CN111106239B - Complementary structure synaptic device based on nanofluid interface type memristor and preparation thereof - Google Patents
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Abstract
The invention belongs to the technical field of microelectronics and nanometer, and discloses a complementary structure synapse device based on a nanofluid interface type memristor and a preparation method thereof, wherein the device comprises at least two parallel nanometer channels which are functionally divided into two types in total; after the nano channels with different functional classifications are contacted with the first liquid, the wall surfaces of the nano channels with different positive and negative electric properties are brought, the nano channels with the first and second functions show different ion selective trafficability to the first liquid, and do not show the ion selective trafficability to the second liquid; under the action of an external electric field, the conductance changes of the two types of functional nano channels are opposite, and the artificial synapse device with a complementary structure is realized. According to the invention, through the integral cooperation of the first liquid, the second liquid and the two types of parallel functional nano channels, different liquid interfaces move in the nano channels under the same external electric field, so that the enhancement type and inhibition type nano-fluid memristor units can be obtained correspondingly, and a synapse device with a complementary structure is realized.
Description
Technical Field
The invention belongs to the technical field of microelectronics and nanometer, and particularly relates to a synapsis device with a complementary structure based on a nanofluid interface type memristor and a preparation method thereof][PF6]According to the nanofluid memristor, two different nano-channel materials and structures are designed, the combination of an enhancement type synaptic memristor unit and a suppression type synaptic memristor unit can be completed on the same substrate through a traditional semiconductor preparation process, and then a complementary structure synaptic device based on the nanofluid interface type memristor is obtained.
Background
With the size reduction of the traditional semiconductor device and the increase of the design scale of the integrated circuit, the traditional integrated circuit technology has the limitation that the traditional integrated circuit technology cannot be eliminated, the development of artificial intelligence cannot be separated from the design of the integrated circuit, and brain-like calculation and deep learning need a proper special integrated circuit to be realized, so that the realization of functions of reading and writing of human hearing and speaking and the like is completed.
A memristor (memristor) is a fourth type of passive element inferred by "zeisu" in the 1970 s when studying the relationship between charge, current, voltage and magnetic flux, and it is proposed that memristors represent the relationship between charge and magnetic flux. The resistance of a memristor changes with the amount of charge flowing through it and is able to maintain its previous resistance state when the applied current is turned off. When considering designing a circuit simulating a nerve morphological structure, a structural unit replacing synapses of a human brain is needed, so that the design of a neural network circuit is finished by considering using memristors to realize synapse functions.
Between human brain neurons, there are reinforced synapses and inhibitory synapses, and for the same bioelectric impulse signals, reinforcement or reduction of synaptic weights can be respectively realized, so as to obtain corresponding learning or memory functions. On the other hand, the current memristive neural network has a complex design structure, and an additional circuit or multiple layers of complex auxiliary circuits are needed to complete the simultaneous realization of enhanced synapses and inhibited synapses, so that corresponding functional algorithms are realized; in the aspect of integrated circuit design, enhancement type and inhibition type synapse devices are prepared at the same time in the same process flow rarely.
Therefore, there is a need for a suitable complementary synaptic structure to achieve both enhanced and inhibited synaptic function.
Disclosure of Invention
Aiming at the above defects or improvement requirements of the prior art, the invention aims to provide a synapse device with a complementary structure based on a nanofluid interface type memristor and a preparation method thereof, wherein through the overall cooperation effect of a first liquid, a second liquid and two types of parallel nanochannels, the two types of parallel nanochannels are utilized to generate an ion selection effect on the first liquid and not generate an ion selection effect on the second liquid, and further, different liquid interfaces are generated in the two parallel nanochannels to move in the same external electric field direction by utilizing the difference of the electric charge of the first liquid and the surface hydrolysis of the two parallel nanochannels, so that an enhancement type nanofluid memristor unit and an inhibition type nanofluid memristor unit are correspondingly obtained, the coexistence of an enhancement type device and an inhibition type device in an artificial synapse device is realized, and the synapse device with the complementary structure is functionally realized, and the simplification of the preparation flow is realized, and the improvement of the traditional circuit structure is completed.
To achieve the above object, according to one aspect of the present invention, there is provided a synapse device based on a complementary structure of a nanofluidic interface memristor, comprising at least two parallel nanochannels functionally divided into two types, a first liquid channel and a second liquid channel disposed at two ends of the nanochannels, wherein any one of the nanochannels is used to communicate the first liquid channel with the second liquid channel; and, the nanochannels are all located on a first substrate, the first liquid channel and the second liquid channel are both located on a second substrate, and the first substrate and the second substrate are laminated together to form a monolithic structure; wherein the content of the first and second substances,
the first liquid channel is used for containing a first liquid and is connected with the first electrode; the second liquid channel is used for containing a second liquid and is connected with the second electrode; the first liquid and the second liquid have difference in conductivity and are not mutually soluble;
the nanometer channels can be functionally classified into two types, namely a first type of functional nanometer channel and a second type of functional nanometer channel; the two types of functional nano channels can generate different hydrolysis reactions after being contacted with the first liquid to generate ions with different positive and negative electric properties, so that the wall surfaces of the two types of functional nano channels show electric properties with different positive and negative electric properties, and the two types of functions can be divided by utilizing the difference of the positive and negative electric properties; the two types of functional nano-channels are respectively marked as a first type of functional nano-channel and a second type of functional nano-channel, wherein the first type of functional nano-channel can make the wall surface show negative charge after being contacted with the first liquid, and the second type of functional nano-channel can make the wall surface show positive charge after being contacted with the first liquid; due to the fact that positive and negative electric properties of the wall surface are different, the first type of functional nano-channel and the second type of functional nano-channel can show different ion selective permeability for the first liquid, and meanwhile, the two types of functional nano-channels can not show ion selective permeability for the second liquid;
the first electrode and the second electrode are used for applying an external voltage to the nano channels so as to introduce an external electric field effect to the nano channels; the external voltage can generate external electric fields in the same direction in the nano channels, and under the action of the external electric fields, the electric charges on the wall surfaces of the two types of functional nano channels are different, so that the conductance changes of the two types of functional nano channels are opposite, and the synapsis device with the complementary structure of the nano-fluid interface type memristor is realized.
In a further preferred embodiment of the present invention, the inner wall material of the first-type functional nanochannel is a material capable of carrying negative ions or negative groups after being hydrolyzed with the first liquid, and is preferably SiO2(ii) a The inner wall material adopted by the second type of functional nano-channel is a material which can be hydrolyzed with the first liquid and then carries electropositive ions or electropositive groups, and is preferably Al2O3。
As a further preference of the present invention, the first liquid is an aqueous solution of a compound salt, preferably an aqueous solution of KCl; the second liquid is an ionic conductor or a conductive organic compound immiscible with an aqueous solution of a salt of the compound, preferably [ BMIM][PF6]。
As a further optimization of the invention, the depth of any one of the nanometer channels is 80-200nm, the width is 50-300nm, and the length is 10-100 um.
As a further preferred aspect of the present invention, the first liquid channel specifically includes a first micron channel, and at least 2 liquid reservoirs connected by the first micron channel; the depth of the first micron channel is 50-1000um, the width is 1-5um, and the length is 1-2 cm;
the second liquid channel specifically comprises a second micron channel and at least 2 liquid storage tanks connected through the second micron channel; the depth of the second micron channel is 50-1000um, the width is 1-5um, and the length is 1-2 cm;
1 first electrode disposed in a reservoir connected to said first microchannel;
1 second electrode disposed in a reservoir connected to said second microchannel;
preferably, the number of the liquid storage tanks is 4, two of the liquid storage tanks are respectively distributed at two ends of the first micron channel, and the other two liquid storage tanks are respectively distributed at two ends of the second micron channel.
As a further preferred of the present invention, the first substrate is SiO2The second substrate is a PDMS substrate.
According to another aspect of the invention, the invention provides a preparation method for preparing the synapse device based on the complementary structure of the nanofluid interface type memristor, which is characterized by comprising the following steps:
(1) in SiO2Obtaining at least two parallel nano channels on a substrate through a semiconductor processing technology, wherein the semiconductor processing technology comprises electron beam lithography and plasma etching, and then removing photoresist; then, the nanometer channels are divided functionally in advance, wherein at least one nanometer channel is divided into a first type of functional nanometer channel in advance, and at least one nanometer channel is divided into a second type of functional nanometer channel; the nanometer channels pre-divided into the first type of functional nanometer channels are kept unchanged; the nano channel pre-divided into the second type of functional nano channel needs to be subjected to electron beam evaporation through a photoresist exposure mask after the plasma etching process is finished, and after stripping is finished, the inner wall of the nano channel is modified, so that the wall surface obtained after modification is a material which can be hydrolyzed with the first liquid and then is positively charged; therefore, the preparation of the nanometer channels with the first type of function and the second type of function which are functionally divided into two types in total is realized;
(2) preparing a PDMS substrate having a first liquid channel and a second liquid channel;
preferably, the step (2) specifically comprises the following operations: preparing another SiO2The substrate is coated with photoresist in a spinning mode, is aligned through a mask plate in an alignment mode, is exposed, is developed by using corresponding developing solution, and is dried and formed; then, a PDMS reagent is used for carrying out mould inversion, drying and forming are carried out, and then the PDMS forming module is formed from the SiO2Taking off the substrate to obtain the film with the second layerA PDMS substrate having a liquid channel and a second liquid channel; wherein, the exposure is preferably performed by an ultraviolet photoetching machine;
(3) subjecting the SiO obtained in the step (1) to2And (3) aligning, bonding and packaging the substrate and the PDMS substrate obtained in the step (2), so that any one of the nano channels can be communicated with the first liquid channel and the second liquid channel.
As a further preferred of the present invention, the preparation method further comprises the steps of:
(4) correspondingly injecting a first liquid and a second liquid into the first liquid channel and the second liquid channel respectively, wherein the first liquid and the second liquid have difference in conductivity and are not mutually soluble; the two types of functional nano channels can generate different hydrolysis reactions after being contacted with the first liquid to generate ions with different positive and negative electric properties, so that the wall surfaces of the two types of functional nano channels have different positive and negative electric properties; wherein the first type of functional nanochannel is capable of rendering the wall surface negatively charged upon contact with the first liquid and the second type of functional nanochannel is capable of rendering the wall surface positively charged upon contact with the first liquid; due to the fact that positive and negative electric properties of the wall surface are different, the first type of functional nano-channel and the second type of functional nano-channel can show different ion selective permeability for the first liquid, and meanwhile, the two types of functional nano-channels can not show ion selective permeability for the second liquid.
In a further preferred embodiment of the present invention, the wall material of the second-type functional nano-channel is Al2O3Correspondingly, in the step (1), when the electron beam evaporation technology is adopted to modify the nano channel pre-divided into the second type of functional nano channel, the material used by the electron beam evaporation is Al, specifically, evaporation is performed first, and after the evaporation is completed, the nano channel is contacted with air to be oxidized, so that Al is generated2O3。
As a further preferred aspect of the present invention, in the step (3), after the alignment bonding is completed, any one of the nano channels is perpendicular to the first liquid channel and the second liquid channel.
Compared with the prior art, the technical scheme provided by the invention realizes the synapse device with the complementary structure with the coexistence of the enhancement type and the inhibition type. The device consists of a microchannel plus two parallel nanochannels with different functions (each nanochannel of one function comprises at least one nanochannel) spanning across it, all nanochannels being used to contain two liquids, namely a first liquid and a second liquid. The first liquid and the second liquid in the nano channel are mutually insoluble and have difference in conductivity, meanwhile, the first liquid can enable the wall surface of the nano channel to generate hydrolysis action so as to bring wall surface charges, and then the channel generates ion selection action on ions in the first liquid; the different functional classifications of the nanometer channel can be realized by the modification of different nanometer channel inner wall materials, and the different nanometer channel inner wall materials lead the surfaces of the two types of functional nanometer channels to generate different hydrolysis reactions when being contacted with the first liquid, thereby leading the polarity of the charges carried by the wall surfaces of the nanometer channels to be different; when a voltage is applied to two ends of the device, because of the selective permeability of the nano-channels to ions, a number of single-polarity ions which occupy a dominant position exist in each channel, and the ions can move under the action of an external electric field, so that a liquid interface between first liquid and second liquid in the nano-channels continuously moves under the action of the electric field. Because of the significant difference in conductivity between the first liquid and the second liquid, the conductance of the channel changes when the position of the interface between the first liquid and the second liquid in the channel changes (i.e., the length occupied by the first liquid and the second liquid in the channel changes). Because the surface of different channels is charged with opposite polarities, the moving directions of liquid interfaces in different channels are opposite under the condition of the same external electric field. That is, when the first liquid contacts the surfaces of the two parallel nano-channels, the electrical conductance of the two parallel nano-channels increases in one type and decreases in the other type under the same external electric field direction by utilizing the difference of the polarities of charges carried by the wall surfaces after hydrolysis reaction, and the electrical conductance of the two parallel nano-channels respectively corresponds to the enhancement type nano-fluid memristor unit and the inhibition type nano-fluid memristor unit, so that the synapse device with the complementary structure is functionally realized. According to the invention, by utilizing a parallel nano-channel structure, two mutually insoluble solutions with different conductivities are driven to move in a nano-channel by an electric field, so that opposite conductivity changes of different channels are realized, and a complementary synapse device of an interface type memristor based on nanofluid is constructed.
Compared with the traditional brain-like neural network circuit design, in the traditional technology, when an enhanced synapse and an inhibitory synapse are designed and prepared, or when enhancement or reduction of synaptic weights is completed, an additional auxiliary circuit needs to be designed, for example, when a spiking neural network algorithm ReSuMe is completed, an additional auxiliary circuit needs to be designed to achieve simultaneous enhancement and reduction of synaptic weights in the weight adjustment process. The invention provides the weight change of the enhanced synapse unit and the inhibited synapse unit at the same time under the same electric field or pulse, thereby simplifying and improving the neural network circuit design, reducing the complexity of the hardware structure and reducing the power consumption required by the realization of the neural network function.
The nano channel in the invention is consistent with the conventional definition, namely, the channel is the nano channel as long as one dimension of the parameters of the length, the width and the height of the channel is a nano scale; the invention preferably adopts a nanometer channel with channel depth and width parameters of nanometer, wherein, the depth can be preferably controlled to be 80-200nm, and the width can be preferably controlled to be 50-300 nm. The size condition can ensure that the solution in the channel can be regulated by surface charges, and simultaneously enough liquid flows into the nano channel, so that the current of the whole device reaches a more ideal range, and the difficulty in device preparation is reduced. If the width of the nano-channel is too wide, such as larger than 300nm, the regulation and control effect of the surface charge on ions in the channel will begin to gradually decrease, so that the concentration of the ions in the nano-channel is very similar to that of the solution outside the channel, and the selective permeability of the nano-channel on the ions is reduced. If the width of the nano-channel is too narrow (e.g. less than 50nm) and the depth is also reduced (e.g. less than 50nm), the total amount of solution flowing into the nano-channel is significantly reduced, the current signal range of the device is also significantly reduced, and the device is easily affected by various noises during the testing process. Meanwhile, the requirement for device preparation is higher due to further reduction of the size, and the yield of the device can be reduced.
The principle that the nano channels with different functional classifications have different polarity charges in the invention is that the surfaces of the two types of functional nano channels with different functional classifications are contacted with the first liquid to generate different hydrolysis reactions and different positive and negative ions, so that the wall surfaces are provided with different charges. The two different functions of the nanochannel can be achieved by applying different surface modifications to the inner wall of the channel (of course, a combination of applying and not applying surface modifications can also be used). Based on SiO with nano-channels2Substrate for example, for a nanochannel without surface modification, the hydrolysis reaction that occurs is SiO2The reaction of hydrolysis into silicic acid, the silicic acid is decomposed into silicate and hydrogen ions in the solution, the hydrogen ions enter the solution and the silicate ions are left on the wall surface, so that the wall surface is charged with negative charges; for the channel after surface modification, the surface of the channel is Al2O3For example, when contacting with the first liquid, hydrolysis reaction occurs to generate aluminum hydroxide, which is decomposed into aluminum ions and hydroxide ions in the solution, and the hydroxide ions enter the solution to leave the aluminum ions, so that the wall surface of the channel is positively charged; so as long as the nanochannel is successfully surface Al-modified (Al can be deposited, in particular by evaporation, since Al is easily oxidized, the surface will be mainly covered by aluminum oxide), the surface will be charged with different polarities when in contact with the first liquid. Here, the polarity of the charge carried by the channel surface in contact with the first liquid mainly depends on the kind of ionic groups left on the surface after the modification material and the first liquid undergo a chemical reaction when the channel surface is modified, and the valence of the ionic groups. In particular, the solid oxide surface is charged in an aqueous suspension. Thus, they associate with water molecules through charge-dipole interactions, thereby forming hydrophilicity. Thereby forming either a positive or negative surface charge on the solid-liquid surface in contact with the first solution. With Al2O3Modification if Al is carried out2O3And (3) modifying, namely, leaving positive ionic groups on the surface of the nano channel, wherein the surface of the nano channel is charged with positive surface charges after being contacted with the first liquid.
The invention can modify the surfaces of a plurality of parallel nanometer channels, can realize a first type of functional nanometer channel and a second type of functional nanometer channel with two types of different functions, and finally realizes a synapse device with a complementary structure by utilizing the integral arrangement of different detailed structures in the device. Correspondingly, in the aspect of the preparation method, the whole process flow of the preparation method is controlled according to the structural characteristics, and a convenient and fast mode is provided for the preparation of the synapse device with the complementary structure. In order to make the manufacturing steps relatively simpler, the nano-channel is manufactured by adopting a structural basis that the wall surface is hydrolyzed and has negative charges; although the nano-channel surface modification method is based on the surface modification method which is published by researchers and applied to the manufacturing of the nano-fluidic diode, the method utilizes the nano-channel surface modification method to realize the first type of functional nano-channel and the second type of functional nano-channel with different functions, and finally obtains the synapse device with the complementary structure, and the application directions of the memristor are completely different.
The invention designs a new preparation method based on the synapse device with the complementary structure, and further optimally controls parameter conditions and the like in the preparation method. Although the synapse device with the complementary structure is based on the nanofluid interface type memristor, due to the particularity of the channel, the preparation method of the synapse device is greatly different from that of the common nanofluid interface type memristor, and is different from the method that the nanometer channel and the micron channel are jointly prepared on the same silicon chip in the previous research results of the inventor.
Especially for the preparation of parallel nano-channels, when the nano-channels are prepared by ultraviolet lithography, specific parameters need to be selected to achieve a relatively ideal lithography effect, for example, considering the parameters of the resolution of lithography and the current magnitude during lithography, the exposure parameters can be controlled at an exposure dose of 300-2The current can be controlled between 4nA and 5nA, but the current needs to be controlled to the minimum value of the achievable precision when the nano-structure exposure is carried out, for example, 100-300pA, so as to keep the nano-structure being completely etched and achieve the ideal exposure effect. And then carrying out plasma etching after development to deepen the depth of the channel, strictly controlling etching parameters in the etching process to avoid insufficient depth of the channel or over-depth of the channel, wherein the specific etching rate can be kept at 2nm-2.5nm/s, and the etching time can be selected according to the desired depth (for example, the etching time can be controlled to be about 100s for reaching the depth within the range of 80 nm-200 nm). And then, surface modification is carried out on the channel, a layer of photoresist can be firstly coated on the surface of the device in a spin mode, alignment is carried out by using a mask plate with a pre-designed pattern, then ultraviolet exposure is carried out, and the exposure time can be controlled within 2-3 s. The purpose of this step is to use photoresist to mask, facilitate the subsequent channel surface modification to at least one of the plurality of nanochannels. Metal evaporation is then performed, and the thickness of the metal may preferably be 5-10nm, in order to avoid undesirable effects of too thick or too thin metal films. Then a metal stripping operation is carried out, in which case two nano-channels with functionally different functions can be distinguished, at least one of which has been surface-modified.
For the preparation process of the PDMS micron channel, firstly, SiO is needed2The substrate was coated with photoresist and UV lithographed MJB4 on SiO2The exposure of the micron channel pattern is carried out on the substrate, and the exposure time can be preferably controlled to be about 30s, so that the condition of underexposure or overexposure is avoided. After development, the mold was dried, and the PDMS reagent was used for inversion. In the process, the time and temperature for processing the PDMS reagent and drying and molding need to be controlled, for example, PDMS and a curing agent can be uniformly stirred,the ratio can be fine tuned according to the desired PDMS morphology and can generally be maintained at a ratio of 1: 10. And then drying and forming are carried out, the temperature can be controlled at 60 ℃, and the forming can be carried out after drying for about 1 hour. Then, the nano channel and the micro channel are aligned and bonded, at this stage, the PDMS micro channel and the nano channel can be put into a plasma cleaning machine for cleaning, and the oxygen pressure and the cleaning time can be preferably controlled in the cleaning process, so that the condition that the surface is not cleaned to an ideal degree and cannot be bonded is avoided; for example, the oxygen pressure may be controlled at a rate of 100ml/s, and the purging time may be kept within 1 minute. After cleaning, alignment bonding operation can be carried out under a microscope, the micron channel and the parallel nanometer channel need to be aligned to ensure communication, and the micron channel can be perpendicular to the parallel nanometer channel in the alignment process.
Drawings
FIG. 1 is a device structure diagram of a complementary structure synapse device based on a memristor of the nanofluidic interface type in accordance with the present invention.
Fig. 2 is a schematic diagram of an enhanced nanofluidic channel cell.
Fig. 3 is a schematic diagram of a suppressor nanofluidic channel cell.
Fig. 4 is a schematic view of a first nanochannel under an optical microscope.
FIG. 5 is a first nanochannel AFM characterization.
FIG. 6 is a schematic view of a PDMS device mold.
The meaning of the reference symbols in fig. 1 is as follows: the device comprises a silicon chip substrate 1, a Polydimethylsiloxane (PDMS) substrate 2, an Ag/AgCl doped electrode 3, a liquid storage tank 4, a first nano channel 5, a second nano channel 6 and a micron channel 7.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is described in further detail below with reference to the accompanying drawings and embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention. In addition, the technical features involved in the embodiments of the present invention described below may be combined with each other as long as they do not conflict with each other.
Example 1
As shown in fig. 1, the synapse device of complementary structure of the memristor in nanofluid interface type of the present invention has four liquid reservoirs in total, the liquid reservoirs are respectively interconnected with the corresponding micron channels, parallel nano channels perpendicular to the micron channels are arranged between the two parallel micron channels, so as to interconnect the micron channels and the nano channels, and the nano channels and the micron channels on the PDMS substrate can be respectively obtained on the silicon substrate through a semiconductor process.
KCl salt solution is injected into the left liquid storage tank of the device, and ion conductor such as [ BMIM ] is injected into the right liquid storage tank][PF6](ii) a In the first nanometer channel, the inner wall of the channel is SiO2The material and KCl solution generate solid-liquid hydrolysis to make the inner wall of the channel have negative charge, so that the channel has ion selective permeability and cation K is mainly in the channel+When an electric field is applied, ions in the channel move under the action of the electric field force, and at the moment, the number of cations in the channel is dominant, so that the cations in the channel can drive liquid to flow under the action of the electric field force, so that an immiscible liquid interface in the channel moves, and the integral conductance of the first nano channel is increased; in the parallel second nano channel, the channel inner wall is Al2O3The material contacts with KCl solution to generate solid-liquid hydrolysis, so that the inner wall of the channel is positively charged, the channel also has ion selective permeability, and anions Cl are mainly in the channel-When an electric field is applied in the same direction, most of the anions Cl in the channel are similar to those in the above-The liquid is driven to flow by the forced movement, so that the immiscible liquid level interface in the channel moves, and the moving direction is opposite to the moving direction in the first nano channel, so that the integral conductance of the second nano channel is reduced.
FIG. 2 is a schematic diagram of an enhancement type nano-fluid channel unit, in which the inner wall of the channel is SiO2The material and the injected KCl solution generate solid-liquid hydrolysis to make the inner wall of the channel negatively charged, so that the channel is formedHas ion selective permeability, and the channel is mainly provided with cations K+When an electric field is applied, cations K in the channel+The liquid is driven to flow by the forced movement, so that an immiscible liquid interface in the channel moves, the KCl solution ratio in the channel rises, and the ion conductor [ BMIM ]][PF6]The ratio is reduced, so that the overall conductance of the first nano-channel is increased, and the enhanced nano-fluid memristor unit is realized.
FIG. 3 is a schematic diagram of the principle of the suppressive nanofluidic channel cell, in the second nano-channel in parallel, since the inner wall of the channel is Al2O3The material contacts with KCl solution to generate solid-liquid hydrolysis, so that the inner wall of the channel is positively charged, the channel also has ion selective permeability, and anions Cl are in the channel-When an electric field in the same direction is applied, anions Cl in the channel-The liquid is driven to flow by the forced movement, so that the immiscible liquid level interface in the channel moves, the moving direction is opposite to the moving direction in the first nano channel, the KCl solution ratio in the channel is reduced, and the ion conductor [ BMIM ]][PF6]The ratio is increased, so that the overall conductance of the second nano-channel is reduced, and the restrained nanofluid memristor unit is realized.
The specific embodiment takes a specific nano channel as an example, and the channel is an enhanced nano channel.
(1) As shown in fig. 4, a first nano-channel is obtained on a first substrate 1 by a semiconductor processing technique including electron beam lithography followed by development and then plasma ICP etching.
(2) The depth of the nano-channel is characterized by AFM, and as shown in FIG. 5, the depth of the nano-channel in the region is about 140nm, the width is 200nm, and the length is 20 um.
When the parallel complementary nanometer channels are prepared, the channel size parameters are selected, and the first nanometer channel and the second nanometer channel can be the same or close to each other as much as possible.
(3) During the preparation of the microchannel 7 containing the first and second liquids, an ultraviolet lithography machine MJB4 was used on SiO2On a substrate 1The preparation of the channel comprises the following specific operations: spin-coating photoresist, aligning by mask plate alignment, exposing, developing with corresponding developing solution, and drying for molding. Using PDMS reagent to perform reverse molding, drying at 65 ℃ for 12h for molding, and taking the PDMS molding module 2 from SiO2And taking down the substrate 1, wherein the depth of the first micron channel and the second micron channel is controlled to be 50-1000um, the width is controlled to be 1-5um, and the length is controlled to be 1-2 cm. The molded PDMS device was then punched at the location of the label reservoir using a special punching tool as shown in fig. 6, and after bonding the device, injection was performed from the hole to inject the first and second liquids into the reservoir.
(4) And aligning, bonding and packaging the processed parallel nano channels and the micron channels on the PDMS molding module 2, wherein the process comprises the steps of putting the PDMS module 2 and the silicon wafer substrate 1 into a plasma cleaning machine to clean the surfaces of the PDMS module and the silicon wafer substrate 1, and aligning and bonding the PDMS module 2 and the silicon wafer substrate 1 under a microscope to complete packaging after cleaning. During alignment, the micron channel and the parallel nanometer channel need to be aligned to ensure communication, and the micron channel can be perpendicular to the parallel nanometer channel in the alignment process; in addition, the alignment bonding can be performed under a high-precision microscope, and a plasma cleaning machine or a high-temperature heating method is adopted in the bonding process.
(5) Respectively injecting KCl solution and ion conductor [ BMIM ] into the left liquid storage tank and the right liquid storage tank][PF6]And inserting Ag/AgCl doped electrodes respectively to finish the preparation of the synapse device with the complementary structure of the nano-fluid interface type memristor.
The 2 parallel nano channels are arranged in parallel, and the included angle between the nano channels and the micron channel can adopt other angles besides the nano channels are arranged perpendicular to the micron channel. The liquid storage tank can be a cylindrical liquid storage tank, and the whole synapse device with the complementary structure is provided with at least 2 liquid storage tanks, wherein 1 liquid storage tank is connected with the first micron channel, and the other 1 liquid storage tank is connected with the second micron channel; the number and location of the reservoirs may be other numbers and locations than shown in fig. 1, as long as the reservoirs are capable of connecting to the first microchannel or the second microchannel and providing them with the first liquid or the second liquid.
In addition, the specific types of the first liquid and the second liquid, and the specific inner wall materials of the first nanochannel and the second nanochannel may be other materials besides the specific combinations given in the above embodiments, as long as the first liquid and the second liquid have a difference in electrical conductivity and are not mutually soluble, and the first liquid and the surfaces of the two parallel nanochannels have different electrical properties when in contact, and the two nanochannels have ion permselectivity for the first liquid and do not generate ion permselectivity for the second liquid.
The above embodiment only takes one kind of functional nanochannels corresponding to only one nanochannel as an example, but based on the present invention, there is no specific requirement on the total number of nanochannels, as long as the two kinds of functional nanochannels exist at the same time, and the combination of two or more nanochannels can realize synapses with complementary structures. Each channel corresponds to a specific conductance variation range, if a plurality of nano channels are parallel, the conductance variation range of the whole device is enlarged, and the conductance variation interval is adjusted along with the variation of the number of the channels with surface charges with different polarities. Assuming that the conductance variation range corresponding to one nanochannel is 3-6 (both the positively and negatively charged channels are the same), if three channels with negative charges on the surface and one channel with positive charges on the surface are provided, the conductance variation range obtained by theoretical calculation is 15-21 (i.e., 3 x 3+ 6-6 x 3+6), although in practice, the conductance variation may be additionally varied (for example, in practice, under the same electric field, the variation of conductance of different channels is different, which may cause the conductance variation range to be shifted).
As a supplementary note, the wall charge density can be changed by adjusting the pH of the first liquid, or applying a bias, for example, and the above-described embodiment of the present invention selects the first liquid having a neutral property (so that the degree of hydrolysis will be kept constant), so that experimental verification can be performed without changing the wall charge density.
It will be understood by those skilled in the art that the foregoing is only a preferred embodiment of the present invention, and is not intended to limit the invention, and that any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the scope of the present invention.
Claims (10)
1. A preparation method of a synapse device with a complementary structure based on a nano fluid interface type memristor is characterized in that the synapse device with the complementary structure comprises at least two parallel nano channels which are functionally divided into two types, a first liquid channel and a second liquid channel are arranged at two ends of the nano channels, and any one of the nano channels is used for communicating the first liquid channel with the second liquid channel; and, the nanochannels are all located on a first substrate, the first liquid channel and the second liquid channel are both located on a second substrate, and the first substrate and the second substrate are laminated together to form a monolithic structure; wherein the content of the first and second substances,
the first liquid channel is used for containing a first liquid and is connected with the first electrode; the second liquid channel is used for containing a second liquid and is connected with the second electrode; the first liquid and the second liquid have difference in conductivity and are not mutually soluble;
the nanometer channels can be functionally classified into two types, namely a first type of functional nanometer channel and a second type of functional nanometer channel; the two types of functional nano channels can generate different hydrolysis reactions after being contacted with the first liquid to generate ions with different positive and negative electric properties, so that the wall surfaces of the two types of functional nano channels show electric properties with different positive and negative electric properties, and the two types of functions can be divided by utilizing the difference of the positive and negative electric properties; the two types of functional nano-channels are respectively marked as a first type of functional nano-channel and a second type of functional nano-channel, wherein the first type of functional nano-channel can make the wall surface show negative charge after being contacted with the first liquid, and the second type of functional nano-channel can make the wall surface show positive charge after being contacted with the first liquid; due to the fact that positive and negative electric properties of the wall surface are different, the first type of functional nano-channel and the second type of functional nano-channel can show different ion selective permeability for the first liquid, and meanwhile, the two types of functional nano-channels can not show ion selective permeability for the second liquid;
the first electrode and the second electrode are used for applying an external voltage to the nano channels so as to introduce an external electric field effect to the nano channels; the external voltage can generate external electric fields in the same direction in the nano channels, and under the action of the external electric fields, the electric charges on the wall surfaces of the two types of functional nano channels are different, so that the conductance changes of the two types of functional nano channels are opposite, and the synaptronic structure device of the nano-fluid interface type memristor is realized;
the preparation method comprises the following steps:
(1) in SiO2Obtaining at least two parallel nano channels on a substrate through a semiconductor processing technology, wherein the semiconductor processing technology comprises electron beam lithography and plasma etching, and then removing photoresist; then, the nanometer channels are divided functionally in advance, wherein at least one nanometer channel is divided into a first type of functional nanometer channel in advance, and at least one nanometer channel is divided into a second type of functional nanometer channel; the nanometer channels pre-divided into the first type of functional nanometer channels are kept unchanged; the nano channel pre-divided into the second type of functional nano channel needs to be subjected to electron beam evaporation through a photoresist exposure mask after the plasma etching process is finished, and after stripping is finished, the inner wall of the nano channel is modified, so that the wall surface obtained after modification is a material which can be hydrolyzed with the first liquid and then is positively charged; therefore, the preparation of the nanometer channels with the first type of function and the second type of function which are functionally divided into two types in total is realized;
(2) preparing a PDMS substrate having a first liquid channel and a second liquid channel;
(3) subjecting the SiO obtained in the step (1) to2And (3) aligning, bonding and packaging the substrate and the PDMS substrate obtained in the step (2), so that any one of the nano channels can be communicated with the first liquid channel and the second liquid channel.
2. The method according to claim 1, wherein the inner wall material of the first functional nano-channel is SiO2；
The step (2) specifically comprises the following operations: preparing another SiO2The substrate is coated with photoresist in a spinning mode, is aligned through a mask plate in an alignment mode, is exposed, is developed by using corresponding developing solution, and is dried and formed; then, a PDMS reagent is used for carrying out mould inversion, drying and forming are carried out, and then the PDMS forming module is formed from the SiO2And taking down the substrate to obtain the PDMS substrate with the first liquid channel and the second liquid channel.
3. The method according to claim 2, wherein in the step (2), the exposure is performed by using an ultraviolet lithography machine.
4. The method of claim 1, further comprising the steps of:
(4) correspondingly injecting a first liquid and a second liquid into the first liquid channel and the second liquid channel respectively, wherein the first liquid and the second liquid have difference in conductivity and are not mutually soluble; the two types of functional nano channels can generate different hydrolysis reactions after being contacted with the first liquid to generate ions with different positive and negative electric properties, so that the wall surfaces of the two types of functional nano channels have different positive and negative electric properties; wherein the first type of functional nanochannel is capable of rendering the wall surface negatively charged upon contact with the first liquid and the second type of functional nanochannel is capable of rendering the wall surface positively charged upon contact with the first liquid; due to the fact that positive and negative electric properties of the wall surface are different, the first type of functional nano-channel and the second type of functional nano-channel can show different ion selective permeability for the first liquid, and meanwhile, the two types of functional nano-channels can not show ion selective permeability for the second liquid.
5. The method according to claim 4, wherein in the step (4), the first liquid is an aqueous solution of a compound salt, and the second liquid is an ionic conductor or a conductive organic compound immiscible with the aqueous solution of the compound salt.
6. The method of claim 5, wherein in the step (4), the first liquid is an aqueous solution of KCl, and the second liquid is [ BMIM ]][PF6]。
7. The method according to claim 1, wherein the wall material of the second type of functional nanochannel is Al2O3Correspondingly, in the step (1), when the electron beam evaporation technology is adopted to modify the nano channel pre-divided into the second type of functional nano channel, the material used by the electron beam evaporation is Al, specifically, evaporation is performed first, and after the evaporation is completed, the nano channel is contacted with air to be oxidized, so that Al is generated2O3。
8. The method according to claim 1, wherein in the step (3), after the alignment bonding is completed, any one of the nanochannels is perpendicular to the first liquid channel and the second liquid channel.
9. The method of claim 1, wherein the depth of any one of the nano-channels is 80-200nm, the width is 50-300nm, and the length is 10-100 um.
10. The method of claim 1, wherein the first fluid channel comprises a first microchannel, and at least 2 reservoirs connected by the first microchannel; the depth of the first micron channel is 50-1000um, the width is 1-5um, and the length is 1-2 cm;
the second liquid channel specifically comprises a second micron channel and at least 2 liquid storage tanks connected through the second micron channel; the depth of the second micron channel is 50-1000um, the width is 1-5um, and the length is 1-2 cm;
1 first electrode disposed in a reservoir connected to said first microchannel;
1 second electrode disposed in a reservoir connected to said second microchannel;
the number of the liquid storage tanks is 4, two of the liquid storage tanks are respectively distributed at two tail ends of the first micron channel, and the other two liquid storage tanks are respectively distributed at two tail ends of the second micron channel.
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