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Zn-doped CuAlS

transparent p-type conductive thin ﬁlms deposited

by pulsed plasma deposition

Ming Yang, Yinghua Wang, Guifeng Li, Zhan Shi, and Qun Zhang

a兲

Department of Materials Science, Fudan University, 220 Han-Dan Road, Shanghai 200433,

People’s Republic of China

共Received 27 March 2009; accepted 14 September 2009; published 14 October 2009兲

CuAl

0.90

0.10

thin ﬁlms were deposited by pulsed plasma deposition. The dependence of

structural, surface morphology, electrical, and optical properties of the ﬁlms on substrate

temperature was investigated. X-ray diffraction patterns reveal that the ﬁlm be amorphous structure.

The electrical properties are sensitive to the substrate temperature. A typical sample with

conductivity of 50.9 S cm

−1

, carrier mobility of 3.13 cm

−1

, carrier concentration of 1.41

⫻10

−3

, and average transmission of 74% in visible range of 400–700 nm was obtained. A

transparent p-CuAlS

:Zn/ n-In

:W heterogeneous diode was also fabricated and exhibits

rectifying current-voltage characteristics. The ratio of forward current to the reverse current exceeds

80 within the range of applied voltages of −3.0–+3.0 V and the turn-on voltage is approximately

I. INTRODUCTION

p-type transparent conductive oxide 共 p-TCO兲 thin ﬁlms

have attracted interest in the emerging ﬁeld of “transparent

electronics.”

Recently, a series of p-TCOs such as delafos-

site CuMO

共M =Al, Cr, Ga, In, Sc, Y, B兲,

2–8

SrCu

ox-

ysulﬁdes of LaCuOCh 共Ch= S, Se兲,

10,11

binary oxides of

NiO,

codoped p-ZnO,

13–15

etc., have been reported with

various deposition techniques. However, although p-type

conductivity has already been demonstrated in these wide

band gap oxide semiconductors, the rather low value 共mostly

⬃1Scm

−1

兲 is still not high enough to match that of com-

mercially used n-TCOs 共

␴

⬎10

Scm

−1

兲 nowadays, which

greatly limits their application in active semiconductor de-

vices, where the pn junction is a key structure. It is needed to

explore novel material systems other than the oxides to get

improved conductivity. Sulﬁdes have been studied as a

promising candidate in recent years. Park et al.

found the

higher covalency of the Cu–S interactions in BaCu

rela-

tive to the Cu–O interactions in the oxides. Higher covalency

is expected to lead to broader bands, smaller effective

masses, hence higher mobility and smaller dopant ionization

energies, which could effectively improve the hole conduc-

tivity. Huang et al. focused on another kind of sulﬁde

CuAlS

, which has a chalcopyrite structure and a superlattice

of the zinc blende, with a wide band gap of ⬃3.5 eV. It

contains an ordered tetrahedral array of ﬂattened CuS

and

undistorted AlS

. This tetrahedral symmetry and the associ-

ated crystal-ﬁeld splitting impart a strong Cu 3d and S 3p

hybridization at the valence band maximum 共VBM兲. Mean-

while, the distortion of CuS

causes dispersion at the VBM,

which facilitates hole conduction.

The bulk of Zn-doped

CuAlS

had been studied and the thin ﬁlm had been tried to

be prepared.

For further research, the detailed investiga-

tions on the ﬁlm properties are required.

In this article, Zn-doped CuAlS

thin ﬁlms were prepared

using the pulsed plasma deposition

共PPD兲 method. The de-

pendence of structural, surface morphology, electrical, and

optical properties of the ﬁlms on the substrate temperature

was studied. A transparent heterojunction diode of

p-CuAlS

:Zn/ n-In

:W 共IWO兲 was also fabricated and

the current-voltage 共I-V兲 curve was characterized.

II. EXPERIMENTAL DETAILS

CuAl

0.90

0.10

ceramic target was provided by Liu et

al.

The ﬁlms were prepared using a PPD system 共previ-

ously called CSA,

Organic Spintronics Corporation, Italy兲.

The vacuum chamber was evacuated down to a pressure of

1⫻10

−2

Pa prior to deposition. The ﬁlms with about 200 nm

were deposited on glass substrates in Ar 共99.99%兲 ambient.

The glass substrate was cleaned in pure water, alcohol, and

acetone for 20 min in an ultrasonic bath, respectively. The

working pressure was maintained at 2.4 Pa during ﬁlm depo-

sition. The discharge gas type was chosen as Ar. High volt-

age dc power supply 共HCL 140-20000兲 was used to provide

the high accelerating voltage. The voltage and current were

set at 18.0 kV and 4.8 mA, respectively. Thus the strength of

electrical ﬁeld between the trigger 共⬃0V兲 and hollow cath-

ode 共⬃18 kV兲 is estimated to be 10

V/ m, while that be-

tween the cathode and target is also about 2⫻10

V/ m. The

acceleration quartz tube has a diameter of 2 mm and a length

of 10 cm. The extracted electron current density was in the

order of 1 A / cm

. The distance between the end of tube and

surface center of target was about 4 mm.

The full width at

half maximum of the pulse was about 100 ns.

The substrate

was heated from 300 to 500 °C by an infrared lamp and the

temperature was measured by a thermocouple 共Eliwell

EWTQ 915, Invensys, Italy兲. More details about PPD work-

ing principles could reference early reports by Witke et al.

X-ray diffraction 共XRD兲 patterns of the samples were ob-

tained 共Rigaku D/Max–2550 V兲 using Cu K

␣

radiation 共␭

=0.154 18 nm兲. The surface morphology was measured us-

a兲

Electronic mail: zhangqun@fudan.edu.cn

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