CN101671020A - Silicon nanowire-based fluorescence chemical logic switch and preparation method thereof - Google Patents
Silicon nanowire-based fluorescence chemical logic switch and preparation method thereof Download PDFInfo
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- CN101671020A CN101671020A CN200810239879A CN200810239879A CN101671020A CN 101671020 A CN101671020 A CN 101671020A CN 200810239879 A CN200810239879 A CN 200810239879A CN 200810239879 A CN200810239879 A CN 200810239879A CN 101671020 A CN101671020 A CN 101671020A
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Abstract
The invention belongs to the field of fluorescence chemical logic switches in a one-dimensional nanostructure, in particular relates to a silicon nanowire-based fluorescence chemical logic switch anda preparation method thereof. The method comprises the following steps: carrying out surface treatment on a silicon nanowire prepared by a vapor deposition method, wherein the surface treatment comprises surface plasma treatment, laser radiation, ion surface bombardment or surface activation by chemical methods; and then, modifying the surface of the dry silicon nanowire after the surface treatment so that dansylamide with a logic switch function is arranged on the surface by covalent modification to obtain the silicon nanowire-based fluorescence chemical logic switch. The silicon nanowire-based fluorescence chemical logic switch can be used for preparing photochemical logic devices with smaller volumes and higher integration degrees.
Description
Technical field
The invention belongs to the fluorescence chemical logic switch field of one dimension Nano structure, particularly based on the preparation method of the fluorescence chemical logic switch of silicon nanowires, and the fluorescence chemical logic switch based on silicon nanowires that obtains by this method.
Background technology
Because organic molecule can carry out multifarious design and controlledly synthesis, in recent years, the light shutter device of forming with organic molecule is as potential important component part in the following digital processing system, and correlative study has caused people's great interest.Can pass through the input of light, electricity, magnetic, chemical signal, the output of the light of change organic molecule, electricity, magnetic signal so just can realize binary conversion, thereby be implemented in the logical operation on the molecular scale by the coding of input, output signal.In various input and output signals,, be a kind of ideal output signal because fluorescent signal is simple to operate, highly sensitive, the time of response is short, can carry out radio operation at single molecules level.AND, OR, INH, XOR, XNOR, NOR, various logical operations such as Half-adder, Half-subtractor based on organic molecule all have been widely studied, but the practical application of molecule logical operation reaches single molecules level far away.Therefore, but research practical application small-sized logical operation device be necessary.The different functionalities organic molecule is assembled on the enough little carrier, just might realizes the target of molecule logical operation.The research that polymer nano granules is used to photoswitch once had one piece of relevant report (Nature Materials, 2006, A.P.deSilva), but the close-packed mode of nano particle often makes the real contact area of itself and surrounding environment be far smaller than theory expectation, particularly under liquid environment, because the effect of surface tension of liquid, liquid is difficult to be deep into internal particle, makes problem particularly serious, thereby has reduced its actual responsiveness; Therefore, brought inconvenience to practical application.Silicon nanowires is because preparation is simple, finishing easily, conveniently make nano-array, by the nano material in the array being carried out the modification of difference in functionality switch respectively, help realizing nano-array multiple logical operation, can combining nano the simplicity of linear array preparation and organic synthesis diversity, can be compatible mutually with the conventional semiconductor technology, all these characteristics may make silicon nanowires become suitable molecular switch carrier.
Summary of the invention
The objective of the invention is to make full use of the small size of silicon nanowires and the accessibility of silicon nanowire array preparation, the dansyl amide that will have logic switch function is modified the surface of silicon nanowires, thereby a kind of preparation method of the fluorescence chemical logic switch based on silicon nanowires is provided.
A further object of the present invention provides the fluorescence chemical logic switch based on silicon nanowires that is prepared by purpose one method, the problem of utilizing the organic molecule logical switch to be faced with solution.
Method of the present invention is to carry out surface treatment by the silicon nanowires that the vapour deposition process preparation obtains, and its surface treatment is surface plasma processing, laser radiation, ion surface bombards or carry out surface active with chemical process; Then the surface of surface-treated exsiccant silicon nanowires is being modified, the dansyl amide of logic switch function is being arranged, obtaining fluorescence chemical logic switch based on silicon nanowires at its surperficial covalent modification.
The preparation method of the fluorescence chemical logic switch based on silicon nanowires of the present invention may further comprise the steps:
1) surface treatment of silicon nanowires:
Is to handle 1-3 hour in 90-150 ℃ the oxygen plasma silicon nanowires in temperature; Or be that the continuous laser of 325 nanometers was to silicon nanowires irradiation 0.5-2 hour with wavelength; Or with calcium ion source bombardment silicon nanowires 0.5-2 hour; Or carrying out surface active with chemical process, it is 98% the vitriol oil (H that silicon nanowires is put into mass concentration
2SO
4) and mass concentration be 30% hydrogen peroxide (H
2O
2) mixed solution in (H
2SO
4: H
2O
2Volume ratio be 7: 3), be to boil under 60-90 ℃ 10-60 minute in temperature, be chilled to room temperature, be washed to neutrality with second distillation repeatedly, put into H then
2O: H
2O
2: NH
3.H
2The volume ratio of O is 3-5: 0.2-1: in 1 the mixed solution 1-3 hour, take out, and be washed to neutrality with second distillation repeatedly, vacuum-drying;
2) finishing of silicon nanowires:
In being connected with the container of water trap (as round-bottomed flask), add surface-treated exsiccant silicon nanowires and the 40mL dry toluene that the 20mg step 1) obtains, rare gas element (as nitrogen etc.) protection down, be heated to 140 ℃ of component distillations and remove moisture, after steaming 30mL toluene, be cooled to 60-90 ℃ and add the N-3-triethoxysilylpropyl dansyl amide of 0.6mmol-1.8mmol, being 60-90 ℃ in temperature stirred 12-48 hour down, reduce to room temperature, filter the thick product of silicon nanowires that obtains finishing with microfilter; Thick product carries out ultrasonic cleaning repeatedly in organic solvent, filter, and removes unreacted N-3-triethoxysilylpropyl dansyl amide, and vacuum-drying obtains the fluorescence chemical logic switch based on silicon nanowires.
Described silicon nanowires can obtain with the vapour deposition process preparation.As 3 gram SiO are positioned in the middle of the aluminum oxide boiler tube of horizontal pipe furnace, the aluminum oxide boiler tube is evacuated to 10
-2Handkerchief feeds the mixed gas of argon gas and hydrogen then in the aluminum oxide boiler tube, wherein hydrogen content account for the mixed gas volume 1%～10% between; With the stable gas pressure of aluminum oxide boiler tube at 10000 handkerchiefs between 50000 handkerchiefs, the tube furnace temperature is elevated to 1290 ℃-1350 ℃, and kept this temperature 3-8 hour, then, tube furnace is lowered the temperature naturally, finally the cold zone at tube furnace obtains silicon nanowires.
Described silicon nanowires diameter is at 15～25nm, and length is at 1um～10um.
Described thick product carries out ultrasonic cleaning in organic solvent be successively at toluene, and methylene dichloride carries out ultrasonic cleaning in the ethanol.
Step 2) dry toluene that preferably newly steams of described dry toluene.
When the fluorescence chemical logic switch based on silicon nanowires that the inventive method is obtained carries out fluoroscopic examination, be the fluorescence chemical logic switch based on silicon nanowires to be scattered in form suspension in the deionized water, carry out the test of switching function with fluorescence spectrophotometer.The excitation wavelength 330nm of used laser, wavelength of transmitted light 535nm.Fluorescence spectrophotometer detects the change in fluorescence based on the fluorescence chemical logic switch surface N-3-triethoxysilylpropyl dansyl amide of silicon nanowires, is fluorescence enhancing or the cancellation that detects based on the fluorescence chemical logic switch surface N-3-triethoxysilylpropyl dansyl amide of silicon nanowires.
The one dimension Nano structure of described fluorescence chemical logic switch based on silicon nanowires this to carry out in being scattered in deionized water in the fluoroscopic examination be chaotic distribution, or oldered array distributes.
Beneficial effect of the present invention:
The present invention is by carrying out finishing to silicon nanowires, realized fluorescence chemical logic switch based on silicon nanowires, and, the volume of silicon nanowires is little, make array easily, and these provide a kind of new thinking and method for the higher photochemistry logical device of preparation littler, the integrated degree of volume.
The present invention is further illustrated below in conjunction with specific embodiment and accompanying drawing.
Description of drawings
Fig. 1. the finishing of silicon nanowires and switching process synoptic diagram among the present invention.
Fig. 2. among the embodiment of the invention 1-9 based on the fluorescence chemical logic switch of the silicon nanowires fluorescence spectrum figure under the 1-8 condition below input; Wherein, 1-8 is followed successively by dansyl amide modification silicon nanowires+chlorion, dansyl amide modification silicon nanowires, dansyl amide modification silicon nanowires+mercury ion+chlorion, dansyl amide modification silicon nanowires+mercury ion, dansyl amide modification silicon nanowires+hydrogen ion, dansyl amide modification silicon nanowires+chlorion+hydrogen ion, dansyl amide modification silicon nanowires+mercury ion+chlorion+hydrogen ion, dansyl amide modification silicon nanowires+mercury ion+hydrogen ion.
Fig. 3. dansyl amide modifies that silicon nanowires obtains among the embodiment of the invention 1-9 based on the response to various positively charged ions (A) and negatively charged ion (B) of the fluorescence chemical logic switch of silicon nanowires; Wherein, the response of when 2mM different metal ion (A) and different anions (B) are represented in the response that on behalf of 2mM different metal ion (A) and different anions (B), the black histogram dansyl amide is modified silicon nanowires fluorescence, white histogram with the coexistence of 0.2mM mercury ion dansyl amide being modified silicon nanowires fluorescence.
Fig. 4. dansyl amide is modified the fluorescence chemical logic switch synoptic diagram based on silicon nanowires that silicon nanowires obtains among the present invention.
Embodiment
3 gram SiO are positioned in the middle of the aluminum oxide boiler tube of horizontal pipe furnace, then the aluminum oxide boiler tube are evacuated to 10
-2Handkerchief feeds the mixed gas of argon gas and hydrogen then in the aluminum oxide boiler tube, wherein hydrogen content account for the mixed gas volume 5% between.With the stable gas pressure of aluminum oxide boiler tube at 10000 handkerchiefs.Then the tube furnace temperature is elevated to 1290 ℃, and keeps temperature after 6 hours, tube furnace is lowered the temperature naturally.Finally the cold zone at tube furnace obtains silicon nanowires, and the silicon nanowires diameter is at 15-25nm, and length is at 1um～10um.
The silicon nanowires that obtains in being 150 ℃ oxygen plasma, temperature was handled 3 hours.In being connected with the 100mL round-bottomed flask of water trap, add silicon nanowires and the new dry toluene that steams of 40mL that the 20mg oxygen plasma treatment is crossed; under the nitrogen protection; be heated to 140 ℃ of component distillations and remove moisture; after steaming 30mL toluene; reduce to 90 ℃ and add the N-3-triethoxysilylpropyl dansyl amide of 0.60mmol; 90 ℃ were stirred 48 hours, reduced to room temperature, filtered with microfilter and obtained the thick product of finishing silicon nanowires.Thick product is repeatedly successively at toluene, and methylene dichloride carries out ultrasonic cleaning in the ethanol, filters, and removes unreacted N-3-triethoxysilylpropyl dansyl amide, and vacuum-drying obtains the fluorescence chemical logic switch based on silicon nanowires.
The fluorescence chemical logic switch based on silicon nanowires that obtains is scattered in respectively forms suspension in the deionized water, based on the one dimension Nano structure of the fluorescence chemical logic switch of silicon nanowires this to carry out in being scattered in deionized water in the fluoroscopic examination be chaotic distribution, or oldered array distributes.Dropping contains ion solution in suspension respectively, by measuring the influence of the fluorescence intensity of N-3-triethoxysilylpropyl dansyl amide on the various ion pair silicon nanowires, finds pH, Hg (II) and Cl
-Or Br
-The fluorescence of the silicon nanowires that N-3-triethoxysilylpropyl dansyl amide is modified has special response (Fig. 2 and Fig. 3).Respectively with pH, Hg (II) and Cl
-Or Br
-As three inputs, to the experiment condition defined threshold, be 1 when existing, be 0 when not existing; The fluorescence of the silicon nanowires that N-3-triethoxysilylpropyl-dansyl amide is modified is 1 as output when fluorescence intensity is higher than threshold value, is 0 when being lower than threshold value, obtains spectrum and truth table (table 1, Fig. 2) under the different experimental conditions; Simultaneously, this logical switch has good freedom from jamming to other metal ion.And, can make logical switch return to original state by the acidity that adds disodium EDTA and regulator solution.
In the middle of this embodiment, also can select for use, Ge nanoline, zinc oxide (ZnO) nano wire, ZnS nano wire, germanium oxide (GeO
2) replacements such as nano wire, Cadmium oxide nano wire, other condition is constant, and same final nano wire can be used as the logical switches of three inputs.In this embodiment, silicon nanowires can adopt the preparation of chemo-selective lithographic method.
3 gram SiO are positioned in the middle of the aluminum oxide boiler tube of horizontal pipe furnace, then the aluminum oxide boiler tube are evacuated to 10
-2Handkerchief feeds the mixed gas of argon gas and hydrogen then in the aluminum oxide boiler tube, wherein hydrogen content account for the mixed gas volume 8% between.With the stable gas pressure of aluminum oxide boiler tube at 40000 handkerchiefs.Then the tube furnace temperature is elevated to 1320 ℃, and kept temperature 8 hours, tube furnace is lowered the temperature naturally then.Finally the cold zone at tube furnace obtains silicon nanowires, and the silicon nanowires diameter is at 15-25nm, and length is at 1um～10um.
The silicon nanowires that obtains was shone 0.5 hour with wavelength 325 nanometer continuous lasers.In being connected with the 100mL round-bottomed flask of water trap, add silicon nanowires and the 40mL dry toluene that the 20mg oxygen plasma treatment is crossed; under the nitrogen protection; be heated to 140 ℃ of component distillations and remove moisture; after steaming 30mL toluene; reduce to 70 ℃ and add the N-3-triethoxysilylpropyl dansyl amide of 1.20mmol; 70 ℃ were stirred 24 hours, reduced to room temperature, filtered with microfilter and obtained the thick product of finishing silicon nanowires.Thick product is successively at toluene, and methylene dichloride carries out ultrasonic cleaning in the ethanol, filters, and removes unreacted N-3-triethoxysilylpropyl dansyl amide, and vacuum-drying obtains the fluorescence chemical logic switch based on silicon nanowires.
The fluorescence chemical logic switch based on silicon nanowires that obtains is scattered in respectively forms suspension in the deionized water, based on the one dimension Nano structure of the fluorescence chemical logic switch of silicon nanowires this to carry out in being scattered in deionized water in the fluoroscopic examination be chaotic distribution, or oldered array distributes.Dropping contains ion solution in suspension respectively, by measuring the influence of the fluorescence intensity of N-3-triethoxysilylpropyl dansyl amide on the various ion pair silicon nanowires, finds pH, Hg (II) and Cl
-Or Br
-The fluorescence of the silicon nanowires that N-3-triethoxysilylpropyl dansyl amide is modified has special response (Fig. 2 and Fig. 3).Respectively with pH, Hg (II) and Cl
-Or Br
-As three inputs, to the experiment condition defined threshold, be 1 when existing, be 0 when not existing; The fluorescence of the silicon nanowires that N-3-triethoxysilylpropyl-dansyl amide is modified is 1 as output when fluorescence intensity is higher than threshold value, is 0 when being lower than threshold value, obtains spectrum and truth table (table 1, Fig. 2) under the different experimental conditions; Simultaneously, this logical switch has good freedom from jamming to other metal ion.And, can make logical switch return to original state by the acidity that adds disodium EDTA and regulator solution.
In the middle of this embodiment, also can select for use, Ge nanoline, zinc oxide (ZnO) nano wire, ZnS nano wire, germanium oxide (GeO
2) replacements such as nano wire, Cadmium oxide nano wire, other condition is constant, and same final nano wire can be used as the logical switches of three inputs.In this embodiment, silicon nanowires can adopt the preparation of chemo-selective lithographic method.
3 gram SiO are positioned in the middle of the aluminum oxide boiler tube of horizontal pipe furnace, then the aluminum oxide boiler tube are evacuated to 10
-2Handkerchief feeds the mixed gas of argon gas and hydrogen then in the aluminum oxide boiler tube, wherein hydrogen content account for the mixed gas volume 8% between.With the stable gas pressure of aluminum oxide boiler tube at 40000 handkerchiefs.Then the tube furnace temperature is elevated to 1320 ℃, and kept temperature 8 hours, tube furnace is lowered the temperature naturally then.Finally the cold zone at tube furnace obtains silicon nanowires, and the silicon nanowires diameter is at 15-25nm, and length is at 1um～10um.
The silicon nanowires that obtains is used wavelength 325 nanometer continuous laser radiation treatment 2 hours.In being connected with the 100mL round-bottomed flask of water trap, add silicon nanowires and the new dry toluene that steams of 40mL that the 20mg oxygen plasma treatment is crossed; under the nitrogen protection; be heated to 140 ℃ of component distillations and remove moisture; after steaming 30mL toluene; reduce to 60 ℃ and add the N-3-triethoxysilylpropyl dansyl amide of 1.80mmol; 60 ℃ were stirred 12 hours, reduced to room temperature, filtered with microfilter and obtained the thick product of finishing silicon nanowires.Thick product is repeatedly successively at toluene, and methylene dichloride carries out ultrasonic cleaning in the ethanol, filters, and removes unreacted N-3-triethoxysilylpropyl dansyl amide, and vacuum-drying obtains the fluorescence chemical logic switch based on silicon nanowires.
The fluorescence chemical logic switch based on silicon nanowires that obtains is scattered in respectively forms suspension in the deionized water, based on the one dimension Nano structure of the fluorescence chemical logic switch of silicon nanowires this to carry out in being scattered in deionized water in the fluoroscopic examination be chaotic distribution, or oldered array distributes.Dropping contains ion solution in suspension respectively, by measuring the influence of the fluorescence intensity of N-3-triethoxysilylpropyl dansyl amide on the various ion pair silicon nanowires, finds pH, Hg (II) and Cl
-Or Br
-The fluorescence of the silicon nanowires that N-3-triethoxysilylpropyl dansyl amide is modified has special response (Fig. 2 and Fig. 3).Respectively with pH, Hg (II) and Cl
-Or Br
-As three inputs, to the experiment condition defined threshold, be 1 when existing, be 0 when not existing; The fluorescence of the silicon nanowires that N-3-triethoxysilylpropyl-dansyl amide is modified is 1 as output when fluorescence intensity is higher than threshold value, is 0 when being lower than threshold value, obtains spectrum and truth table (table 1, Fig. 2) under the different experimental conditions; Simultaneously, this logical switch has good freedom from jamming to other metal ion.And, can make logical switch return to original state by the acidity that adds disodium EDTA and regulator solution.
In the middle of this embodiment, also can select for use, Ge nanoline, zinc oxide (ZnO) nano wire, ZnS nano wire, germanium oxide (GeO
2) replacements such as nano wire, Cadmium oxide nano wire, other condition is constant, and same final nano wire can be used as the logical switches of three inputs.In this embodiment, silicon nanowires can adopt the preparation of chemo-selective lithographic method.
Embodiment 4
3 gram SiO are positioned in the middle of the aluminum oxide boiler tube of horizontal pipe furnace, then the aluminum oxide boiler tube are evacuated to 10
-2Handkerchief feeds the mixed gas of argon gas and hydrogen then in the aluminum oxide boiler tube, wherein hydrogen content account for the mixed gas volume 1% between.With the stable gas pressure of aluminum oxide boiler tube at 50000 handkerchiefs.Then the tube furnace temperature is elevated to 1350 ℃, and kept temperature 3 hours, tube furnace is lowered the temperature naturally then.Finally the cold zone at tube furnace obtains silicon nanowires, and the silicon nanowires diameter is at 15-25nm, and length is at 1um～10um.
Silicon nanowires was handled 2 hours with the calcium ion source bombardment.The silicon nanowires and the 40mL dry toluene that in being connected with the 100mL round-bottomed flask of water trap, add the above-mentioned processing of 20mg; under the nitrogen protection; be heated to 140 ℃ of component distillations and remove moisture; after steaming 30mL toluene; reduce to 90 ℃ and add the N-3-triethoxysilylpropyl dansyl amide of 1.4mmol; 90 ℃ were stirred 36 hours, reduced to room temperature, filtered with microfilter and obtained the thick product of finishing silicon nanowires.Thick product is successively at toluene, and methylene dichloride carries out ultrasonic cleaning in the alcohol solvent, filters, and removes unreacted N-3-triethoxysilylpropyl dansyl amide, and vacuum-drying obtains the fluorescence chemical logic switch based on silicon nanowires.
The fluorescence chemical logic switch based on silicon nanowires that obtains is scattered in respectively forms suspension in the deionized water, based on the one dimension Nano structure of the fluorescence chemical logic switch of silicon nanowires this to carry out in being scattered in deionized water in the fluoroscopic examination be chaotic distribution, or oldered array distributes.Dropping contains ion solution in suspension respectively, by measuring the influence of the fluorescence intensity of N-3-triethoxysilylpropyl dansyl amide on the various ion pair silicon nanowires, finds pH, Hg (II) and Cl
-Or Br
-The fluorescence of the silicon nanowires that N-3-triethoxysilylpropyl dansyl amide is modified has special response (Fig. 2 and Fig. 3).Respectively with pH, Hg (II) and Cl
-Or Br
-As three inputs, to the experiment condition defined threshold, be 1 when existing, be 0 when not existing; The fluorescence of the silicon nanowires that N-3-triethoxysilylpropyl-dansyl amide is modified is 1 as output when fluorescence intensity is higher than threshold value, is 0 when being lower than threshold value, obtains spectrum and truth table (table 1, Fig. 2) under the different experimental conditions; Simultaneously, this logical switch has good freedom from jamming to other metal ion.And, can make logical switch return to original state by the acidity that adds disodium EDTA and regulator solution.
In the middle of this embodiment, also can select for use, Ge nanoline, zinc oxide (ZnO) nano wire, ZnS nano wire, germanium oxide (GeO
2) replacements such as nano wire, Cadmium oxide nano wire, other condition is constant, and same final nano wire can be used as the logical switches of three inputs.In this embodiment, silicon nanowires can adopt the preparation of chemo-selective lithographic method.
3 gram SiO are positioned in the middle of the aluminum oxide boiler tube of horizontal pipe furnace, then the aluminum oxide boiler tube are evacuated to 10
-2Handkerchief feeds the mixed gas of argon gas and hydrogen then in the aluminum oxide boiler tube, wherein hydrogen content account for the mixed gas volume 5% between.With the stable gas pressure of aluminum oxide boiler tube at 20000 handkerchiefs.Then the tube furnace temperature is elevated to 1300 ℃, and kept temperature 6 hours, tube furnace is lowered the temperature naturally then.Finally the cold zone at tube furnace obtains silicon nanowires, and the silicon nanowires diameter is at 15-25nm, and length is at 1um～10um.
It is 98% the vitriol oil (H that the silicon nanowires that obtains is put into mass concentration
2SO
4) and mass concentration be 30% hydrogen peroxide (H
2O
2) mixed solution in (dense H
2SO
4: H
2O
2Volume ratio be 7: 3), 90 ℃ were boiled 30 minutes, were chilled to room temperature, were washed to neutrality with second distillation repeatedly, put into the H of 5: 1: 1 (volume ratio)
2O: H
2O
2: NH
3.H
2Room temperature is 3 hours in the O mixed solution, is washed to neutrality with second distillation repeatedly, vacuum-drying.
The dring silicon nano wire and the 40mL dry toluene that in being connected with the 100mL round-bottomed flask of water trap, add the above-mentioned processing of 20mg; under the nitrogen protection; be heated to 140 ℃ of component distillations and remove moisture; after steaming 30mL toluene; reduce to 90 ℃ and add the N-3-triethoxysilylpropyl dansyl amide of 1.8mmol; 90 ℃ were stirred 48 hours, reduced to room temperature, filtered with microfilter and obtained the thick product of finishing silicon nanowires.Thick product is repeatedly successively at toluene, and methylene dichloride carries out ultrasonic cleaning in the ethanol, filters, and removes unreacted N-3-triethoxysilylpropyl dansyl amide, and vacuum-drying obtains the fluorescence chemical logic switch based on silicon nanowires.
The fluorescence chemical logic switch based on silicon nanowires that obtains is scattered in respectively forms suspension in the deionized water, based on the one dimension Nano structure of the fluorescence chemical logic switch of silicon nanowires this to carry out in being scattered in deionized water in the fluoroscopic examination be chaotic distribution, or oldered array distributes.Dropping contains ion solution in suspension respectively, by measuring the influence of the fluorescence intensity of N-3-triethoxysilylpropyl dansyl amide on the various ion pair silicon nanowires, finds pH, Hg (II) and Cl
-Or Br
-The fluorescence of the silicon nanowires that N-3-triethoxysilylpropyl dansyl amide is modified has special response (Fig. 2 and Fig. 3).Respectively with pH, Hg (II) and Cl
-Or Br
-As three inputs, to the experiment condition defined threshold, be 1 when existing, be 0 when not existing; The fluorescence of the silicon nanowires that N-3-triethoxysilylpropyl-dansyl amide is modified is 1 as output when fluorescence intensity is higher than threshold value, is 0 when being lower than threshold value, obtains spectrum and truth table (table 1, Fig. 2) under the different experimental conditions; Simultaneously, this logical switch has good freedom from jamming to other metal ion.And, can make logical switch return to original state by the acidity that adds disodium EDTA and regulator solution.
In the middle of this embodiment, also can select for use, Ge nanoline, zinc oxide (ZnO) nano wire, ZnS nano wire, germanium oxide (GeO
2) replacements such as nano wire, Cadmium oxide nano wire, other condition is constant, and same final nano wire can be used as the logical switches of three inputs.In this embodiment, silicon nanowires can adopt the preparation of chemo-selective lithographic method.
Embodiment 6
3 gram SiO are positioned in the middle of the aluminum oxide boiler tube of horizontal pipe furnace, then the aluminum oxide boiler tube are evacuated to 10
-2Handkerchief feeds the mixed gas of argon gas and hydrogen then in the aluminum oxide boiler tube, wherein hydrogen content account for the mixed gas volume 10% between.With the stable gas pressure of aluminum oxide boiler tube at 10000 handkerchiefs.Then the tube furnace temperature is elevated to 1300 ℃, and kept temperature 8 hours, tube furnace is lowered the temperature naturally then.Finally the cold zone at tube furnace obtains silicon nanowires, and the silicon nanowires diameter is at 15-25nm, and length is at 1um～10um.
It is 98% the vitriol oil (H that the silicon nanowires that obtains is put into mass concentration
2SO
4) and mass concentration be 30% hydrogen peroxide (H
2O
2) mixed solution in (dense H
2SO
4: H
2O
2Mol ratio be 7: 3), 90 ℃ were boiled 45 minutes, were chilled to room temperature, were washed to neutrality with second distillation repeatedly, put into the H of 3: 1: 1 (volume ratio)
2O: H
2O
2: NH
3.H
2Room temperature is 3 hours in the O mixed solution, is washed to neutrality with second distillation repeatedly, vacuum-drying.The dring silicon nano wire and the new dry toluene that steams of 40mL that in being connected with the 100mL round-bottomed flask of water trap, add the above-mentioned processing of 20mg; under the nitrogen protection; be heated to 140 ℃ of component distillations and remove moisture; after steaming 30mL toluene; reduce to 90 ℃ and add the N-3-triethoxysilylpropyl dansyl amide of 1.8mmol; 90 ℃ were stirred 48 hours, reduced to room temperature, filtered with microfilter and obtained the thick product of finishing silicon nanowires.Thick product is repeatedly successively at toluene, and methylene dichloride carries out ultrasonic cleaning in the ethanol, filters, and removes unreacted N-3-triethoxysilylpropyl dansyl amide, and vacuum-drying obtains the fluorescence chemical logic switch based on silicon nanowires.
The fluorescence chemical logic switch based on silicon nanowires that obtains is scattered in respectively forms suspension in the deionized water, based on the one dimension Nano structure of the fluorescence chemical logic switch of silicon nanowires this to carry out in being scattered in deionized water in the fluoroscopic examination be chaotic distribution, or oldered array distributes.Dropping contains ion solution in suspension respectively, by measuring the influence of the fluorescence intensity of N-3-triethoxysilylpropyl dansyl amide on the various ion pair silicon nanowires, finds pH, Hg (II) and Cl
-Or Br
-The fluorescence of the silicon nanowires that N-3-triethoxysilylpropyl dansyl amide is modified has special response (Fig. 2 and Fig. 3).Respectively with pH, Hg (II) and Cl
-Or Br
-As three inputs, to the experiment condition defined threshold, be 1 when existing, be 0 when not existing; The fluorescence of the silicon nanowires that N-3-triethoxysilylpropyl-dansyl amide is modified is 1 as output when fluorescence intensity is higher than threshold value, is 0 when being lower than threshold value, obtains spectrum and truth table (table 1, Fig. 2) under the different experimental conditions; Simultaneously, this logical switch has good freedom from jamming to other metal ion.And, can make logical switch return to original state by the acidity that adds disodium EDTA and regulator solution.
In the middle of this embodiment, also can select for use, Ge nanoline, zinc oxide (ZnO) nano wire, ZnS nano wire, germanium oxide (GeO
2) replacements such as nano wire, Cadmium oxide nano wire, other condition is constant, and same final nano wire can be used as the logical switches of three inputs.In this embodiment, silicon nanowires can adopt the preparation of chemo-selective lithographic method.
3 gram SiO are positioned in the middle of the aluminum oxide boiler tube of horizontal pipe furnace, then the aluminum oxide boiler tube are evacuated to 10
-2Handkerchief feeds the mixed gas of argon gas and hydrogen then in the aluminum oxide boiler tube, wherein hydrogen content account for the mixed gas volume 10% between.With the stable gas pressure of aluminum oxide boiler tube at 10000 handkerchiefs.Then the tube furnace temperature is elevated to 1300 ℃, and kept temperature 8 hours, tube furnace is lowered the temperature naturally then.Finally the cold zone at tube furnace obtains silicon nanowires, and the silicon nanowires diameter is at 15-25nm, and length is at 1um～10um.
It is 98% the vitriol oil (H that the silicon nanowires that obtains is put into mass concentration
2SO
4) and mass concentration be 30% hydrogen peroxide (H
2O
2) mixed solution in (dense H
2SO
4: H
2O
2Mol ratio be 7: 3), 90 ℃ were boiled 45 minutes, were chilled to room temperature, were washed to neutrality with second distillation repeatedly, put into the H of 3: 0.2: 1 (volume ratio)
2O: H
2O
2: NH
3.H
2Room temperature is 3 hours in the O mixed solution, is washed to neutrality with second distillation repeatedly, vacuum-drying.The dring silicon nano wire and the 40mL dry toluene that in being connected with the 100mL round-bottomed flask of water trap, add the above-mentioned processing of 20mg; under the nitrogen protection; be heated to 140 ℃ of component distillations and remove moisture; after steaming 30mL toluene; reduce to 90 ℃ and add the N-3-triethoxysilylpropyl dansyl amide of 1.8mmol; 90 ℃ were stirred 48 hours, reduced to room temperature, filtered with microfilter and obtained the thick product of finishing silicon nanowires.Thick product is repeatedly successively at toluene, and methylene dichloride carries out ultrasonic cleaning in the ethanol, filters, and removes unreacted N-3-triethoxysilylpropyl dansyl amide, and vacuum-drying obtains the fluorescence chemical logic switch based on silicon nanowires.
The fluorescence chemical logic switch based on silicon nanowires that obtains is scattered in respectively forms suspension in the deionized water, based on the one dimension Nano structure of the fluorescence chemical logic switch of silicon nanowires this to carry out in being scattered in deionized water in the fluoroscopic examination be chaotic distribution, or oldered array distributes.Dropping contains ion solution in suspension respectively, by measuring the influence of the fluorescence intensity of N-3-triethoxysilylpropyl dansyl amide on the various ion pair silicon nanowires, finds pH, Hg (II) and Cl
-Or Br
-The fluorescence of the silicon nanowires that N-3-triethoxysilylpropyl dansyl amide is modified has special response (Fig. 2 and Fig. 3).Respectively with pH, Hg (II) and Cl
-Or Br
-As three inputs, to the experiment condition defined threshold, be 1 when existing, be 0 when not existing; The fluorescence of the silicon nanowires that N-3-triethoxysilylpropyl-dansyl amide is modified is 1 as output when fluorescence intensity is higher than threshold value, is 0 when being lower than threshold value, obtains spectrum and truth table (table 1, Fig. 2) under the different experimental conditions; Simultaneously, this logical switch has good freedom from jamming to other metal ion.And, can make logical switch return to original state by the acidity that adds disodium EDTA and regulator solution.
In the middle of this embodiment, also can select for use, Ge nanoline, zinc oxide (ZnO) nano wire, ZnS nano wire, germanium oxide (GeO
2) replacements such as nano wire, Cadmium oxide nano wire, other condition is constant, and same final nano wire can be used as the logical switches of three inputs.In this embodiment, silicon nanowires can adopt the preparation of chemo-selective lithographic method.
3 gram SiO are positioned in the middle of the aluminum oxide boiler tube of horizontal pipe furnace, then the aluminum oxide boiler tube are evacuated to 10
-2Handkerchief feeds the mixed gas of argon gas and hydrogen then in the aluminum oxide boiler tube, wherein hydrogen content account for the mixed gas volume 10% between.With the stable gas pressure of aluminum oxide boiler tube at 10000 handkerchiefs.Then the tube furnace temperature is elevated to 1300 ℃, and kept temperature 8 hours, tube furnace is lowered the temperature naturally then.Finally the cold zone at tube furnace obtains silicon nanowires, and the silicon nanowires diameter is at 15-25nm, and length is at 1um～10um.
It is 98% the vitriol oil (H that the silicon nanowires that obtains is put into mass concentration
2SO
4) and mass concentration be 30% hydrogen peroxide (H
2O
2) mixed solution in (dense H
2SO
4: H
2O
2Mol ratio be 7: 3), 80 ℃ were boiled 60 minutes, were chilled to room temperature, were washed to neutrality with second distillation repeatedly, put into the H of 5: 0.2: 1 (volume ratio)
2O: H
2O
2: NH
3.H
2Room temperature is 1 hour in the O mixed solution, is washed to neutrality with second distillation repeatedly, vacuum-drying.The dring silicon nano wire and the 40mL dry toluene that in being connected with the 100mL round-bottomed flask of water trap, add the above-mentioned processing of 20mg; under the nitrogen protection; be heated to 140 ℃ of component distillations and remove moisture; after steaming 30mL toluene; reduce to 80 ℃ and add the N-3-triethoxysilylpropyl dansyl amide of 1.8mmol; 80 ℃ were stirred 36 hours, reduced to room temperature, filtered with microfilter and obtained the thick product of finishing silicon nanowires.Thick product is repeatedly successively at toluene, and methylene dichloride carries out ultrasonic cleaning in the ethanol, filters, and removes unreacted N-3-triethoxysilylpropyl dansyl amide, and vacuum-drying obtains the fluorescence chemical logic switch based on silicon nanowires.
The fluorescence chemical logic switch based on silicon nanowires that obtains is scattered in respectively forms suspension in the deionized water, based on the one dimension Nano structure of the fluorescence chemical logic switch of silicon nanowires this to carry out in being scattered in deionized water in the fluoroscopic examination be chaotic distribution, or oldered array distributes.Dropping contains ion solution in suspension respectively, by measuring the influence of the fluorescence intensity of N-3-triethoxysilylpropyl dansyl amide on the various ion pair silicon nanowires, finds pH, Hg (II) and Cl
-Or Br
-The fluorescence of the silicon nanowires that N-3-triethoxysilylpropyl dansyl amide is modified has special response (Fig. 2 and Fig. 3).Respectively with pH, Hg (II) and Cl
-Or Br
-As three inputs, to the experiment condition defined threshold, be 1 when existing, be 0 when not existing; The fluorescence of the silicon nanowires that N-3-triethoxysilylpropyl-dansyl amide is modified is 1 as output when fluorescence intensity is higher than threshold value, is 0 when being lower than threshold value, obtains spectrum and truth table (table 1, Fig. 2) under the different experimental conditions; Simultaneously, this logical switch has good freedom from jamming to other metal ion.And, can make logical switch return to original state by the acidity that adds disodium EDTA and regulator solution.
In the middle of this embodiment, also can select for use, Ge nanoline, zinc oxide (ZnO) nano wire, ZnS nano wire, germanium oxide (GeO
2) replacements such as nano wire, Cadmium oxide nano wire, other condition is constant, and same final nano wire can be used as the logical switches of three inputs.In this embodiment, silicon nanowires can adopt the preparation of chemo-selective lithographic method.
Embodiment 9
3 gram SiO are positioned in the middle of the aluminum oxide boiler tube of horizontal pipe furnace, then the aluminum oxide boiler tube are evacuated to 10
-2Handkerchief feeds the mixed gas of argon gas and hydrogen then in the aluminum oxide boiler tube, wherein hydrogen content account for the mixed gas volume 10% between.With the stable gas pressure of aluminum oxide boiler tube at 10000 handkerchiefs.Then the tube furnace temperature is elevated to 1300 ℃, and kept temperature 8 hours, tube furnace is lowered the temperature naturally then.Finally the cold zone at tube furnace obtains silicon nanowires, and the silicon nanowires diameter is at 15-25nm, and length is at 1um～10um.
It is 98% the vitriol oil (H that the silicon nanowires that obtains is put into mass concentration
2SO
4) and mass concentration be 30% hydrogen peroxide (H
2O
2) mixed solution in (dense H
2SO
4: H
2O
2Mol ratio be 7: 3), 60 ℃ were boiled 45 minutes, were chilled to room temperature, were washed to neutrality with second distillation repeatedly, put into the H of 5: 1: 1 (volume ratio)
2O: H
2O
2: NH
3.H
2Room temperature is 13 hours in the O mixed solution, is washed to neutrality with second distillation repeatedly, vacuum-drying.The dring silicon nano wire and the 40mL dry toluene that in being connected with the 100mL round-bottomed flask of water trap, add the above-mentioned processing of 20mg; under the nitrogen protection; be heated to 140 ℃ of component distillations and remove moisture; after steaming 30mL toluene; reduce to 90 ℃ and add the N-3-triethoxysilylpropyl dansyl amide of 1.2mmol; 90 ℃ were stirred 24 hours, reduced to room temperature, filtered with microfilter and obtained the thick product of finishing silicon nanowires.Thick product is repeatedly successively at toluene, and methylene dichloride carries out ultrasonic cleaning in the ethanol, filters, and removes unreacted N-3-triethoxysilylpropyl dansyl amide, and vacuum-drying obtains the fluorescence chemical logic switch based on silicon nanowires.
The fluorescence chemical logic switch based on silicon nanowires that obtains is scattered in respectively forms suspension in the deionized water, based on the one dimension Nano structure of the fluorescence chemical logic switch of silicon nanowires this to carry out in being scattered in deionized water in the fluoroscopic examination be chaotic distribution, or oldered array distributes.Dropping contains ion solution in suspension respectively, by measuring the influence of the fluorescence intensity of N-3-triethoxysilylpropyl dansyl amide on the various ion pair silicon nanowires, finds pH, Hg (II) and Cl
-Or Br
-The fluorescence of the silicon nanowires that N-3-triethoxysilylpropyl dansyl amide is modified has special response (Fig. 2 and Fig. 3).Respectively with pH, Hg (II) and Cl
-Or Br
-As three inputs, to the experiment condition defined threshold, be 1 when existing, be 0 when not existing; The fluorescence of the silicon nanowires that N-3-triethoxysilylpropyl-dansyl amide is modified is 1 as output when fluorescence intensity is higher than threshold value, is 0 when being lower than threshold value, obtains spectrum and truth table (table 1, Fig. 2) under the different experimental conditions; Simultaneously, this logical switch has good freedom from jamming to other metal ion.And, can make logical switch return to original state by the acidity that adds disodium EDTA and regulator solution.
In the middle of this embodiment, also can select for use, Ge nanoline, zinc oxide (ZnO) nano wire, ZnS nano wire, germanium oxide (GeO
2) replacements such as nano wire, Cadmium oxide nano wire, other condition is constant, and same final nano wire can be used as the logical switches of three inputs.In this embodiment, silicon nanowires can adopt the preparation of chemo-selective lithographic method.
Dansyl amide is modified three input truth tables of silicon nanowires logical switch in table 1. the foregoing description 1～9
Claims (7)
1. the preparation method based on the fluorescence chemical logic switch of silicon nanowires is characterized in that, this method may further comprise the steps:
1) surface treatment of silicon nanowires:
Is to handle 1-3 hour in 90-150 ℃ the oxygen plasma silicon nanowires in temperature; Or be that the continuous laser of 325 nanometers was to silicon nanowires irradiation 0.5-2 hour with wavelength; Or with calcium ion source bombardment silicon nanowires 0.5-2 hour; Or carry out surface active with chemical process, and silicon nanowires is put into the mixed solution of the vitriol oil and hydrogen peroxide, be to boil under 60-90 ℃ 10-60 minute in temperature, be chilled to room temperature, be washed till neutrality with distilled water, put into H then
2O: H
2O
2: NH
3.H
2The volume ratio of O is 3-5: 0.2-1: in 1 the mixed solution 1-3 hour, take out, and be washed till neutrality with distilled water, vacuum-drying;
2) finishing of silicon nanowires:
In being connected with the container of water trap, add surface-treated silicon nanowires and the 40mL dry toluene that the 20mg step 1) obtains, under the protection of inert gas, be heated to 140 ℃ of component distillations and remove moisture, after steaming 30mL toluene, be cooled to 60-90 ℃ and add the N-3-triethoxysilylpropyl dansyl amide of 0.6mmol-1.8mmol, be 60-90 ℃ in temperature and stirred 12-48 hour down, reduce to room temperature, filter the thick product of silicon nanowires that obtains finishing with strainer; Thick product carries out ultrasonic cleaning in organic solvent, filter, and removes unreacted N-3-triethoxysilylpropyl dansyl amide, and vacuum-drying obtains the fluorescence chemical logic switch based on silicon nanowires.
2. method according to claim 1 is characterized in that: described silicon nanowires diameter is at 15～25nm, and length is at 1um～10um.
3. method according to claim 1 is characterized in that: in the mixed solution of the described vitriol oil and hydrogen peroxide, the vitriol oil: the mol ratio of hydrogen peroxide is 7: 3.
4. method according to claim 1 is characterized in that: described thick product carries out ultrasonic cleaning in organic solvent be successively at toluene, and methylene dichloride carries out ultrasonic cleaning in the ethanol.
5. method according to claim 1 is characterized in that: step 2) described dry toluene is the new dry toluene that steams.
6. fluorescence chemical logic switch that obtains by each method of claim 1～5 based on silicon nanowires.
7. the fluorescence chemical logic switch based on silicon nanowires according to claim 6, it is characterized in that: based on the one dimension Nano structure of the fluorescence chemical logic switch of silicon nanowires this to carry out in being scattered in deionized water in the fluoroscopic examination be chaotic distribution, or oldered array distributes.
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