Mixed metal oxide-based memristor

FIELD: chemistry.

SUBSTANCE: memristor devices are nonvolatile memory devices and can be used to design computer systems based on an artificial neural network architecture. The present device consists of an active layer situated between two current-conducting layers with which it is in electrical contact. The active layer has a resistive switching property and is a double-layer oxide structure HfAlxOy/HfO2. The HfAlxOy layer has high solubility and high equilibrium concentration of oxygen vacancies, and HfO2 is a layer with low solubility of vacancies. The current-conducting layers are made of titanium nitride or tungsten nitride. A super-thin layer of ruthenium oxide with thickness of not less than 0.5 nm is deposited on the HfO2/TiN boundary surface.

EFFECT: high stability of modes of switching resistance to a low- and high-ohmic state, low switching voltage, high technological compatibility with existing silicon-based microcircuit manufacturing processes.

3 cl, 2 dwg


The invention relates to devices for micro - and nanoelectronics based on advanced materials and can be used in memory devices of computers, microprocessors, portable electronic devices, electronic cards. Memristors device can be used to build computer systems based on the architecture of artificial neural networks.

For the first time the effect of memristive was demonstrated in 2008 for the system Pt-TiO2-TinO2n-1-Pt [D.B. Strukov, G.S. Snider, D.R. Stewart, R.S. Williams. The missing memristor found. Nature, 2008, 453, p.80]. Using such elements demonstrated the ability to implement a new architecture calculations [J. Joshua Yang, Matthew D. Pickett, Xuema Li, Douglas A.A. Ohiberg, Duncan R. Stewart and R. Stanley Williams, Nat. Nanotechnology 2008, 3 429]. As in the traditional system of layers of TiO2-TinO2n-1the distribution of charge carriers (oxygen vacancies) in the film thickness has a random character, special attention is paid to the creation of a controlled distribution profile of impurities in the volume of the active layer for the effective management of the charge carriers in the memristor [Quitoriano N.J., P.J. Kuekes, Yang J. Controlled placement of dopants in memristor active regions. WO 2010085225. 29.07.2010]. To achieve similar results can be achieved by ion implantation of elements having a large number of valence electrons in the volume of the active layer and the latter is a corresponding annealing [Tang D., Xiao H. Method for forming memristor material and electrode structure with memristance. US 20090317958. 24.12.2009]. At a certain depth are formed region rich in vacancies with a negative charge. However, the use of ion implantation allows you to precisely control and flexibility to adjust the number and distribution of implanted atoms and, respectively, regions, enriched by the charge carriers in the film thickness of 10 nm or more. Since the active layer of the memristor often has a thickness of about 3-10 nm, the method of ion implantation is not optimal for the formation of a homogeneous distribution of impurities and, accordingly, does not improve the stability characteristics of the memristor. Therefore, the resistive switching memory elements using non-stoichiometric oxides of transition metals in most cases is not stable: the switch parameters, such as the value of the current in the high resistance and low resistance state, the threshold voltage transitions from one state to another, can vary from cycle to cycle. The total number of switches is small, then, as a rule, the degradation of the structure, which structure is irreversibly enters a low impedance state.

Known memristor-based mixed oxide of the metals of type A + B4+O3, where a is divalent element, and is titanium, or circa the Institute of economy and management, or hafnium [Quitoriano N.J., Ohiberg D.; Kuekes, P.J., Yang J. Using alloy electrodes to dope memristors. WO 2010085226. 29.07.2010].

The disadvantages of the considered technical solutions include:

- at least one of the conductive layers is made of Pt or Au, or alloys based on them;

- when using divalent metal as the second element of the complex oxide formation enthalpy of communication is positive, while the binding energy is quite high. As a result of this the memristor should have relatively low homogeneity and conductivity, which, in turn, leads to non-uniformities in the electric field distribution in the active layer and respectively low stability and repeatability characteristics of the memristor.

The closest in technical essence of the device adopted for the prototype, is the memristor-based mixed oxide of the metals [EN 2472254 C1, 14.11.2011]. In the conditions of the active layer is a mixed oxide, one element of which is titanium or zirconium, or hafnium, and the second element is a trivalent metal ion radius equal to 0,7-1,2 ionic radius titanium, or zirconium, or hafnium, respectively. If mixed metal oxide contains one element zirconium or hafnium, the second element contains scandium, or yttrium or lutetium.

To cons is tkam consider technical solutions include the following:

- functioning of the memristor is caused by the formation under the action of an external field in the active layer two subsoil with different concentration of vacancies. The absence of structural separation subsoil leads to lower stability and repeatability of switching modes, and requires electric mode molding at elevated voltages;

- to obtain a high concentration of charged oxygen vacancies one of the conductive layers is made of palladium. Noble metals such as Pt, Au, Pd, poorly compatible with silicon technology for the production of chips.

The technical result of the proposed invention is to improve the stability of the switching modes of resistance in low - and high-resistance state, a voltage reduction switch, high technological compatibility with existing processes for the production of silicon chips.

The solution of this problem is achieved by the fact that the memristor-based mixed oxide of metals consisting of alternating layers, namely, the active layer, located between two conductive layers, and the active layer includes a mixed oxide according to the invention the active layer consists of two sublayers, one of which is an oxide of hafnium, and the second is a mixed oxide, one element of which one is camping hafnium, and the second aluminum, and also between the conductive and the adjacent layer of hafnium oxide is placed a layer of ruthenium oxide, having a thickness not less than 0.5 nm.

In the particular case as a conductive layer is titanium nitride or tungsten nitride.

In addition, in the mixed oxide, the atomic ratio of the concentrations of aluminum to hafnium is in the range of 0.2-0.5

The invention is illustrated in the following description and the accompanying drawings.

Figure 1 - scheme of the memristor.

The memristor-based mixed metal oxide contains the active layer 1 located between the lower conductive layer 2 and the upper conductive layer 3. The active layer 1 consists of two sublayers: 1a - mixed oxide HfAlxOyand 1b - binary oxide HfO2. Between the upper conductive layer 3 and layer 1b is placed a layer 4 of ruthenium oxide thickness greater than 0.5 nm.

Figure 2 (a) spectra of x-ray photoelectron spectroscopy line Hf4f active layer in contact with RUO Li2line 1 and TiN - line 2; (b) diagram of the band structure and potential distribution in the active layer.

To improve the stability of the frequency of occurrence of switching modes in the active layer is implemented structural separation into two regions: a region containing a high concentration of oxygen vacancies and the source and the battery is a PR job, and the area in which by increasing the concentration of vacancies in the drift of the first area involves condensation of vacancies with the formation of conductive channels. For the formation of the layer, where the condensation of vacancies, the selected binary oxide HfO2with the low solubility of oxygen vacancies. Layer accumulating vacancy must have a high solubility of vacancies and the high equilibrium concentration of vacancies.

In accordance with theoretical calculations [N. W. Zhang, W. Gao, W. Sun, G. Chen, L. Zeng, L.Liu, X. Liu, J. Lu, R. Han, J. Kang, and B. Yu, Appl. Phys. Lett. 96 (2010) 123502] the formation energy of oxygen vacancies in ZrO2and HfO2significantly reduced when adding dopasowywa Al impurities, which leads to higher equilibrium concentration of vacancies. In addition, the films HfAlxOyin a wide interval of concentrations of Al (x>0.1) remain amorphous, which may lead to an increase in the solubility of vacancies. The maximum concentration of oxygen vacancies is observed in the interval x=0.2-0.5. An important factor is that the doped HfO2aluminum does not reduce the width of the forbidden zone. Therefore, as accumulating layer HfAlxOycan be considered as one of the most suitable oxides in the system IU4+IU3+xOy.

When choosing the material for the wire is included layers defining condition, that at least one of the layers should consist of a material having a high work function. Typically such material using one of the noble metals (Pt, Au, Pd). However, the use of these metals in silicon technologies circuits is highly undesirable. It has been found that increasing the effective work function of the electrode made of TiN, up to 5 eV at the interface of TiN/HfO2it is enough to place the ultra-thin layer of conductive ruthenium oxide thickness greater than 0.5 nm. The thickness of the ruthenium oxide is less than 0.5 nm leads to intermediate work function of the electrode in the range of 4.4 to 5.0 eV.

On figa presents XPS spectra line Hf4f for two cases: (1) when the active layer is deposited on the TiN electrode with sublayer RUO Li2and (2) when the active layer is deposited on the TiN electrode without additional sub-layer at the interface.

In case (2) line Hf4f is a single well-resolved doublet Hf4f5/2/Hf4f7/2. This indicates that the active layer is no volume charge and is not observed potential distribution along the depth of the layer.

In case (1), when the active layer is in contact with RUO Li2observed broadening and shift of the line Hf4f, caused by the appearance of a space charge in the active layer. Decomposition of the spectrum line three doublets with different what argemi communication allows to obtain information about the potential distribution in the active layer and to model the band structure (fig.2b). These measurements confirm the assumption that the mixed oxide HfAlxOysource after deposition contains a high equilibrium concentration of charged oxygen vacancies. Upon contact with a conductor having a large work function, vacancies are charged and the Fermi levels are aligned. It can be concluded that the level of charged oxygen vacancies in HfAlxOyequal to 4.3 eV. Therefore, when the contact of the active layer, a TiN layer having a work function of 4.3 to 4.6 eV, vacancies are not charged and remain neutral, and in contact with the ruthenium oxide having a work function of 5.1 eV, vacancies, located in the in the sphere of mixed oxide charge and the active layer there is the potential drop.

Thus, the use of sub-HfAlxOyin the active layer of the memristor allows to obtain a high initial content of neutral oxygen vacancies, and the use of an electrode with an intermediate layer RUO Li2leads to the charging of these positions.

Examples of implementation of the selected memristor

On the oxidized silicon substrate Si-SiO2(the thickness of the oxide 50 nm) by magnetron sputtering deposited conductive layer of TiN with a thickness of 200 nm.

On the substrate formed with the bottom electrode was deposited active layer consists of two sublayers: HfAl0.4Oxthickness of 4 nm and Hf 2thickness of 3 nm. The deposition was carried out by atomic layer deposition at a temperature of 240°C. as precursors used Hf[N(CH3)(C2H5)]4, Al(CH3)3and H2O.

To the active layer not covered by the pads of the lower electrodes and isolating them electrically, before applying the dielectric layer surface of the pads was covered electronic resist the polymethylmethacrylate. After application of the active layer, the resist was removed.

On the surface formed of the active layer through a shadow mask was applied to the upper electrodes. One sample was applied 10 the upper electrode 200 µm in diameter.

The sequence of deposition of the upper electrode:

1) through a shadow mask by pulsed laser deposition deposited layer of ruthenium oxide thickness of 2 nm. The deposition of a layer of ruthenium oxide was carried out by laser ablation of a metallic target EN in the atmosphere of oxygen at a pressure of 10-2Torr;

2) through the same shadow mask by magnetron sputtering deposited TiN layer thickness of 50 nm.

In pairs between the lower and upper electrodes was connected measuring instrument Agilent U2722A, includes power supply and current meter. Measurement of current-voltage characteristics of the voltage range from-2,5 SAR 2.5 V and the switching of the memristor from the high resistance state to low resistance and Vice versa was performed using the standard operating program of the device. The resistance of the high resistance and low resistance States of the memristor was averaged over 100 cycles switch from high resistance to low resistance state and Vice versa.

For ten formed memristors were obtained following characteristics: voltage switch from high resistance to low resistance state was 1.5±0.1 V, the resistance in the high resistance and low resistance States, measured at a voltage of 0.2 V, amounted ROFF=950±40 Ω, RON=50±2 Ohms respectively. The dispersion of the values of the resistances in the resistance in the low resistance state is 5%, the dispersion of the values of the voltage switching does not exceed 6%. These results suggest that the use of the proposed structure allows to obtain a memristor with a highly stable and well reproducible characteristics with high technological compatibility with the processes of production of silicon chips.

1. The memristor-based mixed oxide of metals consisting of alternating layers, namely, the active layer, located between two conductive layers, and the active layer includes a mixed oxide, wherein the active layer consists of two sublayers, one of which is an oxide of hafnium, and the second is a mixed oxide, one element of which is hafnium, and the second is aluminum, and also between conducting the adjacent layer of hafnium oxide is placed a layer of ruthenium oxide, having a thickness not less than 0.5 nm.

2. The memristor according to claim 1, characterized in that the conductive layer is titanium nitride or tungsten nitride.

3. The memristor according to claim 1, characterized in that the mixed oxide, the atomic ratio of the concentrations of aluminum to hafnium is in the range of 0.2-0.5.


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