CN109841736A - One kind accurately constructing organic heterojunction resistive memory and its application based on electrochemical method - Google Patents
One kind accurately constructing organic heterojunction resistive memory and its application based on electrochemical method Download PDFInfo
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- CN109841736A CN109841736A CN201811394320.4A CN201811394320A CN109841736A CN 109841736 A CN109841736 A CN 109841736A CN 201811394320 A CN201811394320 A CN 201811394320A CN 109841736 A CN109841736 A CN 109841736A
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Abstract
The invention belongs to information recording device technical fields, specifically provide one kind based on electrochemical method and accurately construct organic heterojunction resistive memory and its application.The device has hearth electrode, has active layer and dotted top electrode composition to the active layer of volume property, with receptor property, and wherein donor and the electropolymerization method that is all based on of acceptor active layer carry out controllable preparation.When applying different voltages to the organic heterojunction memory device, which shows different resistance states, has information storage function.Have benefited from the advantage of electrochemical method, so that the connection between donor active layer and hearth electrode and between donor active layer and acceptor active layer is even closer, contact resistance is smaller, the injection and transmission of carrier when improving device work.Therefore, memory device has low cut-in voltage, excellent rewritable and stability.It is provided by the invention to prepare hetero-junctions using the method for electropolymerization, it is simple and efficient, it is at low cost, it can large area preparation.
Description
Technical field
A kind of had the invention belongs to information recording device technical field more particularly to based on what electrochemical method accurately constructed
Machine hetero-junctions resistive memory and structure method and its application.
Background technique
Before 50 years, Gordon mole makes a practice of foretelling to the development of chip industry: when price is constant, the performance of silicon chip is every
One times will be promoted every 18-24 months.Like this in more than the 50 years later times, semicon industry is also with the work of Moore's Law
The target made great efforts for industry is developed, and originally it is complete to reduce (keeping all components on chip smaller and smaller) for simple geometric proportion
It can satisfy the demand of people entirely.However, 1970s and the eighties, as Hewlett-Packard's PC, Apple II are calculated
The birth of the personal consumption product such as machine and IBM PC and the growth of information explosion formula, so that function of the people to electronic product
It can diversification and micromation demand increase.Industry is higher and higher to the processing capacity requirement of chip, and volume requirement is smaller and smaller, by
More and more silicon circuits are integrated in same small space, the heat of generation is also increasing, and there are also more bigger problems
Also slowly show, the circuit precision of nowadays top chip manufacturer has reached 14 nanometers, also smaller than most of viruses.But
It is that global semiconductor industry research and development blue print association chairman Borrow's jar (unit of capacitance) Ji Buddhist nun (Paolo Gargini) indicate: " arriving
The year two thousand twenty, from the point of view of most fast development speed, our chip route can achieve 2-3 Nano grade, however in this rank
On can only accommodate 10 atoms, arrived such rank, the behavior of electronics will be limited by the uncertainty of quantum, and transistor will become
It is unreliable to obtain.So people predict that Moore's Law will move towards dusk.Based on this, as a kind of solution, it is believed that benefit
It uses high-molecular organic material as active layer, sandwich type resistance-variable storing device is prepared instead of traditional monocrystalline silicon, with material
Material structure diversification, at low cost, easy processing, flexibility be good, can large area prepare (can by spin coating or inkjet printing, plastics,
Processed above glass, CMOS hydrid integrated circuit), response fast, low in energy consumption, high density storage the advantages that, stored in information
And supercomputing field has a very wide range of applications prospect.
1986, Tang was put forward for the first time double layer heterojunction structure and has been used for organic photovoltaic battery, in this configuration,
Between the electrodes by two organic active layer folders, since it is respectively provided with cavity transmission ability and electron transport ability, Jin Erke
To promote the separation and transmission of electric charge carrier.This research greatly accelerates solar battery, photoelectric detector, transistor
With the development of the efficient photoelectric device such as light emitting diode.But seldom studies have reported that the heterojunction structure is applied to resistive
Memory device.
In addition, the traditional preparation methods of hetero-junctions mainly include solwution method or vapour deposition process.However, these methods are still
So there is some disadvantages, such as cumbersome preparation process, the loss and waste of material, it is difficult to which large area prepares and need valuableness
Equipment.Meanwhile hetero-junctions active layer contact between electrode and active layer based on the preparation of these methods is very poor, usually needs
Electrode is surface modified or additional buffer layer carrys out optimized device performance.Electrochemical polymerization is an outstanding method
Preparation for in-situ film.It is not only easy to operate, and reaction condition is mild, and thickness and shape may be implemented in the film of preparation
It is controllable in looks.Importantly, the film that electrochemistry is prepared can make film and electrode surface have stronger active force,
And then reduce the contact resistance between interface to improve the injection and transmission of charge, improve the efficiency of device.Therefore, electrification is utilized
Method, which prepares hetero-junction thin-film, huge application prospect.
Summary of the invention
Therefore, the advantages of being based on above-mentioned heterojunction structure and electrochemical method, it is an object of that present invention to provide one kind to be based on
Electrochemical method accurately constructs organic heterojunction resistive memory and its application.
The one of purpose of the present invention also resides in the work for proposing a kind of heterojunction structure based on electrochemical method preparation
Property layer.
Present invention further object therein is for the hetero-junctions active layer to be applied in resistive memory, obtains one
Kind is had excellent performance, reliable and stable organic heterojunction resistive memory.
Technical solution of the present invention:
A method of accurately constructing organic heterojunction resistive memory based on electrochemical method, comprising:
Polyphenyl bithiophene and pyrroles (PBTP) active layer are prepared on hearth electrode.
Continue to prepare polythiadiazoles iso-indoles (PTDI) active layer on the PBTP active layer prepared, obtains having heterogeneous
The change resistance layer of junction structure.
Dotted top electrode is grown on hetero-junctions active layer, ultimately forms organic heterojunction resistance-variable storing device.
The method according to the present invention that organic heterojunction resistive memory is accurately constructed based on electrochemical method, into
One step prepares PBTP active layer, comprising:
Using electrochemical method, the growth of direct in-situ electropolymerization prepares PBTP active layer on hearth electrode;
The method according to the present invention that organic heterojunction resistive memory is accurately constructed based on electrochemical method, into
One step prepares PTDI active layer, comprising:
Using electrochemical method, direct in-situ electropolymerization growth preparation PTDI is active on the PBTP active layer prepared
Layer;
The method according to the present invention that organic heterojunction resistive memory is accurately constructed based on electrochemical method, into
One step successively continuously prepares PBTP and PTDI active layer using electrochemical method, obtains the change resistance layer of heterojunction structure, comprising:
Using electrochemical method, electrolyte selects acetonitrile, and electrolyte selects tetra-n-butyl ammonium hexafluorophosphate, and concentration is
The concentration of 0.001-5M, monomer benzothiophene and pyrroles are 0.01-1mM, and electropolymerization preparation PBTP in situ is living in conductive substrates
Property layer;
Using electrochemical method, electrolyte selects acetonitrile, and electrolyte selects tetra-n-butyl ammonium hexafluorophosphate, and concentration is
The concentration of 0.001-5M, pyrrole and diazosulfide is 0.01-1mM, is continued on the above-mentioned PBTP active layer prepared
PTDI donor layer is prepared in electropolymerization in situ;
Using hot evaporation process or magnetron sputtering technique, dotted top is grown on the above-mentioned hetero-junctions change resistance layer being prepared
Electrode.
In the present invention preferably by hot evaporation process, vacuum degree 10-4-10-7Pa, operation electric current 100-150A,
Dotted top electrode is grown on the above-mentioned hetero-junctions change resistance layer being prepared.
The method according to the present invention that organic heterojunction resistive memory is accurately constructed based on electrochemical method, into
One step can be controlled in 20-150nm using the thickness of the PBTP active layer of electropolymerization preparation, and the PTDI using electropolymerization preparation is living
The thickness of property layer can be controlled in 20-150nm, and the thickness for the hetero-junctions change resistance layer being prepared can be controlled in 40-300nm, described
Top electrode with a thickness of 80-300nm, diameter 0.2-0.6mm.
The hearth electrode and top electrode, material is unlimited, including but not limited to conductive metal, such as Au, Ag, Al, Cu, Ti
Deng;Conductive metal oxide, such as ITO, FTO etc..
Top electrode and hearth electrode used can be the same or different.
In one embodiment of the invention, prepared PBTP active layer has electron characteristic, can serve as hole
Transport layer, prepared PTDI active layer have electrophilic characteristic, can serve as electron transfer layer.
The present invention also propose it is a kind of based on electrochemical method preparation organic heterojunction resistance-variable storing device, successively include:
Hearth electrode, PBTP active layer, PTDI active layer and dotted top electrode;Wherein, PBTP and PTDI active layer is all to pass through electropolymerization
It is prepared in situ, two change resistance layer interactions further obtain the change resistance layer of heterojunction structure, the hetero-junctions resistance-change memory
Prepared by device method as described in above-described embodiment forms.
Organic heterojunction resistance-variable storing device is accurately constructed based on electrochemical method the present invention also provides one kind to store in information
With the application in read-write.
In order to realize that information stores, a kind of reading of the resistance-variable storing device with organic heterojunction structure of the embodiment of the present invention
Take method, comprising the following steps: the pulsed bias progress information of application -1.5V is write on the top electrode of the memory device
Enter, applies the reading that a pulsed bias within the scope of 0.5V carries out information on top electrode again, then applied on top electrode
Add a pulsed bias within the scope of 4.5V to carry out the erasing of information, applies an arteries and veins within the scope of 0.5V on top electrode again
Punching is biased into row information reading.
One kind provided by the invention prepares organic heterojunction active layer based on electrochemical method, and it is further applied
In the preparation and application of resistive memory.It is traditional compared to hetero-junctions before to obtain preparation method, it electrochemically prepares different
The advantages that matter knot, which has, to be simple and efficient, easy to operate controllable, and reaction condition is mild, while large area preparation can also be carried out.It is another
Aspect, electropolymerization in situ prepare film, contact even closer between film and electrode and film may be implemented, and then reduce
Contact resistance, conducive to the injection and transmission of electric charge carrier.
The present invention has following advantage:
1. the present invention mention based on electrochemical method on hearth electrode direct electropolymerization preparation PBTP active layer and
PBTP active layer
Direct electropolymerization preparation PTDI active layer can greatly improve active layer and hearth electrode and two active layers it
Between contact, reduce charge transmit energy barrier.
2. the method provided by the invention for preparing organic heterojunction resistive memory based on electrochemical method, may be implemented
The preparation of large area, and preparation method is simple and efficient, it is at low cost, it is completely compatible with traditional CMOS technology.
3. the organic heterojunction resistive memory that the present invention is prepared, electrochemical preparation method and heterogeneous is benefited from
The advantages of knot, has showed the low cut-in voltage of the device, high on-off ratio and multiple read-write circulate operation that can be stable, is organic
The design of resistive memory provides opinion.
Detailed description of the invention
Fig. 1 is the preparation method schematic diagram of organic heterojunction resistive memory;
Fig. 2 is that electropolymerization prepares reaction monomers used in organic heterojunction resistive memory;
Fig. 3 is the section that ITO loads PBTP film (a, c, e, g) and ITO/PBTP loads PTDI film (b, d, f, h)
SEM figure.These films are obtained by 2 circle of electropolymerization scanning, 3 circles, 4 circles and 5 circles respectively;
Fig. 4 is that (the pulse voltage width of application is for the readwrite tests Dependence Results figure of organic heterojunction resistive memory
57ms);
Fig. 5 is the high low resistance state conversion testing result figure of organic heterojunction resistive memory;
Fig. 6 is organic heterojunction resistive memory respectively in the stability test result figure of high low resistance state;
Fig. 7 is organic heterojunction resistive memory structural schematic diagram.
Specific embodiment
With reference to the accompanying drawing, detailed description of the present invention embodiment, so that the features and advantages of the present invention can be brighter
Show understandable.
Embodiment 1
The preparation method schematic diagram of organic heterojunction resistive memory as shown in Figure 1.This method comprises the following steps:
1. preparing PBTP active layer on hearth electrode ITO.
Using cyclic voltammetry, scanning voltage range is -1.0V -1.2V, sweep speed 50mVS-1, electrolyte selection
Acetonitrile, electrolyte select tetra-n-butyl ammonium hexafluorophosphate, and concentration 0.1M, simultaneously the concentration of pyrroles is monomer benzothiophene
0.01M, using ITO as working electrode, continuous scanning 2-5 circle obtains the PBTP active layer of different-thickness.
2. continuing to prepare PTDI active layer on the PBTP active layer prepared, the resistive with heterojunction structure is obtained
Layer.
Using cyclic voltammetry, scanning voltage range is -1.0V -1.2V, sweep speed 50mVS-1, electrolyte selection
Acetonitrile, electrolyte select tetra-n-butyl ammonium hexafluorophosphate, concentration 0.1M, and the concentration of monomer thiadiazoles iso-indoles is 0.01M,
It prepares load using above-mentioned and has the ITO of PTDI active layer as working electrode, continuous scanning 2-5 is enclosed, and obtains different-thickness
PTDI active layer results in the active layer of target heterojunction structure.
Fig. 3 show the section SEM figure of the PBTP active layer being prepared and final double layer heterojunction change resistance layer, by
This can get the thickness of the obtained active layer of different scanning circle number, and difference can accurately be controlled using electrochemical method by also indicating that
The thickness of active layer.
3. growing dotted top electrode on hetero-junctions active layer, organic heterojunction resistance-variable storing device is ultimately formed.
Hot evaporation process is further utilized, dotted Al electrode is grown on the above-mentioned hetero-junctions change resistance layer being prepared, it is thick
It is 0.3mm that degree, which is 120nm diameter,.
Based on above-mentioned steps, organic heterojunction resistive memory can be prepared.
In this embodiment, prepared PBTP active layer has electron characteristic, can serve as hole transmission layer, made
Standby PTDI active layer has electrophilic characteristic, can serve as electron transfer layer.
Embodiment 2
In the present embodiment, the hetero-junctions with a thickness of 103nm is prepared as memory using the method in embodiment 1
The active layer of part, and organic heterojunction memory device is further prepared.Then, the organic heterojunction being prepared is stored
The readwrite tests of device progress information.It is as shown in Figure 3 the read-write loop test result of the organic heterojunction memory device of preparation
Figure.
The storage and read-write that different size of pulse voltage carries out information are applied to the organic heterojunction memory device, specifically
Steps are as follows:
(1) information is read
Apply the pulse voltage of a 0.5V size on the device as reading voltage, at this point, read current is smaller,
5x 10-7A or so, device are in high-impedance state, show that information is not written;
(2) information is written
Apply the pulse voltage an of -1.5V size on the device as write-in voltage, at this point, read current increases suddenly
Greatly, in 0.1A or so, device is converted to low resistance state from high-impedance state, which is to information writing process;
(3) information is read
Apply the pulse voltage of a 0.5V size on the device as voltage is read, at this point, read current is still protected
It holds in higher numerical value, in 0.02A or so, device is still within low resistance state, shows that information is successfully written into, and read and write
The information entered;
(4) information erasing
Apply the pulse voltage of a 4.5V size on the device as erasing voltage, at this point, read current subtracts suddenly
It is small, 10-6A or so, device are converted to high-impedance state from low resistance state, which is the erase process to information;
(5) information is read
Apply the pulse voltage of a 0.5V size on the device as voltage is read, at this point, read current is still protected
It holds in lesser numerical value, in 5x 10-7A or so, device are in high-impedance state, show that the information of write-in has been successfully erased;
High low resistance state conversion testing further is carried out to the organic heterojunction memory device of preparation.It is illustrated in figure 5 preparation
Organic heterojunction memory device high low resistance state conversion testing result figure.
The conversion survey that different size of pulse voltage carries out high low resistance state is continuously applied to the organic heterojunction memory device
Examination, the specific steps are as follows:
Constantly alternately application -1.5V (write-in voltage) on the device, 0.5V (read voltage), 4.5V (erasing voltage) and
0.5 (reading voltage) four pulse voltage, obtains reading the corresponding curent change of voltage as a result, turning for high low resistance state is presented
It changes, and recycles conversion times up to 100 times or more, show that device has and repeat erasable performance.
Then, the read test of high low resistance state stability is carried out to the organic heterojunction memory device of preparation.As shown in Figure 6
For the read test result figure of the high low resistance state stability of the organic heterojunction memory device of preparation.
The read test of high low resistance state stability is carried out to the organic heterojunction memory device of preparation, the specific steps are as follows:
The pulse voltage for applying-a 1.5V first on the device, is written information, then, repeats to apply one to device
The pulse voltage (pulse width is 10 μ s, and the pulse period is 20 μ s) that a size is 0.5V is read out test, is passing through 106It is secondary
After pulse is read, device stills remain in stable high-impedance state.
Then, to the pulse voltage for continuing to a 4.5V on the device, erasure information continues to repeat to apply to device
The pulse voltage (pulse width is 10 μ s, and the pulse period is 20 μ s) that one size is 0.5V is read out test, is passing through 106
After subpulse is read, device stills remain in stable low resistance state.Illustrate that device suffers from preferably in high-impedance state or low resistance state
Stability.
In the present embodiment, the read-write that information has been carried out based on the organic heterojunction memory device prepared in embodiment 1 is surveyed
Examination.Test result shows that the organic heterojunction memory device of preparation has and repeats erasable storage performance, and its reading and
After erasure information, higher stability can be kept.
Above-described embodiment is used to illustrate the present invention, rather than limits the invention, in spirit of the invention and
In claims, to the modifications and changes that the present invention makes, protection scope of the present invention is both fallen within.
Claims (10)
1. a kind of method for accurately constructing organic heterojunction resistive memory based on electrochemical method characterized by comprising
(1) polyphenyl bithiophene and pyrroles's PBTP active layer are prepared on hearth electrode;
(2) continue to prepare polythiadiazoles iso-indoles PTDI active layer on the PBTP active layer prepared, obtain with hetero-junctions
The change resistance layer of structure;
(3) dotted top electrode is grown on hetero-junctions active layer, ultimately forms organic heterojunction resistance-variable storing device.
2. the method according to claim 1 that organic heterojunction resistive memory is accurately constructed based on electrochemical method,
It is characterized in that, preparation PBTP active layer, comprising:
Using electrochemical method, the growth of direct in-situ electropolymerization prepares PBTP active layer on hearth electrode.
3. the method according to claim 1 that organic heterojunction resistive memory is accurately constructed based on electrochemical method,
It is characterized in that, preparation PTDI active layer, comprising:
Using electrochemical method, the growth of direct in-situ electropolymerization prepares PTDI active layer on the PBTP active layer prepared.
4. the method according to claim 1 that organic heterojunction resistive memory is accurately constructed based on electrochemical method,
It is characterized in that, successively continuously preparing PBTP and PTDI active layer using electrochemical method, the change resistance layer of heterojunction structure is obtained,
Specific steps include:
(1) electrochemical method is utilized, electrolyte is acetonitrile, and electrolyte is tetra-n-butyl ammonium hexafluorophosphate, concentration 0.001-
The concentration of 5M, monomer benzothiophene and pyrroles are 0.01-1M, the electropolymerization preparation PBTP active layer in situ in conductive substrates;
(2) electrochemical method is utilized, electrolyte is acetonitrile, and electrolyte is tetra-n-butyl ammonium hexafluorophosphate, concentration 0.001-
5M, the concentration of monomer thiadiazoles iso-indoles are 0.01-1M, continue electropolymerization system in situ on the above-mentioned PBTP active layer prepared
It is standby to obtain PTDI donor layer;
(3) hot evaporation process or magnetron sputtering technique are utilized, grows dotted top on the above-mentioned hetero-junctions change resistance layer being prepared
Electrode.
5. the method according to claim 4 that organic heterojunction resistive memory is accurately constructed based on electrochemical method,
It is characterized in that, caning be controlled in 20-150nm using the thickness of the PBTP active layer of electropolymerization preparation, electropolymerization preparation is utilized
The thickness of PTDI active layer can be controlled in 20-150nm, and the thickness for the hetero-junctions change resistance layer being prepared can be controlled in 40-
300nm, the top electrode with a thickness of 80-300nm, diameter 0.2-0.6mm.
6. the method according to claim 1 that organic heterojunction resistive memory is accurately constructed based on electrochemical method,
The hearth electrode and top electrode, material is unlimited, including but not limited to conductive metal and/or conductive metal oxide;It is described to lead
Electric metal is Au, Ag, Al, Cu or Ti;The conductive metal oxide is ITO or FTO;Top electrode or hearth electrode used can
With same or different.
7. the method according to claim 1 that organic heterojunction resistive memory is accurately constructed based on electrochemical method,
It is characterized in that, prepared PBTP active layer has electron characteristic, hole transmission layer can be served as, prepared PTDI is living
Property layer have electrophilic characteristic, electron transfer layer can be served as.
8. a kind of organic heterojunction resistance-variable storing device accurately constructed based on electrochemical method, which is characterized in that successively include: bottom
Electrode, PBTP active layer, PTDI active layer and dotted top electrode;Wherein, PBTP and PTDI active layer is all by electropolymerization original
Position preparation, two change resistance layer interactions further obtain the change resistance layer of heterojunction structure, the hetero-junctions resistance-variable storing device
It is prepared and is formed by the described in any item methods of claim 1-8.
9. a kind of application for accurately constructing organic heterojunction resistance-variable storing device based on electrochemical method on information is stored and read and write.
10. a kind of realization side for the information storage and read-write for accurately constructing organic heterojunction resistance-variable storing device based on electrochemical method
Formula, which is characterized in that using any one of claim 1-7 the method preparation have organic heterojunction resistance-variable storing device or
Organic heterojunction resistance-variable storing device described in claim 8 carries out voltage scanning, comprising the following steps:
A pulsed bias of application -1.5V carries out information write-in on the top electrode of the memory device, again in top electrode
The upper pulsed bias applied within the scope of 0.5V carries out the reading of information, then applies one within the scope of 4.5V on top electrode
A pulsed bias carries out the erasing of information, and the pulsed bias applied on top electrode within the scope of 0.5V again carries out information reading
It takes.
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