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Register a new userDirect Observation of Localized Radial Oxygen Migration in Functioning Tantalum Oxide Memristors
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Oxygen migration in tantalum oxide, a promising next-generation storage material, is studied using in-operando x-ray absorption spectromicroscopy and is used to microphysically describe accelerated evolution of conduction channel and device failure. The resulting ring-like patterns of oxygen concentration are modeled using thermophoretic forces and Fick diffusion, establishing the critical role of temperature-activated oxygen migration that has been under question lately.
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While the recent establishment of the role of thermophoresis/diffusion-driven oxygen migration during resistance switching in metal oxide memristors provided critical insights required for memristor modeling, extended investigations of the role of oxygen migration during ageing and failure remain to be detailed. Such detailing will enable failure-tolerant design, which can lead to enhanced performance of memristor-based next-generation storage-class memory. Here we directly observed lateral oxygen migration using in-situ synchrotron x-ray absorption spectromicroscopy of HfOx memristors during initial resistance switching, wear over millions of switching cycles, and eventual failure, through which we determined potential physical causes of failure. Using this information, we reengineered devices to mitigate three failure mechanisms, and demonstrated an improvement in endurance of about three orders of magnitude.
Transition metal oxide memristors, or resistive random-access memory (RRAM) switches, are under intense development for storage-class memory because of their favorable operating power, endurance, speed, and density. Their commercial deployment critically depends on predictive compact models based on understanding nanoscale physico-chemical forces, which remains elusive and controversial owing to the difficulties in directly observing atomic motions during resistive switching, Here, using scanning transmission synchrotron x-ray spectromicroscopy to study in-situ switching of hafnium oxide memristors, we directly observed the formation of a localized oxygen-deficiency-derived conductive channel surrounded by a low-conductivity ring of excess oxygen. Subsequent thermal annealing homogenized the segregated oxygen, resetting the cells towards their as-grown resistance state. We show that the formation and dissolution of the conduction channel are successfully modeled by radial thermophoresis and Fick diffusion of oxygen atoms driven by Joule heating. This confirmation and quantification of two opposing nanoscale radial forces that affect bipolar memristor switching are important components for any future physics-based compact model for the electronic switching of these devices.
Unconventional ferroelectricity, robust at reduced nanoscale sizes, exhibited by hafnia-based thin-films presents tremendous opportunities in nanoelectronics. However, the exact nature of polarization switching remains controversial. Here, we investigate epitaxial Hf0.5Zr0.5O2 (HZO) capacitors, interfaced with oxygen conducting metals (La0.67Sr0.33MnO3, LSMO) as electrodes, using atomic resolution electron microscopy while in situ electrical biasing. By direct oxygen imaging, we observe reversible oxygen vacancy migration from the bottom to the top electrode through HZO and reveal associated reversible structural phase transitions in the epitaxial LSMO and HZO layers. We follow the phase transition pathways at the atomic scale and identify that these mechanisms are at play both in tunnel junctions and ferroelectric capacitors switched with sub-millisecond pulses. Our results unmistakably demonstrate that oxygen voltammetry and polarization switching are intertwined in these materials.
Direct evidence of quantum coherence in a single-molecule magnet in frozen solution is reported with coherence times as long as T2 = 630 ns. We can strongly increase the coherence time by modifying the matrix in which the single-molecule magnets are embedded. The electron spins are coupled to the proton nuclear spins of both the molecule itself and interestingly, also to those of the solvent. The clear observation of Rabi oscillations indicates that we can manipulate the spin coherently, an essential prerequisite for performing quantum computations.
Ionic liquid gating can markedly modulate the materials carrier density so as to induce metallization, superconductivity, and quantum phase transitions. One of the main issues is whether the mechanism of ionic liquid gating is an electrostatic field effect or an electrochemical effect, especially for oxide materials. Recent observation of the suppression of the ionic liquid gate-induced metallization in the presence of oxygen for oxide materials suggests the electrochemical effect. However, in more general scenarios, the role of oxygen in ionic liquid gating effect is still unclear. Here, we perform the ionic liquid gating experiments on a non-oxide material: two-dimensional ferromagnetic Cr2Ge2Te6. Our results demonstrate that despite the large increase of the gate leakage current in the presence of oxygen, the oxygen does not affect the ionic liquid gating effect (< 5 % difference), which suggests the electrostatic field effect as the mechanism on non-oxide materials. Moreover, our results show that the ionic liquid gating is more effective on the modulation of the channel resistances compared to the back gating across the 300 nm thick SiO2.
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