Bi₂O₂Se-Based True Random Number Generator for Security Applications

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This article references 50 other publications.

1. 1

   Pang, Y.; Gao, B.; Lin, B.; Qian, H.; Wu, H. Memristors for Hardware Security Applications. Adv. Electron. Mater. 2019, 5, 1800872,  DOI: 10.1002/aelm.201800872

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   Jiang, H.; Belkin, D.; Savel’Ev, S. E.; Lin, S.; Wang, Z.; Li, Y.; Joshi, S.; Midya, R.; Li, C.; Rao, M.; Barnell, M.; Wu, Q.; Yang, J. J.; Xia, Q. A Novel True Random Number Generator Based on a Stochastic Diffusive Memristor. Nat. Commun. 2017, 8, 882,  DOI: 10.1038/s41467-017-00869-x

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   A novel true random number generator based on a stochastic diffusive memristor

   Jiang Hao; Belkin Daniel; Lin Siyan; Wang Zhongrui; Li Yunning; Joshi Saumil; Midya Rivu; Li Can; Rao Mingyi; Yang J Joshua; Xia Qiangfei; Belkin Daniel; Savel'ev Sergey E; Barnell Mark; Wu Qing

   Nature communications (2017), 8 (1), 882 ISSN:.

   The intrinsic variability of switching behavior in memristors has been a major obstacle to their adoption as the next generation of universal memory. On the other hand, this natural stochasticity can be valuable for hardware security applications. Here we propose and demonstrate a novel true random number generator utilizing the stochastic delay time of threshold switching in a Ag:SiO2 diffusive memristor, which exhibits evident advantages in scalability, circuit complexity, and power consumption. The random bits generated by the diffusive memristor true random number generator pass all 15 NIST randomness tests without any post-processing, a first for memristive-switching true random number generators. Based on nanoparticle dynamic simulation and analytical estimates, we attribute the stochasticity in delay time to the probabilistic process by which Ag particles detach from a Ag reservoir. This work paves the way for memristors in hardware security applications for the era of the Internet of Things.Memristors can switch between high and low electrical-resistance states, but the switching behaviour can be unpredictable. Here, the authors harness this unpredictability to develop a memristor-based true random number generator that uses the stochastic delay time of threshold switching.

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3. 3

   Jiang, H.; Li, C.; Zhang, R.; Yan, P.; Lin, P.; Li, Y.; Yang, J. J.; Holcomb, D.; Xia, Q. A Provable Key Destruction Scheme Based on Memristive Crossbar Arrays. Nat. Electron. 2018, 1, 548– 554,  DOI: 10.1038/s41928-018-0146-5

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4. 4

   Yang, L.; Cheng, L.; Li, Y.; Li, H.; Li, J.; Chang, T. C.; Miao, X. Cryptographic Key Generation and In Situ Encryption in One-Transistor-One-Resistor Memristors for Hardware Security. Adv. Electron. Mater. 2021, 7, 2001182,  DOI: 10.1002/aelm.202001182

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   4

   Cryptographic Key Generation and In Situ Encryption in One-Transistor-One-Resistor Memristors for Hardware Security

   Yang, Ling; Cheng, Long; Li, Yi; Li, Haoyang; Li, Jiancong; Chang, Ting-Chang; Miao, Xiangshui

   Advanced Electronic Materials (2021), 7 (5), 2001182CODEN: AEMDBW; ISSN:2199-160X. (Wiley-VCH Verlag GmbH & Co. KGaA)

   The problem of hardware security is exacerbating in the artificial intelligence & Internet of Things era. Phys. unclonable function (PUF) is a promising security primitive that exploits the intrinsic random variations in electronic hardware to produce digital keys. Here, it is shown for the first time that the subthreshold slope (S.S) variations of the transistors can be utilized as the entropy source of the PUF to generate the phys. keys. By combining this S. S PUF with a memristor-based XOR logic function, an in situ encryption/decryption scheme is proposed in a compact one-transistor-one-resistor (1T1R) architecture. It is exptl. demonstrated that the S. S PUF shows great reproducibility, uniqueness, and uniformity. Using the S. S PUF keys, encryption and decryption are successfully implemented for three 16-bit binary sequences in 1T1R devices. The results demonstrate that the unique features of 1T1R can enlighten functional design at the device level against hardware security threats, and the security, memory, and computing can be realized on the same device.

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5. 5

   Kim, G.; In, J. H.; Kim, Y. S.; Rhee, H.; Park, W.; Song, H.; Park, J.; Kim, K. M. Self-Clocking Fast and Variation Tolerant True Random Number Generator Based on a Stochastic Mott Memristor. Nat. Commun. 2021, 12, 2906,  DOI: 10.1038/s41467-021-23184-y

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   5

   Self-clocking fast and variation tolerant true random number generator based on a stochastic mott memristor

   Kim, Gwangmin; In, Jae Hyun; Kim, Young Seok; Rhee, Hakseung; Park, Woojoon; Song, Hanchan; Park, Juseong; Kim, Kyung Min

   Nature Communications (2021), 12 (1), 2906CODEN: NCAOBW; ISSN:2041-1723. (Nature Research)

   The intrinsic stochasticity of the memristor can be used to generate true random nos., essential for non-decryptable hardware-based security devices. Here, we propose a novel and advanced method to generate true random nos. utilizing the stochastic oscillation behavior of a NbOx mott memristor, exhibiting self-clocking, fast and variation tolerant characteristics. The random no. generation rate of the device can be at least 40 kb s-1, which is the fastest record compared with previous volatile memristor-based TRNG devices. Also, its dimensionless operating principle provides high tolerance against both ambient temp. variation and device-to-device variation, enabling robust security hardware applicable in harsh environments.

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6. 6

   Du, N.; Schmidt, H.; Polian, I. Low-Power Emerging Memristive Designs towards Secure Hardware Systems for Applications in Internet of Things. Nano Mater. Sci. 2021, 3, 186– 204,  DOI: 10.1016/j.nanoms.2021.01.001

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7. 7

   Lv, S.; Liu, J.; Geng, Z. Application of Memristors in Hardware Security: A Current State-of-the-Art Technology. Adv. Intell. Syst. 2021, 3, 2000127,  DOI: 10.1002/aisy.202000127

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8. 8

   Lin, B.; Gao, B.; Pang, Y.; Tang, J.; Qian, H.; Wu, H. A Unified Memory and Hardware Security Module Based on the Adjustable Switching Window of Resistive Memory. IEEE J. Electron Devices Soc. 2020, 8, 1257– 1265,  DOI: 10.1109/JEDS.2020.3019266

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9. 9

   Woo, K. S.; Kim, J.; Han, J.; Choi, J. M.; Kim, W.; Hwang, C. S. A High-Speed True Random Number Generator Based on a Cu_XTe_1-x Diffusive Memristor. Adv. Intell. Syst. 2021, 3, 2100062,  DOI: 10.1002/aisy.202100062

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10. 10

    Tian, H.; Wang, X. F.; Mohammad, M. A.; Gou, G. Y.; Wu, F.; Yang, Y.; Ren, T. L. A Hardware Markov Chain Algorithm Realized in a Single Device for Machine Learning. Nat. Commun. 2018, 9, 4305,  DOI: 10.1038/s41467-018-06644-w

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    10

    A hardware Markov chain algorithm realized in a single device for machine learning

    Tian He; Wang Xue-Feng; Gou Guang-Yang; Wu Fan; Yang Yi; Ren Tian-Ling; Tian He; Wang Xue-Feng; Gou Guang-Yang; Wu Fan; Yang Yi; Ren Tian-Ling; Mohammad Mohammad Ali

    Nature communications (2018), 9 (1), 4305 ISSN:.

    There is a growing need for developing machine learning applications. However, implementation of the machine learning algorithm consumes a huge number of transistors or memory devices on-chip. Developing a machine learning capability in a single device has so far remained elusive. Here, we build a Markov chain algorithm in a single device based on the native oxide of two dimensional multilayer tin selenide. After probing the electrical transport in vertical tin oxide/tin selenide/tin oxide heterostructures, two sudden current jumps are observed during the set and reset processes. Furthermore, five filament states are observed. After classifying five filament states into three states of the Markov chain, the probabilities between each states show convergence values after multiple testing cycles. Based on this device, we demo a fixed-probability random number generator within 5% error rate. This work sheds light on a single device as one hardware core with Markov chain algorithm.

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11. 11

    Zhu, J.; Zhang, T.; Yang, Y.; Huang, R. A Comprehensive Review on Emerging Artificial Neuromorphic Devices. Appl. Phys. Rev. 2020, 7, 011312,  DOI: 10.1063/1.5118217

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    A comprehensive review on emerging artificial neuromorphic devices

    Zhu, Jiadi; Zhang, Teng; Yang, Yuchao; Huang, Ru

    Applied Physics Reviews (2020), 7 (1), 011312CODEN: APRPG5; ISSN:1931-9401. (American Institute of Physics)

    The rapid development of information technol. has led to urgent requirements for high efficiency and ultralow power consumption. In the past few decades, neuromorphic computing has drawn extensive attention due to its promising capability in processing massive data with extremely low power consumption. Here, we offer a comprehensive review on emerging artificial neuromorphic devices and their applications. In light of the inner phys. processes, we classify the devices into nine major categories and discuss their resp. strengths and weaknesses. We will show that anion/cation migration-based memristive devices, phase change, and spintronic synapses have been quite mature and possess excellent stability as a memory device, yet they still suffer from challenges in wt. updating linearity and symmetry. Meanwhile, the recently developed electrolyte-gated synaptic transistors have demonstrated outstanding energy efficiency, linearity, and symmetry, but their stability and scalability still need to be optimized. Other emerging synaptic structures, such as ferroelec., metal-insulator transition based, photonic, and purely electronic devices also have limitations in some aspects, therefore leading to the need for further developing high-performance synaptic devices. Addnl. efforts are also demanded to enhance the functionality of artificial neurons while maintaining a relatively low cost in area and power, and it will be of significance to explore the intrinsic neuronal stochasticity in computing and optimize their driving capability, etc. Finally, by looking into the correlations between the operation mechanisms, material systems, device structures, and performance, we provide clues to future material selections, device designs, and integrations for artificial synapses and neurons. (c) 2020 American Institute of Physics.

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12. 12

    Zhao, M.; Gao, B.; Tang, J.; Qian, H.; Wu, H. Reliability of Analog Resistive Switching Memory for Neuromorphic Computing Reliability of Analog Resistive Switching Memory for Neuromorphic Computing. Appl. Phys. Rev. 2020, 7, 011301,  DOI: 10.1063/1.5124915

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    12

    Reliability of analog resistive switching memory for neuromorphic computing

    Zhao, Meiran; Gao, Bin; Tang, Jianshi; Qian, He; Wu, Huaqiang

    Applied Physics Reviews (2020), 7 (1), 011301CODEN: APRPG5; ISSN:1931-9401. (American Institute of Physics)

    As artificial intelligence calls for novel energy-efficient hardware, neuromorphic computing systems based on analog resistive switching memory (RSM) devices have drawn great attention recently. Different from the well-studied binary RSMs, the analog RSMs are featured by a continuous and controllable conductance-tuning ability and thus are capable of combining analog computing and data storage at the device level. Although significant research achievements on analog RSMs have been accomplished, there have been few works demonstrating large-scale neuromorphic systems. A major bottleneck lies in the reliability issues of the analog RSM, such as endurance and retention degrdn. and read/write noises and disturbances. Owing to the complexity of resistive switching mechanisms, studies on the origins of reliability degrdn. and the corresponding optimization methodol. face many challenges. In this article, aiming on the high-performance neuromorphic computing applications, we provide a comprehensive review on the status of reliability studies of analog RSMs, the reliability requirements, and evaluation criteria and outlook for future reliability research directions in this field. (c) 2020 American Institute of Physics.

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13. 13

    Nili, H.; Adam, G. C.; Hoskins, B.; Prezioso, M.; Kim, J.; Mahmoodi, M. R.; Bayat, F. M.; Kavehei, O.; Strukov, D. B. Hardware-Intrinsic Security Primitives Enabled by Analogue State and Nonlinear Conductance Variations in Integrated Memristors. Nat. Electron. 2018, 1, 197– 202,  DOI: 10.1038/s41928-018-0039-7

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14. 14

    Oberoi, A.; Dodda, A.; Liu, H.; Terrones, M.; Das, S. Secure Electronics Enabled by Atomically Thin and Photosensitive Two-Dimensional Memtransistors. ACS Nano 2021, 15, 19815– 19827,  DOI: 10.1021/acsnano.1c07292

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    14

    Secure Electronics Enabled by Atomically Thin and Photosensitive Two-Dimensional Memtransistors

    Oberoi, Aaryan; Dodda, Akhil; Liu, He; Terrones, Mauricio; Das, Saptarshi

    ACS Nano (2021), 15 (12), 19815-19827CODEN: ANCAC3; ISSN:1936-0851. (American Chemical Society)

    The rapid proliferation of security compromised hardware in today's integrated circuit (IC) supply chain poses a global threat to the reliability of communication, computing, and control systems. While there have been significant advancements in detection and avoidance of security breaches, current top-down approaches are mostly inadequate, inefficient, often inconclusive, and resource extensive in time, energy, and cost, offering tremendous scope for innovation in this field. Here, we introduce an energy and area efficient non-von Neumann hardware platform providing comprehensive and bottom-up security solns. by exploiting inherent device-to-device variation, elec. programmability, and persistent photocond. demonstrated by atomically thin two-dimensional memtransistors. We realize diverse security primitives including phys. unclonable function, anticounterfeit measures, intellectual property (IP) watermarking, and IC camouflaging to prevent false authentication, detect recycled and remarked ICs, protect IP theft, and stop reverse engineering of ICs.

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    Wu, P.; Reis, D.; Hu, X. S.; Appenzeller, J. Two-Dimensional Transistors with Reconfigurable Polarities for Secure Circuits. Nat. Electron. 2021, 4, 45– 53,  DOI: 10.1038/s41928-020-00511-7

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    15

    Two-dimensional transistors with reconfigurable polarities for secure circuits

    Wu, Peng; Reis, Dayane; Hu, Xiaobo Sharon; Appenzeller, Joerg

    Nature Electronics (2021), 4 (1), 45-53CODEN: NEALB3; ISSN:2520-1131. (Nature Research)

    Security is a crit. aspect in modern circuit design, but research into hardware security at the device level is rare as it requires modification of existing technol. nodes. With the increasing challenges facing the semiconductor industry, interest in out-of-the-box security solns. has grown, even if this implies introducing novel materials such as two-dimensional layered semiconductors. Here, we show that high-performance, low-voltage, two-dimensional black phosphorus field-effect transistors (FETs) that have reconfigurable polarities are suitable for hardware security applications. The transistors can be dynamically switched between p-FET and n-FET operation through electrostatic gating and can achieve on-off ratios of 105 and subthreshold swings of 72 mV dec-1 at room temp. Using the transistors, we create inverters that exhibit gains of 33.3 and are fully functional at a supply voltage of 0.2 V. We also create a security primitive circuit with polymorphic NAND/NOR obfuscation functionality with sub-1-V operation voltages, and the robustness of the polymorphic gate against power supply variations is tested using Monte Carlo simulations.

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16. 16

    Das, S.; Wali, A.; Kundu, S.; Arnold, A. J.; Zhao, G.; Basu, K. Satisfiability Attack-Resistant Camouflaged Two-Dimensional Heterostructure Devices. ACS Nano 2021, 15, 3453– 3467,  DOI: 10.1021/acsnano.0c10651

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    16

    Satisfiability Attack-Resistant Camouflaged Two-Dimensional Heterostructure Devices

    Wali, Akshay; Kundu, Shamik; Arnold, Andrew J.; Zhao, Guangwei; Basu, Kanad; Das, Saptarshi

    ACS Nano (2021), 15 (2), 3453-3467CODEN: ANCAC3; ISSN:1936-0851. (American Chemical Society)

    Reverse engineering (RE) is one of the major security threats to the semiconductor industry due to the involvement of untrustworthy parties in an increasingly globalized chip manufg. supply chain. RE efforts have already been successful in extg. device level functionalities from an integrated circuit (IC) with very limited resources. Camouflaging is an obfuscation method that can thwart such RE. Existing work on IC camouflaging primarily involves transformable interconnects and/or covert gates where variation in doping and dummy contacts hide the circuit structure or build cells that look alike but have different functionalities. Emerging solns., such as polymorphic gates based on a giant spin Hall effect and Si nanowire field effect transistors (FETs), are also promising but add significant area overhead and are successfully decamouflaged by the satisfiability solver (SAT)-based RE techniques. Here, we harness the properties of two-dimensional (2D) transition-metal dichalcogenides (TMDs) including MoS2, MoSe2, MoTe2, WS2, and WSe2 and their optically transparent transition-metal oxides (TMOs) to demonstrate area efficient camouflaging solns. that are resilient to SAT attack and automatic test pattern generation attacks. We show that resistors with resistance values differing by 5 orders of magnitude, diodes with variable turn-on voltages and reverse satn. currents, and FETs with adjustable conduction type, threshold voltages, and switching characteristics can be optically camouflaged to look exactly similar by engineering TMO/TMD heterostructures, allowing hardware obfuscation of both digital and analog circuits. Since this 2D heterostructure devices family is intrinsically camouflaged, NAND/NOR/AND/OR gates in the circuit can be obfuscated with significantly less area overhead, allowing 100% logic obfuscation compared to only 5% for complementary metal oxide semiconductor (CMOS)-based camouflaging. Finally, we demonstrate that the largest benchmarking circuit from ISCAS'85, comprised of more than 4000 logic gates when obfuscated with the CMOS-based technique, is successfully decamouflaged by SAT attack in <40 min; whereas, it renders to be invulnerable even in more than 10 h when camouflaged with 2D heterostructure devices, thereby corroborating our hypothesis of high resilience against RE. Our approach of connecting material properties to innovative devices to secure circuits can be considered as a one of a kind demonstration, highlighting the benefits of cross-layer optimization.

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    Dodda, A.; Subbulakshmi Radhakrishnan, S.; Schranghamer, T. F.; Buzzell, D.; Sengupta, P.; Das, S. Graphene-Based Physically Unclonable Functions That Are Reconfigurable and Resilient to Machine Learning Attacks. Nat. Electron. 2021, 4, 364– 374,  DOI: 10.1038/s41928-021-00569-x

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    17

    Graphene-based physically unclonable functions that are reconfigurable and resilient to machine learning attacks

    Dodda, Akhil; Subbulakshmi Radhakrishnan, Shiva; Schranghamer, Thomas F.; Buzzell, Drew; Sengupta, Parijat; Das, Saptarshi

    Nature Electronics (2021), 4 (5), 364-374CODEN: NEALB3; ISSN:2520-1131. (Nature Portfolio)

    Abstr.: Graphene has a range of properties that makes it suitable for building devices for the Internet of Things. However, the deployment of such devices will also likely require the development of suitable graphene-based hardware security primitives. Here we report a phys. unclonable function (PUF) that exploits disorders in the carrier transport of graphene field-effect transistors. The Dirac voltage, Dirac conductance and carrier mobility values of a large population of graphene field-effect transistors follow Gaussian random distributions, which allow the devices to be used as a PUF. The resulting PUF is resilient to machine learning attacks based on predictive regression models and generative adversarial neural networks. The PUF is also reconfigurable without any phys. intervention and/or integration of addnl. hardware components due to the memristive properties of graphene. Furthermore, we show that the PUF can operate with ultralow power and is scalable, stable over time and reliable against variations in temp. and supply voltage.

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18. 18

    Wali, A.; Ravichandran, H.; Das, S. A Machine Learning Attack Resilient True Random Number Generator Based on Stochastic Programming of Atomically Thin Transistors. ACS Nano 2021, 15, 17804– 17812,  DOI: 10.1021/acsnano.1c05984

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    18

    A Machine Learning Attack Resilient True Random Number Generator Based on Stochastic Programming of Atomically Thin Transistors

    Wali, Akshay; Ravichandran, Harikrishnan; Das, Saptarshi

    ACS Nano (2021), 15 (11), 17804-17812CODEN: ANCAC3; ISSN:1936-0851. (American Chemical Society)

    A true random no. generator (TRNG) is a crit. hardware component that has become increasingly important in the era of Internet of Things (IoT) and mobile computing for ensuring secure communication and authentication schemes. While recent years have seen an upsurge in TRNGs based on nanoscale materials and devices, their resilience against machine learning (ML) attacks remains unexamd. In this article, we demonstrate a ML attack resilient, low-power, and low-cost TRNG by exploiting stochastic programmability of floating gate (FG) field effect transistors (FETs) with atomically thin channel materials. The origin of stochasticity is attributed to the probabilistic nature of charge trapping and detrapping phenomena in the FG. Our TRNG also satisfies other requirements, which include high entropy, uniformity, uniqueness, and unclonability. Furthermore, the generated bit-streams pass NIST randomness tests without any postprocessing. Our findings are important in the context of hardware security for resource constrained IoT edge devices, which are becoming increasingly vulnerable to ML attacks.

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19. 19

    Wen, C.; Li, X.; Zanotti, T.; Puglisi, F. M.; Shi, Y.; Saiz, F.; Antidormi, A.; Roche, S.; Zheng, W.; Liang, X.; Hu, J.; Duhm, S.; Roldan, J. B.; Wu, T.; Chen, V.; Pop, E.; Garrido, B.; Zhu, K.; Hui, F.; Lanza, M. Advanced Data Encryption Using 2D Materials. Adv. Mater. 2021, 33, 2100185,  DOI: 10.1002/adma.202100185

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    19

    Advanced Data Encryption using 2D Materials

    Wen, Chao; Li, Xuehua; Zanotti, Tommaso; Puglisi, Francesco Maria; Shi, Yuanyuan; Saiz, Fernan; Antidormi, Aleandro; Roche, Stephan; Zheng, Wenwen; Liang, Xianhu; Hu, Jiaxin; Duhm, Steffen; Roldan, Juan B.; Wu, Tianru; Chen, Victoria; Pop, Eric; Garrido, Blas; Zhu, Kaichen; Hui, Fei; Lanza, Mario

    Advanced Materials (Weinheim, Germany) (2021), 33 (27), 2100185CODEN: ADVMEW; ISSN:0935-9648. (Wiley-VCH Verlag GmbH & Co. KGaA)

    Advanced data encryption requires the use of true random no. generators (TRNGs) to produce unpredictable sequences of bits. TRNG circuits with high degree of randomness and low power consumption may be fabricated by using the random telegraph noise (RTN) current signals produced by polarized metal/insulator/metal (MIM) devices as entropy source. However, the RTN signals produced by MIM devices made of traditional insulators, i.e., transition metal oxides like HfO2 and Al2O3, are not stable enough due to the formation and lateral expansion of defect clusters, resulting in undesired current fluctuations and the disappearance of the RTN effect. Here, the fabrication of highly stable TRNG circuits with low power consumption, high degree of randomness (even for a long string of 224 - 1 bits), and high throughput of 1 Mbit s-1 by using MIM devices made of multilayer hexagonal boron nitride (h-BN) is shown. Their application is also demonstrated to produce one-time passwords, which is ideal for the internet-of-everything. The superior stability of the h-BN-based TRNG is related to the presence of few-atoms-wide defects embedded within the layered and cryst. structure of the h-BN stack, which produces a confinement effect that avoids their lateral expansion and results in stable operation.

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20. 20

    Li, T.; Peng, H. 2D Bi₂O₂Se: An Emerging Material Platform for the Next-Generation Electronic Industry. Accounts Mater. Res. 2021, 2, 842– 853,  DOI: 10.1021/accountsmr.1c00130

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    2D Bi2O2Se: An Emerging Material Platform for the Next-Generation Electronic Industry

    Li, Tianran; Peng, Hailin

    Accounts of Materials Research (2021), 2 (9), 842-853CODEN: AMRCDA; ISSN:2643-6728. (American Chemical Society)

    A review. Conspectus: Silicon has been the dominant semiconductor for the microelectronics industry since the late 1950s. Following Moore's law, silicon-based integrated circuit (IC) technol. evolved into a 5 nm node by the end of 2020. However, silicon-based electronics face various challenges such as reduced carrier mobility and increased short-channel effects at sub-10 nm nodes. To overcome these drawbacks, two-dimensional (2D) semiconductors are among the most competitive candidate materials for next-generation electronics, due to their intrinsic at. thickness, flexibility, and dangling-bond-free surfaces. Among all the 2D semiconductors, an air-stable and high-mobility 2D Bi2O2Se semiconductor, a novel ternary material, has some prominent advantages that make it particularly favorable in the electronics industry. First, it demonstrates ultrahigh carrier mobility, moderate band gap, outstanding stability, and excellent mech. properties. Second, it can react with oxygen plasma or oxygen at elevated temps. to form a high-κ native oxide Bi2SeO5. The native oxide Bi2SeO5 forms an atomically sharp interface with Bi2O2Se and can directly serve as a gate dielec. Bi2O2Se is also embodied with some interesting phys. properties such as strong spin-orbit coupling, dimerized selenium vacancies, and ferroelectricity. Taking advantage of these properties, researchers have fabricated high-performance electronic devices, including logic devices, optoelectronics, thermoelecs., sensors, and memory devices. In this account, we will systematically the structure of 2D Bi2O2Se, including its crystal structure, surface structure, point defects, and electronic band structure and how these structures can affect the electron transport in 2D Bi2O2Se. We will then discuss different approaches to synthesize this material including chem. vapor deposition (CVD), metal-org. chem. vapor deposition (MOCVD), mol. beam epitaxy (MBE), and the soln.-assisted method. All these methods show great potential in large-scale prodn. Third, we will discuss how the structure of Bi2O2Se affects its chem. and phys. properties such as chem. reactivity and ferroelec., piezoelec., and electromech. properties. Fourth, we will talk about how to make use of these properties in electronic devices, including field-effect transistors, logic gates, bolometers, photodetectors, thermoelecs., piezoelecs., sensors, and memory devices. Finally, we will put forward our idea on how to pattern large-area Bi2O2Se thin films into isolated channel regions and integrate these devices together into full-functioning circuits. We believe that 2D Bi2O2Se is a promising semiconductor, as a great diversity of high-performance 2D Bi2O2Se-based devices have demonstrated. Hopefully, the unique characteristics of 2D Bi2O2Se can provide addnl. opportunities to complement or replace silicon as the material platform of the next-generation electronics industry. To fill the gap between dreams and reality, there is still much work to be done, esp. in large-scale material synthesis and systematic device integration.

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21. 21

    Wu, J.; Yuan, H.; Meng, M.; Chen, C.; Sun, Y.; Chen, Z.; Dang, W.; Tan, C.; Liu, Y.; Yin, J.; Zhou, Y.; Huang, S.; Xu, H. Q.; Cui, Y.; Hwang, H. Y.; Liu, Z.; Chen, Y.; Yan, B.; Peng, H. High Electron Mobility and Quantum Oscillations in Non-Encapsulated Ultrathin Semiconducting Bi₂O₂Se. Nat. Nanotechnol. 2017, 12, 530– 534,  DOI: 10.1038/nnano.2017.43

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    21

    High electron mobility and quantum oscillations in non-encapsulated ultrathin semiconducting Bi2O2Se

    Wu, Jinxiong; Yuan, Hongtao; Meng, Mengmeng; Chen, Cheng; Sun, Yan; Chen, Zhuoyu; Dang, Wenhui; Tan, Congwei; Liu, Yujing; Yin, Jianbo; Zhou, Yubing; Huang, Shaoyun; Xu, H. Q.; Cui, Yi; Hwang, Harold Y.; Liu, Zhongfan; Chen, Yulin; Yan, Binghai; Peng, Hailin

    Nature Nanotechnology (2017), 12 (6), 530-534CODEN: NNAABX; ISSN:1748-3387. (Nature Publishing Group)

    High-mobility semiconducting ultrathin films form the basis of modern electronics, and may lead to the scalable fabrication of highly performing devices. Because the ultrathin limit cannot be reached for traditional semiconductors, identifying new 2-dimensional materials with both high carrier mobility and a large electronic band gap is a pivotal goal of fundamental research. However, air-stable ultrathin semiconducting materials with superior performances remain elusive at present. Here, the authors report ultrathin films of non-encapsulated layered Bi2O2Se, grown by chem. vapor deposition, which demonstrate excellent air stability and high-mobility semiconducting behavior. The authors observe band gap values of ∼0.8 eV, which are strongly dependent on the film thickness due to quantum-confinement effects. An ultrahigh Hall mobility value of >20,000 cm2 V-1 s-1 is measured in as-grown Bi2O2Se nanoflakes at low temps. This value is comparable to what is obsd. in graphene grown by chem. vapor deposition and at the LaAlO3-SrTiO3 interface, making the detection of Shubnikov-de Haas quantum oscillations possible. Top-gated field-effect transistors based on Bi2O2Se crystals down to the bilayer limit exhibit high Hall mobility values (up to 450 cm2 V-1 s-1), large current on/off ratios (>106) and near-ideal subthreshold swing values (∼65 mV dec-1) at room temp. The results make Bi2O2Se a promising candidate for future high-speed and low-power electronic applications.

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22. 22

    Sun, Y.; Zhang, J.; Ye, S.; Song, J.; Qu, J. Progress Report on Property, Preparation, and Application of Bi₂O₂Se. Adv. Funct. Mater. 2020, 30, 2004480,  DOI: 10.1002/adfm.202004480

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    22

    Progress Report on Property, Preparation, and Application of Bi2O2Se

    Sun, Yuan; Zhang, Jing; Ye, Shuai; Song, Jun; Qu, Junle

    Advanced Functional Materials (2020), 30 (49), 2004480CODEN: AFMDC6; ISSN:1616-301X. (Wiley-VCH Verlag GmbH & Co. KGaA)

    A review. The study of 2D materials has been a significant and fascinating area, at least since the discovery of graphene. As one of the layered bismuth oxychalcogenides, bismuth oxyselenide (Bi2O2Se) has drawn a lot of attention recently. The study of Bi2O2Se was mainly focused on its thermoelec. performance until its ultrathin 2D structure came to the fore. New phys. properties of Bi2O2Se were discovered along with the successful synthesis of 2D Bi2O2Se structures. Few-layer Bi2O2Se exhibits ultrahigh mobility, outstanding stability, tunable bandgaps, and excellent mech. properties, showing remarkable performance in electronics and optoelectronics. In this report, an overview of recent advances in Bi2O2Se research is provided, including structure/property modifications, synthetic methods, and practical applications. Theor. and exptl. results on bulk/few-layer Bi2O2Se are both discussed in this report. Finally, the challenges and outlook for Bi2O2Se are evaluated based on current progress.

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23. 23

    Liu, B.; Zhao, Y.; Verma, D.; Wang, L. A.; Liang, H.; Zhu, H.; Li, L. J.; Hou, T. H.; Lai, C. S. Bi₂O₂Se-Based Memristor-Aided Logic. ACS Appl. Mater. Interfaces 2021, 13, 15391– 15398,  DOI: 10.1021/acsami.1c00177

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    23

    Bi2O2Se-Based Memristor-Aided Logic

    Liu, Bo; Zhao, Yudi; Verma, Dharmendra; Wang, Le An; Liang, Hanyuan; Zhu, Hui; Li, Lain-Jong; Hou, Tuo-Hung; Lai, Chao-Sung

    ACS Applied Materials & Interfaces (2021), 13 (13), 15391-15398CODEN: AAMICK; ISSN:1944-8244. (American Chemical Society)

    The implementation of two-dimensional materials into memristor architectures has recently been a new research focus by taking advantage of their at. thickness, unique lattice, and phys. and electronic properties. Among the van der Waals family, Bi2O2Se is an emerging ternary two-dimensional layered material with ambient stability, suitable band structure, and high cond. that exhibits high potential for use in electronic applications. In this work, we propose and exptl. demonstrate a Bi2O2Se-based memristor-aided logic. By carefully tuning the elec. field polarity of Bi2O2Se through a Pd contact, a reconfigurable NAND gate with zero static power consumption is realized. To provide more knowledge on NAND operation, a kinetic Monte Carlo simulation is carried out. Because the NAND gate is a universal logic gate, cascading addnl. NAND gates can exhibit versatile logic functions. Therefore, the proposed Bi2O2Se-based MAGIC can be a promising building block for developing next-generation in-memory logic computers with multiple functions.

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24. 24

    Chen, W.; Zhang, R.; Zheng, R.; Liu, B. Out-of-Plane Resistance Switching of 2D Bi₂O₂Se at the Nanoscale. Adv. Funct. Mater. 2021, 31, 2105795,  DOI: 10.1002/adfm.202105795

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    24

    Out-of-Plane Resistance Switching of 2D Bi2O2Se at the Nanoscale

    Chen, Wenjun; Zhang, Rongjie; Zheng, Rongxu; Liu, Bilu

    Advanced Functional Materials (2021), 31 (52), 2105795CODEN: AFMDC6; ISSN:1616-301X. (Wiley-VCH Verlag GmbH & Co. KGaA)

    Two-dimensional (2D) bismuth oxyselenide (Bi2O2Se) with high electron mobility shows great potential for nanoelectronics. Although the in-plane properties of Bi2O2Se have been widely studied, its out-of-plane elec. transport behavior remains elusive, despite its importance in fabricating devices with new functionality and high integration d. Here, the out-of-plane elec. properties of 2D Bi2O2Se at nanoscale are revealed by conductive at. force microscope. This work finds that hillocks with tunable heights and sizes are formed on Bi2O2Se after applying a vertical elec. field. Intriguingly, such hillocks are conductive in the vertical direction, resulting in a previously unknown out-of-plane resistance switching in thick Bi2O2Se flakes while ohmic conductive characteristic in thin ones. Furthermore, the transformation is obsd. from bipolar to stable unipolar conduction in thick Bi2O2Se flake possessing such hillocks, suggesting its potential to function as a selector in vertical devices. This work reveals the unique out-of-plane transport behavior of 2D Bi2O2Se, providing the basis for fabricating vertical devices based on this emerging 2D material.

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25. 25

    Yang, F.; Wu, J.; Suwardi, A.; Zhao, Y.; Liang, B.; Jiang, J.; Xu, J.; Chi, D.; Hippalgaonkar, K.; Lu, J. Gate-Tunable Polar Optical Phonon to Piezoelectric Scattering in Few-Layer Bi₂O₂Se for High-Performance Thermoelectrics. Adv. Mater. 2021, 33, 2004786,  DOI: 10.1002/adma.202004786

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    25

    Gate-Tunable Polar Optical Phonon to Piezoelectric Scattering in Few-Layer Bi2O2Se for High-Performance Thermoelectrics

    Yang, Fang; Wu, Jing; Suwardi, Ady; Zhao, Yunshan; Liang, Boyuan; Jiang, Jie; Xu, Jianwei; Chi, Dongzhi; Hippalgaonkar, Kedar; Lu, Junpeng; Ni, Zhenhua

    Advanced Materials (Weinheim, Germany) (2021), 33 (4), 2004786CODEN: ADVMEW; ISSN:0935-9648. (Wiley-VCH Verlag GmbH & Co. KGaA)

    Atomically thin Bi2O2Se has emerged as a new member in 2D materials with ultrahigh carrier mobility and excellent air-stability, showing great potential for electronics and optoelectronics. In addn., its ferroelec. nature renders an ultralow thermal cond., making it a perfect candidate for thermoelecs. In this work, the thermoelec. performance of 2D Bi2O2Se is investigated over a wide temp. range (20-300 K). A gate-tunable transition from polar optical phonon (POP) scattering to piezoelec. scattering is obsd., which facilitates the capacity of drastic mobility engineering in 2D Bi2O2Se. Consequently, a high power factor of more than 400μW m-1 K-2 over an unprecedented temp. range (80-200 K) is achieved, corresponding to the persistently high mobility arising from the highly gate-tunable scattering mechanism. This finding provides a new avenue for maximizing thermoelec. performance by changing the scattering mechanism and carrier mobility over a wide temp. range.

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26. 26

    Diffie, W.; Hellman, M. New Directions in Croptography. IEEE Trans. Inf. Theory 1976, 22, 644– 654,  DOI: 10.1109/TIT.1976.1055638

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    There is no corresponding record for this reference.
27. 27

    Simon, D. K.; Jordan, P. M.; Mikolajick, T.; Dirnstorfer, I. On the Control of the Fixed Charge Densities in Al₂O₃-Based Silicon Surface Passivation Schemes. ACS Appl. Mater. Interfaces 2015, 7, 28215– 28222,  DOI: 10.1021/acsami.5b06606

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    27

    On the Control of the Fixed Charge Densities in Al2O3-Based Silicon Surface Passivation Schemes

    Simon, Daniel K.; Jordan, Paul M.; Mikolajick, Thomas; Dirnstorfer, Ingo

    ACS Applied Materials & Interfaces (2015), 7 (51), 28215-28222CODEN: AAMICK; ISSN:1944-8244. (American Chemical Society)

    A controlled field-effect passivation by a well-defined d. of fixed charges is crucial for modern solar cell surface passivation schemes. Al2O3 nanolayers grown by at. layer deposition contain neg. fixed charges. Elec. measurements on slant-etched layers reveal that these charges are located within a 1. nm distance to the interface with the Si substrate. When inserting addnl. interface layers, the fixed charge d. can be continuously adjusted from 3.5 × 1012 cm-2 (neg. polarity) to 0.0 and up to 4.0 × 1012 cm-2 (pos. polarity). A HfO2 interface layer of one or more monolayers reduces the neg. fixed charges in Al2O3 to zero. The role of HfO2 is described as an inert spacer controlling the distance between Al2O3 and the Si substrate. Probably this spacer alters the nonstoichiometric initial Al2O3 growth regime, which is responsible for the charge formation. From this charge-free HfO2/Al2O3 stack, neg. or pos. fixed charges can be formed by introducing addnl. thin Al2O3 or SiO2 layers between the Si substrate and this HfO2/Al2O3 capping layer. All stacks provide very good passivation of the silicon surface. The measured effective carrier lifetimes are 1-30 ms. This charge control in Al2O3 nanolayers allows the construction of zero-fixed-charge passivation layers as well as layers with tailored fixed charge densities for future solar cell concepts and other field-effect based devices.

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28. 28

    Yang, C.; Chen, T.; Verma, D.; Li, L.; Liu, B.; Chang, W.; Lai, C. Bidirectional All-Optical Synapses Based on a 2D Bi₂O₂Se/Graphene Hybrid Structure for Multifunctional Optoelectronics. Adv. Funct. Mater. 2020, 30, 2001598,  DOI: 10.1002/adfm.202001598

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    28

    Bidirectional All-Optical Synapses Based on a 2D Bi2O2Se/Graphene Hybrid Structure for Multifunctional Optoelectronics

    Yang, Chia-Ming; Chen, Tsung-Cheng; Verma, Dharmendra; Li, Lain-Jong; Liu, Bo; Chang, Wen-Hao; Lai, Chao-Sung

    Advanced Functional Materials (2020), 30 (30), 2001598CODEN: AFMDC6; ISSN:1616-301X. (Wiley-VCH Verlag GmbH & Co. KGaA)

    Neuromorphic computing has been extensively studied to mimic the brain functions of perception, learning, and memory because it may overcome the von Neumann bottleneck. Here, with the light-induced bidirectional photoresponse of the proposed Bi2O2Se/graphene hybrid structure, its potential use in next-generation neuromorphic hardware is examd. with three distinct optoelectronic applications. First, a photodetector based on a Bi2O2Se/graphene hybrid structure presents pos. and neg. photoresponsibility of 88 and -110 A W-1 achieved by the excitation of visible wavelength and UV wavelength light at intensities of 1.2 and 0.3 mW cm-2, resp. Second, this unique photoresponse contributes to the realization of all optically stimulated long-term potentiation or long-term depression to mimic synaptic short-term plasticity and long-term plasticity, which are attributed to the combined effect of photocond., bolometric, and photoinduced desorption. Third, the devices are applied to perform digital logic functions, such as "AND" and "OR," using full light modulation. The proposed Bi2O2Se/graphene-based optoelectronic device represents an innovative and efficient building block for the development of future multifunctional artificial neuromorphic systems.

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29. 29

    Stampfer, B.; Zhang, F.; Illarionov, Y. Y.; Knobloch, T.; Wu, P.; Waltl, M.; Grill, A.; Appenzeller, J.; Grasser, T. Characterization of Single Defects in Ultrascaled MoS₂ Field-Effect Transistors. ACS Nano 2018, 12, 5368– 5375,  DOI: 10.1021/acsnano.8b00268

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    29

    Characterization of single defects in ultrascaled MoS2 field-effect transistors

    Stampfer, Bernhard; Zhang, Feng; Illarionov, Yury Yuryevich; Knobloch, Theresia; Wu, Peng; Waltl, Michael; Grill, Alexander; Appenzeller, Joerg; Grasser, Tibor

    ACS Nano (2018), 12 (6), 5368-5375CODEN: ANCAC3; ISSN:1936-0851. (American Chemical Society)

    MoS2 has received a lot of attention lately as a semiconducting channel material for electronic devices, in part due to its large band gap as compared to that of other 2D materials. Yet, the performance and reliability of these devices are still severely limited by defects which act as traps for charge carriers, causing severely reduced mobilities, hysteresis, and long-term drift. Despite their importance, these defects are only poorly understood. One fundamental problem in defect characterization is that due to the large defect concn. only the av. response to bias changes can be measured. On the basis of such averaged data, a detailed anal. of their properties and identification of particular defect types are difficult. To overcome this limitation, we here characterize single defects on MoS2 devices by performing measurements on ultrascaled transistors (∼65 × 50 nm) which contain only a few defects. These single defects are characterized elec. at varying gate biases and temps. The measured currents contain random telegraph noise, which is due to the transfer of charge between the channel of the transistors and individual defects, visible only due to the large impact of a single elementary charge on the local electrostatics in these small devices. Using hidden Markov models for statistical anal., we ext. the charge capture and emission times of a no. of defects. By comparing the bias-dependence of the measured capture and emission times to the prediction of theor. models, we provide simple rules to distinguish oxide traps from adsorbates on these back-gated devices. In addn., we give simple expressions to est. the vertical and energetic positions of the defects. Using the methods presented in this work, it is possible to locate the sources of performance and reliability limitations in 2D devices and to probe defect distributions in oxide materials with 2D channel materials.

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30. 30

    Huang, P.; Zhu, D. B.; Liu, C.; Zhou, Z.; Dong, Z.; Jiang, H.; Shen, W. S.; Liu, L. F.; Liu, X. Y.; Kang, J. F. RTN Based Oxygen Vacancy Probing Method for Ox-RRAM Reliability Characterization and Its Application in Tail Bits. In Technical Digest - International Electron Devices Meeting, IEDM 2017, 17507985,  DOI: 10.1109/IEDM.2017.8268435

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    There is no corresponding record for this reference.
31. 31

    Illarionov, Y. Y.; Knobloch, T.; Jech, M.; Lanza, M.; Akinwande, D.; Vexler, M. I.; Mueller, T.; Lemme, M. C.; Fiori, G.; Schwierz, F.; Grasser, T. Insulators for 2D Nanoelectronics: The Gap to Bridge. Nat. Commun. 2020, 11, 3385,  DOI: 10.1038/s41467-020-16640-8

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    31

    Insulators for 2D nanoelectronics: the gap to bridge

    Illarionov, Yury Yu.; Knobloch, Theresia; Jech, Markus; Lanza, Mario; Akinwande, Deji; Vexler, Mikhail I.; Mueller, Thomas; Lemme, Max C.; Fiori, Gianluca; Schwierz, Frank; Grasser, Tibor

    Nature Communications (2020), 11 (1), 3385CODEN: NCAOBW; ISSN:2041-1723. (Nature Research)

    A review. Abstr.: Nanoelectronic devices based on 2D materials are far from delivering their full theor. performance potential due to the lack of scalable insulators. Amorphous oxides that work well in silicon technol. have ill-defined interfaces with 2D materials and numerous defects, while 2D hexagonal boron nitride does not meet required dielec. specifications. The list of suitable alternative insulators is currently very limited. Thus, a radically different mindset with respect to suitable insulators for 2D technologies may be required. We review possible soln. scenarios like the creation of clean interfaces, prodn. of native oxides from 2D semiconductors and more intensive studies on cryst. insulators.

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32. 32

    Illarionov, Y. Y.; Knobloch, T.; Waltl, M.; Rzepa, G.; Pospischil, A.; Polyushkin, D. K.; Furchi, M. M.; Mueller, T.; Grasser, T. Energetic Mapping of Oxide Traps in MoS₂ Field-Effect Transistors. 2D Mater. 2017, 4, 025108,  DOI: 10.1088/2053-1583/aa734a

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    32

    Energetic mapping of oxide traps in MoS2 field-effect transistors

    Illarionov, Yury Yu; Knobloch, Theresia; Waltl, Michael; Rzepa, Gerhard; Pospischil, Andreas; Polyushkin, Dmitry K.; Furchi, Marco M.; Mueller, Thomas; Grasser, Tibor

    2D Materials (2017), 4 (2), 025108/1-025108/10CODEN: DMATB7; ISSN:2053-1583. (IOP Publishing Ltd.)

    The performance of MoS2 transistors is strongly affected by charge trapping in oxide traps with very broad distributions of time consts. These defects degrade the mobility and addnl. lead to the hysteresis of the gate transfer characteristics, which presents a crucial performance and reliability issue for these new technologies. Here we perform a detailed study of the hysteresis in double-gated MoS2 FETs and show that this issue is nothing else than a combination of threshold voltage shifts resulting from pos. and neg. bias-temp. instabilities. While these instabilities are well known from silicon devices, they are even more important in 2D devices given the considerably larger defect densities. Most importantly, the magnitudes of these threshold voltage shifts depend strongly on the d. and energetic alignment of the active oxide traps. Based on this, we introduce the incremental hysteresis sweep method which allows for an accurate mapping of these defects and ext. their energy distributions from simulations. By applying our method to analyze the impact of oxide traps situated in the Al2O3 top gate of several devices, we confirm its versatility. Since all 2D devices investigated so far suffer from a similar hysteresis behavior, the incremental hysteresis sweep method provides a unique and powerful way for the detailed characterization of their defect bands.

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33. 33

    Degraeve, R.; Cho, M.; Govoreanu, B.; Kaczer, B.; Zahid, M. B.; Van Houdt, J.; Jurczak, M.; Groeseneken, G. Trap Spectroscopy by Charge Injection and Sensing (TSCIS): A Quantitative Electrical Technique for Studying Defects in Dielectric Stacks. Technol. Dig. - Int. Electron Devices Meet. IEDM 2008, 10479653,  DOI: 10.1109/IEDM.2008.4796812

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    There is no corresponding record for this reference.
34. 34

    Choi, S.; Yang, Y.; Lu, W. Random Telegraph Noise and Resistance Switching Analysis of Oxide Based Resistive Memory. Nanoscale 2014, 6, 400– 404,  DOI: 10.1039/C3NR05016E

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    34

    Random telegraph noise and resistance switching analysis of oxide based resistive memory

    Choi, Shinhyun; Yang, Yuchao; Lu, Wei

    Nanoscale (2014), 6 (1), 400-404CODEN: NANOHL; ISSN:2040-3372. (Royal Society of Chemistry)

    Resistive random access memory (RRAM) devices (e.g. "memristors") are widely believed to be a promising candidate for future memory and logic applications. Although excellent performance has been reported, the nature of resistance switching is still under extensive debate. In this study, we perform systematic investigation of the resistance switching mechanism in a TaOx based RRAM through detailed noise anal., and show that the resistance switching from high-resistance to low-resistance is accompanied by a semiconductor-to-metal transition mediated by the accumulation of oxygen-vacancies in the conduction path. Specifically, pronounced random-telegraph noise (RTN) with values up to 25% was obsd. in the device high-resistance state (HRS) but not in the low-resistance state (LRS). Through time-domain and temp. dependent anal., we show that the RTN effect shares the same origin as the resistive switching effects, and both can be traced to the (re)distribution of oxygen vacancies (VOs). From noise and transport anal. we further obtained the d. of states and av. distance of the VOs at different resistance states, and developed a unified model to explain the conduction in both the HRS and the LRS and account for the resistance switching effects in these devices. Significantly, it was found that even though the conduction channel area is larger in the HRS, during resistive switching a localized region gains significantly higher VO and dominates the conduction process. These findings reveal the complex dynamics involved during resistive switching and will help guide continued optimization in the design and operation of this important emerging device class.

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35. 35

    Song, Y.; Wu, Q.; Wang, X.; Wang, C.; Miao, X. Two Memristors-Based XOR Logic Demonstrated with Encryption/Decryption. IEEE Electron Device Lett. 2021, 42, 1398– 1401,  DOI: 10.1109/LED.2021.3102678

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    35

    Two memristors-based XOR logic demonstrated with encryption/decryption

    Song, Yujie; Wu, Qiwen; Wang, Xingsheng; Wang, Chengxu; Miao, Xiangshui

    IEEE Electron Device Letters (2021), 42 (9), 1398-1401CODEN: EDLEDZ; ISSN:1558-0563. (Institute of Electrical and Electronics Engineers)

    In this study, an optimized XOR logic gate is briefly proposed based on memristors. The proposed XOR exhibits a simple structure that comprises two memristors; it requires merely two steps to complete logic. The inputs of the gate are applied by voltage and memristive resistance, and the output is stored as the resistance value of the output cell. Furthermore, the encryption and decryption based on such a circuit have been verified by performing a parallel elec. test successfully. At the same time, the parallel scheme and the cascaded serial scheme are compared in detail. Moreover, the mentioned energy-efficient circuit helps achieve more complex logic functions. Abiding by Kirchhoff's law, the effect of the memory window and the variation of devices' parameter on the calcn. accuracy has been further analyzed in depth, which helps develop a complete binary logic calcn. theory. On that basis, a digital in-memory calcn. system can be more effectively built based on memristors.

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36. 36

    Li, X.; Zanotti, T.; Wang, T.; Zhu, K.; Puglisi, F. M.; Lanza, M. Random Telegraph Noise in Metal-Oxide Memristors for True Random Number Generators: A Materials Study. Adv. Funct. Mater. 2021, 31, 2102172,  DOI: 10.1002/adfm.202102172

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    36

    Random Telegraph Noise in Metal-Oxide Memristors for True Random Number Generators: A Materials Study

    Li, Xuehua; Zanotti, Tommaso; Wang, Tao; Zhu, Kaichen; Puglisi, Francesco Maria; Lanza, Mario

    Advanced Functional Materials (2021), 31 (27), 2102172CODEN: AFMDC6; ISSN:1616-301X. (Wiley-VCH Verlag GmbH & Co. KGaA)

    Some memristors with metal/insulator/metal (MIM) structure have exhibited random telegraph noise (RTN) current signals, which makes them ideal to build true random no. generators (TRNG) for advanced data encryption. However, there is still no clear guide on how essential manufg. parameters like materials selection, thicknesses, deposition methods, and device lateral size can influence the quality of the RTN signal. In this paper, an exhaustive statistical anal. on the quality of the RTN signals produced by different MIM-like memristors is reported, and straightforward guidelines for the fabrication of memristors with enhanced RTN performance are presented, which are: i. Ni and Ti electrodes show better RTN than Au electrodes, ii. the 50μm × 50μm devices show better RTN than the 5μm × 5μm ones, iii. TiO2 shows better RTN than HfO2 and Al2O3, iv. sputtered-oxides show better RTN than ALD-oxides, and v. 10 nm thick oxides show better RTN than 5 nm thick oxides. The RTN signals recorded have been used as entropy sources in high-throughput TRNG circuits, which have passed the randomness tests of the National Institute of Stds. and Technol. The work can serve as a useful guide for materials scientists and electronic engineers when fabricating MIM-like memristors for RTN applications.

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37. 37

    González-Cordero, G.; González, M. B.; Morell, A.; Jiménez-Molinos, F.; Campabadal, F.; Roldán, J. B. Neural Network Based Analysis of Random Telegraph Noise in Resistive Random Access Memories. Semicond. Sci. Technol. 2020, 35, 25021,  DOI: 10.1088/1361-6641/ab6103

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    37

    Neural network based analysis of random telegraph noise in resistive random access memories

    Gonzalez-Cordero, G.; Gonzalez, M. B.; Morell, A.; Jimenez-Molinos, F.; Campabadal, F.; Roldan, J. B.

    Semiconductor Science and Technology (2020), 35 (2), 025021CODEN: SSTEET; ISSN:0268-1242. (IOP Publishing Ltd.)

    The characterization of random telegraph noise (RTN) signals in resistive random access memories (RRAM) is a challenge. The inherent stochastic operation of these devices, makes this issue more complicated from the math. viewpoint. Nevertheless, the accurate modeling of these type of signals is essential for their use in digital and analog applications. RTN signals are revealed to be linked to the emission and capture of electrons by traps close to the conductive filament that can influence resistive switching operation in RRAMs. RTN features depend on the no. of active traps, on the interaction between these traps at different times, on the occurrence of anomalous effects, etc Using a new representation technique, the locally weighted time lag plot (LWTLP), a highly efficient method in terms of computation, data from current-time (I-t) traces can be represented with a pattern that allows the anal. of important RTN signal features. In addn., self-organizing maps, a neural network devoted to clustering, can be employed to perform an automatic classification of the RTN traces that have similar LWTLP patterns. This pattern anal. allows a better understanding of RTN signals and the physics underlying them. The new technique presented can be performed in a reasonable computing time and it is particularly adequate for long (I-t) traces. We introduce here this technique and the most important results that can be drawn when applied to long RTN traces exptl. obtained in RRAMs.

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38. 38

    González-Cordero, G.; González, M. B.; Zabala, M.; Kalam, K.; Tamm, A.; Jiménez-Molinos, F.; Campabadal, F.; Roldán, J. B. Study of RTN Signals in Resistive Switching Devices Based on Neural Networks. Solid. State. Electron. 2021, 183, 108034,  DOI: 10.1016/j.sse.2021.108034

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    38

    Study of RTN signals in resistive switching devices based on neural networks

    Gonzalez-Cordero, G.; Gonzalez, M. B.; Zabala, M.; Kalam, K.; Tamm, A.; Jimenez-Molinos, F.; Campabadal, F.; Roldan, J. B.

    Solid-State Electronics (2021), 183 (), 108034CODEN: SSELA5; ISSN:0038-1101. (Elsevier Ltd.)

    Random Telegraph Noise (RTN) in Resistive Random Access Memories (RRAM) is an important phenomenon both for the investigation of device physics and for reliability issues. The characteristics of these signals depend on the no. of active traps, on the interaction between these traps at different times, on the occurrence of anomalous effects, etc. Using the Locally Weighted Time Lag Plot (LWTLP), a fast numerical procedure, data from RTN current-time (I-t) traces can be represented with a pattern that allows a deeper understanding of the device physics. In the context of self-organizing maps, a neural network devoted to clustering, we have analyzed the LWTLPs to classify the RTN traces obtained from a long measurement with more than 3 million data points. This RTN pattern classification, obtained in an unsupervised learning scheme, allows a comprehensive characterization of the signals and the physics underlying the device operation.

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39. 39

    Pang, Y.; Yang, Z.; Yang, Y.; Ren, T. Wearable Electronics Based on 2D Materials for Human Physiological Information Detection. small 2020, 16, 1901124,  DOI: 10.1002/smll.201901124

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    Wearable Electronics Based on 2D Materials for Human Physiological Information Detection

    Pang, Yu; Yang, Zhen; Yang, Yi; Ren, Tian-Ling

    Small (2020), 16 (15), 1901124CODEN: SMALBC; ISSN:1613-6810. (Wiley-VCH Verlag GmbH & Co. KGaA)

    A review. Recently, advancement in materials prodn., device fabrication, and flexible circuit has led to the huge prosperity of wearable electronics for human health care monitoring and medical diagnosis. Particularly, with the emergence of 2D materials many merits including light wt., high stretchability, excellent biocompatibility, and high performance are used for those potential applications. Thus, it is urgent to review the wearable electronics based on 2D materials for the detection of various human signals. In this work, the typical graphene-based materials, transition-metal dichalcogenides, and transition metal carbides or carbonitrides used for the wearable electronics are discussed. To well understand the human physiol. information, it is divided into two dominated categories, namely, the human phys. and the human chem. signals. The monitoring of body temp., electrograms, subtle signals, and limb motions is described for the phys. signals while the detection of body fluid including sweat, breathing gas, and saliva is reviewed for the chem. signals. Recent progress and development toward those specific utilizations are highlighted in the Review with the representative examples. The future outlook of wearable health care techniques is briefly discussed for their commercialization.

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40. 40

    Wei, Y.; Li, X.; Wang, Y.; Hirtz, T.; Guo, Z.; Qiao, Y.; Cui, T.; Tian, H.; Yang, Y.; Ren, T. Graphene-Based Multifunctional Textile for Sensing and Actuating. ACS Nano 2021, 15, 17738– 17747,  DOI: 10.1021/acsnano.1c05701

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    40

    Graphene-Based Multifunctional Textile for Sensing and Actuating

    Wei, Yuhong; Li, Xiaoshi; Wang, Yunfan; Hirtz, Thomas; Guo, Zhanfeng; Qiao, Yancong; Cui, Tianrui; Tian, He; Yang, Yi; Ren, Tian-Ling

    ACS Nano (2021), 15 (11), 17738-17747CODEN: ANCAC3; ISSN:1936-0851. (American Chemical Society)

    Textiles are materials that are extensively used in everyday life; textile-based sensors can, therefore, be regarded as ideal devices for a health monitor. However, previously reported textile sensors have limited prospects due to their single function or incompatibility. Traditional textile sensors generally focus on signal detection, which has not been able to be combined with an actuator to provide real-time health status feedback. Thus, to date, there are no well-established health monitoring systems based on intelligent textiles. Herein, we present a wearable batch-prepd. graphene-based textile based on laser-scribing and thermal-transfer technol. Integrated with four functions of strain sensing, pressure sensing, physiol. elec. sensing, and sound emitting, the GT is able to detect human body signals and transduce them to sound signals when the user is in an abnormal phys. state. Moreover, the GT has high linearity for both strain and pressure sensing; the coeffs. of detn. exceed 99.3% and 98.2%, resp. The performance of the device remains stable up to a pressure of 1000 kPa. The response time of the GT possession reaches as low as 85 ms at 4.2 Pa pressure. Therefore, due to their diversified functions and good performance, the research on GT is expected to extend to the fields of health monitoring, sports monitoring, and so forth.

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41. 41

    Liu, B.; Tai, H. H.; Liang, H.; Zheng, E.-Y.; Sahoo, M.; Hsu, C. H.; Chen, T.-C.; Huang, C. A.; Wang, J.-C.; Hou, T.-H.; Lai, C. S. Dimensionally Anisotropic Graphene with High Mobility and a High on-off Ratio in a Three-Terminal RRAM Device. Mater. Chem. Front. 2020, 4, 1756– 1763,  DOI: 10.1039/D0QM00152J

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    41

    Dimensionally anisotropic graphene with high mobility and a high on-off ratio in a three-terminal RRAM device

    Liu, Bo; Tai, Han Hsiang; Liang, Hanyuan; Zheng, En-Yan; Sahoo, Mamina; Hsu, Chih Hsien; Chen, Tsung-Cheng; Huang, Chin An; Wang, Jer-Chyi; Hou, Tuo-Hung; Lai, Chao-Sung

    Materials Chemistry Frontiers (2020), 4 (6), 1756-1763CODEN: MCFAC5; ISSN:2052-1537. (Royal Society of Chemistry)

    In the past decade, graphene has aroused worldwide academic passion in the elect. community, due to its unique two dimen. lattice structure and high mobility properties. Meanwhile, the utilization of graphene for next-generation nano-electronic materials is still under debate due to its intrinsic zero band gap nature. To meet the requirement of logic applications, diversified academic attempts have been carried out to modify its intrinsic band structure, such as doping, bilayer stacking, nano-patterning, or heterostructures. In this work, a tailor made strategy for graphene is proposed and exptl. demonstrated: a dimensionally anisotropic graphene based three terminal resistive random-access memory (RRAM). This device could be operated in two modes, which realized not only high carrier mobility (103 cm2 V-1 s-1) and low gate leakage in field effect mode, but also a high on-off ratio (107) and ultra-low off state current (1 pA) in resistive switching mode. To guarantee the dimensional uniformity and high quality of the graphene, surface polishing and passivation techniques were carried out on Cu foil before graphene CVD synthesis. As demonstrated in this study, the current work paves the way for graphene toward practical logic and memory applications with high performance and low steady state power consumption.

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42. 42

    Park, J.; Lee, Y.; Jeong, H.; Choi, S. Neural Network Physically Unclonable Function: A Trainable Physically Unclonable Function System with Unassailability against Deep Learning Attacks Using Memristor Array. Adv. Intell. Syst. 2021, 3, 2100111,  DOI: 10.1002/aisy.202100111

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    Sun, W.; Gao, B.; Chi, M.; Xia, Q.; Yang, J. J.; Qian, H.; Wu, H. Understanding Memristive Switching via in Situ Characterization and Device Modeling. Nat. Commun. 2019, 10, 3453,  DOI: 10.1038/s41467-019-11411-6

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    Understanding memristive switching via in situ characterization and device modeling

    Sun Wen; Gao Bin; Qian He; Wu Huaqiang; Sun Wen; Chi Miaofang; Sun Wen; Xia Qiangfei; Yang J Joshua

    Nature communications (2019), 10 (1), 3453 ISSN:.

    Owing to their attractive application potentials in both non-volatile memory and unconventional computing, memristive devices have drawn substantial research attention in the last decade. However, major roadblocks still remain in device performance, especially concerning relatively large parameter variability and limited cycling endurance. The response of the active region in the device within and between switching cycles plays the dominating role, yet the microscopic details remain elusive. This Review summarizes recent progress in scientific understanding of the physical origins of the non-idealities and propose a synergistic approach based on in situ characterization and device modeling to investigate switching mechanism. At last, the Review offers an outlook for commercialization viability of memristive technology.

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44. 44

    Baeumer, C.; Valenta, R.; Schmitz, C.; Locatelli, A.; Menteş, T. O.; Rogers, S. P.; Sala, A.; Raab, N.; Nemsak, S.; Shim, M.; Schneider, C. M.; Menzel, S.; Waser, R.; Dittmann, R. Subfilamentary Networks Cause Cycle-to-Cycle Variability in Memristive Devices. ACS Nano 2017, 11, 6921– 6929,  DOI: 10.1021/acsnano.7b02113

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    44

    Subfilamentary networks cause cycle-to-cycle variability in memristive devices

    Baeumer, Christoph; Valenta, Richard; Schmitz, Christoph; Locatelli, Andrea; Mentes, Tevfik Onur; Rogers, Steven P.; Sala, Alessandro; Raab, Nicolas; Nemsak, Slavomir; Shim, Moonsub; Schneider, Claus M.; Menzel, Stephan; Waser, Rainer; Dittmann, Regina

    ACS Nano (2017), 11 (7), 6921-6929CODEN: ANCAC3; ISSN:1936-0851. (American Chemical Society)

    A major obstacle for the implementation of redox-based memristive memory or logic technol. is the large cycle-to-cycle and device-to-device variability. Here, the authors use spectromicroscopic photoemission threshold anal. and operando XAS anal. to exptl. investigate the microscopic origin of the variability. The authors find that some devices exhibit variations in the shape of the conductive filament or in the oxygen vacancy distribution at and around the filament. In other cases, even the location of the active filament changes from one cycle to the next. They propose that both effects originate from the coexistence of multiple (sub)filaments and that the active, current-carrying filament may change from cycle to cycle. These findings account for the obsd. variability in device performance and represent the scientific basis, rather than prior purely empirical engineering approaches, for developing stable memristive devices.

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45. 45

    Lin, A. S.; Pratik, S.; Ota, J.; Rawat, T. S.; Huang, T. H.; Hsu, C. L.; Su, W. M.; Tseng, T. Y. A Process-Aware Memory Compact-Device Model Using Long-Short Term Memory. IEEE Access 2021, 9, 3126– 3139,  DOI: 10.1109/ACCESS.2020.3047491

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46. 46

    Li, C.; Wang, Z.; Rao, M.; Belkin, D.; Song, W.; Jiang, H.; Yan, P.; Li, Y.; Lin, P.; Hu, M.; Ge, N.; Strachan, J. P.; Barnell, M.; Wu, Q.; Williams, R. S.; Yang, J. J.; Xia, Q. Long Short-Term Memory Networks in Memristor Crossbar Arrays. Nat. Mach. Intell. 2019, 1, 49– 57,  DOI: 10.1038/s42256-018-0001-4

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47. 47

    Zhang, X.; Xu, L.; Zhang, H.; Liu, J.; Tan, D.; Chen, L.; Ma, Z.; Li, W. Effect of Joule Heating on Resistive Switching Characteristic in AlO_x Cells Made by Thermal Oxidation Formation. Nanoscale Res. Lett. 2020, 15, 11,  DOI: 10.1186/s11671-019-3229-y

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    Effect of Joule Heating on Resistive Switching Characteristic in AlOx Cells Made by Thermal Oxidation Formation

    Zhang, Xinxin; Xu, Ling; Zhang, Hui; Liu, Jian; Tan, Dingwen; Chen, Liangliang; Ma, Zhongyuan; Li, Wei

    Nanoscale Research Letters (2020), 15 (1), 11CODEN: NRLAAD; ISSN:1556-276X. (Springer)

    The AlOx-based resistive switching memory device is fabricated by an oxidn. diffusion process that involves depositing an Al film on an ITO substrate and annealing at 400°C in a vacuum. An AlOx interface layer with a thickness of ∼ 20 nm is formed as a resistance switching layer. Bipolar and unipolar resistive switching (RS) behaviors are obtained when the compliance current is limited (≥ 1 mA). In the unipolar RS behavior, the devices fail to perform set/reset cycles at a low temp. (40 K), which suggests that Joule heating is essential for the unipolar RS behavior. In the bipolar RS behavior, the abrupt reset transforms into a gradual reset with decreasing temp., which suggests that Joule heating affects the rupture of the conductive filament. In addn., the conductive mechanisms in the high-resistance state and low-resistance state are revealed by the temp. dependence of the I-V curves. For the low-resistance state, the conduction mechanism is due to the electron hopping mechanism, with a hopping activation energy of 9.93 meV. For the high-resistance state, transport mechanism is dominated by the space-charge-limited conduction (SCLC) mechanism.

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48. 48

    Lanza, M.; Wong, H. S. P.; Pop, E.; Ielmini, D.; Strukov, D.; Regan, B. C.; Larcher, L.; Villena, M. A.; Yang, J. J.; Goux, L.; Belmonte, A.; Yang, Y.; Puglisi, F. M.; Kang, J.; Köpe, B. M.; Yalon, E.; Kenyon, A.; Buckwell, M.; Mehonic, A.; Shluger, A. Recommended Methods to Study Resistive Switching Devices. Adv. Electron. Mater. 2019, 5, 1800143,  DOI: 10.1002/aelm.201800143

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    Liu, B.; Liu, Z.; Chiu, I. S.; Di, M.; Wu, Y.; Wang, J. C.; Hou, T. H.; Lai, C. S. Programmable Synaptic Metaplasticity and below Femtojoule Spiking Energy Realized in Graphene-Based Neuromorphic Memristor. ACS Appl. Mater. Interfaces 2018, 10, 20237– 20243,  DOI: 10.1021/acsami.8b04685

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    49

    Programmable Synaptic Metaplasticity and below Femtojoule Spiking Energy Realized in Graphene-Based Neuromorphic Memristor

    Liu, Bo; Liu, Zhiwei; Chiu, In-Shiang; Di, MengFu; Wu, YongRen; Wang, Jer-Chyi; Hou, Tuo-Hung; Lai, Chao-Sung

    ACS Applied Materials & Interfaces (2018), 10 (24), 20237-20243CODEN: AAMICK; ISSN:1944-8244. (American Chemical Society)

    Memristors with rich interior dynamics of ion migration are promising for mimicking various biol. synaptic functions in neuromorphic hardware systems. A graphene-based memristor shows an extremely low energy consumption of less than a femtojoule per spike, by taking advantage of weak surface van der Waals interaction of graphene. The device also shows an intriguing programmable metaplasticity property in which the synaptic plasticity depends on the history of the stimuli and yet allows rapid reconfiguration via an immediate stimulus. This graphene-based memristor could be a promising building block toward designing highly versatile and extremely energy efficient neuromorphic computing systems.

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50. 50

    Liu, B.; Hong, M.-C.; Sahoo, M.; Ong, B. L.; Tok, E. S.; Di, M.; Ho, Y.-P.; Liang, H.; Bow, J.-S.; Liu, Z.; Wang, J. C.; Hou, T.-H; Lai, C. S. A Fluorographene-Based Synaptic Transistor. Adv. Mater. Technol. 2019, 4, 1900422,  DOI: 10.1002/admt.201900422

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    A Fluorographene-Based Synaptic Transistor

    Liu, Bo; Hong, Ming-Chun; Sahoo, Mamina; Ong, Bin Leong; Tok, Eng Soon; Di, MengFu; Ho, Yu-Ping; Liang, Hanyuan; Bow, Jong-Shing; Liu, Zhiwei; Wang, Jer-Chyi; Hou, Tuo-Hung; Lai, Chao-Sung

    Advanced Materials Technologies (Weinheim, Germany) (2019), 4 (10), 1900422CODEN: AMTDCM; ISSN:2365-709X. (Wiley-VCH Verlag GmbH & Co. KGaA)

    Exploring brain-inspired synaptic devices has recently become a new focus of research in nanoelectronic communities. In this emerging field, incorporating 2D materials into three-terminal synaptic transistors has brought various advantages. However, achieving a stable and long-term wt.-modulation in these synaptic transistors, which are typically based on interface charge storage, is still a challenge due to the nature of their spontaneous relaxation. The application of an atomically thin fluorographene layer into the synaptic junction region suppresses this issue and improves the efficiency, tunability, and symmetry of the synaptic plasticity as well as establishing a stable wt.-regulation paradigm. These unique properties can be attributed to the dipolar rotation of C-F in fluorographene. To obtain a better phys. understanding, a vacancy-dependent C-F dipolar rotation model is proposed and supported by hysteresis anal. and d. functional theory calcns. As proposed and demonstrated, the unique fluorographene-based synaptic transistor may be a promising building block for constructing efficient neuromorphic computing hardware.

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