Vol. 63, No. 8, August 2013, pp. 905∼908
New Physics: Sae Mulli, DOI: 10.3938/NPSM.63.905
Study on the Structural and the Electrical Properties of SnO 2 Thin Films Synthesized by Using Sol-gel and Rapid Thermal Annealing Processes
Jong Hoon Lee · Fan Zhang · Hong Seung Kim ∗
Department of Nano Semiconductor Engineering, Korea Maritime University, Busan 606-791, Korea
Jin Hwa Ryu · Kyu-Ha Baek
IoT Convergence Research Department, Electronics and Telecommunication Research Institute, Daejeon 305-700, Korea (Received 20 May 2013 : revised 11 June 2013 : accepted 9 August 2013)
In this study, the structural and the electrical properties of SnO
2thin films were investigated according to the sintering-temperature conditions for the sol-gel process. The SnO
2thin films annealed at temperatures over 800
◦C were shown not to have improved crystallinity and to have a surface morphology with increasing surface unevenness due to recrystallization. The carrier concentrations of the annealed SnO
2thin films were confirmed to be about 10
18∼ 10
19/cm
3, and the carrier concentration decreased with increasing annealing temperature. The mobilities of the SnO
2thin films ranged from 0.83 to 4.74 cm
2/Vs, and the resistivities were confirmed to range from 0.06 to 1.01 Ω·cm.
PACS numbers: 61.66.Fn, 81.40.Ef, 81.20.Fw, 72.20.My Keywords: SnO
2, RTP, Sol-gel, Hall measurement
ú
v Ú-¦ t 0 n É® z º ¶ ¥V R Ëc Ü R SnO 2 U c lT c l8 ý ò k @ Ò × ° Ç% iP «X N Ë; c  \ ¥ U c lT c l8 ý ºX ì Ä,
¹
ÅM X ì Ä ¤V R Ë ì Å
T
ø ¶ B0 å · Fan Zhang · » ý ¡ û B ∗
ô
Dz D G K ª @ / < Æ § / B N õ @ / < Æ ¸ ì ø Í ¸^ / B N < Æõ ,  Òí ß 606-791
©
¼ . > é s · Ù v¦
ô
Dz D G : x ½ ¨" é ¶ IoTÖ 6 x ½ + Ë ½ ¨Â Ò, @ / 305-700
(2013¸ 5 Z 4 20{ 9 ~ Ã Î6 £ §, 2013¸ 6 Z 4 11{ 9 Ã º& ñ : r ~ Ã Î6 £ §, 2013¸ 8 Z 4 9{ 9 > F S X & ñ )
: r ½ ¨\ " f H a % ¦- 0 q / B N& ñ \ " f è : r ¸ ¸| \ É r SnO
2~ Ã Ì} _ ½ ¨ ¸& h , l & h : £ ¤$ í ` ¦ ì r$ 3
% i . ½ ¨ ¸& h : £ ¤$ í \ " f SnO
2~ Ã Ì} É r 800
◦C s © \ " f H 8 s © _ & ñ $ í ¾ Ó © s { 9 # Q t · ú § H
כ
` ¦ S X % i Ü ¼ 9, ~ Ã Ì} _ ³ ð + þ A © s F & ñ o Ð K ³ ð כ ¹^ o =s 7 £ x % i . l & h : £ ¤$ í \
"
f \ P % o ) a SnO
2~ Ã Ì} _ H o # Q H 10
18∼ 10
19/cm
3 Ð% i Ü ¼ 9, \ P % o : r ¸ 7 £ x < Ê\
H o # Q Ã º H y è H â ¾ Ó` ¦ Ð% i . SnO
2~ Ã Ì} _ s 1 l x ¸ H 0.83 \ " f 4.74 cm
2/Vs _ ° ú כ` ¦ t 9, q $ ½ Ó É r 0.06 \ " f Ω· cm ° ú כ` ¦ t H כ ` ¦ S X % i .
PACS numbers: 61.66.Fn, 81.40.Ef, 81.20.Fw, 72.20.My Keywords: SnO
2, RTP, a % ¦- 0 q, f . Ë 8 £ ¤& ñ
∗
E-mail: [email protected]
905
906 New Physics: Sae Mulli, Vol. 63, No. 8, August 2013
I. " e  ] Ø
& ñ í ß oÓ ü t ì ø Í ¸^ SnO
2 H Û ¼G ' p" f_ 8 £ ¤& ñ 6 x ì
ø Í ¸^ Ó ü t| 9 Ð+ V , o 6 x ) a [1–4]. Û ¼ o½ + ËÓ ü t \ SnO
2_ ~ à Ì} s ¸Ø ¦ ÷ & ~ à Ì} _ l ¸$ í É r >
)
a . SnO
2ì ø Í ¸^ _ â Ä º í ß è_ / B N/ B N Ü ¼ Ð < Ês > r F
9, s â Ä º ü @Â Ò\ " f \ P \ -t Å Ò# Qt > ÷ &
Å Ò> Ð 6 x H í ß è/ B N/ B N _ ¸@ / Ð s 1 l x
#
Ä » ÷ &# Q n-+ þ A ì ø Í ¸^ ) a [5]. s ü < ° ú É r SnO
2~ à Ì} \ í ß èl ^ f ¨ à Ì÷ &> ÷ & Ä » H { 9
³ ð _ í ß è l ^ \ í S \ ÷ & { 9 > \ 0 A © # 4 s
+ þ A$ í ÷ &# Q l ¸ ¸ H ± ú t > ) a . ì ø Í@ / Ð í ß è
"
é
¶ ¨ 8 " é ¶ s ÷ & 0 A © # 4 s ± ú 4 R l ¸$ í É r Z
} t > ) a [6]. l > r _ SnO
2~ Ã Ì} É r ª ô Ç ~ ½ ÓZ O Ü ¼
Ð 7 £ x à Ìs 0 p x . rf-sputter, spray pyrolysis, a % ¦- 0 q 1 p x s
6 x ÷ & ¦ e [7–9]. Õ ª × æ a % ¦- 0 q / B N& ñ É r 6 xÓ o\ " f " é ¶
«
Ñ Ó ü t| 9 s Ø ¦ µ 1 Ï # ¦^ Ð è ) a ~ Ã Ì} ` ¦ % 3 H ~ ½ ÓZ O s
. s ü < ° ú É r 6 xÓ o\ " f r ÷ & H ~ ½ ÓZ O É r ª ô Ç W~ ½ Ó Z O
\ & h 6 x s 0 p x ô Ç © & h ` ¦ . á Ô 2 ;à Ô W/ B N& ñ , Û ¼ ß
¼ 2 ;á Ô 2 ;h A, Õ ª q , Õ ª q ` v! Ó / B N& ñ s & h 6 x 0 p x
l M :ë H \ l > r _ / B N` ¦ s 6 x ô Ç 7 £ x à Ì/ B N& ñ Ð
&
h Ä º0 A\ ¦ [10]. t ë ß a % ¦- 0 q / B N& ñ É r Ê ê5 Å q Ü ¼ Ð
~ Ã
Ì} _ è ` ¦ 0 Aô Ç / B N& ñ ` ¦ 9 כ ¹ Ð > ) a . s ü < ° ú
É
r @ /| ¾ Ó Ò q tí ß x 9 / B N& ñ r ç ß _ é ß » ¡ ¤` ¦ 0 AK " f H / å L5 Å q \ P % o
\ ¦ : x ô Ç ~ Ã Ì} o / B N& ñ s 9 כ ¹½ + É כ Ü ¼ Ð ó ø Íé ß ) a . / å L5 Å q
\ P
% o / B N& ñ É r É r / B N& ñ r ç ß Ü ¼ Ð K @ /| ¾ Ó Ò q tí ß s 0
p
x ½ + É÷ r ë ß m $ q 6 x Ü ¼ Ð 0 p x l M :ë H \ $ _
Û ¼G ' p" f ] j \ & h ½ + Ë . / å L5 Å q \ P % o r ~ Ã Ì} _ è
: r ¸ × æ כ ¹ô Ç כ ¹ è × æ s .
: r z ´+ « > É r 500
◦C \ " f 1000
◦C t q §& h  ú ª É r r ç ß 1
l
x î ß \ P % o \ ¦ ½ + É Ã º e H / å L5 Å q\ P % o © q Ð Ê ê5 Å q \ P % o
) a SnO
2~ Ã Ì} _ : £ ¤$ í ` ¦ ½ ¨ ¸& h , l & h Ü ¼ Ð ì r$ 3 # Õ
ª õ \ ¦ Ð ¦ô Ç .
II. ÷ m Ç] M ö U ê s0 n É
: r ½ ¨\ " f 6 x ) a 6 xÓ o É r 6 £ § õ ° ú . 2-methoxy ethanol (CH
3OCH
2CH
2OH, Aldrich) \ 1 M 0 l x ¸_ tin chloride (SnCl
2, Aldrich)\ ¦ À Òü < 1 l x1 p x ô Ç ] t 0 l x ¸_ acetylacetone (CH
3COCH
2COCH
3, Aldrich)` ¦ V , % 3 .
50
◦C _ \ P ó ø Í 0 A\ " f 2r ç ß 1 l x î ß Õ ªW 1h Ë : \ ¦ s 6 x
#
¢ - a 6 x K r ( . \ P í ß o ) a z ´o B H l ó ø Í` ¦ 2 cm × 2 cm l ó ø Íß ¼l Ð Ø Ô ¦ [ j : r õ \ ò ø Í` ¦ 6 xÓ o\ í H
&
h Ü ¼ Ð { " f í6 £ § [ j' l \ ¦ s 6 x # 10ì r ç ß Ä »l
Fig. 1. (Color online) X-ray diffraction patterns of SnO
2thin films annealed from 500 to 1000
◦C.
[
j' ` ¦ % i . t } Ü ¼ Ð íí H Ã ºÓ ü t` ¦ s 6 x # ' ½ ¨
#
Q ? /% 3 . t } Ü ¼ Ð UV-Ozone © q \ l ó ø Í` ¦ V , ¦ 20ì r ç ß 9 þ t o _ ç ` ¦ % i . [ j' ) a l ó ø Í É r ½ + Ë$ í ) a 6 xÓ o` ¦ 1 µm ß ¼l _ syringe 9 ' \ ¦ s 6 x # l ó ø Í0 A\ b # Qä ¼
2 ; Ê ê Û ¼ 2 ; ï' (spin coater) © q \ ¦ s 6 x # 3000 rpm 5
Å
q ¸ Ð 30 íç ß r ¸ í % i . 6 xÓ os ¸ í ) a l ó ø Í` ¦ 5ì r 1 l x î ß y y 120
◦C, 150
◦C, 200
◦C \ " f í H & h Ü ¼ Ð 3 é ß > Ð * $" f \ P ó ø Í0 A\ " f \ P % o \ ¦ % i . s ü < ° ú s
\ P % o ) a l ó ø Í` ¦ / å L5 Å q \ P % o / B N& ñ © q (Rapid ther- mal process, RTP)\ ¦ s 6 x # 500
◦C \ " f 1000
◦C t
100
◦C m 7 £ x r v " f 5ì r 1 l x î ß @ /l ì r 0 Al \ " f
\ P
% o \ ¦ % i .
\ P
% o ) a Ò re ¦ É r X-ray r] X J 8 £ ¤& ñ l , ~ Ã Ì} ¿ ºa 8
£ ¤& ñ l , Å Ò & ³p â , f . Ë 8 £ ¤& ñ © q \ ¦ s 6 x # ~ Ã Ì }
_ ½ ¨ ¸& h l & h : £ ¤$ í x 9 l & h : £ ¤$ í ` ¦ ¸ % i .
III. + s ÇÊ Ý õ m Í w ² o
Figure 1 É r \ P % o ) a SnO
2~ Ã Ì} _ XRD (X-ray diffrac- tion) 8 £ ¤& ñ õ \ ¦ · p כ s . JCPDS 46-1088 × ¼ ü
< q § r x ß ¼ 0 Au H SnO
2 ' aº x ß ¼ü < { 9 u % i Ü ¼ 9, ¸ H x ß ¼ H SnO
2_ & ñ ~ ½ Ó ¾ Ó\ ' a8 £ ¤ ÷ & 9,
É
r Ô ¦í HÓ ü t x ß ¼ H ' a8 £ ¤ ÷ &t · ú § ¤ . \ P % o : r ¸ 7 £ x
< Ê\ (110) x ß ¼_ y © ¸ H 7 £ x % i Ü ¼ 9, x ß ¼ ì ø Íg Ë :; ¤ É r y
è H כ ` ¦ · ú Ã º e . ¢ ¸ô Ç \ P % o : r ¸ 7 £ x < Ê\
& ñ $ í É r ¾ Ó © ÷ & 9, 800
◦C s © \ " f H H : £ ¤$ í ¾ Ó
© ` ¦ 4 R ¸t 3 l w H כ Ü ¼ Ð ó ø Íé ß ) a . 0 A õ a % ¦- 0 q /
B N& ñ \ 6 x ) a ½ ¨^ Ó ü t| 9 x 9 / å L5 Å q ¦ : r \ P % o ì r 0 Al
Study on the Structural and the Electrical Properties of SnO
2Thin Films Synthesized by· · · – Jong Hoon Lee et al. 907
Fig. 2. SEM images showing the top view of SnO
2thin films.
Fig. 3. (Color online) Thickness of SnO
2thin films an- nealed at several RTP temperatures.
\
" f q §& h  ú ª É r r ç ß (5 min) 1 l x î ß \ o ç ß × ¼ Ó ü t| 9 _ \ P ì
r K x 9 ÐW 1s à Ô_ ì r K { 9 # Q SnO
2& ñ $ í ` ¦ t
H כ ` ¦ S X % i .
Figure 2 H SnO
2~ Ã Ì} _ ³ ð & ³ © ` ¦ Å Ò & ³p â Ü
¼ Ð 8 £ ¤& ñ ô Ç s p t s . y y _ \ P % o : r ¸\
~ Ã
Ì} _ ³ ð + þ A © s : r ¸\ o H כ ` ¦ S X
%
i . 500 ∼ 600
◦C \ " f H É r ¸ & ñ { 9 [ þ t s ³ ð
\ + þ A$ í ) a כ ` ¦ S X ½ + É Ã º e Ü ¼ 9, B Ä º ¨ î ò ø Íô Ç : £ ¤$ í
`
¦ Ð% i . t ë ß 700
◦C s © \ " f H ~ Ã Ì} _ { 9 [ þ t s F
& ñ o ÷ & " f ½ ¨+ þ A_ 9 þ t QÛ ¼' (cluster) + þ A © s { 9 Â Ò
'
a8 £ ¤H d` ¦ · ú Ã º e . 800
◦C s © \ " f H ¸ & ñ [ þ t s
ì r í # { 9 Â Ò & ñ w n [ þ t s ì r í ¦ e Ü ¼ 9, 900 ∼ 1000
◦C \ " f H ¦ : r _ \ P % o \ _ K ~ à Ì} ³ ð \ ß ¼Ï þ (crack) s ' a8 £ ¤H d` ¦ S X % i .
Figure 3 É r SnO
2~ Ã Ì} _ \ P % o : r ¸\ É r ¿ ºa 8 £ ¤
&
ñ õ s . Ê ê5 Å q \ P % o : r ¸ 7 £ x < Ê\ ~ Ã Ì} _
¿
ºa ¢ ¸ô Ç y è % i Ü ¼ 9, s H Ä »l Ó ü t _ \ P ì r K \ _ K SnO
2~ Ã Ì} _ x 9 ¸ 7 £ x H כ Ü ¼ Ð ó ø Íé ß ) a . XRD 8
£ ¤& ñ õ 800
◦C ü < 900
◦C s © \ " f H & ñ $ í o
Fig. 4. (Color online) Carrier concentrations, electron mobilities, and resistivities of SnO
2thin films annealed from 500 to 1000
◦C.
\ O
H כ ` ¦ Ò q ty , 900
◦C s © \ " f_ ~ Ã Ì} ¿ ºa y è
H ¦ : r \ P % o \ _ ô Ç ³ ð F 7 £ x µ 1 Ï < Ê É r < H © \ _ ô Ç כ Ü
¼ Ð ó ø Íé ß ) a .
Figure 4 H SnO
2~ Ã Ì} \ " f \ P % o : r ¸\ É r H o
#
Q 0 l x ¸, s 1 l x ¸, q $ ½ Ó o Õ ªA á Ôs . \ P % o : r ¸
7 £ x < Ê\ _ 0 l x ¸ H y è H â ¾ Ó` ¦ t
H כ ` ¦ S X % i . \ P % o : r ¸\ _ Ã º H Ã
º ∼10
19/cm
3\ " f ∼10
18/cm
3Ü ¼ Ð 10C & ñ ¸ y è % i
. s ü < ° ú É r 0 l x ¸_ y è H SnO
2_ ~ Ã Ì} _
\
¦ Ò q t$ í r v H í ß è / B N/ B N õ ° ú É r < Ês ¦ : r \ " f \ P % o
H d \ × ¦ # Q× ¼ H כ Ü ¼ Ð ó ø Íé ß ) a .
s
1 l x ¸ H 900
◦C \ " f © Ä ºÃ º % i Ü ¼ 9, s M : s 1 l x ¸
H 4.74 cm
2·V
−1s
−1° ú כ` ¦ t H כ ` ¦ S X % i . 1000
◦