CN109841736B - Organic heterojunction resistive random access memory device accurately constructed based on electrochemical method and application thereof - Google Patents
Organic heterojunction resistive random access memory device accurately constructed based on electrochemical method and application thereof Download PDFInfo
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Abstract
The invention belongs to the technical field of information storage devices, and particularly provides an organic heterojunction resistive random access memory device accurately constructed based on an electrochemical method and application thereof. The device consists of a bottom electrode, an active layer with donor property, an active layer with acceptor property and a punctiform top electrode, wherein the donor and the acceptor active layers are controllably prepared based on an electropolymerization method. When different voltages are applied to the organic heterojunction memory device, the device shows different resistance states and has an information storage function. Due to the advantages of the electrochemical method, the connection between the donor active layer and the bottom electrode and between the donor active layer and the receptor active layer is tighter, the contact resistance is lower, and the injection and transmission of carriers during the operation of the device are improved. Therefore, the memory device has a low turn-on voltage, excellent re-writability and stability. The method for preparing the heterojunction by utilizing electropolymerization is simple and efficient, has low cost and can be prepared in a large area.
Description
Technical Field
The invention belongs to the technical field of information storage devices, and particularly relates to an organic heterojunction resistive random access memory device accurately constructed based on an electrochemical method, a construction method and application thereof.
Background
Goren-mol predicted the development of the chip industry 50 years ago: when the price is not changed, the performance of the silicon chip is doubled every 18 to 24 months. Thus, over the next 50 years, the semiconductor industry has also developed moore's law as a goal of industry effort, and the initial simple geometric scaling (making all the components on the chip smaller and smaller) has fully satisfied the needs of people. However, in the last 70 th and 80 th century, with the advent of personal consumer products such as the hewlett packard personal computer, Apple II computer, and IBM PC, and the explosive growth of information volume, the demand for the diversification of functions and miniaturization of electronic products has increased. The processing capacity of the chip is required to be higher and smaller in the industry, the generated heat is larger and larger due to the fact that more and more silicon circuits are integrated in the same small space, and the problems are also gradually revealed, and the circuit precision of the top-level chip manufacturer reaches 14 nanometers and is smaller than most viruses. However, the global semiconductor industry development planning blueprint association chairman Paolo Gargini (Paolo Gargini) represents: by 2020, our chip circuitry can reach the 2-3 nm level at the fastest growth rate, however, only 10 atoms can be accommodated at this level, and by that level, the behavior of electrons is limited by quantum uncertainty and the transistors become unreliable. One predicts that moore's law will move toward dusk. Based on this, as a solution, we think that an organic polymer material is used as an active layer to replace the traditional monocrystalline silicon to prepare the sandwich type resistive memory, which has the advantages of diversified material structures, low cost, easy processing, good flexibility, large-area preparation (processing on a plastic, glass or CMOS hybrid integrated circuit can be performed by spin coating or ink-jet printing), fast response, low power consumption, high-density storage, and the like, and has a very wide application prospect in the fields of information storage and high-speed calculation.
In 1986, Tang first proposed a double-layer heterojunction structure in which two organic active layers were sandwiched between electrodes, which, due to their hole transport ability and electron transport ability, respectively, could facilitate the separation and transport of charge carriers, and used in organic photovoltaic cells. This research has greatly accelerated the development of high efficiency photovoltaic devices such as solar cells, photodetectors, transistors, and light emitting diodes. However, there are few studies reporting the application of the heterojunction structure to the resistive memory device.
In addition, the conventional preparation method of the heterojunction mainly includes a solution method or a vapor deposition method. However, these methods still have some disadvantages such as cumbersome preparation processes, loss and waste of materials, difficulty in large-area preparation, and requirement of expensive equipment. Meanwhile, the heterojunction active layer prepared based on these methods has poor contact with the electrode and the active layer, and surface modification of the electrode or an additional buffer layer is often required to optimize device performance. Electrochemical polymerization is an excellent method for in situ film production. The method is simple to operate, the reaction conditions are mild, and the prepared film can be controllable in thickness and shape. More importantly, the film obtained by electrochemical preparation can enable the film and the surface of the electrode to have stronger acting force, so that the contact resistance between interfaces is reduced to improve the injection and transmission of charges, and the efficiency of the device is improved. Therefore, the heterojunction film prepared by the electrochemical method has huge application prospect.
Disclosure of Invention
Therefore, based on the advantages of the heterojunction structure and the electrochemical method, the invention aims to provide an organic heterojunction resistive random access memory device accurately constructed based on the electrochemical method and application thereof.
One of the objects of the present invention is also to propose an active layer of a heterojunction structure based on an electrochemical process.
The invention further aims to apply the heterojunction active layer to a resistive random access memory device to obtain the stable and reliable organic heterojunction resistive random access memory device with excellent performance.
The technical scheme of the invention is as follows:
a method for accurately constructing an organic heterojunction resistive random access memory device based on an electrochemical method comprises the following steps:
a polybenzothiopyrrole (PBTP) active layer was prepared on the bottom electrode.
And continuously preparing a polythiadiazole isoindoline (PTDI) active layer on the prepared PBTP active layer to obtain the resistance change layer with the heterojunction structure.
And growing a point-shaped top electrode on the heterojunction active layer to finally form the organic heterojunction resistive random access memory.
According to the method for accurately constructing the organic heterojunction resistive random access memory device based on the electrochemical method, further, the preparation of the PBTP active layer comprises the following steps:
directly carrying out in-situ electropolymerization growth on the bottom electrode by using an electrochemical method to prepare a PBTP active layer;
according to the method for accurately constructing the organic heterojunction resistive random access memory device based on the electrochemical method, further, the preparation of the PTDI active layer comprises the following steps:
directly carrying out in-situ electropolymerization growth on the prepared PBTP active layer by using an electrochemical method to prepare a PTDI active layer;
according to the method for accurately constructing the organic heterojunction resistive random access memory device based on the electrochemical method, further, the PBTP and the PTDI active layer are sequentially and continuously prepared by the electrochemical method to obtain the resistive layer with the heterojunction structure, and the method comprises the following steps:
preparing a PBTP active layer on a conductive substrate by in-situ electropolymerization by using an electrochemical method, wherein the electrolyte is acetonitrile, the electrolyte is tetra-n-butyl ammonium hexafluorophosphate with the concentration of 0.001-5M and the concentration of a monomer benzothiophenopyrrole of 0.01-1 mM;
by an electrochemical method, the electrolyte is acetonitrile, the electrolyte is tetra-n-butyl ammonium hexafluorophosphate with the concentration of 0.001-5M and the concentration of the monomer pyrrolobenzothiadiazole is 0.01-1mM, and the prepared PBTP active layer is subjected to in-situ electropolymerization to prepare a PTDI donor layer;
and growing a dotted top electrode on the prepared heterojunction resistance-variable layer by utilizing a thermal evaporation process or a magnetron sputtering process.
The thermal vapor deposition process preferably used in the present invention has a degree of vacuum of 10-4-10-7Pa, operating current of 100-150A, and growing a dot-shaped top electrode on the heterojunction resistance-variable layer obtained by the preparation.
According to the method for accurately constructing the organic heterojunction resistive random access memory device based on the electrochemical method, further, the thickness of the PBTP active layer prepared by utilizing electropolymerization can be controlled to be 20-150nm, the thickness of the PTDI active layer prepared by utilizing electropolymerization can be controlled to be 20-150nm, the thickness of the prepared heterojunction resistive random access layer can be controlled to be 40-300nm, the thickness of the top electrode is 80-300nm, and the diameter is 0.2-0.6 mm.
The bottom electrode and the top electrode are made of any material, including but not limited to conductive metals, such as Au, Ag, Al, Cu, Ti, etc.; conductive metal oxides such as ITO, FTO, etc.
The top and bottom electrodes used may be the same or different.
In one embodiment of the present invention, the prepared PBTP active layer has electron donating properties and can function as a hole transport layer, and the prepared PTDI active layer has electron withdrawing properties and can function as an electron transport layer.
The invention also provides an organic heterojunction resistive random access memory prepared based on an electrochemical method, which sequentially comprises the following components: a bottom electrode, a PBTP active layer, a PTDI active layer and a dotted top electrode; the PBTP and PTDI active layers are prepared in situ through electropolymerization, the two resistance change layers interact to further obtain a resistance change layer with a heterojunction structure, and the heterojunction resistive random access memory is prepared by the method in the embodiment.
The invention also provides application of the organic heterojunction resistive random access memory accurately constructed based on the electrochemical method in information storage and reading and writing.
In order to realize information storage, the reading method of the resistive random access memory with the organic heterojunction structure comprises the following steps: applying a pulse bias voltage of-1.5V to the top electrode of the memory device for writing information, applying a pulse bias voltage in the range of 0.5V to the top electrode again for reading information, then applying a pulse bias voltage in the range of 4.5V to the top electrode for erasing information, and applying a pulse bias voltage in the range of 0.5V to the top electrode again for reading information.
The organic heterojunction active layer is prepared based on an electrochemical method and is further applied to preparation and application of a resistive random access memory. Compared with the traditional preparation method of the heterojunction, the electrochemical method for preparing the heterojunction has the advantages of simplicity, high efficiency, simple and controllable operation, mild reaction conditions and the like, and can be used for large-area preparation. On the other hand, the film is prepared by in-situ electropolymerization, so that the film can be in closer contact with the electrode and the film, the contact resistance is further reduced, and the injection and the transmission of charge carriers are facilitated.
The invention has the following advantages:
1. the invention relates to a method for preparing a PBTP active layer on a bottom electrode by direct electropolymerization based on an electrochemical method and a method for preparing the PBTP active layer on the PBTP active layer
The PTDI active layer prepared by direct electropolymerization can greatly improve the contact between the active layer and the bottom electrode and between the two active layers, and reduce the charge transmission energy barrier.
2. The method for preparing the organic heterojunction resistive random access memory device based on the electrochemical method can realize large-area preparation, is simple and efficient, has low cost, and is completely compatible with the traditional CMOS process.
3. The organic heterojunction resistance-change memory device prepared by the invention benefits from the advantages of an electrochemical preparation method and a heterojunction, has low starting voltage, high on-off ratio and stable repeated read-write cycle operation, and provides insight for the design of the organic resistance-change memory device.
Drawings
FIG. 1 is a schematic diagram of a method for manufacturing an organic heterojunction resistive random access memory device;
FIG. 2 shows a reaction monomer used for preparing an organic heterojunction resistive random access memory device through electropolymerization;
FIG. 3 is a cross-sectional SEM of an ITO loaded PBTP film (a, c, e, g) and an ITO/PBTP loaded PTDI film (b, d, f, h). These films were obtained by electropolymerization scanning for 2, 3, 4 and 5 turns, respectively;
fig. 4 is a graph of a read-write test curve result of the organic heterojunction resistive memory device (the applied pulse voltage width is 57 ms);
FIG. 5 is a graph of high and low resistance state transition test results of an organic heterojunction resistive memory device;
fig. 6 is a graph of stability test results of the organic heterojunction resistive memory device in high and low resistance states, respectively;
fig. 7 is a schematic structural diagram of an organic heterojunction resistive random access memory device.
Detailed Description
The features and advantages of the present invention will become more apparent from the following detailed description of the embodiments of the present invention, which is to be read in connection with the accompanying drawings.
Example 1
Fig. 1 is a schematic diagram of a method for manufacturing an organic heterojunction resistive random access memory device. The method comprises the following steps:
1. and preparing a PBTP active layer on the bottom electrode ITO.
By cyclic voltammetry, the scanning voltage range is-1.0V-1.2V, and the scanning rate is 50mVS-1The electrolyte is acetonitrile, the electrolyte is tetra-n-butyl ammonium hexafluorophosphate with the concentration of 0.1M and the concentration of the monomer benzothiophenopyrrole of 0.01M, and the PBTP active layers with different thicknesses are obtained by continuously scanning for 2-5 circles by taking ITO as a working electrode.
2. And continuously preparing the PTDI active layer on the prepared PBTP active layer to obtain the resistive layer with the heterojunction structure.
By cyclic voltammetry, the scanning voltage range is-1.0V-1.2V, and the scanning rate is 50mVS-1The electrolyte is acetonitrile, the electrolyte is tetra-n-butyl ammonium hexafluorophosphate with the concentration of 0.1M, the monomer thiadiazole isoindole with the concentration of 0.01M, the prepared ITO loaded with the PTDI active layer is used as a working electrode, and the PTDI active layer with different thicknesses is obtained by continuously scanning for 2-5 circles, so that the active layer with the target heterojunction structure is obtained.
Fig. 3 is a cross-sectional SEM image of the PBTP active layer prepared and the final bi-layer heterojunction resistive layer, from which the thickness of the active layer obtained for different scan cycles can be obtained, and also shows that the thickness of the different active layers can be precisely controlled by electrochemical methods.
3. And growing a point-shaped top electrode on the heterojunction active layer to finally form the organic heterojunction resistive random access memory.
Further using thermal evaporation technology to grow a point-shaped Al electrode on the heterojunction resistance-change layer prepared by the method, wherein the thickness of the point-shaped Al electrode is 120nm, and the diameter of the point-shaped Al electrode is 0.3 mm.
Based on the steps, the organic heterojunction resistive random access memory device can be prepared.
In this example, the prepared PBTP active layer has electron donating properties and can act as a hole transport layer, and the prepared PTDI active layer has electron withdrawing properties and can act as an electron transport layer.
Example 2
In this example, a heterojunction having a thickness of 103nm was prepared as an active layer of a memory device using the method in example 1, and an organic heterojunction memory device was further prepared. And then, performing information read-write test on the prepared organic heterojunction memory device. Fig. three is a graph showing the read-write cycle test results of the prepared organic heterojunction memory device.
Applying pulse voltages with different sizes to the organic heterojunction memory device to store and read and write information, and specifically comprising the following steps of:
(1) information reading
A pulse voltage of 0.5V is applied to the device as a read voltage, and the read current is small at 5 × 10-7About A, the device is in a high-resistance state, which indicates that information is not written in;
(2) writing of information
Applying a pulse voltage of-1.5V as a writing voltage on the device, wherein the reading current is suddenly increased, the device is switched from a high resistance state to a low resistance state at about 0.1A, and the operation is an information writing process;
(3) information reading
Applying a pulse voltage of 0.5V to the device as a reading voltage, wherein the reading current is still kept at a higher value, and the device is still in a low resistance state at about 0.02A, which indicates that information is successfully written and the written information is read;
(4) information erasure
A pulse voltage of 4.5V is applied to the device as an erase voltage, at which time the read current is abruptly reduced, at 10-6On the left and right sides of A, the device is converted from a low resistance state to a high resistance state, and the operation is an erasing process of information;
(5) information reading
A pulse voltage of 0.5V is applied to the device as a read voltage, while the read current is still kept small at 5x 10-7About A, the device is in a high resistance state, which indicates that the written information has been successfully erased;
and further carrying out high-low resistance state conversion test on the prepared organic heterojunction memory device. Fig. 5 is a graph showing the high and low resistance state transition test results of the prepared organic heterojunction memory device.
The organic heterojunction memory device is continuously applied with pulse voltages with different sizes to carry out high-low resistance state conversion test, and the specific steps are as follows:
four pulse voltages of-1.5V (writing voltage), 0.5V (reading voltage), 4.5V (erasing voltage) and 0.5 (reading voltage) are continuously and alternately applied to the device to obtain a current change result corresponding to the reading voltage, the high-low resistance state conversion is realized, and the cycle conversion times can reach more than 100 times, which shows that the device has the performance of repeated erasing.
And then, performing a read test on the stability of the high and low resistance states of the prepared organic heterojunction memory device. Fig. 6 is a graph showing the read test result of the stability of the high and low resistance states of the prepared organic heterojunction memory device.
The method for reading the stability of the high and low resistance states of the prepared organic heterojunction memory device comprises the following specific steps:
a pulse voltage of-1.5V is applied to the device to write information, and then a pulse voltage of 0.5V (pulse width of 10 μ s and pulse period of 20 μ s) is applied to the device repeatedly for read test, after 10 times6After the sub-pulse reading, the device still maintains a stable high-impedance state.
Then, a 4.5V pulse voltage is continuously applied to the device to erase information, and a 0.5V pulse voltage (with a pulse width of 10 mus and a pulse period of 20 mus) is repeatedly applied to the device to perform a read test, after 10 mus passes6After the sub-pulse reading, the device remains in a stable low resistance state. The device has better stability in a high-resistance state or a low-resistance state.
In this example, information reading and writing tests were performed on the organic heterojunction memory device prepared in example 1. The test result shows that the prepared organic heterojunction memory device has rewritable memory performance and can keep higher stability after information is read and erased.
The above-described embodiments are intended to illustrate rather than to limit the invention, and modifications and variations of the invention are possible within the spirit and scope of the appended claims.
Claims (7)
1. A method for accurately constructing an organic heterojunction resistive random access memory device based on an electrochemical method is characterized by comprising the following steps:
(1) preparing a PBTP active layer of polybenzothiophene and pyrrole on the bottom electrode;
(2) continuously preparing a polythiadiazole isoindoline PTDI active layer on the prepared PBTP active layer to obtain a resistance change layer with a heterojunction structure;
(3) growing a point-like top electrode on the heterojunction active layer to finally form the organic heterojunction resistive random access memory;
preparing a PBTP active layer comprising: directly carrying out in-situ electropolymerization growth on the bottom electrode by using an electrochemical method to prepare a PBTP active layer;
preparing a PTDI active layer comprising:
and (3) directly carrying out in-situ electropolymerization growth on the prepared PBTP active layer by using an electrochemical method to prepare the PTDI active layer.
2. The method for accurately constructing an organic heterojunction resistive memory device based on an electrochemical method as claimed in claim 1, wherein the PBTP and PTDI active layers are sequentially and continuously prepared using an electrochemical method to obtain a resistive layer of a heterojunction structure,
the method comprises the following specific steps:
(1) preparing a PBTP active layer on a conductive substrate by in-situ electropolymerization by using an electrochemical method, wherein the electrolyte is acetonitrile, the electrolyte is tetra-n-butyl ammonium hexafluorophosphate, the concentration of the electrolyte is 0.001-5M, and the concentration of the monomer benzothiophenopyrrole is 0.01-1M;
(2) continuously carrying out in-situ electropolymerization on the prepared PBTP active layer by using an electrochemical method, wherein the electrolyte is acetonitrile, the electrolyte is tetra-n-butyl ammonium hexafluorophosphate, the concentration of the electrolyte is 0.001-5M, the concentration of the monomer thiadiazole isoindole is 0.01-1M, and the prepared PBTP active layer is used for preparing a PTDI donor layer;
(3) and growing a dotted top electrode on the prepared heterojunction resistance-variable layer by utilizing a thermal evaporation process or a magnetron sputtering process.
3. The method for accurately constructing an organic heterojunction resistive-switching memory device based on an electrochemical method as claimed in claim 2, wherein the thickness of the PBTP active layer prepared by using electropolymerization is controlled to be 20-150nm, the thickness of the PTDI active layer prepared by using electropolymerization is controlled to be 20-150nm, the thickness of the prepared heterojunction resistive-switching layer is controlled to be 40-300nm, the thickness of the top electrode is 80-300nm, and the diameter is 0.2-0.6 mm.
4. The method for accurately constructing an organic heterojunction resistive-switching memory device based on an electrochemical method according to claim 1, wherein the bottom electrode and the top electrode comprise a conductive metal and/or a conductive metal oxide; the conductive metal is Au, Ag, Al, Cu or Ti; the conductive metal oxide is ITO or FTO; the top or bottom electrodes used may be the same or different.
5. The method for accurately constructing the organic heterojunction resistive-switching memory device based on the electrochemical method as claimed in claim 1, wherein the prepared PBTP active layer has an electron-donating property and can serve as a hole transport layer, and the prepared PTDI active layer has an electron-withdrawing property and can serve as an electron transport layer.
6. An organic heterojunction resistive random access memory accurately constructed based on an electrochemical method is characterized by sequentially comprising: a bottom electrode, a PBTP active layer, a PTDI active layer and a dotted top electrode; wherein, both the PBTP and the PTDI active layer are prepared in situ by electropolymerization, and the two resistance change layers interact to further obtain a resistance change layer with a heterojunction structure, and the heterojunction resistance change memory is prepared by the method of any one of claims 1 to 5.
7. An implementation mode for accurately constructing information storage and reading and writing of an organic heterojunction resistive random access memory based on an electrochemical method is characterized in that the organic heterojunction resistive random access memory prepared by the method of any one of claims 1 to 5 or the organic heterojunction resistive random access memory of claim 6 is subjected to voltage scanning, and the implementation mode comprises the following steps:
applying a pulse bias voltage of-1.5V to the top electrode of the memory device for writing information, applying a pulse bias voltage in the range of 0.5V to the top electrode again for reading information, then applying a pulse bias voltage in the range of 4.5V to the top electrode for erasing information, and applying a pulse bias voltage in the range of 0.5V to the top electrode again for reading information.
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