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Emerging memory technologies show the potentials of new memory devices to store more data at a lower cost compared to the industry-standard silicon-based devices. Among these, resistive switching random access memory (RRAM) devices, which are based on the metal-insulator-metal (MIM) structure, have shown potential in non-volatile memory applications due to their characteristics of low-power consumption, superior switching speed, excellent reliability, ultimate scaling potential with the simple fabrication process and adaptive aptitudes for the neuromorphic applications [1, 2]. 
The advantage of the biodegradable materials is non-toxic and eco-friendly but the essential material properties remain the major issues in the scaling of biomass-based RRAMs [3]. Biodegradable magnesium fluoride (MgFx) is an insulator with a large bandgap (11.3 eV) which makes it a favorable candidate for biodegradable RRAM devices. Recently, a couple of reports on MgFx based RRAM devices have shown excellent resistive switching and biodegradable properties [2, 4]. Nevertheless, the conduction mechanism and resistive switching mechanism in the MgFx based RRAM devices are not fully understood. The electrodes in RRAM devices may significantly affect the resistive switching (RS) behavior. The effects of electrode materials and operating environment including cryogenic temperature on the device performance have not been studied yet. 
In this study, we report resistive memory devices employing MgFx as the resistive switching layer that is inserted between the platinum and titanium metal electrodes. The MgFx based RRAM devices exhibit electroforming free bipolar resistive switching characteristics at room temperature and open-air environment. We also report the effects of electrode materials (Top: Pt, Au/Ni, ITO, and Bottom: p+ Si, n+ Si, ITO) on MgFx based RRAM devices. It is found that the difference in workfunctions affects the performances of the devices. We have also analyzed the effect of the operating environment as well as temperature from room temperature down to cryogenic temperature. The detailed performance of the devices, their conduction and switching mechanisms, the effects of the electrode materials, and the operating environment including cryogenic temperature will be presented at the virtual conference.


Materials Challenges for Memory

Effects of the electrode materials and operating environment on magnesium fluoride based bipolar RRAMs

electrode materials

cryogenic temperature

vacuum environment

rram


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The energy cost of storing and moving data is enormous, and is growing at such a rapid pace that within a few years the power demand may overwhelm some developed nations. Non-volatile memory (NVM) and neuromorphic computing are enabling critical advances in this area, but there are many scientific and technological challenges. This conference will cover the materials challenges of different memory technologies, from the fundamental processes and mechanisms, to industry perspectives on materials specifications and manufacturing.

poster

Interfacial exchange coupling and proximity effects in antiferromagnetic/ferromagnetic (AFM/FM) bilayers are the key that control the exchange bias phenomena exploited in most spintronic devices. In both cases, spin fluctuations in the AFM layer during the temperature-driven magnetic phase transition at the Néel temperature (TN) are commonly used to understand the magnitude of the exchange bias field (HE), the onset of HE, referred as the Blocking temperature (TB ≤TN), and the enhancement of the coercive field (HC). Here we show that the magnetic domain structure during the magnetization reversal of the FM layer controls the mentioned effects. Temperature-dependent measurements performed in a V2O3/Co bilayer after different field cooling (FC) procedures reveal that these effects depend strongly on the FC angle and are associated with a different domain structure of a FM layer that has a well-defined uniaxial magnetic anisotropy. Remarkably, a wide temperature window for TB (c.a. 35 K) and up to a factor of two in HE are found. All experimental observations can be explained within the Random-Field Model for the interfacial exchange coupling in AFM/FM bilayers with a fixed (nanometre-sized) AFM domain structure in contact with a variable (angle-dependent) FM domain structure. Our results highlight the importance of the domain structure and magnetization reversal of the FM layer in the exchange coupling phenomena, paving the way to enhance and/or control interfacial effects in future spintronic devices.

Tailoring interfacial phenomena in hybrid V2O3/Co bilayers

This experimental study measures interface spin Seebeck effect (SSE), spin current generation by a temperature gradient, in two antiferromagnetic crystals using optical pump-Terahertz emission spectroscopy. We utilise the absorption of a femtosecond optical pulse in an adjacent Pt thin layer to create a strong temperature discontinuity at the interface, which subsequently generates an incoherent spin current. The Pt layer also converts the spins to a charge current, generating a single-cycle Terahertz electric field pulse. The ultra-fast probing technique enables focusing the interpretation to only the interface effect. Strong THz emissions from both antiferromagnets indicate their excellent interface quality for spin transport. We observe disparate nature of the SSE signal dependence on temperature in the two antiferromagnets, which unambiguously reveals the influence of magnon resonant frequency.

Probing Interfacial Spin Transport in Antiferromagnets using Terahertz Spin Seebeck Effect

Most optoelectronic and memristive devices are fabricated using a vertically aligned configuration, where one or more layers of the active material(s) are “sandwiched” between the metal electrodes. Coplanar electrode architectures on the other hand, may offer many advantages, such as lower power consumption, faster operating speed, greater sensitivity and higher-level of integration. Furthermore, using nanogap (<15 nm)-separated coplanar electrodes, extreme downscale of the active layer thickness can be achieved, resulting in fast response speed photodetectors and low-power resistive switching in memristive devices.
Herein, we show memristive devices based on coplanar nanogap electrodes. These have been fabricated at a wafer scale with an inexpensive nanopatterning technique, compatible with flexible substrates, named adhesion lithography. We demonstrate memristors based on empty and metal oxide, polymer and carbon-nanotube materials, discuss the mechanism dominating their operation and showcase their ability to be integrated in arrays.

Nanogap electrode-based memristive devices

The paper presents the results of numerical modeling and experimental studies of the regularities of the manifestation of the memristor effect of oxide nanodots obtained by the method of local anodic oxidation.

Memristive properties of titanium oxide nanodot structures for resistive memory

High density, high-speed and low power consuming nonvolatile memories are currently being vigorously explored for use in next-generation computation, particularly due to the performance gap between the logic and memory elements of the current computational architecture.[1–3] Of various explored material systems, electrically switchable spontaneous polarization of ferroelectric materials enables a robust nonvolatile memory solution.[4–6] Using ultrathin films of ferroelectric materials as a tunnel barrier in metal/ferroelectric/metal trilayer structure, so called ferroelectric tunnel junctions (FTJ), is being explored widely as a potential nonvolatile memory elements. Unlike to ferroelectric RAM (FeRAM), FTJ offers nondestructive readout, in addition to low operation energy and high operation speed.[7]
In this work,[8] we have demonstrated FTJs with a very large OFF/ON resistance ratio and relatively low resistance area product (RA) with ~ 1 nm thick Zr doped HfO2 (HZO) ferroelectric tunnel barrier. We stabilized ferroelectricity in ultrathin films of rhombohedral HZO (R-HZO) through the substrate-induced compressive strain. The resistance area product at the bias voltage (~ 300 mV) required for one-half of the zero-bias TER ratio is three orders of magnitude lower than reported value with relatively thick ferroelectric barriers. [9, 10] The OFF/ON resistance ratio of 135 achieved with ~ 1 nm barrier, which is enhanced to 105 with increasing the barrier thickness to 2.5 nm, is the highest reported value for HZO barrier based FTJs. These results set the stage for further exploration of Hafnia-based FTJs for non-volatile memory applications.

References
[1] S. Manipatruni, D. E. Nikonov, I. A. Young, Nat.
Phys. 2018, 14, 338.
[2] H. S. P. Wong, S. Salahuddin, Nat. Nanotechnol.
2015, 10, 191.
[3] B. Prasad, Y. L. Huang, R. V. Chopdekar, Z. Chen,
J. Steffes, S. Das, Q. Li, M. Yang, C. C. Lin, T.
Gosavi, D. E. Nikonov, Z. Q. Qiu, L. W. Martin, B.
D. Huey, I. Young, J. Íñiguez, S. Manipatruni, R.
Ramesh, Adv. Mater. 2020, 32, 1.
[4] S. Manipatruni, D. E. Nikonov, C.-C. Lin, T. A.
Gosavi, H. Liu, B. Prasad, Y.-L. Huang, E.
Bonturim, R. Ramesh, I. A. Young, Nature 2019,
565, 35
[5] S. Oh, H. Hwang, I. K. Yoo, APL Mater. 2019,
091109 7.

Hf0.5Zr0.5O2 ferroelectric tunnel barriers for nonvolatile memory applications

Phase change alloys have seen widespread use from rewritable optical discs to the present day interest in their use in emerging neuromorphic computing architectures. In spite of this enormous commercial interest, the physics of carriers in these materials is still not fully understood. In particular, the role of non-thermal process in the switching physics of PCM is still debated. Here, we describe the time and space dependence of the coupling between photoexcited carriers and the lattice in both the amorphous and crystalline states of one phase change material, GeTe. Our work reveals a clear evolution of the electron-phonon coupling during the phase transformation as the spectra of photoexcited acoustic phonons in the amorphous (a-GeTe) and crystalline (α-GeTe) phases are different. In particular and surprisingly, our analysis of the photoinduced acoustic pulse duration in crystalline GeTe suggests that a part of the energy deposited during the photoexcitation process takes place over a distance that clearly exceeds that defined by the pump light skin depth. In the opposite, the lattice photoexcitation process remains localized within that skin depth in the amorphous state. We then demonstrate that this is due to supersonic diffusion of photoexcited electron-hole plasma in the crystalline state. Consequently these findings prove the existence of a non-thermal transport of energy which is much faster than lattice heat diffusion.

Non-thermal transport of energy driven by photoexcited carriers in switchable solid states of GeTe

Resistive switching devices based on metal-insulator-metal (MIM) structures have substantial potentials in both non-volatile memories (NVM) and neuromorphic computing circuits. Most of the MIM devices are highly insulating at the pristine state and requires a large bias (electroforming step) to set the devices to the operable resistive switching situation. Electroforming step may cause the stochastic characteristics of the conductive filament formation, corresponding to poor synaptic characteristics.
In the present work, we employed a WOx/ZrOx stack with Ta/Pt electrodes to achieve an electroforming-free Ta/WOx/ZrOx/Pt resistive switching device. This device is also self-rectifying because the ZrOx/Pt interface creates a Schottky barrier, which provides an opportunity to solve the sneak-path-current problem in memristive crossbar array. Furthermore, Ta/WOx/ZrOx/Pt devices show analog-switching behavior, which allow us to demonstrate the synaptic plasticity via pulse stimulation with different amplitude or interval pulse. Then, synaptic functions of potentiation/depression cycles, paired-pulse facilitation (PPF) and spike-timing plasticity (STDP) have been successfully simulated. The excellent linearity and repeatability potentiation/depression cycles in the Ta/WOx/ZrOx/Pt device were applied to model the synaptic weight update in neural network (NN) simulation platform for pattern recognition accuracy using the MINST dataset of hand-written digits. The resulting NN inference accuracy of the Ta/WOx/ZrOx/Pt synaptic devices reaches 97.7% after 100 epochs, indicating that this device make it very suitable for on-chip training of artificial neural network.

Electroforming-free resistive switching of WOx/ZrOx stack for neuromorphic computing systems

Currently, there is a high demand for developing shape memory alloys that can be used at high temperatures such as aerospace and Ti50Pd50-XRuX is found to be one of the promising alloy. This is due to their shape memory effect and super elasticity. Previous studies revealed that the alloy is mechanically stable above 25 at. % Ru with a positive C^' at 0 K. So, an understanding of its transformation temperature behaviour is required, which is currently not clear. The self-consistent-charge density functional tight binding (SCC-DFTB) approach was used to develop parameters for Ti50Pd50-XRuX employing the parameterization technique. The structural and electronic properties were determined to check stability on derived potentials using DFTB+ code. As part of the validation for the developed set, the results are in good agreement to within 5 % as compared with Dmol3 findings. Furthermore, the SCC sets of parameters were also used to determine the lattice expansions to check the transformation temperature of ternary Ti50Pd50-XRuX. It was observed that the addition of Ru reduces the transformation temperature. The findings imply that the SCC-DFTB approach was able to predict the stability and transformation behaviour of Ti50Pd50-XRuX alloys.

Parameterization and transformation temperature of Ti50Pd50-XRuX using SCC-DFTB approach

With rapid development of information technology and artificial intelligence, optically controlled ferroelectric junctions are becoming promising candidates for data storage and logics [1]. We have recently reported that the resistance state of a BaTiO3 ferroelectric tunnel barrier can the switched from ON to OFF states by illumination with a suitable wavelength (blue laser, λ = 405 nm) if an imprint field (EIMP ≈ -2.8MV/cm) exists that unbalances the equilibrium polarization up/down domain configuration. The observation that smaller energy photons (red laser, λ = 648 nm) does not produce such effect strongly suggests that photocarriers play major role on polarization and resistance switching. Here we explore in greater detail the possible role of thermal effects and potential thermally induced suppression of polarization. A number of experiments, including the time-dependent response, its sensitivity to illumination power and recovery processes, have been performed. Data shows the prominence of electronic process (photocarriers and polarization screening) as the ultimate reason for light-induced resistive switching [2].

References
[1] Uchino, Kenji. Ferroelectric devices. CRC press, 2018.
[2] Long, Xiao, et al. "Non-volatile optical switch of resistance in photoferroelectric tunnel junctions." Nature communications 12.1 (2021): 1-9.


Disentangling electronic and thermal contributions to the observed light-induced resistance switching in BaTiO3 ferroelectric tunnel junction

The atomic-scale interfaces of 3D transition-metals oxides are the fascinating playground for several atomic-scale interactions of spins. Novel physical phenomena such as magnetoelectric coupling, unconventional exchange bias (EB) coupling, etc. which originate at such interfaces have huge potential for next-generation nanoscale spintronic devices. Among them, EB is the most studied due to its importance for device applications such as high-density memory and sensor. Here, we demonstrate EB coupling (EB shift, HEB~40 Oe at 2 K) at the interface of epitaxially grown ferromagnetic (FM) La0.67Sr0.33MnO3 (LSMO) – ferroelectric (FE) BaTiO3 (BTO) bilayer thin films on SrTiO3 (STO) single crystal substrates in absence of any conventional antiferromagnetic (AFM) material. Such EB is only observed when the thickness of LSMO is only a few unit cells (<10nm). Importantly, we find that the EB coupling follows training effect, bias field dependency, and temperature dependency. By X-ray magnetic circular dichroism (XMCD) measurement, it is observed that in such epitaxial heterostructure Ti of BTO poses magnetisation at 2K and can reversibly switch between two distinct magnetization states by switching external applied magnetic field. A remanent magnetization (MR) in Ti is also observed. The magnetization of Ti as well the EB vanishes at high temperature (300K) which confirms the EB coupling between Ti of BTO and Mn of LSMO at low temperature. This is an important step towards creating EB coupling between FM and FE materials without conventional AFM materials, which may enable a new class of multi-state memory devices by switching magnetization, FE polarisation and EB coupling in the same device.

Effects of the electrode materials and operating environment on magnesium fluoride based bipolar RRAMs

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