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46713-B10
Exploring Defect Level Position and Occupation in Metamorphic Heterostructures for Multi-junction Photovoltaic Converters
Timothy H. Gfroerer, Davidson College
Technological improvement of the conversion efficiency in
state-of-the-art high efficiency solar cells depends, in part, on the development
and refinement of high-bandgap alloys that can be grown on GaAs
substrates.� The bandgap in alloys like
GaAsP and GaInP can be tuned to match design parameters that capitalize on the
power available in the high-energy portion of the solar spectrum.� However, the atomic spacing in these crystals
differs from that of the underlying GaAs, so a higher concentration of
crystalline defects is expected in GaAsP and GaInP epilayers.� These defects impair solar cell performance
by providing new pathways for photo-excited charge carriers to recombine rather
than generate electricity.
At Davidson College, we are using
three different experimental techniques to characterize defects in GaAsP and
GaInP.� In the first, we use
spatially-integrated measurements of photoluminescence spectra and radiative
efficiency to investigate collective properties of defect-related
transitions.� In the second, we use
transient capacitance measurements to explore transport into and out of
defect-related states.� And in the third,
which is a new experiment for us in 2008, we use a digital CCD camera to obtain
photoluminescence images showing the defect distribution and carrier depletion
via recombination at defects.

I.� Photoluminescence spectra from 1.75eV GaAsP
are shown in Figure 1.� The broad
defect-related (D-R) peak below the band-to-band (B-B) emission indicates that
radiative recombination is occurring through relatively shallow defect levels
in this alloy.� At higher temperatures
these transitions become nonradiative and, with increasing temperature, the
defect states become thermally depleted.�
Analysis of the radiative efficiency (the radiative divided by the total
recombination rate) provides further evidence that a broad band of shallow
states exists in this material.� Running
a rigorous computational algorithm to minimize the error between experimental
measurements and theoretical predictions of radiative efficiency vs. photo-excitation
produces the results shown in Figure 2.�
The inset graph shows the computer-generated density of states (DOS)
distribution between the valence and conduction band edges (Ev
and Ec).�
We find that a high density of defect levels just below Ec is required to obtain the best fit.
II. Transient
capacitance measurements on diodes during and after the application of a bias
pulse can be used to monitor the capture and emission of carriers into and out
of defect-related traps.�
Representative
transients on devices incorporating 1.75eV GaAsP are shown in Figure 3.� The capture and escape response deviates
strongly from conventional exponential behavior.� Such non-exponential behavior is often
attributed to the presence of a broad band of defect energies, with shallow
levels emptying quickly at early times and slower deeper levels contributing at
later times.� However, with
non-exponential behavior occurring during both the introduction and exclusion of
carriers from the depletion region, we assign the behavior to anomalous
transport rather than the filling and thermally-activated emptying of defect
states.� For example, if carriers are
hopping between defect sites, quick motion would be expected between nearby
sites, while slower motion would occur during more distant hops.� We fit the temperature-dependent response to
the stretched exponential function shown in the graph, holding the stretching
parameter d and amplitude A fixed.� Arrhenius plots of the resulting capture and
emission rates (k) are linear and
yield comparable capture and escape activation energies (see Figure 4),
providing further evidence for the transport-limited interpretation noted
above.� Indeed, we also observe a
thermally-activated, stretched-exponential response in 2.0eV GaInP, suggesting
that the simultaneous incorporation of Gallium and Phosphorous may be
responsible for this effect.
III. This summer, we undertook a new
experiment to image the photoluminescence generated by these materials using a
high-sensitivity CCD camera.� We observed
striking spatial inhomogeneity in the luminescence
brightness, even in nominally lattice-matched GaAs.� We also noted that the size of the
defect-related features depends strongly on the laser excitation intensity (see
Figure 5). ��At low density, carriers
diffuse more readily to defective regions rather than recombining radiatively, producing larger effective �dead� areas.� We model the behavior by assigning a large
defect recombination rate to the defect position and allowing diffusion to
control the density of carriers in adjacent regions (see Figure 6).� The results are consistent with our
observations, but a more sophisticated model will be required to achieve better
quantitative agreement with experiment.�
At this stage, we can conclude that (1) if the defect recombination rate
is non-uniform throughout the sample, diffusion will contribute to a reduction
in net efficiency and (2) even for high-quality semiconductors with few
defects, diffusion can lead to significant defect recombination at low
excitation intensity.� Preliminary images
from GaAsP grown lattice-mismatched on GaAs suggest that a hypothetical network
of defective pixels will be required to reconcile our diffusion-limited model
with experiment.� Since the defect
concentration in these structures is much higher, we expect photo-excited
carriers to find defects more readily, raising the photo-excitation intensity
threshold for good solar cell performance.
�
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