Nonvolatile Modulation Research Articles

Giant tunnel electroresistance through a Van der Waals junction by external ferroelectric polarization

The burgeoning interest in two-dimensional semiconductors stems from their potential as ultrathin platforms for next-generation transistors. Nonetheless, there persist formidable challenges in fully obtaining high-performance complementary logic components and the underlying mechanisms for the polarity modulation of transistors are not yet fully understood. Here, we exploit both ferroelectric domain-based nonvolatile modulation of Fermi level in transitional metal dichalcogenides (MoS2) and quantum tunneling through nanoscale hexagonal boron nitride (h-BN). Our prototype devices, termed as vertical tunneling ferroelectric field-effect transistor, utilizes a Van der Waals MoS2/h-BN/metal tunnel junction as the channel. The Fermi level of MoS2 is bipolarly tuned by ferroelectric domains and sensitively detected by the direct quantum tunneling strength across the junction, demonstrating an impressive electroresistance ratio of up to 109 in the vertical tunneling ferroelectric field-effect transistor. It consumes only 0.16 fJ of energy to open a ratio window exceeding 104. This work not only validates the effectiveness of tailored tunnel barriers in manipulating electronic flow but also highlights a new avenue for the design flexibility and functional versatility of advanced ferroelectric memory technology.

Room-temperature modulation of microwave conductivity in ferroelectric-gated correlated oxides

We report the nonvolatile modulation of microwave conductivity in ferroelectric PbZr0.2Ti0.8O3-gated ultrathin LaNiO3/La0.67Sr0.33MnO3 correlated oxide channel visualized by microwave impedance microscopy. Polarization switching is obtained by applying a tip bias above the coercive voltage of the ferroelectric layer. The microwave conductivity of the correlated channel underneath the up- and down-polarized domains has been quantified by finite-element analysis of the tip-sample admittance. At room temperature, a resistance on/off ratio above 100 between the two polarization states is sustained at frequencies up to 1 GHz, which starts to drop at higher frequencies. The frequence-dependence suggests that the conductance modulation originates from ferroelectric field-effect control of carrier density. The modulation is nonvolatile, remaining stable after 6 months of domain writing. Our work is significant for potential applications of oxide-based ferroelectric field-effect transistors in high-frequency nanoelectronics and spintronics.

Electric field control of spin-orbit torque in annealed Ta/CoFeB/HfO x heterostructures via interfacial oxidation modulation

Electric field control of spin-orbit torque (SOT) exhibits promising potential in advanced spintronic devices through interfacial modulation. In this work, we investigate the influence of electric field and interfacial oxidation on SOT efficiency in annealed Ta/CoFeB/HfO x heterostructures. By varying annealing temperatures, the damping-like SOT efficiency reaches its peak at the annealing temperature of 320 °C, with an 80% field-free magnetization switching ratio induced by SOT having been demonstrated. This enhancement is ascribed to the annealing-induced modulation of oxygen ion migration at the CoFeB/HfO x interface. By applying voltages across the Ta/CoFeB/HfO x heterostructures, which drives the O2‒ migration across the interface, a reversible, bipolar, and non-volatile modulation of SOT efficiency was observed. The collective influence of annealing temperature and electric field effects on SOT carried out in this work provides an effective approach into facilitating the optimization and control of SOT in spintronic devices.

Electrical Control Grain Dimensionality with Multilevel Magnetic Anisotropy.

In alignment with the increasing demand for larger storage capacity and longer data retention, the electrical control of magnetic anisotropy has been a research focus in the realm of spintronics. Typically, magnetic anisotropy is determined by grain dimensionality, which is set during the fabrication of magnetic thin films. Despite the intrinsic correlation between magnetic anisotropy and grain dimensionality, there is a lack of experimental evidence for electrically controlling grain dimensionality, thereby impairing the efficiency of magnetic anisotropy modulation. Here, we demonstrate an electric field control of grain dimensionality and prove it as the active mechanism for tuning interfacial magnetism. The reduction in grain dimensionality is associated with a transition from ferromagnetic to superparamagnetic behavior. We achieve a nonvolatile and reversible modulation of the coercivity in both the ferromagnetic and superparamagnetic regimes. Subsequent electrical and elemental analysis confirms the variation in grain dimensionality upon the application of gate voltages, revealing a transition from a multidomain to a single-domain state, accompanied by a reduction in grain dimensionality. Furthermore, we exploit the influence of grain dimensionality on domain wall motion, extending its applicability to multilevel magnetic memory and synaptic devices. Our results provide a strategy for tuning interfacial magnetism through grain size engineering for advancements in high-performance spintronics.

Nonvolatile Phase-Only Transmissive Spatial Light Modulator with Electrical Addressability of Individual Pixels.

Active metasurfaces with tunable subwavelength-scale nanoscatterers are promising platforms for high-performance spatial light modulators (SLMs). Among the tuning methods, phase-change materials (PCMs) are attractive because of their nonvolatile, threshold-driven, and drastic optical modulation, rendering zero-static power, crosstalk immunity, and compact pixels. However, current electrically controlled PCM-based metasurfaces are limited to global amplitude modulation, which is insufficient for SLMs. Here, an individual-pixel addressable, transmissive metasurface is experimentally demonstrated using the low-loss PCM Sb2Se3 and doped silicon nanowire heaters. The nanowires simultaneously form a diatomic metasurface, supporting a high-quality-factor (∼406) quasi-bound-state-in-the-continuum mode. A global phase-only modulation of ∼0.25π (∼0.2π) in simulation (experiment) is achieved, showing ten times enhancement. A 2π phase shift is further obtained using a guided-mode resonance with enhanced light-Sb2Se3 interaction. Finally, individual-pixel addressability and SLM functionality are demonstrated through deterministic multilevel switching (ten levels) and tunable far-field beam shaping. Our work presents zero-static power transmissive phase-only SLMs, enabled by electrically controlled low-loss PCMs and individual meta-molecule addressable metasurfaces.

Electric field control of perpendicular magnetic tunnel junctions with easy-cone magnetic anisotropic free layers.

Magnetic tunnel junctions (MTJs) are the core element of spintronic devices. Currently, the mainstream writing operation of MTJs is based on electric current with high energy dissipation, and it can be notably reduced if an electric field is used instead. In this regard, it is promising for electric field control of MTJ in the multiferroic heterostructure composed of MTJ and ferroelectrics via strain-mediated magnetoelectric coupling. However, there are only reports on MTJs with in-plane anisotropy so far. Here, we investigate electric field control of the resistance state of MgO-based perpendicular MTJs with easy-cone anisotropic free layers through strain-mediated magnetoelectric coupling in multiferroic heterostructures. A remarkable, nonvolatile, and reversible modulation of resistance at room temperature is demonstrated. Through local reciprocal space mapping under different electric fields for Pb(Mg1/3Nb2/3)0.7Ti0.3O3 beneath the MTJ pillar, the modulation mechanism is deduced. Our work represents a crucial step toward electric field control of spintronic devices with non-in-plane magnetic anisotropy.

Monolithic back-end-of-line integration of phase change materials into foundry-manufactured silicon photonics

Monolithic integration of novel materials without modifying the existing photonic component library is crucial to advancing heterogeneous silicon photonic integrated circuits. Here we show the introduction of a silicon nitride etch stop layer at select areas, coupled with low-loss oxide trench, enabling incorporation of functional materials without compromising foundry-verified device reliability. As an illustration, two distinct chalcogenide phase change materials (PCMs) with remarkable nonvolatile modulation capabilities, namely Sb2Se3 and Ge2Sb2Se4Te1, were monolithic back-end-of-line integrated, offering compact phase and intensity tuning units with zero-static power consumption. By employing these building blocks, the phase error of a push-pull Mach–Zehnder interferometer optical switch could be reduced with a 48% peak power consumption reduction. Mirco-ring filters with >5-bit wavelength selective intensity modulation and waveguide-based >7-bit intensity-modulation broadband attenuators could also be achieved. This foundry-compatible platform could open up the possibility of integrating other excellent optoelectronic materials into future silicon photonic process design kits.

Approaching the Zero-Power Operating Limit in a Self-Coordinated Organic Protonic Synapse.

High-performance artificial synapse with nonvolatile memory and low power consumption is a perfect candidate for brainoid intelligence. Unfortunately, due to the energy barrier paradox between ultra-low power and nonvolatile modulation of device conductances, it is still a challenge at the moment to construct such ideal synapses. Herein, a proton-reservoir type 4,4',4″,4'''-(Porphine-5,10,15,20-tetrayl) tetrakis (benzenesulfonic acid) (TPPS) molecule and fabricated organic protonic memristors with device width of 10µm to 100nm is synthesized. The occurrence of sequential proton migration and interfacial self-coordinated doping will introduce new energy levels into the molecular bandgap, resulting in effective and nonvolatile modulation of device conductance over 64 continuous states with retention exceeding 30min. The power consumptions of modulating and reading the device conductance approach the zero-power operating limits, which range from 16.25pW to 2.06nW and 6.5fW to 0.83pW, respectively. Finally, a robust artificial synapse is successfully demonstrated, showing spiking-rate-dependent plasticity (SRDP) and spiking-timing-dependent plasticity (STDP) characteristics with ultra-low power of 0.66 to 0.82pW, as well as 100 long-term depression (LTD)/potentiation (LTP) cycles with 0.14%/0.30% weight variations.

Nonvolatile Modulation of Light Emission from Delocalized and Defect-Bound Excitons in Monolayer MoS2 Using the Remnant Polarization in the Ferroelectric Polymer P(VDF-TrFE): Implications for Optical Memory

Nonvolatile Modulation of Light Emission from Delocalized and Defect-Bound Excitons in Monolayer MoS₂ Using the Remnant Polarization in the Ferroelectric Polymer P(VDF-TrFE): Implications for Optical Memory

In Memory Energy Application for Electrochemical Random Access Memory

This work explores the innovative concept of a hybrid dual-behavior device, based on emerging nonvolatile memory technology, for both data retention and energy storage. Electrochemical random access memory (ECRAM) is considered a major candidate as next-generation memory, thanks to its promising performances in terms of scalability and CMOS process compatibility. In particular, three-terminal synaptic transistors (SynT) offer an ion conductor-gated control from which ion doping content can be monitored with high energy efficiency via redox reactions, thus decoupling write-read actions and improving the linearity of programming states for neuromorphic computing1. Its working mechanisms, based on faradaic processes, motivate the study on the feasibility of operating ECRAM also as energy storage element.To evaluate the energy capability, various electrochemical characterizations are presented. Cyclic voltammetry tests reveal that the cells behave as standard electrochemical storage elements when investigating the impact of the scan rate, maximum positive voltage, and area on the reduction peak. Storage capability amounts up to 1.5µAh.cm-2 have been obtained, two decades higher than deep trench capacitor existing solutions, while showing outstanding synaptic behavior: A nonvolatile conductance modulation (<75 nS) is achieved through reversible lithium intercalation into the channel, and synaptic functions, such as long-term potentiation/depression involve ultralow switching energy of 2 fJ μm−2. Moreover, this SynT shows excellent endurance (>105 weight updates) and recognition accuracy (>95% on the MNIST data test using crossbar simulations). Finally, design concepts are proposed, where ECRAM “in-memory energy” technology would be a newfangled approach to meet the needs of various emerging and standard applications.Reference Nguyen, N. et al. An Ultralow Power Li x TiO 2 -Based Synaptic Transistor for Scalable Neuromorphic Computing. Adv. Electron. Mater. 2200607, 2200607 (2022). Figure 1. Schematic view of the elaborated SynT, and corresponding dual energy and data storage properties: vertical gate stack is a nanobattery with energy storage function while lateral architecture allows for conductance modulation and data storage. Figure 1

Tunable structural transmissive color in fano-resonant optical coatings employing phase-change materials

Reversible, nonvolatile, and pronounced refractive index modulation is an unprecedented combination of properties enabled by chalcogenide phase-change materials (PCMs). This combination of properties makes PCMs a fast-growing platform for active, low-energy nanophotonics, including tunability to otherwise passive thin-film optical coatings. Here, we integrate the PCM Sb2Se3 into a novel four-layer thin-film optical coating that exploits photonic Fano resonances to achieve tunable structural colors in both reflection and transmission. We show, contrary to traditional coatings, that Fano-resonant optical coatings (FROCs) allow for achieving transmissive and reflective structures with narrowband peaks at the same resonant wavelength. Moreover, we demonstrate asymmetric optical response in reflection, where Fano resonance and narrow-band filtering are observed depending upon the light incidence side. Finally, we use a multi-objective inverse design via machine learning (ML) to provide a wide range of solution sets with optimized structures while providing information on the performance limitations of the PCM-based FROCs. Adding tunability to the newly introduced Fano-resonant optical coatings opens various applications in spectral and beam splitting, and simultaneous reflective and transmissive displays, diffractive objects, and holograms.

Reconfigurable and nonvolatile terahertz lithography-free photonic devices based on phase change films

High-performance terahertz (THz) devices with reconfigurable features are highly desirable in many promising THz applications. However, most of the existing reconfigurable THz elements are still limited to volatile responses, single functionality, and time-consuming multistep manufacturing procedures. In this paper, we report a lithography-free approach to create reconfigurable and nonvolatile THz components by exploring the reversible, nonvolatile, and continuous THz modulation capability of the phase change material Ge2Sb2Te5 . As a proof of concept, THz gratings with significant Rayleigh anomalies and diffraction as well as ultrathin THz flat lenses with subwavelength and ultra-broadband focusing capabilities are designed and fabricated on ultrathin Ge2Sb2Te5 films using the presented photo-imprint strategy. Moreover, such a method can also be adopted to create more complex THz devices, such as Pancharatnam–Berry phase metasurfaces and grayscale holographic plates. With these findings, the proposed method will provide a promising solution to realize reconfigurable and nonvolatile THz elements.

Edge-Based Two-Dimensional α-In2Se3–MoS2 Ferroelectric Field Effect Device

Heterostructures based on two-dimensional materials offer the possibility to achieve synergistic functionalities, which otherwise remain secluded by their individual counterparts. Herein, ferroelectric polarization switching in α-In2Se3 has been utilized to engineer multilevel nonvolatile conduction states in a partially overlapping α-In2Se3-MoS2-based ferroelectric semiconducting field effect device. In particular, we demonstrate how the intercoupled ferroelectric nature of α-In2Se3 allows to nonvolatilely switch between n-i and n-i-n type junction configurations based on a novel edge state actuation mechanism, paving the way for subnanometric scale nonvolatile device miniaturization. Furthermore, the induced asymmetric polarization enables enhanced photogenerated carriers' separation, resulting in an extremely high photoresponse of ∼1275 A/W in the visible range and strong nonvolatile modulation of the bright A- and B- excitonic emission channels in the overlaying MoS2 monolayer. Our results show significant potential to harness the switchable polarization in partially overlapping α-In2Se3-MoS2 based FeFETs to engineer multimodal, nonvolatile nanoscale electronic and optoelectronic devices.

Giant and Nonvolatile Control of Exchange Bias in Fe3GeTe2/Irradiated Fe3GeTe2/MgO Heterostructure Through Ultralow Voltage

AbstractThe discovery of van der Waals magnets has provided a new platform for the electrical control of magnetism. Recent experiments have demonstrated that the magnetic properties of van der Waals magnets can be tuned by various gate modulations, although most of them are volatile and require gate voltages no lower than several volts. Here, the realization of nonvolatile control of exchange bias and coercive fields in Fe3GeTe2/MgO heterostructures, and the gate voltage is as low as tens of mV which is two orders of magnitude smaller than those in previous experiments is presented. The discovery of an ionic‐irradiated phase formed in Fe3GeTe2 by MgO sputtering revealed that an exchange bias effect can be obtained in this heterostructure and tuned from ≈700 to 0 Oe through voltages ranging from 5 to 20 mV. Owing to the high stability of oxidized Fe3GeTe2, the voltage‐driven oxygen incorporated into Fe3GeTe2 from the irradiated phase induces a nonvolatile magnetism modulation that can be retained after turning off the gate voltage. These findings demonstrate a methodology to modulate the magnetism of van der Waals magnets, opening new opportunities to fabricate all‐solid, long‐retention, and low‐dissipation nano‐electronic devices using van der Waals materials.

Selective Dual-Ion Modulation in Solid-State Magnetoelectric Heterojunctions for In-Memory Encryption.

Nanoionic technologies are identified as a promising approach to modulating the physical properties of solid-state dielectrics, which have resulted in various emergent nanodevices, such as nanoionic resistive switching devices and magnetoionic devices for memory and computing applications. Previous studies are limited to single-type ion manipulation, and the investigation of multiple-type ion modulation on the coupled magnetoelectric effects, for developing information devices with multiple integrated functionalities, remains elusive. Here, a dual-ion solid-state magnetoelectric heterojunction based on Pt/HfO2- x /NiOy /Ni with reconfigurable magnetoresistance (MR) characteristics is reported for in-memory encryption. It is shown that the oxygen anions and nickel cations can be selectively driven by voltages with controlled polarity and intensity, which concurrently change the overall electrical resistance and the interfacial magnetic coupling, thus significantly modulate the MR symmetry. Based on this device, a magnetoelectric memory prototype array with in-memory encryption functionality is designed for the secure storage of image and digit information. Along with the advantages including simple structure, multistate encryption, good reversibility, and nonvolatile modulation capability, this proof-of-concept device opens new avenues toward next-generation compact electronics with integrated information functionalities.

Controllably modulated asymmetrical photoresponse with a nonvolatile memory effect in a single CH3NH3PbI3 micro/nanowire for photorectifiers and photomemory.

Nanostructured hybrid organic-inorganic perovskites exhibit remarkable photodetection performance due to their abundant surface states and high responsivity to visible light. However, in traditional photodetectors with a symmetrical configuration of two-terminal electrodes, the photoresponse is independent of bias polarity. Moreover, for self-powered photodetectors, an asymmetric structure of the chemical composition, such as p-n and Schottky junctions, and two different electrodes are necessary. Herein, we demonstrate a modulable asymmetrical photoresponse by packing only one electrode end in a single CH3NH3PbI3 micro/nanowire with two symmetrical Ag electrodes. This not only enables the high performance of light- and bias-modulated multifunctional photorectifiers and self-powered photodetectors, but also allows controllable implementation of nonvolatile photomemory with a tunable spectral responsivity and range. At an unpacked electrode interface, trace moisture in the environment promotes a good bonding of Ag+ and I-, substantially decreasing the interface barrier. Conversely, at a packed electrode interface, abundant surface states can be well preserved, leading to a high interface barrier. Notably, under a large voltage and strong light, the redox of Ag/AgI at the unpacked electrode interface and the injection and ejection of holes at the packed electrode interface can be reversibly conducted by inverting the voltage polarity, enabling a controllable nonvolatile modulation. Therefore, by clarifying the actual origin of the photoelectrical response of CH3NH3PbI3 micro/nanowires at electrode interfaces, high-performance multifunctional photorectifiers and self-powered photodetectors based on asymmetrical interface photovoltaic effects with two symmetrical electrodes can be controllably realized. Furthermore, by precise cooperative modulation of two electrode interface states with a large voltage and strong illumination, nonvolatile photomemory with a tunable spectral responsivity and range can be implemented.

Reversible and Nonvolatile Manipulation of the Spin-Orbit Interaction in Ferroelectric Field-Effect Transistors Based on a Two-Dimensional Bismuth Oxychalcogenide

The spin-orbit interaction (SOI) offers a nonferromagnetic scheme to realize spin polarization through utilizing an electric field. Electrically tunable SOIs through electrostatic gates have been investigated; however, the relatively weak and volatile tunability limits their practical applications in spintronics. Here, we demonstrate the nonvolatile electric field control of the SOI via constructing ferroelectric Rashba architectures, i.e., two-dimensional ${\mathrm{Bi}}_{2}{\mathrm{O}}_{2}\mathrm{Se}/\mathrm{Pb}({\mathrm{Mg}}_{1/3}{\mathrm{Nb}}_{2/3}){\mathrm{O}}_{3}$-${\mathrm{PbTiO}}_{3}$ ferroelectric field-effect transistors. The experimentally observed weak antilocalization (WAL) cusp in ${\mathrm{Bi}}_{2}{\mathrm{O}}_{2}\mathrm{Se}$ films implies the Rashba-type SOI that arises from the asymmetric confinement potential. Significantly, taking advantage of the switchable ferroelectric polarization, the WAL-to-weak-localization-transition trend reveals the competition between spin relaxation and the dephasing process, and the variation of carrier density leads to a reversible and nonvolatile modulation of the spin-relaxation time and the spin-splitting energy of ${\mathrm{Bi}}_{2}{\mathrm{O}}_{2}\mathrm{Se}$ films by this ferroelectric gating. Our work provides a scheme to achieve nonvolatile control of the Rashba SOI with the utilization of ferroelectric remanent polarization.

Remote surface optical phonon scattering in ferroelectric Ba0.6Sr0.4TiO3 gated graphene

We report the effect of remote surface optical (RSO) phonon scattering on carrier mobility in monolayer graphene gated by ferroelectric oxide. We fabricate monolayer graphene transistors back-gated by epitaxial (001) Ba0.6Sr0.4TiO3 films, with field effect mobility up to 23 000 cm2 V−1 s−1 achieved. Switching ferroelectric polarization induces nonvolatile modulation of resistance and quantum Hall effect in graphene at low temperatures. Ellipsometry spectroscopy studies reveal four pairs of optical phonon modes in Ba0.6Sr0.4TiO3, from which we extract RSO phonon frequencies. The temperature dependence of resistivity in graphene can be well accounted for by considering the scattering from the intrinsic longitudinal acoustic phonon and the RSO phonon, with the latter dominated by the mode at 35.8 meV. Our study reveals the room temperature mobility limit of ferroelectric-gated graphene transistors imposed by RSO phonon scattering.

Analog Tunnel Memory Based on Programmable Metallization for Passive Neuromorphic Circuits.

Although experimental implementations of memristive crossbar arrays have indicated the potential of these networks for in-memory computing, their performance is generally limited by an intrinsic variability on the device level as a result of the stochastic formation of conducting filaments. A tunnel-type memristive device typically exhibits small switching variations, owing to the relatively uniform interface effect. However, the low mobility of oxygen ions and large depolarization field result in slow operation speed and poor retention. Here, we demonstrate a quantum-tunneling memory with Ag-doped percolating systems, which possesses desired characteristics for large-scale artificial neural networks. The percolating layer suppresses the random formation of conductive filaments, and the nonvolatile modulation of the Fowler-Nordheim tunneling current is enabled by the collective movement of active Ag nanocrystals with high mobility and a minimal depolarization field. Such devices simultaneously possess electroforming-free characteristics, record low switching variabilities (temporal and spatial variation down to 1.6 and 2.1%, respectively), nanosecond operation speed, and long data retention (>104 s at 85 °C). Simulations prove that passive arrays with our analog memory of large current-voltage nonlinearity achieve a high write and recognition accuracy. Thus, our discovery of the unique tunnel memory contributes to an important step toward realizing neuromorphic circuits.

An Ultralow Power LixTiO2‐Based Synaptic Transistor for Scalable Neuromorphic Computing

AbstractArtificial synapses based on electrochemical synaptic transistors (SynTs) have attracted tremendous attention toward massive parallel computing operations. However, most SynTs still suffer from downscaling limitations and high energy consumption. To overcome such drawbacks, a complementary metal–oxide–semiconductor (CMOS) back‐end‐of‐line compatible solid‐state SynT is presented, which includes an ultrathin (10 nm thick) quasiamorphous LixTiO2 channel. A nonvolatile conductance modulation (&lt;75 nS) is achieved through reversible lithium intercalation into the channel, and synaptic functions, such as long‐term potentiation/depression involve ultralow switching energy of 2 fJ µm−2. Moreover, this SynT shows excellent endurance (&gt;105 weight updates) and recognition accuracy (&gt;95% on the MNIST data test using crossbar simulations). Furthermore, a comprehensive electrochemical study allows deeper insight into the specific pseudocapacitive mechanism at the origin of conductance modulation. These results underline the high potential of LixTiO2‐based SynTs for energy‐efficient neuromorphic applications.