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Electrical conductivity measurement of silicon wire prepared by CVD

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Đây là một bài báo khoa học về dây nano silic trong lĩnh vực nghiên cứu công nghệ nano dành cho những người nghiên cứu sâu về vật lý và khoa học vật liệu.Tài liệu có thể dùng tham khảo cho sinh viên các nghành vật lý và công nghệ có đam mê về khoa học

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a r t i c l e i n f o

Article history:

Received 11 October 2008

In final form 27 November 2008

Available online 6 December 2008

a b s t r a c t

The electrical resistivity of a silicon nanowire formed from Si2H6by CVD was measured using micro-probes equipped with SEM The resistivity of 6.58  105Xcm at room temperature was obtained from the current–voltage (I–V) curve for the wire with both ends fused to the probes The non-linear I–V curve measured only by contacting the wire with the probes could be explained by the resistivity in a series of silicon and dielectric thin oxide films formed on the silicon nanowires

Ó 2008 Elsevier B.V All rights reserved

1 Introduction

Silicon nanowires (SiNWs) are potential materials for nanoscale

electronic and chemical devices[1–4]due to their quantum

con-finement effects and peculiar structures with a high aspect ratio

in nano size Most SiNWs have been formed by bottom-up

pro-cesses, such as laser ablation[5], thermal evaporation[6–8], solid

reaction[9], and chemical vapor deposition (CVD)[10,11] In each

case, SiNWs are synthesized by essentially utilizing a vapor–

liquid–solid (VLS) mechanism[12] SiNWs are single crystalline

and grow along the h1 1 1i or h1 1 2i direction with sizes of

3–1000 nm in diameter and 10lm – several mm in length[5,7]

Among several physical and chemical properties of SiNWs, there

have been several reports on electrical conductance

measure-ments, in which the single wire was placed on the patterned

elec-tric circuit fabricated by lithography and 2- and 4-terminal

methods were applied to measure the resistances[1,2,4] In

gen-eral, SiNWs are covered with a thin silicon oxide film formed

dur-ing the growth process or after exposure to air after the formation

[5–11] Oxide films have been removed so that the silicon crystals

directly contact the electrodes [13] However, the effect of such

thin oxide film on the electrical resistance measurement of SiNWs

has not been clarified

In the present work, the direct measurement of electrical

resis-tance of a silicon nanowire was attempted using micro probes

manipulated in a scanning electron microscope

2 Experimental procedures

2.1 Preparation of materials

Silicon nanowires were grown on {1 0 0} silicon wafers with a

thin gold film The silicon wafer had a rectangular shape (10 mm

long, 4 mm wide, and 0.5 mm thick) and was covered with gold film of approximately 2 nm in thickness The gold film as a catalyst growing SiNWs[3,11]was formed by sputtering The substrate was put into a stainless tube and placed inside a vacuum chamber so that the flow of the reactant gas could be controlled After evacuat-ing the chamber up to 1  105Pa, the substrate was heated at

569 K A 10% Si2H6gas diluted with H2and argon gas were then introduced into the chamber The disilane and argon gases were run at constant rates of 0.0167 cc/s and 0.33 cc/s, respectively The total pressure was set at 0.667 kPa The disilane gas was chem-ically decomposed to form SiNWs on the substrate through form-ing a liquid Au–Si eutectic, followed by silicon nanowire growth underneath the liquid eutectic droplet[12] After the deposition

of SiNWs for 1200 s, the structure of SiNWs was examined with

a scanning electron microscope (JEOL JSM-6700F) equipped with

an energy dispersive X-ray spectrometer (EDS) and high-resolution transmission electron microscope (JEOL JEM-3000F TEM) with a Gatan GIF Tridiem energy-filter system Plasmon-loss images were taken using the Gatan GIF system

2.2 Electrical resistance measurements The SiNWs formed on the substrate were manipulated with a Zyvex S100 system installed in LEO 1550 FE-SEM The manipula-tion system consisted of four tungsten probes One nanowire was picked up with the probes, and the current–voltage relations were measured at room temperature using 4-terminal and 2-terminal methods

3 Results 3.1 Silicon nanowires

Fig 1shows the morphology of SiNWs formed on a silicon wa-fer at 569 K The size of the wires ranged from 5 to 100 nm in diam-eter and 10 – several hundred lm in length The EDS analysis

0009-2614/$ - see front matter Ó 2008 Elsevier B.V All rights reserved.

* Corresponding author Fax: +81 29 859 2100.

E-mail address: noda.tetsuji@nims.go.jp (T Noda).

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indicated the presence of oxygen along with a strong Si peak in the

spectra of SiNWs

The typical microstructure of a SiNW taken by TEM is shown in

Fig 2 The SiNWs are crystalline and grow parallel to the h1 1 0i

direction A high-resolution lattice image shows that the SiNWs

consist of a crystalline core and an amorphous sheath The

diffrac-tion pattern indicates that the [1 1 1] zone axis of silicon single

crystal and additional 1/3{4 2 2} spots appeared The 1/3{4 2 2}

reflection has been reported elsewhere as well[14] The

appear-ance of these spots is reported due to the effect of the infinite

structure of the nanowire[14] The surface amorphous layer is

con-sidered as thin silicon oxide formed by oxidation in a small amount

of residual oxygen in the reaction chamber during the growth of

Fig 1 Morphology of SiNWs formed for 1200 s at 569 K.

Fig 2 TEM micrograph and diffraction pattern of a SiNW The diffraction pattern was taken for a square region of the lattice image of the nanowire.

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crystal of 19 nm covered with silicon oxide of around 1.8 nm in

thickness Other SiNWs with different diameters were also

exam-ined by TEM Most SiNWs were found to be covered with oxide

film with a thickness ranging from around 1 nm to several tens nm

3.2 Electrical resistance measurements

One SiNW with length longer than 100lm was pulled out from

bundled SiNWs formed on a silicon wafer by manipulating four

tungsten probes in a vacuum

Fig 4shows how to measure the electrical resistance of a SiNW

by the probes The SiNWs had enough stiffness to be held by the

probes The wire was pushed with four probes that were

alternately positioned so that the contact between the wire and

tungsten probes could be sufficiently obtained (seeFig 4a) A

con-stant electrical current was applied between the outer two probes

The voltage between the inner two probes was then measured

with a voltmeter The diameter of the SiNW examined in this

experiment was 850 nm The distance between the two inner

probes was 2.82lm

Fig 5 shows the result of a 4-terminal measurement for the

sample shown inFig 4 The current increases with the measured

voltage, but no linear relationship in current versus voltage (I–V)

behavior was observed The slope of the I–V curve gradually

in-creased with the voltage The linear I–V relation can be assumed

at a certain voltage range The slope gives an approximate

resistiv-ity of 3.1  106

Xcm at 0–10 V, 1.7  106

Xcm at 10–15 V, and 6.9  105Xcm at 30–38 V

The result ofFig 5seems to be caused by the effect of surface

oxide surrounding the silicon core Then, the applied current

in-creased, resulting in the melting of the end of the SiNW contacting

the tungsten probe InFig 4b, the features of the contacts of the

fused SiNW on the two tungsten probes are shown It is evident

that the end of the SiNW contacting the probe was melted and

cov-ered the probe According to the binary phase diagram for Si–W

system, W2Si phase appears at temperatures lower than the

melt-ing point of silicon[17].This means that the tungsten silicide could

be formed at the interface between the fused silicon wire and the

tungsten tip The silicon wire therefore firmly adhered to the

tung-sten probe and the contact resistivity between the silicon wire and

the tungsten tip is considered to be negligibly small The length of

the SiNW between the two probes was 38.6lm The I–V relation

was then measured The linear relation was obtained as shown in

Fig 6 The slope gives a resistivity of 6.58  105

Xcm for the SiNW

of 850 nm in diameter and 38.6lm in length The present result is

in good agreement with an intrinsic resistivity in the order of

105

Xcm for silicon[18] This value corresponds to p- or n-type

impurity concentration of 109–1010/cm3[19] Assuming the

num-ber of silicon atoms in a cubic centimeter as 5  1022, the purity

of the present SiNW is to be better than 11 N Furthermore, the

of the tungsten probes showed a clear linear relation The resistiv-ity obtained fromFig 6was 6.58  105Xcm, which corresponds

to the resistivity of silicon crystal with a purity better than 11 N

InFig 5, the resistivity decreases with increasing voltage and came close to the value of that ofFig 6 The value of 6.9  105Xcm at 30–38 V was described in the previous section The surface silicon oxide is essentially an insulator and has ionic conductive property

By applying voltage, the ionic current gradually increases with increasing the electric field, and finally, a dielectric breakdown phenomenon occurs at high electric fields

The ionic current, I, through a dielectric material is given as Eq

(1) [20]:

Fig 4 SEM micrographs of a SiNW contacted with 4 tungsten probes (a), and the same SiNW of which both ends were fused to the probes (b) The electrical measurements were conducted with the 4-terminal method (a) and the 2-terminal

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I ¼ K sinhðkqE=2kTÞ; ð1Þ

where k is the ionic jump distance, q, the charge, E, the electric field,

k, the Boltzmann constant, and T, the temperature K is a constant at

the measured temperature

Fig 7is a schematic drawing of the electrical measurement of

the SiNW covered with the silicon oxide layer The total resistance,

R, is the sum of those of SiNW and silicon oxide as

where R1 is 6.58  105

Xcm and is taken from the present experiment

R2is given as a function of electric field, E, as expected from Eq

(1)

The total voltage, VT, is then

V1and V2are applied voltages to the silicon wire and the surface

oxide layer, respectively

Assuming T = 298 K, k = 0.491 nm of the lattice parameter for

the (1 0 0) plane of quartz [21], q = 3.2  1019C for the oxygen

ion, and the average thickness of oxide of 12.5 nm as a result of

the observation of the fractured surface of the SiNW described in

the previous section, the I–V relationship can be obtained by giving

proper K and V2values In the present case, the ratio of V2/VT, r, was

assumed to be constant independently of VT

Fig 8is the result of curve fitting using Eq.(3), where the K va-lue and r were assumed to be 1.1  1011A and 0.055 A fairly good coincidence between the experimental and simulation results is observed The electric field, E, estimated from the r value, was changed from 4 kV/mm at VT of 1 V and 44 kV/mm at 15 V The reported breakdown electrical field for silicon oxide film is around

40 kV/mm[22] As described in the previous section, the resistivity measured by the 4-terminal method started to decrease at around 10–15 V of the applied voltage The dielectric breakdown was as-sumed to be completed at 30 V since the resistivity value measured with the 4-terminal method agrees with that with the 2-terminal method at around the applied voltage That means that the break-down of the surface oxide film was considered to gradually occur

at lower voltage than 30 V

Fig 5 I–V curve for the SiNW measured with the 4-terminal method.

Fig 7 Schematic illustration of the electrical circuit of SiNW.

Fig 8 Fitting the estimated I–V curve using Eq (3) to the experimental data

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(1) The prepared SiNWs were single crystalline and grow

paral-lel to the h1 1 0i direction The SiNWs were covered with thin

silicon oxide film

(2) The I–V curve for the SiNW of 850 nm in diameter measured

with the 4-terminal method using micro probes showed a

non-linear relationship that might have been caused by

the effect of surface silicon oxide on the SiNWs

(3) The 2-terminal measurement, in which both ends of a SiNW

were fused to the probes, indicated a linear I–V curve giving

the resistivity of 6.58  105

Xcm This value corresponds to that of bulk silicon with purity better than 11 N

(4) The I–V curve obtained with the 4-terminal method could be

explained by the resistivity in a series of silicon and thin

oxide film

[10] Z.Q Liu et al., Chem Phys Lett 341 (2001) 523.

[11] H Suzuki, H Araki, M Tosa, T Noda, Mat Trans 48 (2007) 2202.

[12] R.S Wagner, W.C Ellis, Appl Phys Lett 4 (1964) 89.

[13] J Hu, M Ouyang, P Yang, C.M Lieber, Nature 399 (1999) 48.

[14] D.C Bell, Y Wu, C.J Barrelet, S Gradecak, J Xiang, B.P Timko, C.M Lieber, Microsc Res Tech 64 (2004) 373.

[15] Q Hu, H Suzuki, H Gao, H Araki, W Yang, T Noda, Chem Phys Lett 378 (2003) 299.

[16] K Sasaki, S Tsukimoto, M Konno, T Kamino, H Saka, J Microsc 203 (2001) 203.

[17] S.V.N Naidu, A.M Sriramamurthy, P.R Rao, J Alloy Phase Diag 5 (1989) 149 [18] F.J Morin, J.P Maita, Phys Rev 96 (1954) 28.

[19] W.R Runyan, Silicon Semiconductor Technology, McGraw-Hill Book Company, New York, 1965, p 106.

[20] M Kosaki, K Sugiyama, M Ieda, J Appl Phys 42 (1971) 3388.

[21] G Roma, Y Limoge, S Baroni, Phys Rev Lett 86 (2001) 4564.

[22] G Siddall, Vacuum 9 (1960) 274.

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