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Physica E 23 (2004) 1–4

www.elsevier.com/locate/physe

Junjie Niua, Jian Shaa;b, Niansheng Zhangb, Yujie Jia, Xiangyang Maa, Deren Yanga;∗

a State Key Lab of Silicon Materials, Department of Material Science and Engineering, Zhejiang University, Zheda Lu 38,

Hangzhou 310027, People’s Republic of China

b Department of Physics, Zhejiang University, Hangzhou 310027, People’s Republic of China

Received 8 November 2003; accepted 27 November 2003

Abstract

Tiny SiO2nano-wires (SiO2-NWs) were synthesized on a p-Si (1 1 1) wafer by the chemical-vapor-deposition method The minimum diameter of the nano-wires was around 9 nm, and the length was longer than 10 m The results of transmission electron microscopy shows that the amorphous nano-wires were composed of Si and O with an approximate atomic ratio of 1:2 Furthermore, the photoluminescence behavior of the SiO2-NWs has been also checked

? 2004 Elsevier B.V All rights reserved

PACS: 71.55.Cn; 81.05.Ys; 81.15.Gh

Keywords: Tiny SiO2 nano-wires; Synthesis; PL spectrum

1 Introduction

Quasi-one dimensional nano-materials have

stim-ulated much interest for their potential applications

in nano-electronics, optics, Bat face display, etc

con-Fnement eGect, the diameter of the one-dimensional

nano-materials should be very small (e.g 1 nm) It

has been reported that the minimum diameter of

car-bon tubes could be 0:4 nm [10], and that of silicon

potential photoluminescence and wave-guide

attention [12] Several techniques have been used to

fabricate SiO2-NWs, such as sol–gel, laser ablation,

Corresponding author Tel.: 571-8795-1667; fax:

+86-571-8795-2322.

E-mail address: mseyang@dial.zju.edu.cn (D Yang).

catalyzed thermal decomposition, carbothermal re-duction, chemical-vapor-deposition (CVD) and so on [13–17] By means of CVD method, it was reported

50 nm [18]

In this paper, we report the synthesis of the large

scale tiny (about 9 nm in diameter) and long (∼ m)

of compatibility with integrated circuits, silicon sub-strates were used in our experiments The nano-wires were checked by means of a scanning electron mi-croscopy (SEM), transmission electron mimi-croscopy (TEM), energy dispersive X-ray spectroscopy (EDX), and photoluminescence (PL) spectroscopy

2 Experiment The heavily boron-doped p-type Si (1 1 1) wafers as substrates was Frst cleaned for 30 min in the acetone

1386-9477/$ - see front matter ? 2004 Elsevier B.V All rights reserved.

doi:10.1016/j.physe.2003.11.274

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2 J Niu et al / Physica E 23 (2004) 1–4

by ultrasound The substrates were about 20 mm in

width and 40 mm in length Next, a magnetic

sputter-ing method was used to deposit Ni as a catalyst on the

substrates Then the substrates were placed in a quartz

tube furnace The furnace chamber was pumped down

to 10 Pa and heated When the temperature reached

1000C, a mixture gas of argon, hydrogen, and silane

(Bow ratio 100:20:15) was allowed into the chamber

The pressure and temperature in the chamber were

kept at 2000 Pa and 1000C during the deposition

After that, the substrates were removed from the

fur-nace for the SEM (JSM-T20, JEOL) and PL (F-4500,

Hitachi) measurement, respectively The PL spectra

of the deposited matters on the substrates were

mea-sured at room temperature in the spectral range of

200–900 nm using a general Xe-light source with a

wavelength 206 nm as the excitation source

Further-more, the deposited matters on the substrates were

dis-solved in an ethanol solution, and then the dropwise

was placed on a copper grid covered with a very thin

carbon Flm, so that the deposited materials could be

analyzed with a TEM (Phillip CM200) equipped with

an EDX

3 Results and discussion

Top view of the large-scale entangled tiny

nano-wires synthesized on the silicon substrates is

shown in Fig.1 The as-grown nano-wires have length

Fig 1 Top view SEM image of the densely tiny nano-wires that

grew on a silicon substrate.

Fig 2 TEM image of the as-grown SiO2 -NWs Most of the smooth SiO2-NWs have uniform diameter of about 9 nm, while the others have a diameter of 20 nm The corresponding EDX data (upper right inset) of the SiO2-NWs shows that they are composed of Si and O with an approximate atomic ratio of 1:2 C and Cu peaks originated from Cu grid for TEM analysis.

up to tens of micrometers, and most of them have di-ameter around 9 nm and a few of them have diam-eter around 20 nm, as shown in Fig 2 The smooth

ob-served The EDX spectrum (Fig.2, upper right) shows that the nano-wires were composed of Si and O with

an approximate atomic ratio of 1:2 C and Cu peaks

in the spectrum originated from the Cu grid used for TEM analysis The high-magniFcation TEM image of

a SiO2-NW is given in Fig 3 A clear Ni particle can be seen as the catalyst attached to the tip of the SiO2-NW The SAED pattern (inset of Fig.3) shows

no diGraction spots, indicating the amorphous nature

of the SiO2-NW, which was of the same nature as that

in the previous work [18]

The PL measurements at an excitation wave-length of 206 nm were carried out with a general Xe-light source Fig.4shows the PL spectrum of the

a normal emission band at around 544 nm, which

is believed to be due to neutral oxygen vacancies

of SiO2-NWs [18,19] Furthermore, a new emission band at 595 nm with very weak density could be also observed At present, the exact mechanism of

experiments will be needed

According to the vapor–liquid–solid (VLS) mecha-nism, the catalyst as islands can induce the deposition

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J Niu et al / Physica E 23 (2004) 1–4 3

Fig 3 TEM image of a single SiO2-NWs A Ni–Si droplet attached

to the tip of the SiO2-NW (the white arrow, lower inset) The

SAED pattern in the upper right indicates the amorphous nature

of the SiO2-NW.

Fig 4 PL spectrum of SiO2 -NWs measured at room temperature.

atoms to form droplets so that nano-wires can grow

[20] The diameter of the nanowires is dependent on

the size of the catalyst In most of the cases these two

sizes are very close In our experiments, the size of the

catalyst was uniform and very small (¡ 10 nm in

di-Fig 5 The sketch graphs of the SiO2-NWs growth.

ameter as shown in Fig.3) Those small catalyst par-ticles could easily form nuclei so that the nano-wires with smaller diameter could be grown on them

In the beginning of the nano-wire growth, the round

Ni particle and the Si atoms deposited from silane form

with more and more Si atoms melting, the droplets gradually reach supersaturation The Si atoms in the droplet will segregate when more Si atoms joined The segregation has an equal probability in the 360area around the droplets that place on the smooth silicon substrates Therefore, the segregated Si atoms would grow around the droplet with the crystal directions Si (1 1 1), Si (2 2 0), Si (3 1 1), etc (Fig.5b) According

to the lowest energy theory, the Si (1 1 1) direction will dominate the Fnal growth, for it is the lowest en-ergy Because the consumed Si atoms, due to the earli-est growth of Si (1 1 1) direction, gradually to reach a homeostasis with the deposited Si atoms, the growth of other new Si (1 1 1) directions will not appear around the droplet (Fig.5c) Thus with the prolonged grow-ing time, the Si atoms along with (1 1 1) direction

moved forward slowly accompanying the growth of the SiNWs One thing must be mentioned: the newly formed SiNWs will be oxidized rapidly to amorphous

degree and the impure reaction gases in the quartz

tube Since the temperature (∼ 1000 ◦C) is much lower than the crystalline temperature of the SiO2-NWs, this

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4 J Niu et al / Physica E 23 (2004) 1–4

induces the original nano-silicon structure to an

amor-phous SiO2-NWs and round-belt SiO2 structure (see

the TEM image in Fig.3)

In the primary phase of the SiNWs, the droplets are

pushed forward slowly with the continued growth If

only one droplet exists on the silicon wafer, the droplet

will be pushed to one direction straightly Therefore,

the SiNWs will be uniform and straight growing under

this condition (Fig 5d) In fact, hundreds and

thou-sands of droplets on the substrates collide unavoidably

during the co-instantaneous growth When a moving

droplet encounters another moving droplet, the two

droplets will commix to a bigger droplet (Fig.5e,

be-cause the outside silicon ring is very thin, we ignore

its very weak eGect) When Si atoms drop in, the new

droplet will reach supersaturation again to segregate

and will keep the former SiNWs to grow continually

But the growth velocity (Fig.5f) has been slower in

comparison with the original SiNWs (Fig.5c) A

cer-tain angle  (in Fig.5f) between the two diGerent

di-rectional SiNWs induces the SiNWs to grow curly (see

Fig.5g) The SiNWs formed under this condition are

commonly curving (see the circular regions in Fig.2)

Obviously, the number of commixed SiNWs droplets

is very small Even the encountering of three or more

than three droplets is much less (Fig.5h) The

major-ity is that one droplet forms a SiNW and its diameter

is relatively straight, as shown Fig.2 A deeper

might contribute to the successful synthesis and

de-vice application of one-dimensional quantum wires

4 Conclusions

about 9 nm and a length of more than 10 m were

synthesized on a p-Si (1 1 1) wafer The experiments

of SEM and TEM found that nano-wires were

com-posed of Si and O with an approximate atomic ratio

of 1:2 and were of amorphous nature Besides the

nor-mal emission band at 544 nm, a new weak emission

also observed

Acknowledgements This work was supported by the National Natu-ral Science Foundation of China (No 50272057 and 60225010) and Zhejiang Provincial Natural Science Foundation (No 601092) The authors also express their gratitude to Prof Youwen Wang for the TEM measurement

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