Journal of the Korean Physical Society, Vol. 55, No. 3, September 2009, pp.

1272∼1277

Effect of Deposition Angle on the Optical and the Structural Properties of

Ta2 O5 Thin Films Fabricated by Using Glancing Angle Deposition

K. M. A. Sobahan, Yong Jun Park and Chang Kwon Hwangbo∗

Department of Physics, Inha University, Incheon 402-751

(Received 26 August 2008)

In this paper, the effect of deposition angle on the optical and the structural properties of Ta2 O5
thin films fabricated by using electron beam evaporation with a glancing angle deposition (GLAD)
technique is reported. The refractive index and the porosity at various deposition angles are studied.
We see that the refractive index decreases and the porosity increases with increasing deposition
angle. The calculated in-plane birefringence of GLAD Ta2 O5 films shows a maximum value of 0.04
at a deposition angle of 70◦ . The microstructure and the morphology are also investigated by using
scanning electron microscope (SEM). The cross-sectional SEM images illustrate a highly oriented
microstructure composed of slanted columns and voids due to the shadowing effect and limited
adatom diffusion. Therefore, the glancing angle deposition technique is an original way to control
the columnar microstructure with an enhanced birefringence.

PACS numbers: 77.55.+f, 78.55.Mb, 78.20.-e

Keywords: Glancing angle deposition, Ta2 O5 thin films, Birefringence

I. INTRODUCTION research on account of its remarkable properties, such

as good thermal and chemical stability, excellent trans-
Glancing angle deposition (GLAD) is a sophisticated parency, high refractive index, and compatibility with
physical evaporation technique for fabricating thin films, standard microelectronic processes [15–18]. This ma-
in which oblique angle deposition and substrate rota- terial is widely used in optical waveguides, antireflec-
tion are employed to tailor the columnar microstructures tion coatings, MOS devices, interference filter coatings,
of the thin films with controlled porosity and shapes. and corrosion-resistant protective coatings [19–24]. How-
This technique was first reported in 1959 [1] and later ever, to our best knowledge, no systematic studies have
by others [2–4]. With different ways of the oblique sub- been done on the optical and the structural properties of
strate rotation, a wide variety of microstructures, such Ta2 O5 thin films fabricated by using GLAD technique.
as inclined columns [5], straight pillars [6], helix shapes Hence, there is need to study how varying the depo-
[7], and zigzag shapes [8], can be tailored. Structures sition angle affects the properties of the GLAD Ta2 O5
fabricated using GLAD technique have attracted much films. In this paper, the effect of the deposition angle on
attention in recent years, with many potential appli- the optical and the structural properties of Ta2 O5 thin
cations in microelectronics, magnetic-storage media [9], films fabricated by using GLAD technique is reported.
and flat-panel displays [10], as well as photonic [11] and Various deposition angles were employed to control the
biomedical devices [12] and microsensors [13]. More- microstructure of the films. The refractive index, the
over, the microstructures of the thin films fabricated porosity, and the in-plane birefringence at various de-
by using GLAD induce optical anisotropy [14]. The position angles are described. The microstructure and
degree of this anisotropy strongly depends on the de- morphology were also investigated by using a scanning
position angle, the material, and the deposition condi- electron microscope (SEM).
tions. Based on the optical anisotropy induced by us-
ing the GLAD technique, many researchers have demon-
strated optical retardation plates, anisotropic antire-
II. EXPERIMENTAL PROCEDURE
flection coatings, birefringent omnidirectional reflectors,
three-dimensional photonic band-gap crystals, and so on.
Tantalum pentaoxide (Ta2 O5 ) is an interesting mate- Ta2 O5 thin films were deposited on B270 glass and
rial in fundamental studies and in applications-oriented polished n-Si (100) wafer substrates in an electron-beam
evaporation system by using the GLAD technique. The
∗ E-mail:[email protected]; GLAD technique is detailed elsewhere [25,26] and is il-
Tel: +82-32-860-7657; Fax: +82-32-876-1403 lustrated schematically in Fig. 1. High-purity (99.8%)
-1272-
Effect of Deposition Angle on the Optical and the Structural Properties· · · – K. M. A. Sobahan et al. -1273-

yses, and those deposited on silicon wafers were used

for structural analyses. The transmittance spectra were
measured by using a spectrophotometer (Carry 500, Var-
ian) in the wavelength range from 400 to 800 nm. A
linear polarizer was used to measure the transmittance
spectra in two mutually orthogonal directions: The x-
direction is a projection of the vapor flux’s direction on
the substrate and the y-direction is perpendicular to it,
as illustrated in Fig. 1(b). The refractive index and
the thickness of the films were determined by using an
envelope method. The cross-sectional structure and the
surface morphology of the films were characterized by
using a scanning electron microscope (SEM).

III. RESULTS AND DISCUSSION

1. Optical Characterizations

The transmittance spectra and the effective refractive

indices of the GLAD Ta2 O5 films are plotted as functions
of the deposition angle in Fig. 2. From Fig. 2(a), the
transmittance of these films clearly increases gradually
with increasing deposition angle, and the transmittances
of the films fabricated at deposition angles of 80◦ and
85◦ are higher than that of the substrate. This result
indicates that the Ta2 O5 films deposited by using GLAD
technique are anti-reflectance films at 80◦ and 85◦ .
Figure 2(b) illustrates the effective refractive indices
of the same films, which were calculated based on trans-
mittance spectra by using the envelope method [27].
The dispersion curves at wavelengths of 400 − 800 nm
were fitted by using the Cauchy dispersion equation:
n(λ) = A + B/λ2 + C/λ4 . We found that the effective
refractive index of the Ta2 O5 films decreased as the de-
position angle was increased and at a wavelength of 633
Fig. 1. (a) Schematic diagram of the glancing angle de-
position (GLAD) technique, and (b) vapor flux, column, and
nm, it decreased from 2.05 to 1.42, which is much smaller
growth orientation with angle definitions: α is the deposition than for the corresponding bulk materials (n = 2.2). A
angle, and β is the column angle. similar behavior was observed in TiO2 , ZrO2 , MgF2 , SiO,
and CaF2 films deposited by using the GLAD technique
[25,28–30]. This can be attributed to the porous struc-
Ta2 O5 in the form of a tablet was used as an evaporation ture in the GLAD films, which will inevitably result in a
source. Pre-evaporation of this material was performed decrease in the effective refractive index and an increase
for 5 minutes prior to the main evaporation. The de- in the transmittance. As can been seen in Fig. 2(b),
position was performed in a vacuum chamber at a base at deposition angles of 80◦ and 85◦ , the effective refrac-
pressure of ∼5 × 10−6 Torr. The electron-beam evap- tive indices of the Ta2 O5 films are about 1.46 and 1.42,
oration used a 3-cm crucible pocket located at 45 cm respectively, which are lower than the refractive index
directly beneath the substrate. The deposition rate and of the B270 glass substrate (n = 1.52). Therefore, the
the thickness of the growing films were measured by using GLAD technique can control the refractive index by tai-
a quartz-crystal sensor placed near the substrate. The loring the microstructures of the films, and the films fab-
deposition rate was maintained at 0.5 nm/s. Various de- ricated at high deposition angles are antireflection films
position angles, α (0◦ , 30◦ , 45◦ , 60◦ , 70◦ , 80◦ and 85◦ ), [31].
also known as vapor flux incident angles and defined as The packing density and, hence, the porosity of the
the angle between the incident vapor flux and the sub- GLAD Ta2 O5 films can be calculated based on the
strate surface normal as illustrated in Fig. 1(a), were Bruggeman effective-medium approximation [32]:
employed to control the microstructure. The films de- εA − ε εB − ε
posited on glass substrates were used for optical anal- pA + pB =0 (1)
εA + 2ε εB + 2ε
-1274- Journal of the Korean Physical Society, Vol. 55, No. 3, September 2009

Fig. 2. Optical properties of Ta2 O5 films fabricated at Fig. 3. (a) Porosity and (b) in-plane birefringence of Ta2 O5
various deposition angles: (a) transmittance spectra and (b) films for different deposition angles at 633 nm.
refractive indices.

determined from Tx and Ty , respectively, by using the

where ε, εA , and εB are the dielectric functions of the envelope method. Fig. 3(b) clearly demonstrates the
effective medium, material A, and material B, respec- effect of deposition angle on the in-plane birefringence
tively. The pA and pB represent the packing densities (∆n = ny − nx ) for the GLAD Ta2 O5 films. The in-
of materials A and B, respectively. Fig. 3(a) shows the plane birefringence increases with increasing deposition
porosity of the GLAD Ta2 O5 films as a function of the angle and reaches a maximum value of ∆n = 0.04 at an
deposition angle. From this figure, the porosities of the angle of α = 70◦ . After that, it decreases with the fur-
films in the x- and the y- directions are seen to increase ther increases in the deposition angle. Hodgkinson and
with increasing deposition angle, and the porosity in the Wu [20] also reported the maximum birefringence at α =
x-direction is higher than that in the y-direction. The 70◦ for Ta2 O5 films grown under the serial bideposition
film deposited at α = 0◦ becomes compact; hence, the technique. The films deposited at very high deposition
porosity is very small because the incoming vapor flux angles give rise to a very porous structure, which does
arrives normal to the substrate surface symmetrically. not favor improved optical birefringence.
However, at a deposition angle of 85◦ , the porosity in-
creases to 0.609 in the x-direction and to 0.592 in the
y-direction due to atomic shadowing effects and limited 2. Structural Properties
adatom diffusion.
When the transmittance spectra are measured with
two orthogonal directions of incident linear polarized Scanning electron microscopic cross-sectional images
light, Tx in the x-direction and Ty in the y-direction, of Ta2 O5 films deposited at angles of 0◦ , 30◦ , 70◦ , and
as illustrated in Fig. 1(b), the in-plane birefringence is 85◦ are shown in Figs. 4(a)∼(d). Inspection of the cross-
defined as the difference between the two in-plane refrac- sectional view ensures that the GLAD Ta2 O5 films are
tive indices [33]. The refractive indices nx and ny are composed of slanted columns and inter-columnar gaps
Effect of Deposition Angle on the Optical and the Structural Properties· · · – K. M. A. Sobahan et al. -1275-

Table 1. Deposition, tangent, and column angles of Ta2 O5

films
Deposition angle Calculated column angle Measured column
(deg.) from “Tangent rule” (deg.) angle (deg.)
0 0 0
30 16.1 10
60 40.89 29
70 53.95 37.4
85 80.07 52.6

surface normal and the long axis of the slanted columns,

are measured from the cross-section SEM images. As
can be seen, the inter-columnar gap and the column an-
gles, as well as the column inclination, of the GLAD
Ta2 O5 films increase with increasing deposition angle.
At higher deposition angles, the columns become sepa-
rated and distinguishable. These effects are the result of
the shadowing effect and limited adatom diffusion. Table
1 shows the calculated and the measured values of the
columnar angles for the Ta2 O5 films deposited at various
deposition angles. The column angle, β, is well known
to be less than the deposition angle, α, and to follow the
empirical tangent rule, tan β = (1/2)tanα [34]. However,
the measured columnar angles in our experiment deviate
from the empirical tangent rule, as summarized in Table
1. Thus, a modified tangent rule, tan (β/C) = (1/2)tanα
[28], is used, where C is a parameter that depends on the
materials and the deposition conditions. The parameter
C for the Ta2 O5 films in our experiment was found to
be 0.69, which is smaller than the C = 1.0 for the em-
pirical tangent rule. The highly-oriented nanostructure
of the slanted columns indicates that the GLAD Ta2 O5
films are anisotropic [35], with the long axis parallel to
the columnar growth direction. The anisotropic struc-
ture will introduce an anisotropic dependence into the
thermal, electrical, magnetic, and optical properties of
thin films [36].
The surface morphologies of the Ta2 O5 films deposited
at angles of 0◦ , 70◦ , and 85◦ are presented in Fig. 5. As
can be seen in Fig. 5(a), the surface of the film deposited
at 0◦ is smooth, but the pinholes and many voids are
observed in the case of the films deposited at angles of 70◦
and 85◦ , as shown in Figs. 5(b) and (c), respectively, and
they increase with increasing deposition angle. Higher
deposition angles lead to pinholes and many voids in the
surface, larger column angles, larger separations between
Fig. 4. Cross-sectional SEM images of Ta2 O5 films fabri- neighboring columns, and highly porous thin films. The
cated at various deposition angles: (a) α = 0◦ , (b) α = 30◦ , shapes of the voids on the film’s surface also appear to be
(c) α = 70◦ , and (d) α = 85◦ . asymmetric in the x- and the y-directions, and the voids
in the x-direction are more porous. This result shows
good agreement with the result of Fig. 3(a) in which the
porosity increases with increasing deposition angle due
(voids). The columns are also seen to be inclined towards to shadow effect, and the porosity in the x-direction is
the direction of the incoming vapor flux. The column higher than that in the y-direction. It also implies that
angles (β), defined as the angle between the substrate the structural asymmetry of columns and voids induces
-1276- Journal of the Korean Physical Society, Vol. 55, No. 3, September 2009

the maximum value is found 0.04 at a deposition angle

of 70◦ . Examination of SEM images reveals that the
GLAD Ta2 O5 films are highly-oriented nanostructures
composed of slanted columns separated by voids. We
also find that the column angle increases with increasing
deposition angle. The voids and the pinholes observed on
the surfaces of the films are asymmetric in the x- and the
y-directions and increase with increasing deposition an-
gle. These results indicate that glancing angle deposition
is an effective technique for controlling the microstruc-
tures and, hence, the optical properties of Ta2 O5 films.

ACKNOWLEDGMENT

This work was supported by Inha University Research

grant.

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