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When organic compounds are pre-oxidized before coagulation, the disinfection byproducts are usually generated in the following chlorination process in drinking water treatment. In this study, the effects of pre-oxidation on carbon removal and generation of disinfection byproducts were investigated by using common oxidants of ozone, permanganate and ferrate. It was demonstrated that turbidities were reduced by 35%, 37.5% and 38.3%, and dissolved organic carbon was reduced by 18.8%, 26.5% and 20.8%, respectively, with the pre-oxidation of ozone, permanganate and ferrate under optimal dosage but inorganic carbon was not affected. Turbidity, dissolved organic carbon and dissolved organic matter showed an initial decrease and then increase pattern with increase in ozone and permanganate concentrations, but a different continuously decreasing pattern was demonstrated by ferrate. The results indicated that pre-oxidation of organic compounds was incomplete and may include steps of colloid destabilization, cell lysis and partial mineralization. The removal rates of total disinfection byproducts under optimal concentrations were 31.69%, 45.36% and 39.35%, respectively. Eleven disinfection byproducts were identified and quantified, and the major species were chloroform, trichloroacetaldehyde and dichloroacetonitrile, which were either generated directly from organic compounds or converted from other species of disinfection byproducts. The highest LC50 of disinfection byproducts were dibromo- and bromochloro- acetonitriles, indicating the cytotoxicity was mostly contributed by the nitrogen-containing disinfection byproducts, which combined accounted for 79.6% to 83.4% of the total toxicity.

Silicon is considered as a blooming candidate material for next-generation lithium-ion batteries due to its low electrochemical potential and high theoretical capacity. However, its commercialization has been impeded by the poor cycling issue associated with severe volume changes (∼380%) upon (de)lithiation. Herein, an organic-inorganic hybrid film of titanicone via molecular layer deposition (MLD) is proposed as an artificial solid electrolyte interphase (SEI) layer for Si anodes. This rigid-soft titanicone coating with Young's modulus of 21 GPa can effectively relieve stress concentration during the lithiation process, guaranteeing the stability of the mechanical structure of a Si nanoparticles (NPs)@titanicone electrode. Benefiting from the long-strand (Ti-O-benzene-O-Ti-) unit design, the optimized Si NPs@70 cycle titanicone anode delivers a high Li+ diffusion coefficient and a low Li+ diffusion barrier, as revealed by galvanostatic intermittent titration (GITT) investigations and density functional theory (DFT) simulations, respectively. Ultimately, the Si NPs@70 cycle titanicone electrode shows high initial Coulombic efficiency (84%), long cycling stability (957 mAh g-1 after 450 cycles at 1 A g-1), a stable SEI layer, and good rate performances. The molecular-scale design of the titanicone-protected Si anodes may bring in new opportunities to realize the next-generation lithium-ion batteries as well as other rechargeable batteries.

In this work, a highly stretchable and sensitive strain sensor using silver nanowires (Ag NWs)/multi-walled carbon nanotubes (MWCNTs) on hair band is proposed. The fabrication process of such sensors enabled scalable and facile production with low cost by dipping hair band into Ag NWs/MWCNTs composites suspension. The sensing performance of the sensors was optimized by tuning the Ag NWs/MWCNTs mass ratio. The hair band based strain sensor with Ag NWs/MWCNTs mass ratio of 30 exhibited the best performance with high sensitivity of 416.0 and good stretchability up to 70%. Moreover, great repeatability and long-term stability could be achieved over 7500 cycles of stretch-release. This Ag NWs/MWCNTs-hair band sensor can be used for monitoring human motions and swallowing action.

In this work, zinc sulfide (ZnS) on hydroxylated multi-walled carbon nanotubes (MWCNTs) composite was prepared for lithium-ion batteries (LIBs) anode. It is demonstrated that atomic layer deposition (ALD) enables a conformal, uniform, and ultrathin ZnS (~ 7 nm) layer onto the surface of hydroxylated MWCNTs. The resulting MWCNTs@ZnS core–shell composite displays excellent electrochemical performances as LIBs anode, accounting for high capacity, stable cyclability, high rate capability, and exceptional coulombic efficiency. The MWCNTs@ZnS composite can exhibit a stable discharge capacity, sustaining 520 mAh g−1 versus 108 mAh g−1 for commercial ZnS powders after 200 cycles at 100 mA g−1. The improved electrochemical performances are attributed to the synergistic effect from MWCNTs and ALD ZnS film. MWCNTs have good conductivity and huge surface area while the ALD ZnS film has high Li storage capability. This study verifies that ALD is highly flexible in developing excellent electrodes of LIBs.

Metal nanogaps can confine electromagnetic field into extremely small volumes, exhibiting strong surface plasmon resonance effect. Therefore, metal nanogaps show great prospects in enhancing light–matter interaction. However, it is still challenging to fabricate large-scale (centimeter scale) nanogaps with precise control of gap size at nanoscale, limiting the practical applications of metal nanogaps. In this work, we proposed a facile and economic strategy to fabricate large-scale sub-10 nm Ag nanogaps by the combination of atomic layer deposition (ALD) and mechanical rolling. The plasmonic nanogaps can be formed in the compacted Ag film by the sacrificial Al2O3 deposited via ALD. The size of nanogaps are determined by the twice thickness of Al2O3 with nanometric control. Raman results show that SERS activity depends closely on the nanogap size, and 4 nm Ag nanogaps exhibit the best SERS activity. By combining with other porous metal substrates, various sub-10 nm metal nanogaps can be fabricated over large scale. Therefore, this strategy will have significant implications for the preparation of nanogaps and enhanced spectroscopy.

Gd and Si co-doped HfO2 gate dielectric thin films were prepared by atomic layer deposition (ALD), while Gd[N(SiMe3)2]3, Hf[NEtMe]4, and H2O are chosen to be precursors. The Gd and Si were successfully co-doped into HfO2 films using only one doping precursor Gd[N(SiMe3)2]3. The doping concentration can be facilely tuned by controlling ALD recipe. The atomic percentages of Si/(Si + Gd + Hf) and Gd/(Si + Gd + Hf) increase from 11.5 to 28.9% and from 6.8 to 28.4% when changing the ALD cycle ratio of GdxSiyO to HfO2 from 1:9 to 1:1. The band gap and band alignment were investigated by X-ray photoelectron spectroscopy. The results imply that the band gap of Gd/Si co-doped HfO2 films has a positive relation with doping concentration. Moreover, the valence band offset decreases with doping concentration first but then increases, while the change of conduction band offset is opposite. The (1:6)-HfxGdySizO films with 11.6 at.% Gd/(Gd + Hf) exhibit the maximum accumulation capacitance and dielectric constant, which are only slightly smaller than those of the HfO2 films. Compared to HfO2 films, the leakage current density of (1:6)-HfxGdySizO films is decreased by at least one order of magnitude. Therefore, Gd and Si co-doping can improve the electrical properties of HfO2 films.

The photoelectrochemical (PEC) water oxidation performance of α-Fe2O3 photoanodes is jointly restricted by their high charge recombination and sluggish water oxidation kinetics. Herein, through coupling Ag and CdS nanoparticles with an α-Fe2O3 nanorod film, a new kind of α-Fe2O3/Ag/CdS ternary heterojunction film was constructed and investigated as a photoanode for solar water oxidation. The resultant α-Fe2O3/Ag/CdS photoanode can take full advantages of the α-Fe2O3/CdS heterojunction and the properties of Ag nanoparticles. Specifically, the formation of the α-Fe2O3/CdS heterojunction improves the charge separation and transfer efficiency of the α-Fe2O3 photoanode through band potential differences. Meanwhile, the presence of Ag nanoparticles enlarges the absorption edge of α-Fe2O3/CdS and decreases the electron–hole recombination through their surface plasmon resonance (SPR) effect. In addition, the electrocatalytic properties of Ag nanoparticles could initiate the water oxidation on the α-Fe2O3/Ag/CdS photoanode jointly. As a result, a higher photocurrent density of 3.25 mA cm−2 at 1.23 V vs. RHE was achieved on the α-Fe2O3/Ag/CdS photoanode during water oxidation, which is 2.5 times higher relative to the photocurrent of the α-Fe2O3 photoanode. Furthermore, the onset potential of water oxidation on the α-Fe2O3/Ag/CdS photoanode was negatively shifted about 220 mV relative to the α-Fe2O3 photoanode due to its faster kinetics. With the protection of the amorphous TiO2 layer, the water oxidation activity of the α-Fe2O3/Ag/CdS photoanode can be steadily maintained even after 10 h of reaction at 1.23 V vs. RHE. The present work provides an efficient strategy for the development of α-Fe2O3-based ternary heterojunction photoanodes for solar water oxidation.

Lithium-ion batteries with conversion-type anode electrodes have attracted increasing interest in providing higher energy storage density than those with commercial intercalation-type electrodes. However, conversion-type materials exhibit severe structural instability and capacity fade during cycling. In this work, a molecular layer deposition (MLD)-derived conductive Al2O3/carbon layer was employed to stabilize the structure of the cactus-like NiCo2O4 nanocrystal (NC) anode. The conductive Al2O3/carbon network and cactus-like NiCo2O4 NCs are beneficial for fast Li+/e− transport. Moreover, the Al2O3/carbon buffer-layer can prevent the NiCo2O4 NCs from agglomeration and form a steady solid electrolyte interphase (SEI), thus hampering the penetration of the electrolyte. Owing to these advantages, the assembled NiCo2O4@Al2O3/carbon half battery shows a high reversible capacity (931.2 mA h g−1 at 2 A g−1) and long-term stability of 290 mA h g−1 at 5 A g−1 over 500 cycles. Quantitative analyses further reveal the fast kinetics and the capacitance-battery dual model mechanism in the 3D core–shell structures. The design and introduction of MLD-derived hybrid coating may open a new way to conversion-type and alloy-type anode materials beyond NiCo2O4 to achieve high cyclability.

In this work, commercial anatase TiO2 powders were modified using ultrathin Fe2O3 layer by atomic layer deposition (ALD). The ultrathin Fe2O3 coating having small bandgap of 2.20 eV can increase the visible light absorption of TiO2 supports, at the meantime, Fe2O3/TiO2 heterojunction can effectively improve the lifetime of photogenerated electron–hole pairs. Results of ALD Fe2O3 modified TiO2 catalyst, therefore, showed great visible light driven catalytic degradation of methyl orange compared to pristine TiO2. A 400 cycles of ALD Fe2O3 (~ 2.6 nm) coated TiO2 powders exhibit the highest degradation efficiency of 97.4% in 90 min, much higher than pristine TiO2 powders of only 12.5%. Moreover, an ultrathin ALD Al2O3 (~ 2 nm) was able to improve the stability of Fe2O3-TiO2 catalyst. These results demonstrate that ALD surface modification with ultrathin coating is an extremely powerful route for the applications in constructing efficient and stable photocatalysts.

HfOx-based resistive random-access memory devices have shown great potential in next-generation non-volatile memory devices, but they are not optimized as synaptic devices for neuromorphic systems. In this paper, the fabrication and biological synaptic behavior of HfO2/HfOx bilayered ultrathin memory devices is studied. 4 nm non-stoichiometric HfOx films were prepared on the TiN-coated Si substrate by plasma-enhanced atomic layer deposition (PEALD) using Hf[N(C2H5)CH3]4 (TEMAH) and hydrogen plasma. 2 nm stoichiometric HfO2 films were then deposited by thermal atomic layer deposition (TALD) using TEMAH and H2O precursors. X-ray photoelectron spectroscopy and electron energy loss spectroscopy were used to analyze the oxygen vacancy concentrations in HfO2/HfOx bilayer films. The effect of oxygen vacancy concentration in non-stoichiometric HfOx layers on resistive switching characteristics of Pt/HfO2/HfOx/TiN bilayered memristive devices has been explored. The memristor with 12.1% oxygen vacancy content in the HfOx layer shows better comprehensive properties with the optimal pulse energy consumption, reset switching speed and DC endurance and retention properties. Each operation is evaluated in a range of approximately ten-picojoules. Some important biological synaptic functions such as nonlinear transmission characteristics, short-term and long-term plasticity, paired-pulse facilitation, spike-timing-dependent plasticity and conditioned reflex have also been demonstrated in optimized memristive devices. This HfO2/HfOx ultrathin memristor is used for an attractive large-scale hardware implementation of neuromorphic simulations.

To address the issues of large volume expansion and low electrical conductivity of ZnO anode nanomaterials during lithium ion battery operation, herein we engineered a rod-like ZnO anode with robust and conductive TiO2 quantum dot (QD)@carbon coating derived from molecular layer deposited titanicone, in which the TiO2 QDs are well confined inside the carbon layer. Transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) confirm the formation of TiO2 QDs and carbonization of fumaric acid in hybrid films after annealing in H2 atmosphere at 700 °C. Benefiting from a unique protective layer design, the prepared TiO2 QD@carbon@ZnO nanorod (NR) anodes display outstanding cycling performance with a discharge capacity of 1154 mA h g−1 after 100 cycles and 70% capacity retention, along with a high rate capacity of 470 mA h g−1 for 500 cycles at 2 A g−1. Moreover, our work demonstrates an innovative and promising approach toward a robust and conductive metal oxide QD@carbon nanocomposite layer for electrode materials in the future.

In this letter, biologic synaptic functions of organic-inorganic hybrid memristors using novel Ti-based maleic acid (Ti-MA)/TiO2 ultrathin films have been demonstrated. The memristive functional layer consists of 4-nm Ti-MA and 4-nm TiO2, which was fabricated at 160° C by molecular layer deposition (MLD)/atomic layer deposition (ALD), respectively. A typical bipolar resistive switching characteristic has been confirmed in the TaN/Ti-MA/TiO2/Pt bilayer memristors with the space charge limited current model. Using different electrical pulse modules, several important biologic synaptic functions such as nonlinear transmission characteristics, short-/long-term plasticity, paired-pulse facilitation, and spike-timing-dependent plasticity have been achieved. The organic-inorganic hybrid memristors of ultrathin bilayer Ti-MA/TiO2 derived by low temperature MLD/ALD are attractive for neuromorphic simulation and flexible neuroscience applications.

To solve the poor cyclability of faradic supercapacitors (SCs), the authors reported a unique porous carbon (PC) coating with “gap shell” structure on carbon fiber cloth (CFC)/NiS2 materials. This gap shell PC coating was fabricated by combining atomic layer deposition (ALD) Al2O3 and molecular layer deposition alucone, followed by carbonization and etching. The as-prepared CFC/NiS2/PC composites were directly used as binder-free electrodes for SCs. Benefited from its novel nanostructure, the CFC/NiS2/PC electrode shows a large specific capacitance of 1034.6 F/g at 1 A/g and considerable rate capability of 67% capacitance, retaining ratio within 1–20 A/g. The cyclability of the CFC/NiS2/PC electrode is enhanced by 50% relative to the mere CFC/NiS2 after 2000 cycles, which is attributed to the gap and electrically conductive PC coating. Hence, this work provides a promising approach to design gap shell layer for improved cyclability of faradic SCs and other practical applications in energy storage electronics.

A dense Al2O3 interlayer was inserted into TiN to enhance the tribological and anti-corrosion properties of TiN hard coating via a hybrid process of magnetron sputtering and atomic layer deposition (ALD). The influence of the ALD-Al2O3 layer on the microstructure, mechanical, tribological and anti-corrosion properties of TiN was examined. The TiN-Al2O3 coating exhibits low friction coefficient and specific wear rate, due to the structure change and columnar refinement caused by the addition of amorphous ALD-Al2O3 interlay which improves the mechanical properties of hard coating. The improved corrosion properties of TiN are attributed to the fact that the insulating ALD-Al2O3 used as a sealing layer can prevent the corrosive chlorine ions migrating into the lower TiN layer and block the charge transport in coatings. Moreover, raising the insertion position of ALD-Al2O3 layer away from the steel substrate results in a further increase in the anti-corrosion property of TiN-Al2O3 composite coating.

Combining wide-bandgap and narrow-bandgap perovskites to construct monolithic all-perovskite tandem solar cells offers avenues for continued increases in photovoltaic (PV) power conversion efficiencies (PCEs). However, actual efficiencies today are diminished by the subpar performance of narrow-bandgap subcells. Here we report a strategy to reduce Sn vacancies in mixed Pb–Sn narrow-bandgap perovskites that use metallic tin to reduce the Sn4+ (an oxidation product of Sn2+) to Sn2+ via a comproportionation reaction. We increase, thereby, the charge-carrier diffusion length in narrow-bandgap perovskites to 3 μm for the best materials. We obtain a PCE of 21.1% for 1.22-eV narrow-bandgap solar cells. We fabricate monolithic all-perovskite tandem cells with certified PCEs of 24.8% for small-area devices (0.049 cm2) and of 22.1% for large-area devices (1.05 cm2). The tandem cells retain 90% of their performance following 463 h of operation at the maximum power point under full 1-sun illumination. Improvements in the efficiency and stability of low-bandgap perovskite solar cells are key to enabling all-perovskite solar cells. Here, Lin et al. use metallic tin to prevent oxidation in such low-gap perovskite and demonstrate 24.8%-efficient tandems that are stable for over 400 h under operating conditions.

Uniform C-Al2O3 composite coating with homogeneous thickness was adopted to improve the electrochemical properties of LiNi0.6Co0.2Mn0.2O2 by the pyrolysis of molecular layer deposited alucone in argon. Compared with LiNi0.6Co0.2Mn0.2O2 coated atomic layer deposited Al2O3, C-Al2O3 coated electrode delivered high discharge capacity, good rate capability and durable cyclic stability, even at elevated temperature. Such enhanced electrochemical performance could be attributed to the synergistic effect between the amorphous Al2O3 and conductive carbon in the dual-functional C-Al2O3 composite coating, resulting in the improved structural stability and electrochemical kinetics of LiNi0.6Co0.2Mn0.2O2 cathode. The network of carbon in C-Al2O3 composite coating supplied high electrical conductivity, and lowers the charge transfer resistance on the surface of electrode. Meanwhile, the uniform amorphous Al2O3 with its flexible structure improved the structural stability of cathode and favored the diffusion of Li+ ions.

The wide applications of ultrathin group IV metal oxide films (TiO2, ZrO2 and HfO2) probably expose materials to potentially reactive etchants and solvents, appealing for extraordinary chemical stability and corrosion resistance property. In this paper, TiO2 ultrathin films were deposited on Si at 200 °C while ZrO2 and HfO2 were grown at 250 °C to fit their growth temperature window, by thermal atomic layer deposition (TALD) and plasma-enhanced ALD (PEALD). A variety of chemical liquid media including 1 mol/L H2SO4, 1 mol/L HCl, 1 mol/L KOH, 1 mol/L KCl, and 18 MΩ deionized water were used to test and compare chemical stability of all these as-deposited group IV metal oxides thin films, as well as post-annealed samples at various temperatures. Among these metal oxides, TALD/PEALD HfO2 ultrathin films exhibit the best chemical stability and anti-corrosion property without any change in thickness after long time immersion into acidic, alkaline and neutral solutions. As-deposited TALD ZrO2 ultrathin films have slow etch rate of 1.06 nm/day in 1 mol/L HCl, however other PEALD ZrO2 ultrathin films and annealed TALD ones show better anti-acid stability, indicating the role of introduction of plasma O2 in PEALD and post-thermal treatment. As-deposited TiO2 ultrathin films by TALD and PEALD are found to be etched slowly in acidic solutions, but the PEALD can decrease the etching rate of TiO2 by ~41%. After post-annealing, TiO2 ultrathin films have satisfactory corrosion resistance, which is ascribed to the crystallization transition from amorphous to anatase phase and the formation of 5% Si-doped TiO2 ultrathin layers on sample surfaces, i.e. Ti-silicate. ZrO2, and TiO2 ultrathin films show excellent corrosion endurance property in basic and neutral solutions. Simultaneously, 304 stainless steel coated with PEALD-HfO2 is found to have a lower corrosion rate than that with TALD-HfO2 by means of electrochemical measurement. The pre-treatment of plasma H2 to 304 stainless steel can effectively reduce interfacial impurities and porosity of overlayers with significantly enhanced corrosion endurance. Above all, the chemical stability and anti-corrosion properties of IV group metal oxide coatings can be improved by using PEALD technique, post-annealing process and plasma H2 pre-treatment to substrates.

Metal–insulator–metal (MIM) capacitors fabricated with Zr-Sn-Ti-O dielectrics by the plasma-enhanced atomic layer deposition (PEALD) were first demonstrated. By changing the pulse cycle ratio and cycle number of PEALD, the comprehensive electrical properties of the Zr-Sn-Ti-O MIM capacitors were optimized to meet the requirements of system-level chips for the high-density MIM capacitors. When the cycle ratio of ZrO2:SnO2:TiO2 is 2:10:2, the sample of Zr0.45Sn0.06Ti0.48O2 shows the best electrical properties: a capacitance density of 10.8 fF/ $\mu \text{m}^{{2}}$ , a quadratic voltage linearity of −83 ppm/V2, a leakage current density of $5\times 10^{{-7}}$ A/cm2 at 3 V, a breakdown voltage of 6.8 V, and a temperature linearity coefficient of 95.1 ppm/°C. These results indicate that PEALD Zr-Sn-Ti-O dielectrics are promising candidates for future high-density MIM capacitor applications in radio frequency and analog-/mixed-signal integrated circuits.

In this work, Ni3S2/Ni foam was successfully synthesized using a facile gas-phase method of annealing Ni foam in H2S atmosphere. It was used as a binder free electrode for high-performance supercapacitors. The areal capacitance increases rapidly in the initial charge-discharge cycling and then reaches a stable stage. An ultrahigh areal capacitance of 9.88 F cm−2 at the current density of 10 mA cm−2 is achieved in the stable charge-discharge stage, which is around 88 times of initial capacitance (112.5 mF cm−2). Further studies reveal that surface Ni3S2 transforms into porous Ni(OH)2 during charge-discharge process, and surface area increases more than 100 times. The soaring specific surface area is the dominant factor contributing to the increased areal capacitance. More importantly, this self-formed porous structure exhibits ultra-stable long-time cycling ability, as no capacity fading is observed even after 60000 cycles of charge-discharge at high current density (150 mA cm−2). These results indicate that self-formed porous Ni(OH)2 structure during electrochemical cycling maybe a promising electrode for high performance supercapacitor applications.

In this work, we propose a new design of flexible strain sensors based on biomimetic patterned-polydimethylsiloxane (P-PDMS) and multi-walled carbon nanotubes (MWCNTs) decorated with Ir nanoparticles (NPs) deposited by atomic layer deposition (ALD). The biomimetic flexible strain sensors of Ir NPs@MWCNTs on patterned PDMS show superior sensitivity (34.96), larger sensing range (0–30%), better stability (＞10,000 stretch and release cycles), and fairly faster response time (150 ms) under optimal 200 ALD Ir cycles. This is attributed to the synergic effect of utilizing patterned PDMS films copied from duck webs as substrates and Ir@CNTs as sensing materials. Furthermore, the flexible strain sensors can detect not only stretch but also bend stress rapidly and accurately. Above all, a simple, green, and low cost method has been developed to fabricate the flexible biomimetic strain sensors with patterned PDMS and Ir NPs@MWCNTs, exhibit promising prospects in human motion detection, wearable electronics, human-machine interfaces, etc.

Ti-based maleic acid (MA) hybrid films were successfully fabricated by molecular layer deposition (MLD) using organic precursor MA and inorganic precursor TiCl4. The effect of deposition temperature on the growth rate, composition, and bonding mode of hybrid thin films has been investigated systematically. With increasing temperature from 140 to 280 °C, the growth rate decreases from 1.42 to 0.16 A per MLD cycle with basically unchanged composition ratio of C:O:Ti in the films. Fourier transform infrared spectra indicate that all hybrid films show preference for bidentate bonding mode. Further analyses of X-ray photoelectron spectroscopy and in situ quartz crystal microbalance elucidate that as-deposited MLD Ti-MA hybrid films consist of inorganic Ti-O-Ti units and organic-inorganic Ti-MA units. In addition, the density functional theory calculation was performed to investigate the possible reaction mechanism of the TiCl4-MA MLD process, which is well consistent with experimental results. More importantly, upon comparison with the TiCl4-fumaric acid MLD system, it is demonstrated that the cis- and trans-configurations of butenedioic acid influence the MLD growth, bonding mode, stability, and charging ability of MLD hybrid films. Ti-MA hybrid films exhibit better stability and charging ability than Ti-FA hybrid films, benefiting from the inorganic Ti-O-Ti units in the hybrid films.

A charge trapping memory device using Ta2O5/Al2O3/TiO2/Al2O3/Ta2O5 (TATiAT) nanocomposite high-k dielectrics as charge trapping layer (CTL) and amorphous Al2O3 as the tunneling and blocking layers has been investigated, in which all the high-k dielectric films were fabricated by atomic layer deposition (ALD) technique. A large memory window of 10.0 V with higher charge trap density of 1.10 × 1013 cm−2 at gate voltage of ±10 V has been achieved. The better storage characteristic is attributed to the inter-diffusion between nanocomposite high-k oxides and the formation of more oxygen vacancies in CTL. The device shows the fast P/E speed and excellent endurance characteristics. A 70% initial memory window can be maintained after 10 years of retention by using the extrapolation method. The large conduction band offsets of 1.02 eV between TATiAT and Al2O3 is beneficial to retention characteristic due to the deep trap level.