, we address this challenge by developing a surface functionalization technique for the selective adsorption of these contaminants. Our approach involves atomic layer deposition (ALD) followed by vapor-phase silanization of porous substrates. We utilized porous silica gel powder (∼100 µm particles, 89 m2/g surface area, ∼30 nm pores) as an initial substrate. This powder was first coated with ∼0.5 nm ALD Al2O3, followed by vapor-phase grafting of a thiol-functional silane. The modified powder, particularly in acidic conditions (pH = 4), showed high selectivity in adsorbing Cd(II), As(V), Pb(II), Hg(II), and Cu(II) heavy metal ions in mixed ion solutions over common benign ions (e.g., Na, K, Ca, and Mg). Langmuir adsorption isotherms and breakthrough adsorption studies were conducted to assess heavy metal binding affinity and revealed the order of Cd(II) < Pb(II) < Cu(II) < As(V) < Hg(II), with a significantly higher affinity for As(V) and Hg(II) ions. Time-dependent uptake studies demonstrated rapid removal of heavy metal ions from aqueous environments, with Hg(II) exhibiting the fastest adsorption kinetics on thiol-modified surfaces. These findings highlight the potential of ALD and vapor-phase silanization to create effective adsorbents for the targeted removal of hazardous contaminants from water.

Ultrahigh Sensitivity for Thermographic Human-Machine Interface via Precious Metals Atomic Layer Deposition on V-MXene: Computational and Experimental Exploration.

Global healthcare based on the Internet of Things system is rapidly transforming to measure precise physiological body parameters without visiting hospitals at remote patients and associated symptoms monitoring. 2D materials and the prevailing mood of current ever-expanding MXene-based sensing devices motivate to introduce first the novel iridium (Ir) precious metal incorporated vanadium (V)-MXene via industrially favored emerging atomic layer deposition (ALD) techniques. The current work contributes a precise control and delicate balance of Ir single atomic forms or clusters on the V-MXene to constitute a unique precious metal-MXene embedded heterostructure (Ir-ALD@V-MXene) in practical real-time sensing healthcare applications to thermography with human-machine interface for the first time. Ir-ALD@V-MXene delivers an ultrahigh durability and sensing performance of 2.4% °C-1 than pristine V-MXene (0.42% °C-1), outperforming several conventionally used MXenes, graphene, underscoring the importance of the Ir-ALD innovative process. Aberration-corrected advanced ultra-high-resolution transmission/scanning transmission electron microscopy confirms the presence of Ir atomic clusters on well-aligned 2D-layered V-MXene structure and their advanced heterostructure formation (Ir-ALD@V-MXene), enhanced sensing mechanism is investigated using density functional theory (DFT) computations. A rational design empowering the Ir-ALD process on least explored V-MXene can potentially unfold further precious metals ALD-process developments for next-generation wearable personal healthcare devices.

The surface chemistry of the atomic layer deposition of metal thin films.

In this perspective we discuss the progress made in the mechanistic studies of the surface chemistry associated with the atomic layer deposition (ALD) of metal films and the usefulness of that knowledge for the optimization of existing film growth processes and for the design of new ones. Our focus is on the deposition of late transition metals. We start by introducing some of the main surface-sensitive techniques and approaches used in this research. We comment on the general nature of the metallorganic complexes used as precursors for these depositions, and the uniqueness that solid surfaces and the absence of liquid solvents bring to the ALD chemistry and differentiate it from what is known from metalorganic chemistry in solution. We then delve into the adsorption and thermal chemistry of those precursors, highlighting the complex and stepwise nature of the decomposition of the organic ligands that usually ensued upon their thermal activation. We discuss the criteria relevant for the selection of co-reactants to be used on the second half of the ALD cycle, with emphasis on the redox chemistry often associated with the growth of metallic films starting from complexes with metal cations. Additional considerations include the nature of the substrate and the final structural and chemical properties of the growing films, which we indicate rarely retain the homogeneous 2D structure often aimed for. We end with some general conclusions and personal thoughts about the future of this field.

Comparative Study of Plasma-Enhanced-Atomic-Layer-Deposited Al2O3/HfO2/SiO2 and HfO2/Al2O3/SiO2 Trilayers for Ultraviolet Laser Applications.

High-performance thin films combining large optical bandgap Al2O3 and high refractive index HfO2 are excellent components for constructing the next generation of laser systems with enhanced output power. However, the growth of low-defect plasma-enhanced-atomic-layer-deposited (PEALD) Al2O3 for high-power laser applications and its combination with HfO2 and SiO2 materials commonly used in high-power laser thin films still face challenges, such as how to minimize defects, especially interface defects. In this work, substrate-layer interface defects in Al2O3 single-layer thin films, layer-layer interface defects in Al2O3-based bilayer and trilayer thin films, and their effects on the laser-induced damage threshold (LIDT) were investigated via capacitance-voltage (C-V) measurements. The experimental results show that by optimizing the deposition parameters, specifically the deposition temperature, precursor exposure time, and plasma oxygen exposure time, Al2O3 thin films with low defect density and high LIDT can be obtained. Two trilayer anti-reflection (AR) thin film structures, Al2O3/HfO2/SiO2 and HfO2/Al2O3/SiO2, were then prepared and compared. The trilayer AR thin film with Al2O3/HfO2/SiO2 structure exhibits a lower interface defect density, better interface bonding performance, and an increase in LIDT by approximately 2.8 times. We believe these results provide guidance for the control of interface defects and the design of thin film structures and will benefit many thin film optics for laser applications.

Tailoring Mechanical Reliability in Transparent ZnO-Zincone Thin-Film Electrodes with Organic Interlayer Interfaces and Thickness.

To address the inherent brittleness of conventional transparent conductive oxides, researchers have focused on enhancing their flexibility. This is achieved by incorporating organic films to construct organic-inorganic hybrid layer-by-layer nanostructures, where the interlayer thickness and interface play pivotal roles in determining the properties. These factors are contingent on the type of material, processing conditions, and specific application requirements, making it essential to select the appropriate conditions. In this study, ZnO-zincone nanolaminate thin films were fabricated using atomic layer deposition and molecular layer deposition in various structural configurations. Transmission electron microscopy, X-ray diffraction, and scanning electron microscopy were used to conduct a thorough analysis of the thin-film growth and structural transformations resulting from the deposition conditions. Furthermore, the influence of structural differences at the interfaces on the mechanical properties of the films was investigated by employing both tensile and compression-bending fatigue tests. This comprehensive examination reveals noteworthy variations in the mechanical responses of the films. Thin films characterized by internal porosity and an intermixed amorphous structure demonstrated enhanced compressive toughness, whereas rigid organic layers improved flexibility. These findings offer valuable insights into the development of flexible, transparent multilayer films.

Controlled NiOx Defect Engineering to Harnessing Redox Reactions in Perovskite Photovoltaic Cells via Atomic Layer Deposition.

Albeit the undesirable attributes of NiOx, such as low conductivity, unmanageable defects, and redox reactions occurring at the perovskite/NiOx interface, which impede the progress in inverted perovskite solar cells (i-PSCs), it is the most favorable choice of technology for industrialization of PSCs. In this study, we propose a novel Ni vacancy defect modulate approach to leverage the conformal growth and surface self-limiting reaction characteristics of the atomic layer deposition (ALD)-fabricated NiOx by varying the O2 plasma injection time (tOE) to induce self-doping. Consequently, NiOx thin films with enhanced conductivity, an appropriate Ni3+/Ni2+ ratio, stable surface states, and ultrathinness are realized as hole-transporting layers (HTLs) in p-i-n PSCs. As a result of these improvements, ALD-NiOx-based devices exhibit the highest power conversion efficiency (PCE) of 19.86% and a fill factor (FF) of 81.86%. Notably, the optimal interfacial defects effectively suppressed the severe reaction between the perovskite and NiOx. This suppression is evidenced by the lowest decay rate observed in a harsh environment, lasting for 500 consecutive hours. The proposed approach introduces the possibility of a hierarchical distribution of defects and offers feasibility for the fabrication of large-area, uniform, and high-quality films.

Regulation of Interface Ion Transport by Electron Ionic Conductor Construction toward High-Voltage and High-Rate LiNi0.5Co0.2Mn0.3O2 Cathodes in Lithium Ion Battery.

Simultaneously achieving high-energy-density and high-power-density is a crucial yet challenging objective in the pursuit of commercialized power batteries. In this study, atomic layer deposition (ALD) is employed combined with a coordinated thermal treatment strategy to construct a densely packed, electron-ion dual conductor (EIC) protective coating on the surface of commercial LiNi0.5Co0.2Mn0.3O2 (NCM523) cathode material, further enhanced by gradient Al doping (Al@EIC-NCM523). The ultra-thin EIC effectively suppresses side reactions, thereby enhancing the stability of the cathode-electrolyte interphase (CEI) at high-voltages. The EIC's dual conduction capability provides a potent driving force for Li+ transport at the interface, promoting the formation of rapid ion deintercalation pathways within the Al@EIC-NCM523 bulk phase. Moreover, the strategic gradient doping of Al serves to anchor the atomic spacing of Ni and O within the structure of Al@EIC-NCM523, curbing irreversible phase transitions at high-voltages and preserving the integrity of its layered structure. Remarkably, Al@EIC-NCM523 displays an unprecedented rate capability (114.7 mAh g-1 at 20 C), and a sustained cycling performance (capacity retention of 74.72% after 800 cycles at 10 C) at 4.6 V. These findings demonstrate that the proposed EIC and doping strategy holds a significant promise for developing high-energy-density and high-power-density lithium-ion batteries (LIBs).

Interface-Engineered Atomic Layer Deposition of 3D Li4Ti5O12 for High-Capacity Lithium-Ion 3D Thin-Film Batteries.

Upcoming energy-autonomous mm-scale Internet-of-things devices require high-energy and high-power microbatteries. On-chip 3D thin-film batteries (TFBs) are the most promising option but lack high-rate anode materials. Here, Li4Ti5O12 thin films fabricated by atomic layer deposition (ALD) are electrochemically evaluated on 3D substrates for the first time. The 3D Li4Ti5O12 reveals an excellent footprint capacity of 20.23 µAh cm-2 at 1 C. The outstanding high-rate capability is demonstrated with 7.75 µAh cm-2 at 5 mA cm-2 (250 C) while preserving a remarkable capacity retention of 97.4% after 500 cycles. Planar films with various thicknesses exhibit electrochemical nanoscale effects and are tuned to maximize performance. The developed ALD process enables conformal high-quality spinel (111)-textured Li4Ti5O12 films on Si substrates with an area enhancement of 9. Interface engineering by employing ultrathin AlOx on the current collector facilitates a required crystallization time reduction which ensures high film and interface quality and prospective on-chip integration. This work demonstrates that 3D Li4Ti5O12 by ALD can be an attractive solution for the microelectronics-compatible fabrication of scalable high-energy and high-power Li-ion 3D TFBs.

Atomic Layer Deposition of Zirconia on Titanium Implants Improves Osseointegration in Rabbit Bones.

Purpose: Atomic layer deposition (ALD) is a method that can deposit zirconia uniformly on an atomic basis. The effect of deposited zirconia on titanium implants using ALD was evaluated in vivo. Methods: Machined titanium implants (MTIs) were used as the Control. MTIs treated by sandblasting with large grit and acid etching (SA) and MTIs deposited with zirconia using ALD are referred to as Groups S and Z, respectively. Twelve implants were prepared for each group. Six rabbits were used as experimental animals. To evaluate the osteogenesis and osteocyte aspects around the implants, radiological and histological analyses were performed. The bone-to-implant contact (BIC) ratio was measured and statistically analyzed to evaluate the osseointegration capabilities. Results: In the micro-CT analysis, more radiopaque bone tissues were observed around the implants in Groups S and Z. Histological observation found that Groups S and Z had more and denser mature bone tissues around the implants in the cortical bone area. Many new and mature bone tissues were also observed in the medullary cavity area. For the BIC ratio, Groups S and Z were significantly higher than the Control in the cortical bone area (P < 0.017), but there was no significant difference between Groups S and Z. Conclusion: MTIs deposited with zirconia using ALD (Group Z) radiologically and histologically showed more mature bone formation and activated osteocytes compared with MTIs (Control). Group Z also had a significantly higher BIC ratio than the Control. Within the limitations of this study, depositing zirconia on the surface of MTIs using ALD can improve osseointegration in vivo.

Ultrasensitive Monolithic Dopamine Microsensors Employing Vertically Aligned Carbon Nanofibers.

Brain-on-Chip devices, which facilitate on-chip cultures of neurons to simulate brain functions, are receiving tremendous attention from both fundamental and clinical research. Consequently, microsensors are being developed to accomplish real-time monitoring of neurotransmitters, which are the benchmarks for neuron network operation. Among these, electrochemical sensors have emerged as promising candidates for detecting a critical neurotransmitter, dopamine. However, current state-of-the-art electrochemical dopamine sensors are suffering from issues like limited sensitivity and cumbersome fabrication. Here, a novel route in monolithically microfabricating vertically aligned carbon nanofiber electrochemical dopamine microsensors is reported with an anti-blistering slow cooling process. Thanks to the microfabrication process, microsensors is created with complete insulation and large surface areas. The champion device shows extremely high sensitivity of 4.52× 104 µAµM-1·cm-2, which is two-orders-of-magnitude higher than current devices, and a highly competitive limit of detection of 0.243 nM. These remarkable figures-of-merit will open new windows for applications such as electrochemical recording from a single neuron.

Surface and grain boundary coating for stabilizing LiNi0.8Mn0.1Co0.1O2 based electrodes.

The widespread use of high-capacity Ni-rich layered oxides such as LiNi0.8Mn0.1Co0.1O2 (NMC811), in lithium-ion batteries is hindered due to practical capacity loss and reduced working voltage during operation. Aging leads to defective NMC811 particles, affecting electrochemical performance. Surface modification offers a promising approach to improve cycle life. Here, we introduce an amorphous lithium titanate (LTO) coating via atomic layer deposition (ALD), not only covering NMC811 surfaces but also penetrating cavities and grain boundaries. As NMC811 electrodes suffer from low structural stability during charge and discharge, We combined electrochemistry, operando X-ray diffraction (XRD), and dilatometry to understand structural changes and the coating protective effects. XRD reveals significant structural evolution during delithiation for uncoated NMC811. The highly reversible phase change in coated NMC811 highlights enhanced bulk structure stability. The LTO coating retards NMC811 degradation, boosting capacity retention from 86% to 93% after 140 cycles. This study underscores the importance of grain boundary engineering for Ni-rich layered oxide electrode stability and the interplay of chemical and mechanical factors in battery aging.