CN104966778B - A kind of frequency response learner of long-term memory and preparation method thereof - Google Patents
A kind of frequency response learner of long-term memory and preparation method thereof Download PDFInfo
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- CN104966778B CN104966778B CN201510230713.1A CN201510230713A CN104966778B CN 104966778 B CN104966778 B CN 104966778B CN 201510230713 A CN201510230713 A CN 201510230713A CN 104966778 B CN104966778 B CN 104966778B
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Abstract
The invention discloses frequency response learner of a kind of long-term memory and preparation method thereof.It includes the hearth electrode, dielectric layer and the top electrode that set gradually, dielectric layer be when being arranged on Semiconductor Organic nitride layer of the hearth electrode on and being arranged on top electrode on polyelectrolyte floor.Its preparation method, comprise the following steps：1) coating semiconductor organic matter layer in the one side of the hearth electrode on non-deposited conductive substrate；Then the coated polymer dielectric substrate in Semiconductor Organic nitride layer, drying, obtains being arranged on the dielectric layer on hearth electrode；2) mask plate is added on polyelectrolyte floor, top electrode is deposited on mask plate, mask plate is removed, that is, obtains learner.Adaptive frequency selectivity response can occur in input stimulus threshold range in the present invention, and this selectivity has long time-effect, and the device is the frequency dependence learner for having long-term memory, has the preferable simulation to nerve synapse.
Description
Technical field
The present invention relates to frequency response learner of a kind of long-term memory and preparation method thereof, belong to information electronic materials
Technical field.
Background technology
Analog neuron synaptic plasticity, it is current information, material, computer, neuroscience field to realize that class brain calculates
The problem of scientists and engineers pay close attention to jointly.Many memristors are invented and have carried out analog neuron synaptic plasticity, such as various gold
Belong to oxide, the resistance-variable storing device of metallic conduction filament types etc., can be with the time correlation plasticity of analog neuron cynapse
And frequency dependence plasticity (SRDP) (STDP).However, these devices differ distant with the property of true biological synapse, example
Such as, working media is unclear, mechanism is unintelligible, does not possess adaptivity under stimulation, synapse weight with stimulate number without
Limit increase, synapse weight increase unlimited increase with frequency of stimulation, or without long time-effect, etc..Therefore there is an urgent need to look for
To the device closer to biological synapse property, to simulate the learning functionality of cynapse, so as to class brain calculating of really marching toward.
The content of the invention
It is an object of the invention to provide frequency response learner of a kind of long-term memory and preparation method thereof, the present invention can
Responded with occurring adaptive frequency selectivity in input stimulus threshold range, and this selectivity has long time-effect.
Frequency response learner provided by the invention, it includes hearth electrode, dielectric layer and the top electrode set gradually, and it is special
Sign is：The dielectric layer is the Semiconductor Organic nitride layer being arranged in the hearth electrode one side and is arranged on the top electrode one
Polyelectrolyte floor on face；
The Semiconductor Organic nitride layer is the derivative of soluble p-phenylene vinylene or soluble p-phenylene vinylene, described poly-
Polymer electrolyte layer is PEO doping metals complex salts.
Above-mentioned learner, the learner also include conductive substrate；
The non-one side for setting the dielectric layer of the hearth electrode is deposited on si substrates by transition zone, and the Si substrates are
Si (100) substrate aoxidized by 300nm；
The transition zone is Ti layers, and the thickness of the transition zone can be 20nm.
Above-mentioned learner, the thickness of the hearth electrode can be 50~300nm, concretely 150nm；
In the dielectric layer, the thickness of the Semiconductor Organic nitride layer can be 50~100nm, concretely 70nm, institute
The thickness for stating polyelectrolyte floor can be 7~10 μm, concretely 8 μm；
The thickness of the top electrode can be 60~100nm, concretely 70nm.
Above-mentioned learner, the hearth electrode and the top electrode are made of platinum (Pt), golden (Au) or palladium (Pd)；
In the polyelectrolyte floor, in the PEO ethylene oxide monomer and the metal complex salt
The mol ratio of metal cation can be 16~32：1, concretely 16：1.
Above-mentioned learner, the derivative of the soluble p-phenylene vinylene (abbreviation PPV) for it is poly- [2- methoxyl groups -5 (2 ' -
Ethyl hexyl oxy) -1,4- phenylacetylenes] (abbreviation MEH-PPV), cyano group polyphenylene ethylene (abbreviation CN-PPV) or poly- [2- methoxyl groups -
5- (3 ', 7 '-dimethyl-octa epoxide) -1,4- phenylacetylenes] (abbreviation MDMO-PPV)；
The metal complex salt is LiCF3SO3、KCF3SO3、Ba(CF3SO3)2、Ca(CF3SO3)2、Nd(CF3SO3)3With
CsClO4At least one of.
Above-mentioned learner, the molecular weight of the soluble p-phenylene vinylene can be 150000~250000；
The molecular weight of the derivative of the soluble p-phenylene vinylene can be 150000~250000；
The molecular weight of the PEO can be 70000~200000, concretely 100000.
Present invention also offers the preparation method of above-mentioned learner, comprise the following steps：1) conductive described in non-deposited
Spreading out for the soluble p-phenylene vinylene or the soluble p-phenylene vinylene is coated in the one side of the hearth electrode on substrate
Biology, drying, obtains the Semiconductor Organic nitride layer；Then the PEO is coated in the Semiconductor Organic nitride layer
(PEO) aqueous solution of doping metals complex salts, the polyelectrolyte floor is obtained, dried, obtain being arranged on the bottom electricity
Dielectric layer on extremely；
2) mask plate is added on the polyelectrolyte floor, the top electrode is deposited on the mask plate, removed
The mask plate, that is, obtain the learner.
Above-mentioned method, the hearth electrode is deposited on the conductive substrate and uses physical vaporous deposition, the present invention uses
Commercially available Pt pieces are deposited on SiO2On substrate；
Coating the Semiconductor Organic nitride layer and use rotary coating, the speed of the rotary coating can be 1500~
2500rpm, concretely 2000rpm, time can be 50~80s, concretely 70s；
Dry the derivative of the soluble p-phenylene vinylene or the soluble p-phenylene vinylene temperature can be 40~
70 DEG C, concretely 50 DEG C, the time can be 5~12h, concretely 5.5h；
The mass percentage concentration of the aqueous solution of the PEO doping metals complex salts can be 0.5~2wt%；
The temperature for drying the aqueous solution of the PEO doping metals complex salts can be 65~100 DEG C, specifically may be used
For 75 DEG C, the time can be 10~30min, concretely 20min.
Above-mentioned method, the mask plate are the metal provided with circular hole figure, line pattern, camber line figure or broken line figure
Plate, the metallic plate are made of stainless steel, when the mask plate is the metallic plate provided with circular hole figure, the circular hole
Diameter can be 100nm~0.3mm, concretely 0.3mm；
The condition of the evaporation is：Vacuum is less than 10-8Torr, sedimentation rate are 0.03~0.05nm/s.
Frequency response learner of the present invention is applied in analog neuron cynapse field, learns in application frequency response of the present invention
During device, the frequency separation of response is 1Hz~200Hz；In use, the learner has frequency dependence plasticity, i.e. SRDP,
Suppression is produced under low frequency stimulating, is produced under high frequency stimulation excited.
During using frequency response learner of the present invention, its ability of learning and memory includes but is not limited to：To in input stimulus
Pulse signal in threshold range produces selective frequency response, and response is in suppression when being stimulated compared with low frequency (1Hz~80Hz)
Property processed, i.e., stimulate the response weight of (1Hz) to change relative to fundamental frequency and be less than 100%；And upper frequency (80Hz~200Hz) stimulates
When produce excitability response, i.e., relative to fundamental frequency stimulate (1Hz) response weight change be more than 100%.The selection of frequency response
Property there is long-range effect, suppression/excitement response can maintain more than 10 minutes.By being tested in general pulse device of the present invention
Extra " inhibition " of preceding progress or " excitability " stimulates, thus it is possible to vary device switchs to excited threshold value frequency by suppressing in test
Rate.
The present invention has advantages below：
1st, adaptive frequency selectivity response, and this selection can occur in input stimulus threshold range in the present invention
Property has long time-effect, and the device is the frequency dependence learner for having long-term memory.
2nd, memory capability of the invention switchs to excitatoty threshold value by inhibition and can be modulated by advance stimulation.
3rd, the present invention realizes learning and memory function by Ion transfer, all has in performance and the aspect of structure two to nerve
The preferable simulation of cynapse.
Brief description of the drawings
Fig. 1 is the structural representation of the present invention.
Fig. 2 be frequency response learner of the present invention voltage x current scan round curve map, wherein Fig. 2 (a) be voltage-
Scan round figure in the range of 2V~2V, Fig. 2 (b) are scan round figure of the voltage in the range of 0~2V, and 2 (c) is voltage 0
Scan round figure in the range of~-2V.
Fig. 3 is that the pulse frequency of frequency response learner of the present invention relies on plastic linearity curve (SRDP) figure.
Fig. 4 is the pulse test result figure of frequency response learner of the present invention, wherein, Fig. 4 (a) is that the pulse used is surveyed
Examination, Fig. 4 (b) are the figure that reverse current peak value changes with impulse stimulation number.
Fig. 5 is the long-range linearity curve figure of the frequency dependence learning performance of frequency response learner of the present invention.
Fig. 6 is the threshold value curve of sliding figure of frequency response learner of the present invention.
Embodiment
Experimental method used in following embodiments is conventional method unless otherwise specified.
Material used, reagent etc., unless otherwise specified, are commercially obtained in following embodiments.
The present invention is further described with specific embodiment below in conjunction with the accompanying drawings, but the invention is not limited in this,
Any modifications, equivalent replacements and improvementsmade within the spirit and principles of the invention, etc., it should be included in the present invention's
Within protection domain.
Embodiment 1, Pt/MEH-PPV/PEO-LiCF3SO3/ Pt frequency response learners
1) the transition zone Ti on commercially available Si substrates by 20nm is coated with 150nm thickness Pt substrates, Si substrates are oxidation
300nm Si (100)), it is cleaned by ultrasonic 4-8 minutes successively with acetone, alcohol and deionized water, is dried up with nitrogen.After cleaning
Substrate be placed on glue evenning table, μ l methoxyl groups -5 (2 '-ethyl hexyl oxy)-Isosorbide-5-Nitrae-p-phenylene vinylene (MEH- of rotary coating 3.5
PPV, molecular weight are 150000~250000), rotating speed 2000rpm, spin-coating time 70s, then dried using drying glue platform at 50 DEG C
It is dry 5.5 hours.
2) in MEH-PPV Semiconductor Organic nitride layer (thickness 70nm) the μ l of drop coating 3.5 polymer dielectric.The polymerization
Thing electrolyte is by PEO (PEO, molecular weight 100000) and trifluoromethanesulfonic acid lithium (LiCF3SO3) blending aqueous solution structure
Into, mass fraction 2wt%, oxirane monomers (EO):Metal cation (Li+)=16:1.By the substrate after drop coating again
It is placed on drying glue platform, is toasted 20 minutes with 75 DEG C of temperature, obtains the polymer dielectric of 8 μ m-thicks.
3) preparing two-layered medium layer (organic semiconductor layer thickness is that 70nm+ polyelectrolyte floor thickness is 8 μm)
Substrate on after mask plate (thickness be 100 μm) of the addition provided with circular aperture 0.3mm, be integrally placed at electron beam evaporation plating coating machine
Chip bench on, be evacuated to vacuum less than 10-8Torr, open electron gun evaporation Pt, control sedimentation rate be 0.03~
0.05nm/s, acquisition thickness are 70nm island Pt top electrodes.After the completion of electron beam evaporation plating, to the vacuum of electron beam evaporation plating coating machine
It is atmospheric pressure that high pure nitrogen to vacuum indoor pressure is filled with room, takes out, that is, obtains frequency response learner of the present invention.
Embodiment 2, Pt/MEH-PPV/PEO-LiCF3SO3The electrical properties of/Pt frequency response learners
Property 1, voltage-current curve are in loop line pattern, negative differential resistance (NDR) effect occur, as shown in Figure 2.
Fig. 2 (a) is scan round of the voltage in the range of -2V~2V, and NDR is appeared in by during negative sense to forward scan
0.6V position.Fig. 2 (b) is scan round of the voltage in the range of 0~2V, does not occur obvious NDR phenomenons, but
Nearby there is current breakpoint in 0.1V, illustrates that resistance changes.Fig. 2 (c) is scan round of the voltage in the range of 0~-2V, nothing
NDR or current breakpoint occur, and illustrate that the dissymmetrical structure of learner two-layered medium layer of the present invention result in electric property not
Symmetry.
The compression rate of above-mentioned scan round process is 100V/s.
Property 2, the square wave/triangular pulse signal for applying different frequency, the weight obtained by the Current calculation that recoils have
There is the selectivity to frequency：With the rising of frequency, weight first reduces and increased afterwards, that is, responds and switch to excitability by inhibition, obtain
Obtain selective pulse frequency and rely on plasticity (SRDP) curve, as shown in Figure 3.
Square-wave pulse signal is continuous 40 arteries and veins that array frequency is respectively f (f=1Hz, 10Hz, 20Hz ... 142Hz)
Rush signal, amplitude 0.1V, pulsewidth 0.5ms.
Triangular pulse signal is that array frequency is respectively continuous 40 of f (f=1Hz, 10Hz, 20Hz ... ... 142Hz)
Pulse signal, amplitude 03V, compression rate 100V/s.
The computational methods of weight are as follows：After frequency of use is stimulated learner of the present invention for f set of pulses signal,
Measure the current value (A points in Fig. 4) of back discharge after each end-of-pulsing.From Fig. 4 (b) it can be seen that with impulse stimulation time
Several increases, the absolute value of the current peak of device of the present invention first increase, and are stabilized to a fixed value afterwards, remember the fixed current
It is worth for If.Calculate If/IF=1Hz× 100% numerical value, it is the weighted value under frequency f.
The suppression of response/excitability method of discrimination is as follows：Response of the weight calculation less than 100% responds for inhibition, power
Response of the re-computation more than 100% responds for excitability.
Property 3, the frequency of learner of the present invention selection study property have long-range effect, and " inhibition " or " excitability " rings
It should can maintain more than 10 minutes, as shown in Figure 5.As shown in Figure 5, for the exciting signal of high frequency, frequency of stimulation is higher,
Excitement response is stronger, and the time needed for excitement failure is also longer, i.e., with more preferable long-range.
The method of testing that " inhibition " or " excitability " response is held time is as follows：On top electrode, first apply 1Hz
Pulse is stimulated, then is applied a certain specific frequency f pulse and stimulated, and then reuses 1Hz at regular intervals
Pulse stimulated, as " reading " signal, weight is calculated using previously described weighing computation method respectively, so as to do
Go out the weight versus time curve to a certain specific frequency f, as shown in Fig. 5.
Property 4, extra " inhibition " or " excitability " thorn by being carried out to device of the present invention before general pulse is tested
Swash, thus it is possible to vary learner of the present invention is switched to the threshold frequency of excitability response by inhibition response in test.As shown in fig. 6,
Before normal pulse frequency relies on plasticity (SRDP) test, apply one group of 10Hz suppression sexual stimulus, the present invention to device
The transformation threshold value of " suppression-excitement response " of frequency response learner increases to 130Hz by 25Hz.
Claims (9)
1. a kind of frequency response learner, it includes hearth electrode, dielectric layer and the top electrode set gradually, it is characterised in that：Institute
State dielectric layer be when being arranged on Semiconductor Organic nitride layer of the hearth electrode on and being arranged on the top electrode on it is poly-
Polymer electrolyte layer；
The Semiconductor Organic nitride layer is the derivative of soluble p-phenylene vinylene or soluble p-phenylene vinylene, the polymer
Dielectric substrate is PEO doping metals complex salts；
The hearth electrode and the top electrode are made of platinum, gold or palladium；
In the polyelectrolyte floor, the PEO ethylene oxide monomer and metal in the metal complex salt
The mol ratio of cation is 16~32：1.
2. learner according to claim 1, it is characterised in that：The learner also includes conductive substrate；
The non-one side for setting the dielectric layer of the hearth electrode is deposited on si substrates by transition zone；
The transition zone is Ti layers.
3. learner according to claim 1 or 2, it is characterised in that：The thickness of the hearth electrode is 50~300nm；
In the dielectric layer, the thickness of the Semiconductor Organic nitride layer is 50~100nm, the thickness of the polyelectrolyte floor
Spend for 7~10 μm；
The thickness of the top electrode is 60~100nm.
4. learner according to claim 1 or 2, it is characterised in that：The derivative of the soluble p-phenylene vinylene is
Poly- [(2 '-ethyl hexyl oxy) -1,4- of 2- methoxyl groups -5 phenylacetylenes], cyano group polyphenylene ethylene or it is poly- [2- methoxyl groups -5- (3 ',
7 '-dimethyl-octa epoxide) -1,4- phenylacetylenes]；
The metal complex salt is LiCF3SO3、KCF3SO3、Ba(CF3SO3)2、Ca(CF3SO3)2、Nd(CF3SO3)3And CsClO4
At least one of.
5. learner according to claim 1 or 2, it is characterised in that：The molecular weight of the soluble p-phenylene vinylene is
150000~250000；
The molecular weight of the derivative of the soluble p-phenylene vinylene is 150000~250000；
The molecular weight of the PEO is 70000~200000.
6. the preparation method of the learner any one of claim 2-5, comprises the following steps：1) led described in non-deposited
The soluble p-phenylene vinylene or the soluble p-phenylene vinylene are coated in the one side of the hearth electrode on electric substrate
Derivative, drying, obtains the Semiconductor Organic nitride layer；Then the polycyclic oxygen second is coated in the Semiconductor Organic nitride layer
The aqueous solution of alkane doping metals complex salts, the polyelectrolyte floor is obtained, dry, obtain being arranged on the hearth electrode
Dielectric layer；
2) mask plate is added on the polyelectrolyte floor, is deposited the top electrode on the mask plate, described in removing
Mask plate, that is, obtain the learner.
7. according to the method for claim 6, it is characterised in that：The hearth electrode is deposited on the conductive substrate and uses physics
Vapour deposition process；
Coat the Semiconductor Organic nitride layer and use rotary coating, the speed of the rotary coating is 1500~2500rpm, the time
For 50~80s；
The temperature for drying the derivative of the soluble p-phenylene vinylene or the soluble p-phenylene vinylene is 40~70 DEG C, when
Between be 5~12h；
The mass percentage concentration of the aqueous solution of the PEO doping metals complex salts is 0.5~2wt%；
Dry the aqueous solution of the PEO doping metals complex salts temperature be 65~100 DEG C, the time be 10~
30min。
8. the method according to claim 6 or 7, it is characterised in that：The mask plate is provided with circular hole figure, rectilinear
The metallic plate of shape, camber line figure or broken line figure；
The condition of the evaporation is：Vacuum is less than 10-8Torr, sedimentation rate are 0.03~0.05nm/s.
9. application of the learner in analog neuron cynapse field any one of claim 1-5.
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| CN108987565B (en) * | 2018-04-17 | 2021-01-05 | 张晗 | Synapse device based on metal cation modified black phosphorus and preparation method thereof |
| CN109378383A (en) * | 2018-09-17 | 2019-02-22 | 南开大学 | A kind of preparation method based on organic nano ion/electronics hybrid material both ends neurobionics electronic device |
| CN111323654B (en) * | 2020-02-28 | 2021-08-06 | 北京大学 | Synapse simulation method and system of resistive device |
| CN112103388B (en) * | 2020-09-23 | 2022-10-04 | 南开大学 | Based on Ti 3 C 2 Preparation method of artificial synapse device with-MXene/electrolyte structure |
| CN112909166B (en) * | 2021-01-26 | 2022-11-25 | 天津理工大学 | Nerve synapse bionic device based on polyelectrolyte double-layer structure |
| ES2927156B2 (en) * | 2021-04-30 | 2023-03-13 | Univ Valencia | MEMRISTIVE DEVICES BASED ON SEMICONDUCTOR POLYMER MATERIALS THROUGH THE PHENOMENON OF IONIC MIGRATION |
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