Transparent Anti-Radiative Ferroelectric Heterostructure Based on

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Functional Inorganic Materials and Devices

Transparent Anti-Radiative Ferroelectric Heterostructure Based on Flexible Oxide Heteroepitaxy Chun-Hao Ma, Jie Jiang, Pao-Wen Shao, Qiangxiang Peng, Chun-Wei Huang, Ping-Chun Wu, Jyun-Ting Lee, Yu-Hong Lai, Din Ping Tsai, Jyh Ming Wu, Shen-Chuan Lo, Wen-Wei Wu, Yichun Zhou, Po-Wen Chiu, and Ying-Hao Chu ACS Appl. Mater. Interfaces, Just Accepted Manuscript • DOI: 10.1021/acsami.8b10272 • Publication Date (Web): 17 Aug 2018 Downloaded from http://pubs.acs.org on August 19, 2018

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ACS Applied Materials & Interfaces

Transparent Anti-Radiative Ferroelectric Heterostructure Based on Flexible Oxide Heteroepitaxy Chun-Hao Ma1,2, Jie Jiang3, Pao-Wen Shao2, Qiang-Xiang Peng3, Chun-Wei Huang2,4, PingChun Wu2, Jyun-Ting Lee5, Yu-Hong Lai2, Din-Ping Tsai6, Jyh-Ming Wu5, Shen-Chuan Lo4, Wen-Wei Wu2, Yi-Chun Zhou3, Po-Wen Chiu1,7*, and Ying-Hao Chu2,4,8* 1

Department of Electrical Engineering, National Tsing Hua University, 30013 Hsinchu, Taiwan

2

Department of Materials Science and Engineering, National Chiao Tung University, Hsinchu

30010, Taiwan 3

Key Laboratory of Low Dimensional Materials and Application Technology of Ministry of

Education, Xiangtan University, Hunan 411105, China 4

Material and Chemical Research Laboratories, Industrial Technology Research Institute,

Hsinchu 31040, Taiwan 5

Department of Materials Science and Engineering, National Tsing Hua University, Hsinchu

30013, Taiwan 6

Research Center for Applied Sciences, Academia Sinica, Taipei 11529, Taiwan

ACS Paragon Plus Environment

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ACS Applied Materials & Interfaces 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

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Institute of Atomic and Molecular Sciences, Academia Sinica, Taipei 10617, Taiwan

8

Center for Emergent Functional Matter Science, National Chiao Tung University, Hsinchu

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30010, Taiwan KEYWORDS : ferroelectric, transparent, flexible, anti-radiative, PLZT, mica, van der Waals epitaxy

ABSTRACT

In the era of Internet of Things, the demand for flexible and transparent electronic devices has shifted to the forefront of materials science research. However, the radiation damage to key performance of transparent devices under radiative environment remains as a critical issue. Here, we present a promising technology for nonvolatile transparent electronic devices based on flexible oxide heteroepitaxy. A direct fabrication of epitaxial lead lanthanum zirconate titanate on transparent flexible mica substrate with indium tin oxide electrodes is presented. The transparent flexible ferroelectric heterostructures not only retain their superior performance, thermal stability, reliability and mechanical durability, but also exhibit remarkably robust properties against to a strong radiation exposure. Our study demonstrates an extraordinary concept to realize transparent flexible nonvolatile electronic devices for the design and development of next-generation smart devices with potential application in electronics, automotive, aerospace and nuclear systems.


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INTRODUCTION With increasing demand on Internet of Things, wearable and flexible electronics becomes an important research direction to integrate more functionalities. Along this research direction, transparent components serve as a necessary ingredient in lots of devices, such as panels, glasses, windshield, windows etc. Thus, transparent flexible electronics have attracted much interest as novel technical solution for next-generation consumer electronics towards a convenient and smart living future.1-4 To realize these transparent flexible electronic systems, it is necessary to compose the system with ubiquitous components such as image displays,5 logics,6 information storages,7 and sensors.8 Moreover, most transparent components are required to use under radiation exposure, the radiation loss of key performance becomes a critical feature.9-10 Among the components of transparent electronics, an important integral part of the electronic circuits is an element of nonvolatile memory which can be used to store and retrieve information as required. Several types of non-volatile memories that feature transparency in visible light have been reported, such as a memory with In-Ga-Zn-O semiconductor charge storage layer,11-12 the polymer ferroelectric memory based on poly(vinylidene fluoride trifluoroethylene),13-14 graphene based resistive switching memory etc.15-16 They all show superior advantages with tremendous potentials in applications. However, none of them showed promising feature against radiation yet. Oxide materials are ubiquitous in modern science due to their fascinating physical properties and promising applications in next generation technologies. For instance, ferroelectric oxides have gained great interest due to its large polarization, fast switching time, low coercive field, and a high piezoelectric coefficient.17-18 More importantly, they also show superior radiation tolerance.19 Thus, it is promising to realize high-speed, high storage density, low-power consumption and low cost non-volatile memory based on ferroelectric oxides. However, no transparent flexible


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ferroelectric memory based on complex oxides have been reported. Therefore, to build up a transparent flexible oxide based ferroelectric memory is a big challenge and an important step in transparent flexible applications. In order to construct a ferroelectric memory featuring optical transparency and mechanical flexibility, three key ingredients have to be integrated: 1. Transparent ferroelectric layer. In the search of transparent ferroelectrics, perovskite lead lanthanum zirconate titanate (Pb1-xLax(ZryTi1y)O3;

PLZT) is an important one showing high transmittance, relatively low coercive field, and

high remnant polarization.20-22 2. Transparent conducting oxides.23 Among them, indium tin oxide (ITO) is the most common one due to its high conductivity and good optical transmittance. It can also serve as a potential solution to solve the issue of ferroelectric fatigue in the heterostructure since oxide electrodes are favorable.24-25 However, typically the process for ferroelectric oxides require a thermal treatment at high oxygen pressure in order to reduce leakage current, while transparent conducting oxides need a relatively reducing atmosphere to produce oxygen vacancies as the source for the generation of charge carriers. Thus, the optimization of growth process to satisfy the needs of both materials is an essential step. 3. Transparent and flexible substrates. Recently, due to its atomically smooth surface, high thermal stability, high transparency and mechanical flexibility, muscovite mica has been reported to be a proper substrate for oxide heteroepitaxy.26-27 Various flexible heterostructures composed oxide heteroepitaxy were delivered, providing a new platform for flexible electronics.28-30 In this study, we build up a transparent ferroelectric system composed of ITO/PLZT/ITO/muscovite heteroepitaxy to combine these key parts for transparent flexible memory (Figure 1a). In our investigation, the ITO/PLZT/ITO/mica heteroepitaxy not only retain the superior optical and ferroelectric properties but also exhibit good mechanical flexibility, durability, and thermal stability. As shown in the inset of Figure 1b, the


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photograph of ITO/PLZT/ITO/mica clearly highlights high optical transparency of the heterostructure with mechanical flexibility. The optical transmittance spectrum of the heterostructure in the ultraviolet-visible-infrared regime is shown in Figure 1b. An average visible transmittance of 80% of the heterostructure can be observed. Our results represent an important milestone in the advancement of transparent flexible ferroelectric applications via oxide heteroepitaxy. RESULT AND DISCUSSION In the heterostructure, the local ferroelectricity was probed by piezoresponse force microscopy (PFM) based on the patterns written on the PLZT layer with an application of electric field via a conducting tip. A tip bias of +6V was applied to pole the region of 3 μm x 3 μm, followed by another poling with a tip bias of -8V in the central area of 1 μm x 1 μm. The surface topography and the corresponding out-of-plane polarization signal are shown in Figure 1c and d, respectively. In Figure 1d, a PFM phase image shows the regions with clear bright and dark contrast corresponding to downward and upward polarizations, respectively. After the poling, the area of 3 μm x 3 μm and 1 μm x 1 μm show uniform bright contrast and dark contrast, respectively. This result indicates the polarization of the PLZT layer is switchable, delivering the local and uniform ferroelectric feature of the heterostructure. Figure S1 shows representative local hysteresis loops extracted from the amplitude and phase signals of PFM. The square loop showing an 180° change in phase signal and a clear butterfly loop in amplitude signal confirms the good ferroelectric switching nature of the PLZT/ITO/mica system. The advances in emerging transparent flexible electronic devices motivate researchers to explore additional requirements in harsh environments. Well-saturated and symmetric polarization-electric field (P-E) hysteresis loops of the heterostructure measured at 1kHz and the temperatures ranging from 25° to 200°C on a virgin


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device are shown in Figure 1e. The typical hysteresis loop with a change in polarization shows effective switching of dipoles. The ferroelectric capacitor exhibits a saturated polarization (Psat) of ~84 μC/cm2, a remnant polarization (Pr) of ~41 μC/cm2 and a coercive field (Ec) of ~290 kV/cm at 25°C, and the temperature evolution is shown in Figure 1f. The superior ferroelectric properties of the heteroepitaxy against temperature can be attributed to high quality and thermal stability of the oxide heteroepitaxy, delivering a potential solution for high-temperature transparent flexible applications.

Figure 1. (a) Schematic representation of PLZT/ITO/mica heterostructure. (b) Optical spectrum of ITO/PLZT/ITO/mica. The (c) surface topography and the (d) out-of-plane phase image. (e) PE hysteresis loops at various temperatures. (f) Remnant, saturation polarizations and coercive field as functions of temperature. The heteroepitaxy and phase identification of the structure were characterized by X-ray diffraction (XRD). In the heterostructure, a very thin ZnO layer (~10 nm) was inserted. Without


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this ZnO layer, it is very difficult to obtain epitaxial ITO bottom layer since the variation of ITO surface energies along different orientations is not very large. However, due to the lowest surface energy of ZnO(00l) and the same symmetry with muscovite, high-quality epitaxial ZnO thin film can be obtained and served as the seeding layer for the sequential growth of high-quality heteroepitaxy. Then, an epitaxial ITO layer as the transparent bottom electrode was inserted for electrical characterizations. After the ITO layer, a PLZT layer was grown on top of the heterostructure. The corresponding growth conditions for each layer can be found in Method session. Figure 2a shows a typical out-of-plane L-scan of the heterostructure. The observation of only PLZT(ll0), ITO(lll) and ZnO(00l) diffraction peaks with muscovite (00l) suggests the epitaxial nature of the heterostructure without other secondary phases. Furthermore, the Φ-scans of PLZT and, ITO, ZnO and muscovite reflections were used to analyze the in-plane structural relationships as shown in Figure 2b. The observation of one primary and two secondary muscovite peaks at 120° intervals indicates different stacking sequences between sheet units along c axis, whereas ZnO {102}, ITO {004} and PLZT {200} exhibit multiple peaks that indicates the growth of epitaxial ZnO, ITO and PLZT films with a multidomain feature on mica substrate. On the basis of

the

XRD

results,

the

epitaxial

relationship

can

be

determined

as

(110)PLZT//(111)ITO//(001)ZnO//(001)mica and (001)PLZT//(1-10)ITO//(010)ZnO//(010)mica for the heterostructure. The multidomain feature and epitaxial relationship of PLZT on ITO is schematically shown in Figure 2c. The rocking curves measured to obtain the critical information about the crystallinity resulted in the full width at half maximum of ~0.71°, ~1.28°, and ~1.77° for ZnO (002), ITO (222), and PLZT (110) peaks, respectively, as shown in Figure 2d. In order to characterize the detailed microstructure on the PLZT/ITO/mica heterostructure and further confirm the heteroepitaxy, the interfaces of the heterostructures were examined by transmission


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electron microscopy (TEM). Figure 2e shows high-resolution cross-sectional TEM images taken along the zone axis of [010]mica, revealing PLZT/STO/ITO and ITO/ZnO/mica interfaces. The STO buffer layer (~10 nm) was chosen to realize high quality epitaxial PLZT on ITO due to the excellent structural compatibility with both PLZT and ITO layers. In addition, it can serve as a transition layer for oxygen stoichiometry since oxygen vacancy is not favorable in the PLZT layer but it is required in the ITO layer. Without this layer, only polycrystalline PLZT could be obtained and all the heterostructures suffered from a severe leakage problem. The corresponding fast Fourier transform patterns of selected area of PLZT, STO, ITO and mica are shown in the right panels, respectively. The reciprocal lattices are also clearly indexed, and the consistency of epitaxial relationships with the XRD results is further confirmed. The interfaces without observable interdiffusion of species across the interfaces indicate high quality of the heterostructure. According to the XRD and TEM results, a good oxide heteroepitaxy system based on PLZT/ITO/muscovite is delivered, which is a key to attain excellent thermal and mechanical stabilities.


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Figure 2. (a) Typical 2θ-θ scan of the heterostructure. (b) Φ-scans at PLZT{200} and {002}, ITO {004}, ZnO {102} and muscovite {203} diffraction peaks. (c) Schematic describing the relationship between the multidomain structures of PLZT grown on ITO layer. (d) Rocking curves of PLZT (110), ITO (222) and ZnO (002). (e) Cross-sectional TEM image of PLZT/ITO/mica interface along with the fast Fourier transform patterns of PLZT, STO, ITO and mica. In the push to practical applications, a series of tests on cyclability of the heteroepitaxy were carried out. The macroscopic ferroelectric performance of the heterostructure against mechanical flexing was evaluated under both tensile and compressive bending modes on the capacitor structure with the top electrode size of 200 μm in diameter. Figure 3a shows the P-E hysteresis loops of the ITO/PLZT/ITO capacitors under various compressive and tensile bending radii (r), whereas Figure 3b shows the change in Psat, Pr and Ec values as a function of bending radius. For the bending radius down to 5 mm, an observation of constant Psat, Pr and Ec values within experimental errors suggests that the ITO/PLZT/ITO capacitor shows stable electrical properties even under mechanical constraints. Moreover, the P-E hysteresis loops under tensile and compressive bending radius of 5 mm before and after 1000 bending cycles and the changes in Psat, Pr and Ec values obtained from the heterostructure exhibit no noticeable change (Figure 3c,d). As shown in Figure S2, no visible cracks or exfoliation show up after 1000 repeated bending cycles. It is easy to understand that due to the relatively weak interaction between film and substrate, and the thickness ratio of film to substrate is completely small, the actual strain applied to the capacitor is too small to influence its performances. Furthermore, for these ferroelectric capacitors to be used in nonvolatile memory applications, ferroelectric reliability issues, such as imprint, retention and fatigue, have to be addressed for their long lifetime operation. The ITO/PLZT/ITO/mica heterostructure exhibits excellent polarization retention (Figure 3e) after 105 s without and under the bending


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situations. The polarization fatigue, which is the reduction in the amount of remnant polarization with repeated switching cycles, of a ITO/PLZT/ITO/mica capacitor is displayed in Figure 3f. The fatigue behavior is stable in the bent states and remains identical before and after 1000 compressive bending cycles. Almost no polarization fatigue is detected after 1010 switching cycles. It is clear from the aforementioned results that the transparent flexible ITO/PLZT/ITO/mica system exhibit stable and superior performance against mechanical bending highly desirable for transparent flexible ferroelectric applications. More importantly, the optical transmittance remains >80% after the mechanical bending tests. Such a feature is attributed to the superior oxide heteroepitaxy built on muscovite substrates. In addition, the piezoelectric response of the heterostructure was tested under bending condition (see the schematic diagram in Figure S3a left-side). As shown in Figure S3a,b, the corresponding open-circuit voltage and short-circuit current generated by bending the sample are 0.3 V and 4 nA, respectively, implying its potential application for transparent piezoelectric devices, self-powered sensors,31 and nanogenerators.32


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Figure 3. (a) P-E hysteresis loops under various tensile and compressive bending radii. (b) Pr, Psat and Ec variation as a function of bending radius. (c) P-E hysteresis loops under tensile and compressive bending of 5 mm before and after 1000 bending cycles. (d) Pr, Psat and Ec variation before and after 1000 bending cycles. (e) Retention and (f) fatigue for the ITO/PLZT/ITO capacitors in unbent and compressively and tensilely bent conditions. A key advantage of ferroelectric memory is the fearlessness of radiation. However, for the applications in aerospace and nuclear, transparent components actually expose to radiation. Thus, it is important to study the ferroelectric performance of the heterostructure after an exposure to strong radiation. Figure 4a shows the P-E hysteresis loops of the ITO/PLZT/ITO/mica system after given a dose of 5 Mrad. The ferroelectric performance of the heterostructure was also studied under both compressive and tensile bending modes, and Figure 4b shows the change in P sat, Pr and Ec values as a function of bending radius. The ferroelectric properties retain constant regardless of the mechanical constraints, and the performance also remains the same before and after exposed to the radiation. These results indicate that the ITO/PLZT/ITO/mica system is robust against radiation. Figure 4c displays stable polarization retention of the ITO/PLZT/ITO capacitors after absorbed 5 Mrad of dose level. Furthermore, Figure 4d shows the evolution of the normalized polarization as a function of the number of switching cycles. The fatigue behavior is both stable in the unbent and bent states, and even maintains the same after 1000 compressive bending cycles. The heterostructure which absorbed the radiation shows no polarization fatigue up to 1010 switching cycles. Therefore, it is evident that the transparent flexible ferroelectric PLZT/mica system exhibit stable performance and can be applied under radiative environment which can play an important role in next-generation aerospace and nuclear applications.


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Figure 4. (a) P-E hysteresis loops under various bending conditions after the heterostructure absorbed radiation at the dose level of 5 Mrad. (b) Pr, Psat and Ec variation as a function of bending radius after the samples exposed to radiation. (c) Retention and (d) fatigue for the heterostructure which was exposed in unbent and compressively and tensilely bent conditions.

CONCLUSIONS In conclusion, high quality transparent flexible ferroelectric element based on the ITO/PLZT/ITO/mica heteroepitaxy has been successfully demonstrated. Furthermore, this capacitor retains its superior electrical performance against temperature variation. Meanwhile, the heterostructure is robust against mechanical and radiation constraints. This study paves the way for an exciting new avenue to next-generation transparent flexible smart electronics. METHOD


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The epitaxial ITO/PLZT/ITO/mica heterostructure was fabricated via pulsed laser deposition using commercial ITO (90% In2O3 and 10% SnO2) and PLZT (Pb0.9La0.1(Zr0.7Ti0.3)O3) targets. A freshly cleaved muscovite mica (1 cm x 1 cm) without any surface treatment or precleaning process was adopted in this study. A KrF excimer laser (λ = 248 nm, Coherent) was operated at 10 Hz laser repetition and laser fluence of 3 J/cm2. The deposition chamber was initially evacuated to a base pressure of 10-6 Torr. The deposition process of 100nm PLZT was carried out at a substrate temperature of 550°C in 100 mTorr oxygen pressure. Both the top (diameter of 200 μm) and bottom ITO layers (50nm) were deposited at the substrate temperature of 400°C and in the oxygen pressure of 5 x 10-4 Torr. Moreover, prior to PLZT and bottom ITO deposition, STO (~10 nm) and ZnO (~10 nm) were deposited as buffer layers, respectively. The STO was grew at a substrate temperature of 550°C in 100 mTorr oxygen pressure, meanwhile the ZnO was deposited at 400°C with oxygen pressure of 5 x 10-4 Torr. The 2θ-θ scan along normal direction and Φ scans were performed at the BL17A at the National Synchrotron Radiation Research Center in Hsinchu to obtain the structural information. The film-substrate interface microstructure was studied by cross-sectional TEM. Cross-sectional TEM specimens were prepared by focused ion beam technique. The optical spectra were collected in the transmission mode using a PerkinElmer Lambda-900 spectrometer. The surface morphology and PFM study were investigated via Asylum Research MPF-3D. The phase-voltage hysteresis loops were measured with a bias window up to 10V. A homemade bending stage was used to perform the evolution of ferroelectricity while the sample was under bending.


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The ferroelectric properties were characterized by a ferroelectric test system (Radiant Technologies Precisionsworkstations RT66A). The P-E hysteresis loops were measured by two tips at a frequency of 1 kHz, and different radii were checked by using the bending stage. A heating stage was used to change the measurement temperature to estimate the P-E variation along with the temperature ranging from 25° to 200°C. Predesigned Teflon molds of fixed bending radii were used to induce the reported compressive and tensile bending strains. For the bending-cycle measurement, a computer-aided homebuilt bending setup combined with optical microscope was used. The ITO/PLZT/ITO/mica was bent from one end while the other end was fixed, and the vertical distance was measured using the microscope as shown in Figure S4. Considering to the radiation environment in outer space, a series of tests on the ITO/PLZT/ITO/mica heterostructure was carried out after the absorbed radiation. The radiation was given by a 60Co γ ray which is at the dose level of 5 Mrad with the dose rate of 50 rad/s. ASSOCIATED CONTENT Supporting Information. Local PFM study, cross-section SEM images, energy generation measurement, and information of home-made bending stage AUTHOR INFORMATION Corresponding Author *E-mail: [email protected] *E-mail: [email protected]


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ORCID Ying-Hao Chu: 0000-0002-3435-9084 Notes The authors declare no competing financial interests. ACKNOWLEDGMENT This work is supported by the Ministry of Science and Technology, Taiwan (Grant Nos. MOST 106-2119-M-009-011-MY3, 106-2628-E-009-001-MY2, 106-2923-M-009-003-MY2) and The SPROUT project of Ministry of Education, Taiwan. REFERENCES 1.

Wager, J. F. Transparent Electronics. Science 2003, 300, 1245−1246.

2.

Yu, X.; Zeng, L.; Zhou, N.; Guo, P.; Shi, F.; Buchholz, D. B.; Ma, Q.; Yu, J.; Dravid, V.

P.; Chang, R. P. H.; Bedzyk, M.; Marks, T. J.; Facchetti, A.; Ultra-flexible, “Invisible” Thin-Film Transistors Enabled by Amorphous Metal Oxide/Polymer Channel Layer Blends. Adv. Mater. 2015, 27, 2390−2399. 3.

Nathan, A.; Lee, S.; Jeon, S.; Robertson, J.; Amorphous Oxide Semiconductor TFTs for

Displays and Imaging. IEEE J. Display Technol. 2014, 10, 917−927. 4.

Lee, S.; Jeon, S.; Chaji, R.; Nathan, A.; Transparent Semiconducting Oxide Technology

for Touch Free Interactive Flexible Displays. Proc. IEEE 2015, 103, 644−664. 5.

Mativenga, M.; Geng, D.; Kim, B.; Jang, J.; Fully Transparent and Rollable Electronics.

ACS Appl. Mater. Interfaces 2015, 7, 11578−1585.


15


6.

Page 16 of 20

Rembert, T.; Battaglia, C.; Anders, A.; Javey, A.; Room Temperature Oxide Deposition

Approach to Fully Transparent, All-oxide Thin-film Transistors. Adv. Mater. 2015, 27, 6090−6095. 7.

Qian, K.; Nguyen, V. C.; Chen, T.; Lee, P. S.; Novel Concepts in Functional Resistive

Switching Memories. J. Mater. Chem. C 2016, 4, 9637−9645. 8.

Adinolfi, V.; Ouellette, O.; Saidaminov, M. I.; Walters, G.; Abdelhady, A. L.; Bakr, O. M.;

Sargent, E. H.; Fast and Sensitive Solution-processed Visible-blind Perovskite UV Photodetectors. Adv. Mater. 2016, 28, 7264−7268. 9.

Bogaerts, J.; Dierickx, B.; Meynants, G.; Uwaerts, D.; Total Dose and Displacement

Damage Effects in A Radiation-hardened CMOS APS. IEEE Trans. Electron Devices 2003, 50, 84−90. 10.

Zou, J.; Gao, K.; Yang, J.; Zhu, J.; Research on Anti-radiation Weapon Confronting Active

Decoys Based on Doppler Frequencies Difference. ICMAE 2016, 262−266. 11.

Zhang, W.-P.; Qian, S.-B.; Liu, W.-J.; Ding, S.-J.; Zhang, D. W.; Novel Multi-level Cell

TFT Memory with An In–Ga–Zn-O Charge Storage Layer and Channel. IEEE Electron. Device Lett. 2015, 36, 1021−1023. 12.

Inoue, H.; Matsuzaki, T.; Nagatsuka, S.; Okazaki, Y.; Sasaki, T.; Noda, K.; Matsubayashi,

D.; Ishizu, T.; Onuki, T.; Isobe, A.; Shionoiri, Y.; Kato, K.; Okuda, T.; Koyama, J.; Yamazaki, S.; Nonvolatile Memory with Extremely Low-leakage Indium-gallium-zinc-oxide Thin-film Transistor. IEEE J. Solid- State Circuits 2012, 47, 2258−2265.


16

Page 17 of 20 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60


13.

Bhansali, U. S.; Khan, M. A.; Alshareef, H. N.; Electrical Performance of Polymer

Ferroelectric Capacitors Fabricated on Plastic Substrate Using Transparent Electrodes. Org. Electron. 2012, 13, 1541−1545. 14.

Yoon, S.-M.; Yang, S.; Byun, C.; Park, S.-H. K.; Cho, D.-H.; Jung, S.-W.; Kwon, O.-S.;

Hwang, C.-S.; Fully Transparent Non-volatile Memory Thin-film Transistors Using An Organic Ferroelectric and Oxide Semiconductor below 200 °C. Adv. Funct. Mater. 2010, 20, 921−926. 15.

Yao, J.; Lin, J.; Dai, Y.; Ruan, G.; Yan, Z.; Li, L.; Zhong, L.; Natelson, D.; Tour, J. M.;

Highly Transparent Nonvolatile Resistive Memory Devices from Silicon Oxide and Graphene. Nat. Commun. 2012, 3, 1101. 16.

Jeong, H. Y.; Kim, J. Y.; Kim, J. W.; Hwang, J. O.; Kim, J.-E.; Lee, J. Y.; Yoon, T. H.;

Cho, B. J.; Kim, S. O.; Ruoff, R. S.; Choi, S.-Y.; Graphene Oxide Thin Films for Flexible Nonvolatile Memory Applications. Nano Lett. 2010, 10, 4381−4386. 17.

Ramesh, R.; Thin Film Ferroelectric Materials and Devices. Springer, 1997.

18.

Izyumskaya, N.; Alivov, Y.-I.; Cho, S.-J.; Morkoç, H.; Lee, H.; Kang, Y.-S.; Processing,

Structure, Properties, and Applications of PZT Thin Films. Crit. Rev. Solid State Mater. Sci. 2007, 32, 111−202. 19.

Sickafus, K. E.; Minervini, L.; Grimes, R. W.; Valdez, J. A.; Ishimaru, M.; Li, F.;

McClellan, K. J.; Hartmann, T.; Radiation Tolerance of Complex Oxides. Science 2000, 289, 748−751.


17


20.

Page 18 of 20

Hu, Z.; Wang, X.; Nan, T.; Zhou, Z.; Ma, B.; Chen, X.; Jones, J. G.; Howe, B. M.; Brown,

G. J.; Gao, Y.; Lin, H.; Wang, Z.; Guo, R.; Chen, S.; Shi, X.; Shi, W.; Sun, H.; Budil, D.; Liu, M.; Sun, N. X.; Non-volatile Ferroelectric Switching of Ferromagnetic Resonance in NiFe/PLZT Multiferroic Thin Film Heterostructures. Sci. Rep. 2016, 6, 32408. 21.

Liu, S. Y.; Chua, L.; Tan, K. C.; Valavan, S. E.; Novel Ferroelectric Capacitor for Non-

volatile Memory Storage and Biomedical Tactile Sensor Applications. Thin Solid Films 2010, 518, 152−155. 22.

Haertling, G. H.; Ferroelectric Ceramics: History and Technology. J. Am. Ceram. Soc.

1999, 82, 797−818. 23.

Hosono, H.; Recent Progress in Transparent Oxide Semiconductors: Materials and Device

Application. Thin Solid Films 2007, 515, 6000−6014. 24.

Ramesh, R.; Chan, W. K.; Wilkens, B.; Gilchrist, H.; Sands, T.; Tarascon, J. M.; Keramidas,

V. G.; Fork, D. K.; Lee, J.; Safari, A.; Fatigue and Retention in Ferroelectric Y-Ba-Cu-O/Pb-ZrTi-O/Y-Ba-Cu-O Heterostructures. Appl. Phys. Lett. 1992, 61, 1537. 25.

Eom, C. B.; Van Dover, R. B.; Phillips, J. M.; Werder, D. J.; Marshall, J. H.; Chen, C. H.;

Cava, R. J.; Fleming, R. M.; Fork, D. K.; Fabrication and Properties of Epitaxial Ferroelectric Heterostructures with (SrRuO3) Isotropic Metallic Oxide Electrodes. Appl. Phys. Lett. 1993, 63, 2570. 26.

Ma, C.-H.; Lin, J.-C.; Liu, H.-J.; Do, T. H.; Zhu, Y.-M.; Ha, T. D.; Zhan, Q.; Juang, J.-Y.;

He, Q.; Arenholz, E.; Chiu, P.-W.; Chu, Y.-H.; Van der Waals Epitaxy of Functional MoO2 Film on Mica for Flexible Electronics. Appl. Phys. Lett. 2016, 108, 253104.


18

Page 19 of 20 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60


27.

Wu, P.-C.; Chen, P.-F.; Do, T. H.; Hsieh, Y.-H.; Ma, C.-H.; Ha, T. D.; Wu, K.-H.; Wang,

Y.-J.; Li, H.-B.; Chen, Y.-C.; Juang, J.-Y.; Yu, P.; Eng, L. M.; Chang, C.-F.; Chiu, P.-W.; Tjeng, L. H.; Chu, Y.-H.; Heteroepitaxy of Fe3O4/muscovite: A New Perspective for Flexible Spintronics. ACS Appl. Mater. Interfaces 2016, 8, 33794−33801. 28.

Chu, Y.-H.; Van der Waals Oxide Heteroepitaxy. npj Quantum Mater. 2017. 2, 67.

29.

Jiang, J.; Bitla, Y.; Huang, C.-W.; Do, T. H.; Liu, H.-J.; Hsieh, Y.-H.; Ma, C.-H.; Jang, C.-

Y.; Lai, Y.-H.; Chiu, P.-W.; Wu, W.-W.; Chen, Y.-C.; Zhou, Y.-C.; Chu, Y.-H.; Flexible Ferroelectric Element Based on Van der Waals Heteroepitaxy. Sci. Adv. 2017, 3, e1700121. 30.

Bitla, Y.; Chen, C.; Lee, H.-C.; Do, T. H.; Ma, C.-H.; Qui, L. V.; Huang, C.-W.; Wu, W.-

W.; Chang, L.; Chiu, P.-W.; Chu, Y.-H.; Oxide Heteroepitaxy for Flexible Optoelectronics. ACS Appl. Mater. Interfaces 2016, 8, 32401−32407. 31.

Fan, F. R.; Tang, W.; Wang, Z. L.; Flexible Nanogenerators for Energy Harvesting and

Self-powered Electronics. Adv. Mater. 2016, 28, 4283−4305 (2016). 32.

Wu, J. M.; Xu, C.; Zhang, Y.; Yang, Y.; Zhou, Y.; Wang, Z. L.; Flexible and Transparent

Nanogenerators Based on A Composite of Lead-free ZnSnO3 Triangular-belts. Adv. Mater. 2012, 24, 6094−6099.


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Transparent Anti-Radiative Ferroelectric Heterostructure Based on

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