JPWO2005060005A1 - Switching element - Google Patents

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JPWO2005060005A1
JPWO2005060005A1 JP2005516353A JP2005516353A JPWO2005060005A1 JP WO2005060005 A1 JPWO2005060005 A1 JP WO2005060005A1 JP 2005516353 A JP2005516353 A JP 2005516353A JP 2005516353 A JP2005516353 A JP 2005516353A JP WO2005060005 A1 JPWO2005060005 A1 JP WO2005060005A1
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switching element
electrode
thin film
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JP4835158B2 (en
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加藤 久人
久人 加藤
川上 春雄
春雄 川上
山城 啓輔
啓輔 山城
恭子 加藤
恭子 加藤
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富士電機ホールディングス株式会社
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    • BPERFORMING OPERATIONS; TRANSPORTING
    • B82NANOTECHNOLOGY
    • B82YSPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
    • B82Y30/00Nanotechnology for materials or surface science, e.g. nanocomposites
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B82NANOTECHNOLOGY
    • B82YSPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
    • B82Y10/00Nanotechnology for information processing, storage or transmission, e.g. quantum computing or single electron logic
    • HELECTRICITY
    • H01BASIC ELECTRIC ELEMENTS
    • H01LSEMICONDUCTOR DEVICES; ELECTRIC SOLID STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H01L27/00Devices consisting of a plurality of semiconductor or other solid-state components formed in or on a common substrate
    • H01L27/28Devices consisting of a plurality of semiconductor or other solid-state components formed in or on a common substrate including components using organic materials as the active part, or using a combination of organic materials with other materials as the active part
    • H01L27/285Integrated circuits with a common active layer, e.g. cross point devices
    • HELECTRICITY
    • H01BASIC ELECTRIC ELEMENTS
    • H01LSEMICONDUCTOR DEVICES; ELECTRIC SOLID STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H01L51/00Solid state devices using organic materials as the active part, or using a combination of organic materials with other materials as the active part; Processes or apparatus specially adapted for the manufacture or treatment of such devices, or of parts thereof
    • H01L51/0032Selection of organic semiconducting materials, e.g. organic light sensitive or organic light emitting materials
    • H01L51/0045Carbon containing materials, e.g. carbon nanotubes, fullerenes
    • H01L51/0046Fullerenes, e.g. C60, C70
    • HELECTRICITY
    • H01BASIC ELECTRIC ELEMENTS
    • H01LSEMICONDUCTOR DEVICES; ELECTRIC SOLID STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H01L51/00Solid state devices using organic materials as the active part, or using a combination of organic materials with other materials as the active part; Processes or apparatus specially adapted for the manufacture or treatment of such devices, or of parts thereof
    • H01L51/05Solid state devices using organic materials as the active part, or using a combination of organic materials with other materials as the active part; Processes or apparatus specially adapted for the manufacture or treatment of such devices, or of parts thereof specially adapted for rectifying, amplifying, oscillating or switching, or capacitors or resistors with at least one potential- jump barrier or surface barrier multistep processes for their manufacture
    • H01L51/0575Solid state devices using organic materials as the active part, or using a combination of organic materials with other materials as the active part; Processes or apparatus specially adapted for the manufacture or treatment of such devices, or of parts thereof specially adapted for rectifying, amplifying, oscillating or switching, or capacitors or resistors with at least one potential- jump barrier or surface barrier multistep processes for their manufacture the devices being controllable only by variation of the electric current supplied or the electric potential applied, to one or more of the electrodes carrying the current to be rectified, amplified, oscillated or switched, e.g. two-terminal devices
    • H01L51/0595Solid state devices using organic materials as the active part, or using a combination of organic materials with other materials as the active part; Processes or apparatus specially adapted for the manufacture or treatment of such devices, or of parts thereof specially adapted for rectifying, amplifying, oscillating or switching, or capacitors or resistors with at least one potential- jump barrier or surface barrier multistep processes for their manufacture the devices being controllable only by variation of the electric current supplied or the electric potential applied, to one or more of the electrodes carrying the current to be rectified, amplified, oscillated or switched, e.g. two-terminal devices molecular electronic devices

Abstract

Provided is a switching element having high switching reproducibility and capable of obtaining a high current value in an on state. In this switching element, a bistable material layer 30 having two kinds of stable resistance values with respect to an applied voltage is arranged as a thin film between the first electrode layer 20a and the second electrode layer 20b, and the bistable The material layer 30 is made of fullerenes, and at least one of the electrodes is an electrode containing gold. The fullerenes are preferably C60 and / or C70, and more preferably the thickness of the bistable material layer 30 is 10 angstroms to 100 μm.

Description

  The present invention relates to a switching element for driving a display panel using an organic EL, a switching element used for a high density memory, and the like, and more particularly to a switching element in which a bistable material is disposed between at least two electrodes.

  In recent years, the characteristics of organic electronic materials have made remarkable progress. In particular, some low-dimensional conductors such as charge transfer complexes have characteristic properties such as metal-insulator transition, and their application to switching elements for driving organic EL display panels and high-density memories is being investigated. Yes.

  Organic bistable materials have attracted attention as materials that can be applied to the above switching elements. An organic bistable material is an organic material that exhibits a so-called non-linear response in which a switching phenomenon is observed when a voltage is applied to the material, and the current of the circuit suddenly increases above a certain voltage.

  FIG. 3 shows an example of voltage-current characteristics of an organic bistable material exhibiting the above switching behavior.

  As shown in FIG. 3, the organic bistable material has two current-voltage characteristics of a high resistance characteristic 51 (off state) and a low resistance characteristic 52 (on state). In the applied state, if the voltage (potential difference) is set to Vth2 or more, it changes from the off state to the on state, and if it is set to Vth1 or less, it has a nonlinear response characteristic that changes from the on state to the off state and the resistance value changes. is doing. That is, a so-called switching operation can be performed by applying a voltage of Vth2 or more or Vth1 or less to the organic bistable material. Here, Vth1 and Vth2 can also be applied as pulse voltages.

  Various organic complexes are known as organic bistable materials exhibiting such a nonlinear response. For example, RSPotember et al., Using a Cu-TCNQ (copper-tetracyanoquinodimethane) complex, prototyped a switching element having two stable resistance values with respect to voltage (see Non-Patent Document 1). .

  Kumai et al. Observed switching behavior due to nonlinear response using a single crystal of K-TCNQ (potassium-tetracyanoquinodimethane) complex (see Non-Patent Document 2).

  Furthermore, Adachi et al. Formed a Cu-TCNQ complex thin film by using a vacuum deposition method, clarified the switching characteristics, and examined the applicability to an organic EL matrix (see Non-Patent Document 3). .

  Moreover, as a memory element using the same material, Yang Yang et al. In a low conductivity material such as aminoimidazole dicarbonitrile (AIDCN), aluminum quinoline, polystyrene, polymethyl methacrylate (PMMA), gold, silver It is disclosed that the above-mentioned bistable characteristics can be stably obtained by forming a high conductivity material such as aluminum, copper, nickel, magnesium, indium, calcium, lithium or the like as a thin film or as dispersed fine particles. (See Patent Document 1).

Here, all of the above switching elements are a two-component system composed of a combination of a donor molecule or a metal element having a donor property and an acceptor molecule such as TCQN, or a low-conductivity material and a high-conductivity material. In the production of a switching element, it is necessary to strictly control the composition ratio of the two components. For this reason, there is a problem that it is difficult to mass-produce switching elements of uniform quality with no variation in bistable characteristics. On the other hand, A. Bandyopadhyay et al. Discloses that bistability can be obtained using Rose Bengal, which is a one-component organic material (see Non-Patent Document 4).
International Publication No. 02/37500 Pamphlet RSPotember et al. Appl. Phys. Lett. 34, (1979) 405 Kumai et al. Solid State Physics 35 (2000) 35 Adachi et al. Proceedings of the Japan Society of Applied Physics Spring 2002 3rd volume 1236 A. Bandyopadhyay et al. Appl. Phys. Lett. 72, (2003) 1215)

  As described above, the two-component switching element is not sufficiently reproducible in the switching phenomenon, and the switching characteristics have not been observed in all elements even in an element manufactured under the same manufacturing conditions. That is, there is a problem that the appearance probability (transition probability) of the element that switches (transitions) is low. Also, when transition is observed, there is a problem that the transition voltage from the off state to the on state is not constant.

Further, in the one-component switching element in Non-Patent Document 4 described above, although switching characteristics can be obtained, the current in the ON state is as low as about 1 mA / cm 2, which is necessary when actually driving an organic EL. There is a problem that it is smaller by one digit or more than the current value of 100 mA / cm 2 .

  The present invention has been made in view of the above-described problems of the prior art, and in a switching element in which a bistable material is disposed between electrodes, switching reproducibility is high and a high current value in an on state can be obtained. An object is to provide a switching element.

  That is, the switching element of the present invention is a switching element in which a bistable material having two kinds of stable resistance values with respect to an applied voltage is arranged as a thin film between at least two electrodes, The stable material is a fullerene, and at least one of the electrodes contains gold. In this case, the fullerene is preferably C60 and / or C70, and the thickness of the thin film made of the fullerene is more preferably 10 Å to 100 μm.

  According to the switching element of the present invention, high reproducibility of switching and a high current value in the on state can be obtained. The reason is considered as follows.

  The fullerene thin film has an electron transport property, and the lowest unoccupied orbital level (LUMO): -3.6 eV of the fullerene thin film is higher than the work function of the gold electrode: -5.1 eV. Therefore, when a negative voltage is applied to the gold electrode, basically no electrons are injected from the gold electrode into the fullerene thin film. Here, when a negative voltage is applied to the gold electrode, it is presumed that positive electric charges injected from the counter electrode accumulate at this interface and the electric field rises locally.

  Although the mechanism of this charge accumulation is not clear, (i) since the gold thin film is in the form of spherical fine particles and the contact area with the fullerene thin film is small, there are many bag paths in the organic film, and charges accumulate there. (Ii) Gold is likely to diffuse into fullerene, and a mechanism such as accumulation of electric charge in the diffused gold is assumed. Both are phenomena caused by physical properties unique to gold.

  Here, when the local electric field exceeds a certain value, dielectric breakdown occurs and electrons are injected from the gold electrode to the fullerene thin film, the resistance at the gold electrode / fullerene thin film interface is extremely reduced, and the device is turned on. It becomes a state. When a positive voltage is applied to the gold electrode, electron injection from the gold electrode to the fullerene thin film is stopped, and the resistance at the gold electrode / fullerene thin film interface returns to the original high resistance state (off state).

  On the other hand, when a positive voltage is applied to the gold electrode, it can be conductive or insulating depending on the work function of the other electrode. However, if a metal having a work function of −4 eV or less is used for the other electrode, In addition, it is easy to inject positive charges into the fullerene thin film, and becomes insulative even when a positive voltage is applied to the gold electrode. Therefore, it is suitable as a bistable element used for driving an organic EL panel, for example. is there.

The mobility of electrons in the fullerene thin film is about 1 cm 2 / Vs. This is several orders of magnitude greater than the mobility of 1 × 10 −3 to 1 × 10 −5 cm 2 / Vs, which is the mobility when an organic compound is used as the bistable material. For this reason, a large on-current can be realized when electrons are injected into the fullerene thin film and turned on.

  According to the present invention, it is possible to obtain a bistability with a very large on-current and to provide a switching element suitable for mass production.

It is a schematic block diagram which shows one Embodiment of the switching element of this invention. 3 is a chart showing current-voltage characteristics of a switching element in Example 1. It is a graph which shows the concept of the voltage-current characteristic of the conventional switching element.

Explanation of symbols

10: Substrate 20a: First electrode layer 20b: Second electrode layer 30: Bistable material layer 51, 71: High resistance state 52, 72: Low resistance state
Vth1: Low threshold voltage (potential difference)
Vth2: High threshold voltage (potential difference)

  Hereinafter, the present invention will be described in detail with reference to the drawings. FIG. 1 is a schematic configuration diagram showing an embodiment of a switching element of the present invention.

  As shown in FIG. 1, the switching element has a configuration in which a first electrode layer 20a, a bistable material layer 30, and a second electrode layer 20b are sequentially stacked on a substrate 10 as a thin film.

  The substrate 10 is not particularly limited as long as it is insulative, but a conventionally known glass substrate or the like is preferably used.

  At least one of the first electrode layer 20a and the second electrode layer 20b needs to be an electrode containing gold, and is preferably a gold electrode. In this case, the other electrode material is a metal material such as aluminum, gold, silver, copper, nickel or iron, an inorganic material such as ITO or carbon, a conjugated organic material, an organic material such as liquid crystal, or a semiconductor material such as silicon. However, it is preferable to use a material having a work function of −4 eV or less.

  This facilitates positive charge injection into the bistable material layer 30 as described above, and becomes insulative when a positive voltage is applied to the gold electrode, and is used, for example, when driving an organic EL panel. It becomes a suitable structure as a bistable element. Specific examples of such a material having a work function of −4 eV or less include aluminum, gold, silver, copper, chromium, nickel, iron, and ITO.

  In addition, in this invention, an electrode is not limited to a thin film, For example, any forms, such as a metal plate, a carbon plate, a thin film, and a conductive coating film, can be used.

  When used in the form of a thin film, it can be used after being thinned by means such as a metal foil, a vapor deposition film, a sputtering film, an electrodeposition film, or a spray pyrolysis film. Alternatively, an electrode can be formed by applying a conductive paint (for example, silver or carbon-containing paint). Here, when an electrode is provided by film formation or coating, the switching element is preferably formed on a substrate 10 as shown in FIG. Moreover, when using plate-shaped electrodes, such as a metal plate and a carbon plate, it is not necessary to use a board | substrate especially.

  As the configuration of the electrodes, as shown in FIG. 1, a sandwich electrode in which electrodes are provided so as to sandwich the bistable material layer 30 may be used. For example, a gap electrode such as a parallel electrode or a comb tooth electrode may be used. There is no particular limitation. Moreover, the film thickness of an electrode can be made arbitrary and is not specifically limited.

  Next, the present invention is characterized in that a thin film made of fullerenes is used as the bistable material layer 30.

Here, fullerenes are generic names for spherical or rugby ball-like carbon clusters made of sp 2 carbon, and generally C60, C70, C76, C78, C84, etc. are known. These are contained in soot produced by vaporizing carbon by arc discharge or resistance heating and quenching with an inert gas such as helium (for example, Kraetschmer et al., Nature, No. 347, 354 (1990)). ), C60 is most contained. And from this soot, the mixture of the said carbon cluster is obtained by extracting with solvents, such as hexane, benzene, toluene, mesitylene, carbon disulfide, for example.

  Further, in order to purify the mixture and isolate each of them, a chromatographic technique usually used for purification of an organic compound (for example, Kraetschmer et al., Nature, No. 347, page 354 (1990)) can be used. . In the present invention, C60 or C70 that can be easily synthesized and isolated, or mixed fullerene obtained by extracting from insoluble soot and removing insoluble impurities is preferably used because it is easily available and low in cost. . In addition, these fullerenes are marketed, for example from Tokyo Chemical Industry etc., and this commercial item can be used.

  The bistable material layer 30 which is a thin film made of fullerenes can be formed by thinning the above fullerenes by various conventionally known film forming methods. For example, a vacuum deposition film, a cast film, a polymer dispersion film, or the like can be used.

The vacuum deposited film is, for example, according to a general vacuum deposition method (Thin Film Handbook, edited by the Japan Society for the Promotion of Science Thin Film No. 131 Committee, Ohmsha (1984), etc.) under a vacuum of 5 × 10 −5 torr or less. A thin film can be formed by heating fullerenes using a metal boat, an alumina boat, or the like, and placing a substrate on the top or bottom. At this time, the substrate may be heated or cooled as necessary. When the substrate is cooled, the thin film is in an amorphous state, and when heated to room temperature or higher, it is obtained in a crystalline state. This vacuum vapor deposition film of fullerenes is stable in air and is very hard and strong.

  The cast film utilizes, for example, the property that fullerenes are dissolved in aromatic hydrocarbons such as benzene, toluene, and mesitylene, carbon disulfide, n-hexane, and the like, and is a means by which a thin film can be easily formed. That is, after dissolving in the above-mentioned solvent and dropping on the substrate, or fixing the substrate on a spinner and dropping the solution, the spinner is rotated at an appropriate number of revolutions to form a thin film or dropped onto the substrate. A film can be formed by thinning the solution by means such as thinning using a bar coater or a doctor blade, and then drying by natural drying or means such as heat or vacuum drying.

  For example, after adding fullerenes in a polymer solution to dissolve or disperse the polymer dispersion film, the polymer dispersion film can be formed by the same means as the cast film. As a dispersion method, a pigment dispersion method such as paint shaker, specs mixer mill, sand mill, ball mill, atrator or kneader can be used.

  Although there is no restriction | limiting in particular as said polymer, For example, vinyl-type polymers, such as saturated polyester, unsaturated polyester, polycarbonate, polyvinyl chloride, polyvinyl acetate, polyvinyl carbazole, styrene, polyvinylidene fluoride, polyvinyl fluoride Examples thereof include fluorinated polymers and copolymers such as styrene-maleic acid. In addition, for example, a liquid crystal polymer such as a polyacrylate liquid crystal polymer or a polysiloxane liquid crystal polymer may be used.

  Regarding the film thickness of the bistable material layer 30, that is, the film thickness of the thin film made of fullerenes, when using a gap electrode, it is sufficient that the thickness is at least one molecule, specifically, 10 angstroms to 100 μm is preferable. More preferably, the thickness is 10 Å to 10 μm. If the thickness is less than 10 angstroms, the thickness is less than a single molecule, so that fullerenes cannot be formed. On the other hand, if it exceeds 100 μm, the transition voltage at the time of switching becomes too high, which is not preferable.

  In addition, when using a sandwich electrode, since a mutual electrode will short-circuit if it is too thin, a certain amount of thickness is required. In this case, the film thickness of the fullerene thin film is preferably in the range of 100 Å to 100 μm, more preferably 200 Å to 10 μm.

Hereinafter, the switching element of the present invention will be described in more detail using examples.
<Example 1>

  A switching element having a configuration as shown in FIG. 1 was prepared by the following procedure.

  A glass substrate is used as the substrate 10, and copper is sequentially used as the first electrode layer 20a, fullerene (C60: manufactured by Tokyo Chemical Industry Co., Ltd.) as the bistable material layer 30, and gold as the second electrode layer 20b by vacuum deposition. A thin film was formed to form the switching element of Example 1.

Note that the first electrode layer 20a, the bistable material layer 30, and the second electrode layer 20b were formed to have thicknesses of 100 nm, 80 nm, and 100 nm, respectively. The vapor deposition apparatus was a diffusion pump exhaust, and was performed at a vacuum degree of 3 × 10 −6 torr. Further, the deposition of copper and gold was performed by a resistance heating method, and the deposition rate was 3 Å / sec, and the deposition of fullerene was performed by a resistance heating method, and the deposition rate was 2 Å / sec. Vapor deposition of each layer was continuously performed with the same vapor deposition apparatus, and the conditions were such that the sample did not come into contact with air during vapor deposition.
<Example 2>

A film was formed under the same conditions as in Example 1 except that fullerene (C70: manufactured by Tokyo Chemical Industry Co., Ltd.) was used as the bistable material layer 30 to obtain a switching element of Example 2.
<Example 3>

A switching element of Example 3 was obtained by forming a film under the same conditions as in Example 1 except that chromium was used instead of copper as the first electrode layer 20a.
<Example 4>

A switching element of Example 4 was obtained by forming a film under the same conditions as in Example 1 except that gold was used as the first electrode layer 20a and copper was used as the second electrode layer 20b.
<Test example>

About the switching element of said Examples 1-4, the current-voltage characteristic was measured in room temperature environment, and the result of having measured the high threshold voltage (potential difference) Vth2 and the current density Ion in an ON state which are the threshold voltages in FIG. These are summarized in Table 1. Here, the voltage (potential difference) is applied to the second electrode layer 20b side. In Examples 1 to 3, the first electrode layer 20a (copper electrode) is set to 0 potential, and the potential of the second electrode layer 20b is In Example 4, the first electrode layer 20a (gold electrode) is set to 0 potential, and the potential of the second electrode layer 20b (copper electrode) is shown. FIG. 2 shows current-voltage characteristics of the switching element of Example 1. In the measurement, the output current of the voltage source was limited to a maximum of 1 A / cm 2 to suppress element damage due to overcurrent.

  From the result of FIG. 2, the bistability of the high resistance state 71 and the low resistance state 72 was obtained in the switching element of Example 1.

That is, in Example 1 of FIG. 2, when the low threshold voltage (potential difference) Vth1 was 0 V, the resistance value changed from the low resistance state 72 to the high resistance state 71 (from the on state to the off state). Further, when the high threshold voltage (potential difference) Vth2 is −7.6 V, the high resistance state 71 transits to the low resistance state 72 (from the off state to the on state). At this time, it can be seen that the current value is 1 A / cm 2 or more in the low resistance state, and the ratio of the low resistance state / high resistance state is at least 10 3 or more.

This bistability was obtained for all the switching elements of Examples 1 to 4. The high threshold voltage (potential difference) Vth2 is −8.2V and −5.8V in Examples 2 and 3, respectively, and 9.4V in Example 4 in which gold is used for the first electrode layer 20a. The on-current was 1 A / cm 2 or more, which is the limiting current value.

The switching element of the present invention can be suitably used for a switching element for driving a display panel such as an organic EL, a high-density memory, or the like.

Claims (3)

  1.   A switching element in which a bistable material having two types of stable resistance values with respect to an applied voltage is arranged as a thin film between at least two electrodes, the bistable material comprising fullerenes, A switching element, wherein at least one of the electrodes contains gold.
  2.   The switching element according to claim 1, wherein the fullerene is C60 and / or C70.
  3.   3. The switching element according to claim 1, wherein the thin film made of the fullerene has a thickness of 10 Å to 100 μm.
JP2005516353A 2003-12-18 2004-12-17 Switching element Active JP4835158B2 (en)

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KR100695166B1 (en) * 2006-01-03 2007-03-08 삼성전자주식회사 Manufacturing method phase-change ram comprising fullerene layer
JP5205670B2 (en) * 2006-03-20 2013-06-05 独立行政法人物質・材料研究機構 Solid element structure and electric / electronic element and electric / electronic device using the same
KR100897881B1 (en) 2006-06-02 2009-05-18 삼성전자주식회사 Memory of fabricating organic memory device employing stack of organic material layer and buckminster fullerene layer as a data storage element
US8110476B2 (en) * 2008-04-11 2012-02-07 Sandisk 3D Llc Memory cell that includes a carbon-based memory element and methods of forming the same

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JPH04158576A (en) * 1990-10-23 1992-06-01 Toshiba Corp Organic thin film device
JPH0629514A (en) * 1992-01-13 1994-02-04 Kawamura Inst Of Chem Res Semiconductor element
JPH07104330A (en) * 1993-10-05 1995-04-21 Hitachi Ltd Nonlinear optical device
JP2002540591A (en) * 1998-12-15 2002-11-26 イー−インク コーポレイション Printing method of a transistor array on a plastic substrate
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