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Synthesis and characterization of silicon nanowires using tin catalyst for solar cells application

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ELSEVI

Contents lists available at ScienceDirect Materials Letters

materials letters

Synthesis and characterization of silicon nanowires using tin catalyst for solar

cells application

Minsung Jeon *, Koichi Kamisako

Department of Electronic and Information Engineering, Tokyo University of Agriculture and Technology, 2-24-16 Nakacho, Koganei, Tokyo 184-8588, Japan

Article history:

Received 20 November 2008

Accepted 6 January 2009

Available online 8 January 2009

Keywords:

Sn-catalyzed SINWs

Reflectance

Solar cells

Phosphorous diffusion

VLS mechanism

Hydrogen radicals

Tin-catalyzed silicon nanowires were synthesized for solar cells application Voluminous silicon nanowires were fabricated on single crystalline silicon wafer Optical reflectance and solar cell efficiency of the synthesized silicon nanowires were explored The reflectance of as-synthesized silicon nanowires was obtained approximately 5% in the short wavelength region (A<500 nm) A short circuit current of 2.3 mA/cm? and open circuit voltage of 520 mV for 1 cm? SiNWs solar cell was obtained

© 2009 Elsevier B.V All rights reserved

1 Introduction

In recent years, nanowires including nanorods based solar cells

have attractive interest due to their characteristics and processing

benefits The nanowires-enabled solar cells allow for decoupling the

light absorption from the direction of carrier transport, such that in

materials where the diffusion length of minority carriers is much

shorter than the thickness of material required for optimal light

absorption, current densities can be improved Nanostructure solar

cells, such as organic—inorganic materials, compound semiconductor

and hetero- or homo-junction silicon structure, have been studied by

many researchers [1-5] Law et al has been demonstrated for dye-

sensitized solar cells using ZnO nanowires and produced an efficiency

of 1.5% [2] Huynh et al have been studied polymer matrix solar cells

using CdSe nanorods, with efficiency of 1.7% [3] These results indicate

that the nanowires are attractive to enhance charge transport in

nanostructures solar cells compared with conventional solar cells or

other nanostructured solar cells

In particular, silicon nanowires (SiNWs) are irresistible materials in

the semiconductor industry because the bulk properties of silicon are

well-known Moreover, it can easily dope impurities to fabricate n- or

p-type Si semiconductor [6,7] The SINWs have been synthesized by

using various methods and metal catalysts via well-known vapor-

liquid-solid (VLS) mechanism [8,9] Moreover, various materials, such

as Au, Al, Ga, In, Pb, Sn and Zn [8-15], have been used for synthesis of

silicon nanostructures Recently, hetero-junction solar cell using

SiNWs have been demonstrated by Tsakalakos et al [4] They fabricated

* Corresponding author Tel./fax: +81 42 388 7446,

E-mail address: joseph@cc.tuat.ac.jp (M Jeon)

0167-577X/$ - see front matter © 2009 Elsevier B.V All rights reserved

doi:10.1016/j.matlet.2009.01.001

Au-catalyzed SiNWs on flexible metal foil and produced a current density of ~ 1.6 mA/cm? for 1.8 cm? cell Similar structures have been demonstrated by Thony et al They fabricated an all-inorganic SINWs solar cell using Au thin film and colloidal nanoparticles The short circuit current (J,.) and open circuit voltage (V,,) of the fabricated cells were 0.53 mA/cm? and 125 mV, respectively [5] As mentioned above,

Au nanoparticles are well-used metal catalyst and it easily synthesizes the SiNWs at low temperature However, it is known to be a deep level impurity in silicon In contrast with Au, tin (Sn) appears to be the favorable catalyst because the Sn-Si alloy has relatively low eutectic temperature of 232 °C [16] and forms with extremely low content of the elemental semiconductors

In our previous work, we successfully synthesized large quantities

of SiNWs using various materials by the hydrogen radical-assisted deposition method including hydrogen radicals pretreatment [12,14,17-19] Moreover, Sn-catalyzed SINWs were easily controlled

by introducing hydrogen flow gas ratios [20] In this letter, we synthesized SiNWs using Sn nanoparticles on single crystalline silicon (c-Si) wafer for solar cell application and their characteristics are explored

2 Experimental details

About 7 2 cm boron-doped Cz silicon (100) wafers were used for fabrication of solar cells Sn metal thin film as catalyst was evaporated

on these c-Si wafers The wafers were dipped in diluted hydrofluoric (5% HF) solution to remove native oxide layer and rinsed in pure water Then, the wafers were immediately located into the evaporation vacuum chamber The Sn metal film was deposited in situ onto the Si wafer by a thermal evaporation source at a rate of less than 1 nm/s.

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Table 1

Synthesis conditions for Sn-catalyzed SINWs fabricated on c-Si (100) wafer

Hydrogen radical treatment Synthesis of SINWs

After depositing a Sn film of approximately 7 nm thickness onto the Si

wafer, the wafer was transferred into the experimental chamber and

heated for 1 h at 400 °C Hydrogen (H2) gas was introduced and then

hydrogen radicals generated by 2.45 GHz microwave were irradiated

on the sample surface to fabricate metal nanoparticles For synthesis

of SINWS, silane gas as Si source was introduced into the experimental

chamber and it was reacted with hydrogen radicals SINWs were

synthesized for 20 min at 400 °C Detailed other synthesis conditions

are summarized in Table 1

The optical and morphological characteristics of the SiNWs

synthesized on c-Si wafer were estimated by spectrophotometer and

field emission scanning electron microscopy (FE-SEM) Furthermore, a

solar cell using the SiNWs synthesized on c-Si wafer was fabricated

after diffusion to form n* emitter The current-voltage (I-V) properties

of the fabricated SiNWs solar cell were investigated by solar simulator

(AM 1.5, 100 mA/cm”)

3 Results and discussion

After synthesis of SiNWs on p-type c-Si wafer, phosphorous diffusion was

performed on the front surface using spin-on phosphors silicate glass (PSG) coating

Then the samples were diffused to fabricate p-n* junction in quartz tube for 30 min at

900 °C in N2 ambient After diffusion, the samples were dipped in 5% HF solution to

remove parasitic layer Fig 1(a) illustrates a schematic of the SINWs solar cell design in

SiNWs

X

Ag contact

this work As shown in the Fig 1(a), the silver (Ag) contacts with thickness of 180 nm were evaporated on the surface of synthesized SiNWs without any transparent conductive oxide (TCO) film To investigate the morphological property of SINWs, a FE-SEM observation was carried out after synthesis of SINWs Fig 1(b) shows the top- view (15° tilted) and cross-section (see inset of Fig 1(b)) FE-SEM images of the SINWs

fabricated on c-Si wafer

As can be seen these figures, voluminous SiINWs were synthesized whisker-like The diameters of SINWs on the bottom and top were approximately 60 nm and thinner than 10 nm, respectively Their lengths extended up to ~1.5 ym Moreover, the SINWs were tapered and catalysts remained on the top of SINWs, It indicates that the Sn- catalyzed SINWs are synthesized via VLS mechanism [8,9] The detailed mechanisms were well described elsewhere [14] After diffusion, the surface morphologies were also observed Here, the doping level in the silicon nanowires, which is measured by secondary ion-microprobe mass spectrometer, was estimated to be 1.4* 107° atom/cm? base on planar Si wafer Fig 1(c) shows the FE-SEM image of the phosphorous-diffused SINWs, The shapes of SINWs after formation of pn junction were slightly curved

As mentioned above, we expect the SiNWs solar cells to show improved optical properties compared with conventional planar Si solar cells Fig 2(a) shows the photograph of the fabricated SINWs solar cell The surface color was dark brown in appearance, To examine the optical properties of the SiNWs solar cell, a reflectance was measured by spectrophotometer with integrating sphere The reflectance of SINWs and typical planar c-Si wafer were compared as shown in Fig 2(b) The reflectance of the fabricated SINWs solar cell represented less than 5% in the short wavelength regions (A<500 nm) In contrast with this result, we have reported SINWs synthesized on c-Si, which have reflectance below 0.5% at A<700 nm [20] The difference of the reflectance might be the effect of synthesis conditions, such as thickness of metal film and SiH, gas flow The reduction of reflectance is very helpful to improve the solar cell performance Therefore, further reduction of the reflectance will be expected from the optimization of the synthesis conditions of SINWs

For analysis of the electrical properties, the I-V curve of the fabricated SINWs solar cell was measured by solar simulator under AM 1.5 (100 mA/cm7) Fig 3 shows the typical dark and light I-V curve of the SiNWs solar cell Clear rectifying behavior and power generation was distinguished in the 1 cm? SiNWs solar cell The short circuit current and open circuit voltage were obtained to 2.3 mA/cm? and 520 mV, respectively These values were higher than that of the hetero-junction SINWs synthesized on metal foil [4] and that of the homo-junction SiNWs solar cell [5] As can be seen in Fig 3, poor I-V characteristics in dark and light conditions were observed It is due to the high series resistance and low shunt resistance Theses limit the efficiency of the fabricated SINWs solar cell Here, the high series resistance may be caused by the unconnected metal Ag contact between the SINWs and neighboring SINWs Moreover, it might be the effect of

nt emitter

Evaporated Al contact

—_—~se

x

TY

» 44

=

we,

4

Fig 1 (a) Schematic of the SiNWs solar cells FE-SEM images of the (b) as-synthesized SiNWs and (c) phosphorous-diffused SiNWs, All the scale bars represent 2.5 um

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M Jeon, K Kamisako / Materials Letters 63 (2009) 777-779 779

300 450 600 750 900 1050 1200

Wavelength [nm]

Fig 2 (a) Photograph of the fabricated SiINWs solar cell (b) The difference of reflectance

between conventional planar c-Si solar cell and SiNWs solar cell

the Schottky barrier between the evaporated Al contact and silicon wafer because of

insufficient annealing conditions For low shunt resistance, it might be the leakage

current from the front metal contact, i.e., local shunting across the solar cell

In addition, the poor results were caused by the unoptimized diameter distribution

and the shapes of the synthesized SINWs It is typically not suitable for the application

of electrical and optical devices Furthermore, unremoved metal nanoparticles caused

the reduction of the carrier lifetime, i.e., increasing surface recombination velocity

Therefore, the sizes and impurity removal must be controlled for further improvement

Moreover, the improvement of the cell performance owing to the deposition of TCO

films, such as indium-tin oxide and fluorine doped tin oxide, on the surface of synthe-

sized SINWs will be expected

4 Conclusion

We have demonstrated tin-catalyzed silicon nanowires solar cells

fabricated by the hydrogen radical-assisted deposition method on a c-

Si wafer This SiINWs solar cell structure is a promising candidate for

future photovoltaic application In particular, it is possible to reduce

0.003

0.002 0.001 0.000

-0.003 F —Sn-catalyzed SiNWs Solar cell 7

-0.004 + L + L ¿ L +

Voltage [V]

Fig 3 I-V characteristics of the fabricated SiNWs solar cell under dark and light

conditions

the thickness of Si base substrate more thinly For improvement of

conversion efficiency of the SiNWs solar cells, the reduction of the

contact resistance and optimization of the nanowire sizes will be considered and the results will be presented near future

References

[1] Baxter JB, Aydil ES Appl Phys Lett 2005;86:053114

[2] Law M, Greene LE, Johnson JC, Saykally R, Yang P Nature Mater 2005;4:455 [3] Huynh WU, Dittmer JJ, Alivisatos AP Science 2002;295:2425,

[4] Tsakalakos L, Balch J, Fronheiser J, Korevaar BA, Sulima O, Rand J Appl Phys Lett 2007;91:233117

[5] Thony P, Delsol R, Jaussaud C, Rondel N, Rouvelere E, Poncet S, et al Proc 23rd European PVSEC, Valencia, Spain; Sep 2008, pp 670-4

[6] Pan L, Lew KK, Redwing JM, Dickey EC J Cryst Growth 2005;277:428

[7] Kimukin I, Islam MS, Williams RS Nanotechnology 2006;17:S240

[8] Wagner RS, Ellis WC Appl Phys Lett 1964;4:89, [9] Givargizov EI J Crystal Growth 1975;31:20, [10] Wang Y, Schmidt V, Senz S, Gosele U Nature Nanotech 2006;1:186

[11] Sunkara MK, Sharma S, Miranda R, Lian G, Dickey EC Appl Phys Lett 2001 ;79:1546 [12] Jeon MS, Kamisako K Mater Lett 2008;62:3903

[13] Zhang J, Jiang F, Yang Y, Li J J Cryst Growth 2007;307:76

[14] Jeon MS, Uchiyama H, Kamisako K Mater Lett 2009;63:246

[15] Yu JY, Chung SW, Heath JR J Phys Chem B 2000;104:11864

[16] Olesinski RW, Abbaschian GJ Bull Alloy Phase Diagr 1984;5:273

[17] Jeon MS, Kamisako K J Nanosci Nanotechnol 2008;8:5188

[18] Jeon MS, Tomitsuka Y, Kamisako K J Ind Eng Chem 2008;14:836

[19] Jeon MS, Kamisako K J Alloys Compd 2008, doi:10.1016/j.jallcom.2008.09.035 [20] Jeon MS, Uchiyama H, Tomitsuka Y, Maishigi K, Kamisako K Proc Renewable Energy 2008, Busan, Korea; Oct 2008

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