1) Effect of polarization on the charge transport in ferroelectric capacitors

One important problem in the case of ferroelectric capacitors, used for microelectronic
applications, is the presence of the dc leakage current (LC). Minimization of LC in
devices used for nonvolatile memories is one hot topic in the field of ferroelectrics.
However, this problem cannot be solved without understanding the conduction
mechanisms leading to the presence of LC in ferroelectric capacitors. This is closely
related with the problem of the interface with the metal electrodes. Traditionally,
ferroelectric materials were regarded as insulating, from the point of view of electrical
conductivity, meaning that the electrodes show an ohmic-like behavior and that the LC is
dominated by the bulk mechanisms like: ohmic conduction, space charge limited currents
(SCLC), or even hopping. More recently, with the enhancement of the deposition
techniques and the possibility to grow very high quality epitaxial films, the insulating
nature of the ferroelectrics became questionable. Many of the experimental results
support the presence of a Schottky-type contact at the ferroelectric-electrode interface,
pointing towards interface controlled conduction mechanisms. The main candidate is the
thermionic emission or Schottky emission over the potential barrier. There are two
possible cases: classic thermionic emission, when the mean free path of the injected
electron is longer than the film thickness, and the bulk-mediated thermionic emission
(drift-diffusion theory), when the mean free path is shorter than the film thickness. The
electron mobility plays an important parameter in the last case.
No matter it is bulk-mediated or not, the important question is: how the polarization
charge, located near the interface, is affecting the charge injection in ferroelectric
capacitors? In order to answer this question we have performed an extended
investigation of conduction mechanisms in epitaxial quality PZT films. The samples were
grown by PLD in collaboration with Max Planck Institute from Halle, Germany [1]. By
the careful manipulation of the deposition parameters it was possible to grow films free
of any extended structural defects, as shown in the inset of figure 1. The current-voltage
characteristics were measured on a wide temperature range and it was found that the
leakage current obeys the following equation:
⎛ 2πmeff kT ⎞
3/ 2
⎛ q ⎛ qE m ⎞⎟ ⎞⎟
⎜
J = 2q ⎜ ⎟ μE exp ⎜− ⎜Φ0 − (1)
h2 ⎟ ⎜ kT ⎜ B
4πε 0 ε op ⎟⎠ ⎟
⎝ ⎠ ⎝ ⎝ ⎠
Here, Em is the maximum field at the reverse-biased Schottky-like contact, considering
also the presence of the polarization charge P [2,3]:
2qN eff V P
Em = + (2)
ε 0ε st ε 0ε st
Considering that the last term in (2) is much larger than the first term (large polarization,
low dielectric constant [4]), it can be shown that the current density is given by:
⎛ 2πmeff kT ⎞
3/ 2 ⎛ q ⎡⎛ qP ⎞ 2q 2 N eff V ⎤ ⎞⎟
J ~ 2q⎜⎜ ⎟⎟ μE exp −⎜ ⎢⎜ ⎟ ⎥
⎜⎜ kT ⎢⎜ Φ B − 4πε 2 ε ε ⎟ − 8πε ε P ⎥ ⎟⎟
0
(3)
⎝ h2 ⎠ ⎝ ⎣⎝ 0 op st ⎠ 0 op
⎦⎠
It can be seen that the polarization contributes with a supplementary reduction of the
potential barrier at zero field. The apparent value is given by:
 ⎡⎛ qP ⎞ 2q 2 N eff V ⎤
Φ B ,app = ⎢⎜ Φ 0B − ⎟− ⎥ (4)
⎢⎜⎝ 4πε 02 ε op ε st ⎟
⎠ 8πε ε P ⎥
⎣ 0 op
⎦

Fig. 1 The current-voltage (I-V)

characteristics for an epitaxial
PZT film grown on a single
crystal SrTiO3 substrate. The
bottom electrode was epitaxial
SrRuO3, and the top electrode
was Pt. The measurements were
performed at different
temperatures (10 K steps)
between 10 K and 360 K. The
inset shows a cross-section TEM
picture before the Pt deposition.

Indeed, from the experimental data (see Fig. 2), a potential barrier of only 0.12 eV is
obtained. This barrier becomes 0.95 eV after making the polarization correction (P is
about 100 μC/cm2 and the static dielectric constant is 80 [4]). This result shows that the
ferroelectric polarization can have a significant impact on the formation of the potential
barrier at the metal-ferroelectric interface.

Fig. 2 The V1/2 dependence of the apparent

potential barrier, as predicted by the
equation (4). The points on the graph were
obtained from the reprezentation.
⎛ J ⎞ ⎛ ⎛ 2πmeff k ⎞ 3 / 2 ⎞ q ⎛ qEm ⎞
Ln⎜ 3 / 2 ⎟ = Ln⎜ 2q⎜⎜ ⎟⎟ μE ⎟ − ⎜Φ0 − ⎟
⎝ T ⎠ ⎜ h 2 ⎟ kT ⎜ B
4πε 0 ε op
⎟
⎝ ⎝ ⎠ ⎠ ⎝ ⎠

[1] Intrinsic ferroelectric properties of strained tetragonal PbZr0.2Ti0.8O3 obtained on layer-by-

layer grown, defect-free single-crystalline films ; Vrejoiu I, Le Rhun G, Pintilie L, Hesse D,
Alexe M, Goesele U, ADVANCED MATERIALS 18 (13): 1657 (2006)
[2] Metal-ferroelectric-metal heterostructures with Schottky contacts. I. Influence of the
ferroelectric properties; Pintilie L, Alexe M, JOURNAL OF APPLIED PHYSICS 98
(12): 123103 (2005)
[3] Ferroelectric polarization-leakage current relation in high quality epitaxial Pb(Zr,
Ti)O3 films; Pintilie L, Vrejoiu I, Hesse D, LeRhun G, Alexe M, PHYSICAL REVIEW
B 75 (10): 104103 (2007)
[4] Extrinsic contributions to the apparent thickness dependence of the dielectric
constant in epitaxial Pb(Zr,Ti)O3 thin films; L. Pintilie, I. Vrejoiu, D. Hesse, G. LeRhun,
and M. Alexe, PHYS. REV. B 75, 224113 (2007)