CN100388410C - Method for producing one-electron device by modulated composite one-dimensional nanometer material - Google Patents

Method for producing one-electron device by modulated composite one-dimensional nanometer material Download PDF

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CN100388410C
CN100388410C CNB021579725A CN02157972A CN100388410C CN 100388410 C CN100388410 C CN 100388410C CN B021579725 A CNB021579725 A CN B021579725A CN 02157972 A CN02157972 A CN 02157972A CN 100388410 C CN100388410 C CN 100388410C
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electron device
tube
carbon nano
electrode
preparation
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CN1510716A (en
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彭练矛
陈清
梁学磊
车仁超
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Peking University
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Peking University
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Abstract

The present invention belongs to the field of nanoelectronics and nanoelectronic devices, more specifically an idea and a method by using modulated complex one-dimensional nanomaterials for building a single electronic device and improving the operating temperature of the single electronic device to a room temperature or even higher. The present invention can change electrical properties of a nanotube by introducing potential barriers into a one-dimensional nanostructure (nanotube) in a control mode in the process of growth (for example, by introducing metal particles, changing components, converting metal to insulators or converting noncrystal to crystal and injecting positioned electrons or ions). The complex nanomaterials can be used for preparing a single electronic device. The operating temperature of the prepared single electronic device can be controlled to reach a room temperature or a higher temperature by adjusting the space of the potential barriers. The present invention is used for the research of nanoelectronics and the preparation of a single electronic device.

Description

Utilize the compound monodimension nanometer material of modulating to prepare the method for single-electron device
Technical field
The invention belongs to nano-electron and nanometer electronic device field, be specially and utilize the compound monodimension nanometer material of modulation to prepare the list device, and improve working temperature to room temperature or higher method.
Background technology
The research of nano-electron device is the of paramount importance field of current nanoscale science and technology, and single-electron device is because its energy consumption is little, does not have advantage such as heat radiation and becomes the important development direction (K.Likharev, Proc.IEEE, 80,60 (1999) .) of nano-electron device.
The key of single-electron device research at present is how to improve its working temperature.The working temperature of single-electron device can be passed through the charging energy E on its " coulomb island " C=e 2/ 2C estimates, requires E C>>K BT (T is a working temperature).Wherein the most key parameter is effective capacitance C.More little its charging of effective capacitance C can E CHigh more, working temperature is also just high more.The key that makes up the elevated operating temperature single-electron device is to reduce its effective capacitance.
Carbon nano-tube becomes the ideal material of preparation single-electron device owing to the caliber of its excellent physical property and nano-scale.But how on carbon nano-tube, to obtain tube axial direction also very little " coulomb island " and be still a difficult problem.Dekker seminar of Dutch Delft university introduces 2 defectives artificially by the carbon Guan Shangyong atomic force microscope of growing (micron number magnitude) at one and has obtained " coulomb island " that be made of one section isolated carbon nano-tube line segment (25 nanometers are long) between calendar year 2001, realized the room temperatureization (H.W.Postma of single-electron device working temperature, T.Teepen, Z.Yao, M.Grifoni and C.Dekker, Nature, 293,76 (2001) .).But this kind method can't be used for large-scale production.
Summary of the invention
The present invention proposes the thought of utilizing the one-dimensional composite nano material preparation single-electron device that modulated structure is arranged.Thereby introduce the electrical properties that potential barrier changes nanotube by control ground in the preparation process of nanotube, realize the nano-scale coulomb island that single-electron device is required with this; By regulating the spacing of potential barrier, control is the working temperature of the single-electron device of preparation thus.
The invention provides a kind of simple and feasible method for preparing single-electron device.Not only can make the working temperature of device bring up to room temperature or higher, and this method go for the production of practicability.
Technical scheme of the present invention is: the method for preparing single-electron device, may further comprise the steps: 1) prepare carbon nano-tube with chemical gaseous phase depositing process, in its growth course, fill excessive metal or nonmetal introducing potential barrier, obtain the compound one dimension carbon nano-tube of modulated structure; 2) prepare electrode with the microelectronics photoetching technique; 3) carbon nano-tube of modulated structure is arranged and electrode is assembled and nanoprocessing with above-mentioned, obtain single-electron device.
Utilize chemical gaseous phase depositing process (being called for short the CVD method) preparation carbon nano-tube, in the CNT (carbon nano-tube) growth course, introduce elementide to CNT (carbon nano-tube) inside.These elementides and carbon pipe interact and form the local potential barrier.Carbon pipe between per two local barrier potentials all can be considered isolated coulomb island.Make single-electron device with traditional microelectronics processes in conjunction with nanoprocessing means such as focused ion beam or electron beam exposures.By the spacing of cluster in the regulating and controlling carbon nano-tube of growth course being controlled the size on coulomb island, thus the working temperature of control device.The working temperature of device can be enhanced room temperature.
Introduce the metal of filling when the potential barrier preparation has the compound one dimension carbon nano-tube of modulated structure and can be Fe, Co, Ni or Ag, the nonmetal of filling can be N or P.
The usefulness that the present invention proposes has simple and easy to do to the CNT (carbon nano-tube) method for processing with atomic-force microscope needle-tip than forefathers of method that the one-dimensional composite nano material construction coulomb island of modulated structure realizes the room temperature single-electron device, a large amount of devices can be prepared simultaneously, a large amount of productions can be used for.By the size of controlling potential barrier spacing control coulomb island and the working temperature of controlling single-electron device, controllability height.
Description of drawings:
The low power pattern picture of the composite Nano carbon pipe that modulation is arranged of Fig. 1 the inventive method preparation.
The high power picture of the composite Nano carbon pipe that modulation is arranged of Fig. 2 the inventive method preparation.
The vertical stratification schematic diagram of the electrode of the single-electron device of Fig. 3 the inventive method preparation.
The nano-electrode of the single-electron device of Fig. 4 the inventive method preparation and the microphoto of carbon pipe.
The voltage-current characteristic of the single-electron device of Fig. 5 the inventive method preparation.
Fig. 5 (a) is the measurement result under the 4.8K.
Fig. 5 (b) is the measurement result under the room temperature.
Embodiment:
Embodiment 1: prepare carbon nano-tube with the CVD method, regularly provide excessive iron to form the local potential barrier in its growth course, prepare electrode with microelectric technique, in conjunction with nanoprocessing means such as focused ion beam or electron beam exposures, finally constitute single-electron device.Concrete steps are as follows:
(1) prepares carbon nano-tube with the CVD method, in its growth course, regularly provide excessive iron, obtained filling the carbon nano-tube of Fe particle.Detailed process is:
A.20mm 2Silicon chip (surface is a silicon dioxide) ultrasonic cleaning 30 minutes in absolute ethyl alcohol is dried, is cleaned.
B. in the CVD stove, place the empty quartz boat of 6 centimetres of length,, load above-mentioned silicon chip in the boat placing second quartz boat with its 875 ℃ of humidity provinces at a distance of 18 centimeters at 300 ℃ of temperature sections.
C. 0.08 gram phthalein cyanogen iron or ferrocene is dissolved in the aromatics organic solvent about 300 milliliters, as dimethylbenzene.
D. according to 15 ℃/min speed intensification CVD stove, the body of ventilating simultaneously, consumption are argon gas 80sccm, hydrogen 65sccm; After arriving 900 ℃, control time and the injection of metering ground are dissolved with the solution of phthalein cyanogen iron or ferrocene and go into stove, must drop in first quartz boat, observe and can inject after last reactant thoroughly consumes next time.
E. after reaction finishes, continue logical argon gas up to cooling.
Shown in accompanying drawing, Fig. 1 is the low power pattern picture by the composite Nano carbon pipe that modulation is arranged of CVD method preparation, Fig. 2 is the high power picture that the composite Nano carbon pipe of modulation is arranged, and scale is 50 nanometers among the figure, the iron particle of filling in the high-visible CNT (carbon nano-tube) from Fig. 2 (showing dark part among the figure).
(2) utilize the microelectronics photoetching technique to go up preparation spacing 100 nanometers to 1 micron, the electrode of live width 100 to 300 nanometers at the silica of 200 nanometer thickness (below be silicon base).Electrode is made by silicon-aluminum.Nano-electrode also utilizes the microelectronics photoetching technique to carry out with the wiring point of millimeter or submillimeter yardstick simultaneously.
(3) carbon nano-tube ultrasonic dispersion back in dichloroethanes is dripped to spill be assembled on the electrode, drip the number of carbon pipe on the solution concentration of spilling and the solution amount control electrode by control.With ESEM or atomic force microscope inspection assembling situation, if directly Zu Zhuan structure is not ideal enough, nanoprocessing means such as available focused ion beam work station or electron beam exposure apparatus are processing and transformation further.Concrete processing, to transform can be that unnecessary nanotube or electrode are cut off, and the nanotube that will not ride on the electrode is connected with electrode with the method for the metal wire of plating nano-scale, will contact imperfect place and add plating and make and contact well.Final formation single-electron device.
(4) use low temperature platform and semi-conductor test instrument to measure the characteristic and the working temperature of single-electron device.
Measurement shows that the platform of tangible single electron effect appears in device current-voltage curve under 4.8K of the inventive method preparation.With the rising of temperature, step narrows down, and still exists up to the 273K step.The working temperature that shows this single-electron device can be up to 273K, i.e. room temperature.
The vertical stratification of the single-electron device electrode of explanation the inventive method preparation shown in Figure 3.Substrate is a silicon, cover the silica of 100-200 nanometer thickness above as insulating barrier, metal electrode above the silica is to be made of silicon-aluminum, and electrode is connected by titanium nitride with the interface of silicon-aluminum, and the live width of electrode and spacing are to make according to designing requirement with the microelectronics photoetching method.Because the size on coulomb island is that the size and the spacing of electrode do not play a crucial role to device performance by the spacing decision of the iron particle of filling, electrode can be live width 100 to 300 nanometers, and spacing 100 nanometers to 1 micron so just can adopt the microelectric technique of maturation.Nanotube will be assembled on the electrode.
Fig. 4 is the nanoelectronic utmost point of the single-electron device of the inventive method preparation and the microphoto of CNT (carbon nano-tube).From left to right bright line is a CNT (carbon nano-tube) among the figure, and five bands up and down are nano-electrode, and white bright part is to utilize the platinum of focused ion beam process technology plating on the electrode, and in order to reduce the contact resistance of carbon pipe and electrode, other parts are insulating layer of silicon oxide.The impressed current source is connected with right 1 electrode with a left side 2 and constitutes the loop with CNT (carbon nano-tube) and make electric current pass through CNT (carbon nano-tube) during measurement, and the left side 3 of centre links to each other with pressure measuring instrument with right 2 electrodes.
The characteristic and the working temperature of the single-electron device of the inventive method preparation are shown in Figure 5 through measurement result, and Fig. 5 (a) is a current-voltage curve under 4.8K, shows the platform of tangible single electron effect.Along with the rising of temperature, step narrows down, and still has (shown in Fig. 5 (b)) up to 273K (under the room temperature) step.This working temperature that shows the single-electron device of the inventive method preparation can be up to 273K, i.e. room temperature, in addition higher than room temperature.
In the single-electron device of the inventive method preparation, the carbon length of tube between middle two electrodes is the hundreds of nanometer, if the device that is made of pure carbon nano-tube generally should not observed single electron effect under the room temperature in this length.The present invention adopts the one-dimensional composite nano material that modulated structure is arranged, and is the CNT (carbon nano-tube) of having filled the iron particle in the present embodiment, has realized room temperature single electron effect.Iron particle and CNT (carbon nano-tube) interact and form the local potential barrier in the present embodiment, and the intergranular CNT (carbon nano-tube) of iron has just constituted a coulomb island.Pass through transmission electron microscope observing.The iron grain spacing of filling in the middle of the CNT (carbon nano-tube) in the present embodiment (coulomb island) can be as small as below 50 nanometers.Just so little coulomb island has caused the appearance of room temperature single electron effect.Simultaneously, because the size on coulomb island is the spacing decision by the iron particle of filling, the size and the spacing of electrode do not play a crucial role to device performance, electrode can be live width 100 to 300 nanometers, spacing 100 nanometers to 1 micron, so just can adopt ripe microelectric technique processing and manufacturing, make the manufacturing of single-electron device real more feasible.
Embodiment 2: adopt the method identical with embodiment 1 to prepare carbon nano-tube, also can fill metal or nonmetal realization modulated structures such as nitrogen, phosphorus such as cobalt, nickel in its growth course, formation local potential barrier; Preparation electrode and carbon nano-tube the process on the electrode of being assembled in can be adopted the method identical with embodiment 1 finally constitutes single-electron device.
Embodiment 3: adopt the periodic variation composition, the transformation of metal and insulator or the electronics of location, ion injection method are introduced the potential barrier preparation the one-dimensional composite nano material of transferring structure.
(1) CVD or arc discharge method prepare pure nano carbon pipe routinely;
(2) make the sieve pattern plate of spacing 20-50 nanometer, live width 10-30 nanometer of electron beam exposure method;
(3) CNT (carbon nano-tube) is tiled on the planar substrates, adds above-mentioned template above;
(4) said structure being exposed to electronics, the ion that can position under high-power electron beam or the ion beam injects.As be exposed under the suitable chemical atmosphere and can realize the periodicity transformation of nanotube composition or the transformation of metal and insulator.
With make electrode with the 1 identical method of implementing and will modulate after carbon nano-tube be assembled on the electrode, finally constitute single-electron device.

Claims (10)

1. a method for preparing single-electron device may further comprise the steps: 1) prepare carbon nano-tube with chemical gaseous phase depositing process, fill excessive metal or nonmetal introducing potential barrier in its growth course, obtain the compound one dimension carbon nano-tube of modulated structure; 2) prepare electrode with the microelectronics photoetching technique; 3) carbon nano-tube of modulated structure is arranged and electrode is assembled and nanoprocessing with above-mentioned, obtain single-electron device.
2. the method for preparing single-electron device according to claim 1 is characterized in that determining the size on the coulomb island of single-electron device working temperature to be determined by the potential barrier spacing.
3. the method for preparing single-electron device according to claim 1 is characterized in that, described have the compound one dimension carbon nano-tube of modulated structure to be assembled on the described electrode after the ultrasonic dispersion in dichloroethanes; The means of described nanoprocessing are focused ion beam work station or electron beam exposure apparatus.
4. the method for preparing single-electron device according to claim 3, it is characterized in that described compound one dimension carbon nano-tube is in dichloroethanes after the ultrasonic dispersion, be assembled on the described electrode by dripping to spill, by the number of carbon pipe on a control solution concentration of spilling and the solution amount control electrode.
5. according to claim 1 or 2 or the 3 or 4 described methods that prepare single-electron device, it is characterized in that the metal of filling when described introducing potential barrier preparation has the compound one dimension carbon nano-tube of modulated structure is Fe, Co, Ni or Ag.
6. the method for preparing single-electron device according to claim 5 is characterized in that it is to be dissolved in gram phthalein cyanogen iron of 0.08 in 300 milliliters of aromatics organic solvents or ferrocene that the preparation of described introducing potential barrier has what use in the compound one dimension carbon nano-tube of modulated structure.
7. the method for preparing single-electron device according to claim 6 is characterized in that described aromatics organic solvent is a dimethylbenzene.
8. according to claim 1 or 2 or the 3 or 4 described methods that prepare single-electron device, what it is characterized in that filling when described introducing potential barrier preparation has the compound one dimension carbon nano-tube of modulated structure nonmetally is N or P.
9. according to claim 1 or 2 or the 3 or 4 described methods that prepare single-electron device, it is characterized in that described electrode, electrode spacing 100 nanometers to 1 micron, live width 100 to 300 nanometers with the preparation of microelectronics photoetching technique.
10. the described application of method in nano-electron research and nanometer electronic device preparation for preparing single-electron device of claim 1.
CNB021579725A 2002-12-20 2002-12-20 Method for producing one-electron device by modulated composite one-dimensional nanometer material Expired - Fee Related CN100388410C (en)

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US6054349A (en) * 1997-06-12 2000-04-25 Fujitsu Limited Single-electron device including therein nanocrystals
CN1278021A (en) * 1999-06-18 2000-12-27 李铁真 Low temp. chemical vapor-phase deposition equipment and method for synthesizing nanometer carbon tube using same

Patent Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US6054349A (en) * 1997-06-12 2000-04-25 Fujitsu Limited Single-electron device including therein nanocrystals
CN1278021A (en) * 1999-06-18 2000-12-27 李铁真 Low temp. chemical vapor-phase deposition equipment and method for synthesizing nanometer carbon tube using same

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