CN111640869B - Multifunctional photoresponsive transistor device, preparation method and application thereof - Google Patents
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Abstract
The invention provides a multifunctional photoresponsive transistor device, a preparation method and application thereof, and belongs to the field of semiconductors. The invention provides a multifunctional light response transistor device, comprising: substrate, active layer and electrode, wherein, the material of active layer includes: an organic semiconductor and chlorophyll. The multifunctional light response transistor device provided by the invention can be used as a photoelectric transistor to realize detection of light signals, and can also be used as a photoelectric detector or a light stimulation synaptic device. When the photoelectric transistor is used, the device has high sensitivity to optical signals, and the output signal and the transfer signal of the transistor can be used as the electrical signals of the response, so that the detection and conversion of the optical signals in different modes are easy to realize. When the multifunctional light response transistor provided by the invention is used as a light stimulation synaptic transistor, the study and forgetting behaviors of synapses can be simulated, and the multifunctional light response transistor has the function of processing graphics.
Description
Technical Field
The invention belongs to the field of semiconductors, and particularly relates to a multifunctional photoresponsive transistor device, a preparation method and application thereof.
Background
Photo-responsive organic field effect transistors have been widely studied for their great potential of application in the fields of communication units, medical imaging instruments, flexible and wearable electronics, etc. In recent years, research hotspots have expanded from single-component organic semiconductor-based light-responsive organic field effect transistors to devices composed of a variety of active materials, such as perovskite-and organic semiconductor-based light-responsive organic field effect transistors, and light-responsive organic field effect transistors having both p-type and n-type semiconductors. Although a variety of active materials are used in these devices, a single photoresponsive function is typically exhibited, for example, much of the previous research has focused on light sensing functions and recent research has focused on light synaptic functions. Currently, few studies on multifunctional photomultiplier tubes are performed, but the research is important. This is because the same device can realize different kinds of functions, and has important significance for high-integration multifunctional organic electronics.
In addition, with the enhancement of environmental awareness of people, biodegradable materials, particularly materials extracted from natural organic matters, have great significance in developing biosafety and environment-friendly organic photoelectric devices. Chlorophyll is the most abundant, green and important natural pigment in plant photosynthesis and biological metabolism. Chlorophyll has been widely studied in photocatalysis and photosynthesis over the past decades. However, chlorophyll-based photodetectors are rare and limited to several studies of graphene/chlorophyll and metal oxide/chlorophyll-based photodetectors.
On the other hand, similar to biological synapses that provide essential functions for the human cerebral nervous system, artificial synapse devices may become an essential component of a neuromorphic network. Studies have shown that synaptic devices have great potential in overcoming the bottleneck of von neumann architecture, and that simulation of human brain neuromorphic computation is an important direction of research in the development of next-generation neuromorphic computer systems.
Disclosure of Invention
The present invention has been made to solve the above-mentioned problems, and an object of the present invention is to provide a device for improving light response performance of an organic field effect transistor by using chlorophyll having light absorption capability, which can realize detection of light signals, particularly weak light; on the other hand, the organic light response transistor can be endowed with a response mode which is adjustable to light by utilizing the function of transistor grid regulation and control. The preparation method and the application of the multifunctional light response transistor device can conveniently and rapidly realize the multifunctional response of the organic transistor to light, and realize the functions of the photoelectric detector and the light stimulation synapse on a single device.
The invention provides a multifunctional light response transistor device, which has the following characteristics: the electrode comprises a substrate, an active layer and an electrode, wherein the material of the active layer comprises an organic semiconductor material and chlorophyll, and the weight of the chlorophyll accounts for 0.1% -90% of the total weight of the active layer.
In the multifunctional photoresponsive transistor device provided by the present invention, it may further have the following features: wherein the chlorophyll is natural chlorophyll, and is artificially synthesized chlorophyll or chlorophyll derivative.
In the multifunctional photoresponsive transistor device provided by the present invention, it may further have the following features: among them, the organic semiconductor may be a high molecular semiconductor or a small molecular semiconductor, preferably an organic semiconductor having a benzene ring structure (e.g., DNTT, C8-BTBT, pentacene, F8T2, phthalocyanine, PTAA, PFO, PPE, PIF) or an organic semiconductor having a thiophene structure (e.g., PDPP4T, pentathiophene, PQT-12, P3HT, PBTTT, NVP, PTVTF, PNDTBT).
In the multifunctional photoresponsive transistor device provided by the present invention, it may further have the following features: wherein the substrate is an inorganic substrate (such as glass substrate, ceramic substrate, silicon substrate, etc.) or an organic substrate (such as PLA substrate, PET substrate), etc.
In the multifunctional photoresponsive transistor device provided by the present invention, it may further have the following features: wherein the electrode is made of conductive metal, conductive alloy or conductive metal oxide.
In the multifunctional photoresponsive transistor device provided by the present invention, it may further have the following features: wherein the number of the electrodes is two, a conductive channel is arranged between the two electrodes, the length of the conductive channel is 4-100 mu m, and the width of the conductive channel is 0.2-10 mm.
The invention provides a preparation method of a multifunctional light response transistor device, which is characterized by comprising the following steps: the method comprises the following steps: step 1, cleaning a substrate, blow-drying, and carrying out OTS treatment on the substrate to obtain an intermediate A; step 2, dripping a natural chlorophyll/organic semiconductor solution on the surface of the intermediate A, and then forming an active layer on the surface of a substrate to obtain an intermediate B, wherein the method for forming the active layer on the surface of the substrate is any one of spin coating, drip coating, lifting or doctor-blading; and 3, evaporating or imprinting electrode materials on the upper surface of the active layer of the intermediate B in a mask mode under a high vacuum condition to form two electrodes, and forming the multifunctional photoresponsive transistor device.
The invention also provides a preparation method of the multifunctional light response transistor device, which has the following characteristics: when the active layer is formed on the surface of the substrate by adopting a spin coating method in the step 2, the spin coating rotating speed is 200r/min-6000r/min, and the spin coating time is 10s-300s.
The invention also provides an application of the multifunctional light response transistor device as a photoelectric detector, which has the technical characteristics that: the gate voltage of the multifunctional photoresponsive transistor device is-5V to-70V.
The invention also provides an application of the multifunctional light response transistor device as a light stimulation synaptic device, which has the technical characteristics that: the gate voltage of the multifunctional photoresponsive transistor device is 5V-70V.
Effects and effects of the invention
According to the multifunctional light response transistor device, the active layer of the multifunctional light response transistor device adopts chlorophyll/organic semiconductors, so that the multifunctional light response transistor device provided by the invention not only can realize detection of light signals and has high sensitivity, but also can be prepared into a three-terminal transistor device, double-voltage driving is realized, and output signals and transfer signals of the transistor can be used as electrical signals for response, so that light signal detection and conversion under different modes are easy to realize, and meanwhile, the preparation process is simple, the cost is low, the use is convenient, and mass production is easy to realize.
According to the application of the multifunctional light response transistor device as the photoelectric detector, the multifunctional light response transistor device can respond to light and dark signals rapidly, and the light-dark current ratio can reach 10 because the gate voltage of-5V to-70V is applied to the multifunctional light response transistor device 6 Has imaging capability.
According to the application of the multifunctional light response transistor device as the light stimulation synaptic device, the multifunctional light response transistor device provided by the invention can show the characteristic of simulating biological synapses for optical signals and realize the functions of dynamic learning, forgetting, graphic processing such as contrast enhancement and network cognition model calculation and identification because the gate voltage of 5-70V is applied to the multifunctional light response transistor device.
Drawings
Fig. 1 is a schematic structural diagram of a multifunctional phototransistor device in embodiment 1 of the present invention;
fig. 2 is a graph showing the output characteristics of the multifunction phototransistor device according to embodiment 1 of the present invention;
fig. 3 is a graph showing transfer characteristics of the multifunction phototransistor device according to embodiment 1 of the present invention;
FIG. 4 is a graph showing the variation of output current with the intensity of illumination signal when the multifunctional phototransistor device according to embodiment 2 of the present invention is used as a photodetector;
FIG. 5 is a graph showing the output current as a function of illumination signal intensity for the multifunction phototransistor device of example 2 according to the present invention;
FIG. 6 is a representation of an imaging application of the multifunctional light-responsive transistor device of embodiment 2 of the present invention as a photodetector;
FIG. 7 is a graph of output current versus optical stimulus signal for a multifunctional light-responsive transistor device of embodiment 3 of the present invention as an optical stimulus synapse device;
FIG. 8 is a diagram showing the dynamic learning and forgetting of the multifunctional light-responsive transistor device of embodiment 3 as a light-stimulated synaptic device in accordance with the present invention;
FIG. 9 is a diagram showing the graphic processing function of the multifunctional light-responsive transistor device of FIG. 3 in an embodiment of the present invention as a light-stimulated synapse device; and
FIG. 10 is a diagram showing the network identification simulation of numbers when the multifunctional light-responsive transistor device of FIG. 3 is used as a light-stimulated synapse device in an embodiment of the invention;
FIG. 11 is a graph showing the output current as a function of illumination signal intensity for the multifunction phototransistor device of example 4 according to the present invention;
fig. 12 is a graph showing the ratio of light to dark current when the multifunctional phototransistor device of embodiment 4 of the present invention is used as a photodetector.
Detailed Description
In order to make the technical means, the creation features, the achievement of the purpose and the effect of the present invention easy to understand, the present invention is specifically described below with reference to the embodiments and the drawings.
Example 1 ]
Fig. 1 is a schematic structural diagram of a multifunctional phototransistor device in embodiment 1 of the present invention.
As shown in fig. 1, the multifunctional light-responsive transistor device 100 provided in this embodiment includes: a substrate 10, an active layer 20 and two gold electrodes 30.
The substrate 10 includes a gate electrode 11 and an insulating layer 12 disposed over the gate electrode 11. In this embodiment the gate 11 is N-doped silicon and the insulating layer 12 is a silicon substrate of silicon dioxide with a thickness of 300 nm. In other embodiments, the insulating layer may also be made of a polymer material such as PLA or PVA as the flexible substrate. In other embodiments, the substrate 10 may be a glass substrate or a ceramic substrate with an insulating and smooth surface.
The active layer 20 consists of chlorophyll and the organic semiconductor PDPP4T (poly [2, 5-bis (2-octyldodecyl) pyrrolo [3,4-c ] pyrrole-1, 4 (2 h,5 h) -dione-3, 6-diyl) -alanine aminotransferase- (2, 2';5',2' "-tetrahydrothiophene-5, 5" -diyl ]), with a weight percentage of chlorophyll of 6.7%. In other embodiments, the chlorophyll content may be 0.1% to 90%. The active layer 20 is disposed over the insulating layer 12 by spin coating.
The structural formula of chlorophyll is shown as follows:
the structural formula of the organic semiconductor PDPP4T is shown as follows:
two gold electrodes 30 are deposited on the upper surface of the active layer 20 by vacuum thermal vapor deposition physical vapor deposition. The length of the conductive channel between the two gold electrodes 30 was 5 μm and the channel width was 0.3mm. In other embodiments, other conductive materials may be used as electrodes, such as silver electrodes, alloy electrodes or metal oxide electrodes, conductive plastics, and the like. In other embodiments, the conductive channel length may be 4 μm to 100 μm and the conductive channel width may be 0.2mm to 10mm.
The preparation method of the multifunctional photoresponsive transistor device provided by the embodiment comprises the following steps:
step 1, ultrasonically cleaning a substrate 10 by using acetone and isopropanol, then flushing by using deionized water and alcohol, drying the surface of the substrate 10 by using nitrogen, and then carrying out OTS treatment on the substrate to obtain an intermediate A;
step 2, placing the intermediate A on a spin coater, dripping chlorophyll/organic semiconductor solution with the chlorophyll weight of 6.7% on the surface, spin-coating, and spin-coating at a rotating speed of 3000r/min for 60 seconds to form an active layer on the surface of the substrate to obtain an intermediate B;
and 3, evaporating gold onto the organic semiconductor under high vacuum in a mask mode to form two gold electrodes 30, wherein a conducting channel between the two electrodes is 5 mu m long, and the channel width is 0.3mm, so that the multifunctional photoresponsive transistor device is formed.
The output characteristic curve and the transfer characteristic curve of the multifunctional optical response organic transistor provided by the embodiment are tested. The testing method comprises the following steps: and under the room temperature and the atmospheric environment, the K-4200 semiconductor tester and the related probe stage are used for scanning in the range of-60V to 60V, so that the output characteristic curve and the transfer characteristic curve of the device are obtained.
Fig. 2 is a graph showing the output characteristics of the multifunctional phototransistor device according to embodiment 1 of the present invention. Fig. 3 is a graph showing transfer characteristics of the multifunction phototransistor device according to embodiment 1 of the present invention.
Example 2 ]
The gate voltage of the multifunctional light response transistor device manufactured in the embodiment 1 is adjusted to-60V, so that the multifunctional light response transistor device can be used as a photoelectric detector.
Irradiating the multifunctional light-responsive organic transistor with LED collimation light source (wavelength 430 nm), and adjusting irradiation light intensity from 0.002-0.271mW/cm 2 And testing the output characteristic curve and the transfer characteristic curve of the OFET by using a semiconductor parameter instrument to obtain the current, mobility and change of threshold voltage of the OFET along with the light intensity.
Fig. 4 is a schematic diagram showing the variation of output current with the intensity of illumination signal when the multifunctional light-responsive transistor device in embodiment 2 of the present invention is used as a photodetector. Fig. 5 is a graph showing the output current as a function of illumination signal intensity when the multifunctional phototransistor device of embodiment 2 of the present invention is used as a photodetector.
As shown in fig. 4, the optical switching ratio of the multifunctional light-responsive transistor device according to embodiment 1 as a photosensor is about 10 6 。
As shown in fig. 5, the output current varies with the light intensity when the multifunctional light-responsive transistor device provided in embodiment 1 is used as a photosensor, indicating that the multifunctional light-responsive transistor device provided in embodiment 1 can also be used as a phototransistor.
At this time, the photo imaging characteristics of the multifunctional photo-responsive transistor device provided as example 1 of the photosensor were studied. An article having a pattern of a specific shape (E-shaped cardboard is used in this example) is overlaid on a 5 x 5 matrix of multi-functional photoresponsive transistor devices, and the matrix of devices is then placed under illumination to test the ratio of the electrical parameters of each device element, such as current, mobility, and threshold voltage, to the electrical parameters of each element without the article being overlaid, giving a photosensitive image of the device matrix for the article.
Fig. 6 is a diagram showing an imaging application of the multifunctional light-responsive transistor device of embodiment 2 as a photodetector.
As shown in fig. 6, the photosensitive device matrix signal output clearly shows the E-shaped pattern, indicating that the multifunctional photoresponsive transistor device prepared in example 1 has good pattern imaging capability.
Example 3 ]
The multifunctional phototransistor device manufactured in example 1 was used as a light-stimulated synaptic device by adjusting the gate voltage to 60V.
The multifunctional light-responsive organic transistor described above was illuminated using an LED collimated light source (wavelength 430 nm). Adjusting irradiation intensity to 0.04-0.48mW/cm 2 The irradiation time was 2 seconds, and the output current curve was detected.
Fig. 7 is a graph of output current versus optical stimulus signal for the multifunctional light-responsive transistor device of embodiment 3 of the present invention as an optical stimulus synapse device.
As shown in fig. 7, the output current curves of the multifunctional light-responsive transistor device manufactured in example 1 under irradiation of light stimuli of different intensities have characteristics similar to those of biological synapses, and can be used as a synaptic device.
The multifunctional light-responsive transistor device manufactured in example 1 as a light-stimulated synaptic device was tested for dynamic learning and forgetting behavior. An article with a pattern of specific shape (in this example, using H-shaped cardboard) was overlaid on a 3 x 3 matrix of multi-functional light responsive transistor devices, and the learning behavior of the light responsive transistor was tested 1 time without light stimulation and after 5 times, 20 times, and the current signal of the matrix was recorded. The light stimulus was then removed and the matrix was tested for output current signal after 1,3,5 minutes.
Fig. 8 is a diagram showing dynamic learning and forgetting of the multifunctional light-responsive transistor device of embodiment 3 as a light-stimulated synaptic device in accordance with the present invention.
The test results are shown in fig. 8, and the matrix signal output of the multifunctional photoresponsive transistor device prepared in the embodiment 1 clearly shows the dynamic learning and forgetting process of the device for optical stimulation.
The multifunctional light-responsive transistor device manufactured in example 1 as a light-stimulated synaptic device was investigated for its processing capability for patterns. We prepared a 3 x 3 array of synaptic transistors that were illuminated with different light intensities at different locations. The current of the matrix device can be read, which is then used as an input signal, resulting in a device having four gray scales.
Fig. 9 is a diagram showing the graphic processing function of the multifunctional light-responsive transistor device of embodiment 3 as a light-stimulated synapse device in accordance with the invention.
The test results are shown in fig. 9, and the device shows an increase in the difference of the current signal with time when the optical stimulus signal is removed. The device exhibited a greater current difference, i.e., pattern contrast enhancement, at 30 seconds and 90 seconds of removal of the optical stimulus signal.
Fig. 10 is a diagram showing a network identification simulation for numbers when the multifunctional light-responsive transistor device in 3 is used as a light-stimulated synapse device in an embodiment of the invention.
The multifunctional light-responsive transistor device manufactured in example 1 as a light-stimulated synaptic device was studied for digital recognition simulation performance. The present example uses the national institute of standards and technology (MNIST) database to demonstrate the learning ability of the light-stimulated synaptic transistors. In the embodiment, a two-layer convolutional neural network is designed, a supervised learning framework is established based on the channel conductance value of the synaptic transistor, and system-level MNIST pattern recognition is simulated. As shown in fig. 10, the present embodiment trains the network with images in the MNIST database, so that a recognition rate of 10 characters from 0 to 9 can be obtained, and the recognition process of the number 0 is shown in the figure.
Example 4 ]
Fig. 1 is a schematic diagram of a structure of a multifunctional phototransistor device according to embodiment 4 of the present invention.
As shown in fig. 1, the active layer 20 is composed of a derivative of chlorophyll and an organic semiconductor PDPP4T (poly [2, 5-bis (2-octyldodecyl) pyrrole [3,4-c ] pyrrole-1, 4 (2 h,5 h) -dione-3, 6-diyl) -alanine aminotransferase- (2, 2';5',2' "-tetrahydrothiophene-5, 5" -diyl ]), the content of chlorophyll derivative being 50%. In other embodiments, the content may be 1% to 80%. The active layer 20 is disposed over the insulating layer 12 by spin coating.
The structural formula of the chlorophyll derivative is shown as follows:
two gold electrodes 30 are deposited on the upper surface of the active layer 20 by vacuum thermal vapor deposition physical vapor deposition. The length of the conductive channel between the two gold electrodes 30 was 30 μm and the channel width was 1mm. In other embodiments, other conductive materials may be used as electrodes, such as silver electrodes, alloy electrodes or metal oxide electrodes, conductive plastics, and the like. In other embodiments, the conductive channel length may be 4 μm to 100 μm and the conductive channel width may be 0.2mm to 10mm.
The preparation method of the photoresponsive transistor device provided by the embodiment is similar to that of the embodiment 1, and comprises the following steps:
step 1, ultrasonically cleaning a substrate 10 by using acetone and isopropanol, then flushing by using deionized water and alcohol, drying the surface of the substrate 10 by using nitrogen, and then carrying out OTS treatment on the substrate to obtain an intermediate A;
step 2, the intermediate A is placed on a spin coater, and chlorophyll/organic semiconductor solution is dripped on the surface, wherein the content of chlorophyll derivative in the embodiment is 50%. Spin coating is carried out at a rotational speed of 2500r/min for 30 seconds, and an active layer is formed on the surface of the substrate to obtain an intermediate B;
and 3, evaporating gold onto the organic semiconductor under high vacuum in a mask mode to form two gold electrodes 30, wherein a conducting channel between the two electrodes is 30 mu m long and a channel width is 1mm, so that the photoresponsive transistor device is obtained.
The transfer characteristic curve test was performed on the optical response organic transistor provided in this embodiment. The testing method comprises the following steps: and under the room temperature and the atmospheric environment, the K-4200 semiconductor tester and the related probe stage are used for scanning within 10V-45V of driving voltage, so that the transfer characteristic curve of the device can be obtained.
In this case, it is used as a photodetector. Irradiating the multifunctional light-responsive organic transistor with LED collimation light source (wavelength 430 nm), and adjusting irradiation light intensity from 0.00068-0.0686mW/cm 2 The output characteristic curve and the transfer characteristic curve of the OFET are tested and recorded by a semiconductor parameter instrument.
Fig. 11 is a schematic diagram showing the variation of output current with the intensity of illumination signal when the multifunctional light-responsive transistor device in embodiment 4 of the present invention is used as a photodetector. It can be seen that as the light intensity increases, the device current continues to increase.
As shown in fig. 12, the optical switching ratio of the multifunctional light-responsive transistor device according to example 4 as a photosensor was about 10 6 . The device has good light response capability and can be used as a photoelectric transistor.
Effects and effects of the examples
According to the multifunctional photoresponsive transistor device in embodiment 1, since the active layer of the multifunctional photoresponsive transistor device adopts chlorophyll/organic semiconductors, the multifunctional photoresponsive transistor device provided in embodiment 1 not only can realize detection of light signals and has high sensitivity, but also can be prepared into a three-terminal transistor device, double-voltage driving is realized, output signals and transfer signals of the transistor can be used as electrical signals for response, detection and conversion of light signals in different modes are easy to realize, and meanwhile, the multifunctional photoresponsive transistor device is simple in preparation process, low in cost, convenient to use and easy to realize mass production.
According to the application of the multifunctional light-responsive transistor device of embodiment 2 as a photodetector, since a gate voltage of-60V is applied to the multifunctional light-responsive transistor device, the multifunctional light-responsive transistor device rapidly responds to light and dark signals, and the light-dark current ratio can reach 10 6 Has imaging capability.
According to the application of the multifunctional light-responsive transistor device according to embodiment 3 as the light-stimulated synaptic device, since the gate voltage of 60V is applied to the multifunctional light-responsive transistor device, the multifunctional light-responsive transistor device can exhibit the characteristics of simulating biological synapses for optical signals, realizing the functions of dynamic learning, forgetting, graphic processing such as contrast enhancement, and network cognitive model calculation recognition.
According to the multifunctional photoresponsive transistor device of example 4, since the active layer is made of chlorophyll derivatives/organic semiconductors, the device of the present invention has good photoresponsive effects on chlorophyll and its derivatives as active materials, and is suitable for use with a wide range of photosensitive materials. Meanwhile, the multifunctional photoresponsive transistor device provided by the embodiment 4 is simple in preparation process, low in cost and easy to produce.
The above embodiments are preferred examples of the present invention, and are not intended to limit the scope of the present invention.
Claims (3)
1. A multifunctional light-responsive transistor device, comprising: a substrate, an active layer and an electrode,
wherein the material of the active layer comprises an organic semiconductor material and chlorophyll, the weight of the chlorophyll accounts for 0.1-90% of the total weight of the active layer,
the chlorophyll is natural chlorophyll, artificially synthesized chlorophyll or chlorophyll derivative,
the organic semiconductor material is an organic semiconductor with benzene ring structure or an organic semiconductor with thiophene structure,
the substrate is a glass substrate, a ceramic substrate, a silicon substrate, a PET substrate or a PLA substrate,
the number of the electrodes is two, a conductive channel is arranged between the two electrodes,
the multifunctional photoresponsive transistor device has the function of a photoelectric detector when the grid voltage is between-5V and-70V,
the multifunctional light response transistor device has the function of a light stimulation synaptic device when the grid voltage is 5V-70V.
2. The multifunctional light-responsive transistor device of claim 1, wherein:
wherein the electrode is made of conductive metal, conductive alloy or conductive metal oxide.
3. The multifunctional light-responsive transistor device of claim 1, wherein:
wherein the length of the conducting channel is 4-100 mu m, and the width of the conducting channel is 0.2-10 mm.
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