Increasing Fluorescent Concentrator Light Collection Efficiency by

Restricting the Angular Emission Characteristic of the Incorporated

Luminescent Material - the “Nano-Fluko” Concept
J.C. Goldschmidt*
, M. Peters
, J. Gutmann
, L. Steidl
, R. Zentel
, B. Bläsi
, M. Hermle
a
a
a
b
b
a
a
Fraunhofer Institute for Solar Energy Systems ISE, Heidenhofstr. 2, 79110 Freiburg, Germany
a
Institut für Organische Chemie, Universität Mainz, Duesberweg 10-14, 55128 Mainz, Germany
b
ABSTRACT
Fluorescent concentrators concentrate both diffuse and direct radiation without requiring tracking of the sun. In
fluorescent concentrators, luminescent materials embedded in a transparent matrix absorb sunlight and emit radiation
with a different wavelength. Total internal reflection traps the emitted light and guides it to solar cells attached to the
concentrator’s edges. The escape cone of total internal reflection, however, limits the light collection efficiency.
Spectrally selective photonic structures, which transmit light in the ab sorption range of the luminescent material and
reflect the emitted light, reduce these losses. In this paper, we review different realizations of such structures and show
th at they increase collection efficiency by 20%. However, light emitted into steep angles in respect to the front surface,
which would be lost without the photonic structures, has a very long effective path inside the concentrator until it reaches
a solar cell. Therefore it suffers from path length dependent losses. We discuss how emission into the unfavorable
directions can be suppressed by integrating the luminescent material into photonic structures, thus reducing these losses.
We present possible realizations both for the concentrator design and for the solar cells used in such systems.
Keywords:
Solar energy, Photovoltaics, Concentrators, Fluorescent concentrators, photonic crystals
1.
INTRODUCTION
Fluorescent concentrators are a special type of light concentrating device. The underlying principle was first used in
scintillation counters
and then their application to concentrate solar radiation was proposed in the late 1970s
. In a
1, 2
3, 4
fluorescent collector, a luminescent material embedded in a transparent matrix absorbs sunlight and emits radiation with
a different wavelen gth. Total internal reflection traps most of the emitted light and guides it to the edges of the collector
(Figure 1). Solar cells op tically coup led to the edges convert this light into electricity.
Fluorescent concentrators are able to concentrate both direct and diffuse radiation. A geometric concentration is
achieved, if the area of the solar cell at the edges is smaller than the illuminated front surface of the collector, i.e. when
th e area from which light is collected is larger than the solar cell area. The ability to concentrate diffuse radiation
presents a great advantage for the application of fluorescent concentrators in temperate climates, such as in middle
Europe, or in indoor applications with relatively high fractions of diffuse radiation. Additionally, fluorescent
concentrators do not require tracking systems that follow the path of the sun, in contrast to concentrator systems that use
lenses or mirrors. This facilitates, for instance, the integration of fluorescent concentrators in buildings.
Fluorescent concen trators were investigated intensively in the early 1980s
. Research at that time aimed at cutting
5, 6
costs by using the concentrator to reduce the need for expensive solar cells. After 20 years of progress in the
development of solar cells and luminescent materials, and with new concepts, several groups such as those of Refs.
7-2 7
are currently reinvestigating the potential of fluorescent concentrators. High efficiencies have been achieved
and
7, 1 0, 24
there has been also considerable progress in the understanding and theoretical description, e.g.
. However,
7 , 8, 12, 27, 28
efficiencies are still too low and system sizes too small for a co mmercial application.
*jan.christoph.goldschmidt@ise.fraunhofer.de, Tel +49 761 4588 5475, www.ise.fraunhofer.de
Photonics for Solar Energy Systems III, edited by Ralf B. Wehrspohn, Andreas Gombert, Proc. of SPIE
Vol. 7725, 77250S · © 2010 SPIE · CCC code: 0277-786X/10/$18 · doi: 10.1117/12.854278
Proc. of SPIE Vol. 7725 77250S-1
Figure 1: Working principle of a fluorescent concentrator (lef). A luminescent material in a matrix absorbs incoming
sunlight (E
) and emits radiation with a different energy (E
). Total internal reflection traps most of the emitted light
1
2
and guides it to solar cells optically coupled to the edges. Emitted light that impinges on the internal surface with an
angle steeper than the critical angle
is lost due to the escape cone of total internal reflection. A part of the emitted
c
light is also re-absorbed, which can be followed by re-emission. On the right, it is shown how the escape cone losses
can be reduced: a selective reflector, realized as a photonic structure, acts as a band stop reflection filter. It allows light
in the absorption range of the dyes to enter the collectors, but reflects light in the emission range.
1.1
Escape cone losses
One fundamental problem limitin g the collection efficiency of fluorescent concentrators is the escape cone of total
internal reflection. All light that impinges on the internal surface with an angle smaller than the critical angle
(
)
c
emit
leaves the collector and is lost (Figure 1 left). The critical angle is given by
1
() ()
. (1)
=
arcsin
c
n
emi t

Integration gives a fraction

() ( )
=
1
-
n
-
2
(2)
t r ap
e mi t
of the emitted photon flux that is trapped in the collector
. For PMMA (Polymethylmethacrylate) with approx.
n
= 1.5,
29
this results in a trapped fraction of around 74%, which means that a fraction of around 26% is lost after every emission
process. The 26% account for the losses through both surfaces. An attached mirror does not change this number, as with
a mirror the light leaves the collector through the front surface after being reflected. The loss of around 26% does not
only occur once, but after every re-absorption and subsequent re-emission.
On the other hand , the Stokes shift between absorption and emission opens the opportunity to reduce these losses
significantly: a selective reflector, which transmits the light in the absorp tion range of the luminescent material and
reflects the emitted light, would trap nearly all the emitted light inside the collector
. The concept is illustrated in Figure
30
1 on the right. There are several ways to realize such selective reflectors. For instance, in
hot mirrors were proposed to
17
serve as selective reflectors and in
photonic structures. In the fist part of the paper, we will show experimental results
18
on how different photonic structures affect the efficiency of fluorescent concentrator systems.
Even with photonic structures, however, light emitted into the former escape cone is more frequently subject to loss
events. This light is emitted into steep angles in respect to the front surface. Therefore it has a very long effective path
inside the concentrator until it reaches a solar cell. In consequence, it suffers quite strongly from path length dependent
losses, such as re-absorption by the dye, absorption in the matrix, scattering etc. In the second part of the paper, we
discuss integration of the luminescent material into photonic structures that suppress emission into the unfavorable
directions to reduce these losses. We present possible realizations both for th e concentrator design as well as for the solar
cells that are to be used in such systems.
Proc. of SPIE Vol. 7725 77250S-2
2.
REDUCING ESCAPE CONE LOSSES WITH PHOTONIC STRUCTURES
2.1
Multilayer system
To reduce the escape cone losses, a selective reflector is necessary that shows a high transmission in the absorption range
of the luminescent material and high reflection in the emission range. A possible realization of such a selective reflector
is a so-called Rugate filter. It features a continuously varying refractive index profile that results in a single reflection
peak. However, some unwanted side lobes remain. Optimized Rugate filters
show only one single reflection peak for a
certain wavelength and almost no other reflectio ns. In this work, such optimized Rugate filters are used, which were
an d they were optimized for
produced at the company mso-jena by Ion-Assisted-Deposition (IAD. Their size is 5x5cm
th e used dye material. The filters had an antireflection coating adapted to the absorptio n range of the used dye. The used
material is denoted BA241 and was develop during the first research period in the 1980s
The reflection of the filter,
the absorption and the photoluminescence of the BA241fluorescent concentrator are shown in Figure 2. The filter
transmits the light in the absorption range of the dye and it reflects the emitted light and therefore has exactly the desired
properties.
Figure 2: Reflection spectrum of the used photonic structure and the absorption and photoluminescence of the fluorescent
concentrator the filter was designed for. The reflection of the structure very nicely fits the emission peak of the dye in
the concentrator.
To investigate how the filter increases the light guiding efficiency of the concentrators we attached a 21 x 3 mm
GaInP
2
solar cell on one rim of a 3 mm thick fluorescent concentrator with a size of 2 x 6 cm
(the cell was attached to the 2 cm
rim). A white BaSO
bottom reflector was placed under the system and the EQE of the system was measured, with and
4
with out the filter on top. During the EQE measurement, the system was illuminated with a 3 mm wide spot in 1 cm
distance to the solar cell. Figure 3 sh ows the comparison of the two measurements and additionally the reflection of the
filter. Obviously the filter reduces the efficiency in the region where it is reflective, which is the case for the wan ted
reflection above 550 nm and also for the unwanted reflection below 380 nm. On the other hand, the filter increases
efficiency significantly over a broad spectral range, because it traps the emitted light.
We also realized a system with a 5 mm thick, 5 x 10 cm
fluorescent concentrator to which one GaInP solar cell was
2
coupled with silico ne. The solar cell had an active area of 5 x 49 mm
.
Hence the relation between illuminated
2
fluorescent concentrator area and solar cell area constitutes a geometric concentration ratio of 20x. The so lar cell had an
efficiency of 16.7% under AM1.5g illumination. White PTFE served as bottom reflector and also as reflector at the
edges that were not covered by solar cells. Without the filter this system had an efficiency of 2.6±0.1% (uncertainty is
for relative comparison) in reference to the 50 cm
area of the system. The filter increased the efficiency to 3.1±0.1%,
2
which constitutes an efficiency increase of around 20% relative. With the achieved efficiency of 3.1% and the
concentration ratio of 20, the realized fluorescent concentrator produces about 3.7 times more energy than the GaInP
solar cell had produced on its own.
Proc. of SPIE Vol. 7725 77250S-3
Figure 3: External Quantum Efficiency (EQE) measurement of a system with a GaInP solar cell attached to a fluorescent
collector of 3 mm thickness made from BA241 under which a BaSO
bottom reflector was placed with and without a
4
photonic structure on top of the collector. Additionally the reflection of the photonic structure is shown. The efficiency
is increased significantly over a broad spectral range, because more emitted light is trapped and guided to the sides.
Figure 4 shows the spatially resolved light collection efficiency as it was measured with a Light Beam Induced Current
(LBIC) setup on this system with a photonic structure on top. One can see that the collection efficiency is highest close
to the solar cell. The efficiency drops with increasing distance to the solar cell and closer to the solar cell free edges.
Interestingly, the collection efficiency increases as well close to the edge opposite the solar cell. This effect was observed
in different systems of varying sizes. Therefore it cannot be considered a simple measurement artifact. Very likely, light
outside the absorption range of the dye is somehow redirected to the solar cell by the bottom and the edge reflector, or by
the actual edge of the collector. However, a precise explanation is yet to be developed.
Figure 4: Light Beam Induced Current (LBIC) scan of the 10 x 5 cm
sample described above. A photonic structure was
2
placed on top of the fluorescent concentrator during the measurement. A white reflector made from PTFE was placed at
the bottom and the edges without solar cells. The edge with the attached solar cell is located at the right in this picture.
Not the full collector area was scanned to avoid contact of the scanning head with the wiring of the system. One can see
that the collection efficiency is highest close to the solar cell. The efficiency drops with increasing distance to the solar
cell and closer to the edges.
Proc. of SPIE Vol. 7725 77250S-4
Figure 5: Averaged linescans in x-direction from an LBIC scan with and without photonic structure. Close to the solar cell
the efficiency is lower with the photonic structure, because it reduces the effectiveness of the bottom reflector for small
distances. Over most of the fluorescent concentrator, however, collection efficiency is significantly higher with a
photonic structure, resulting in a relative efficiency increase of 20%.
Figure 5 compares the averaged linescans in the x-direction of the LBIC scan shown in Figure 4 and of a scan without
photonic structure. The average was taken from 1.25 to 2.5 cm in the y-direction. Close to the solar cell the efficiency is
lo wer with the photonic structure. The reason is that light, which enters the collector close to the solar cell, can be
reflected directly to the solar cell by the bottom reflector. This absorption-less light collection works as well for the light
outside the absorption range of the dye, which is still in the spectral region that can be used by the solar cell. This light
outside the absorption range, however, is blocked by the photonic structure. Nevertheless, over most of the fluorescent
concentrator, collection efficiency is significantly higher with a photonic structure, resulting in the relative efficiency
increase of 20%. This is a clear demonstration of how photonic structures can help to increase the collection efficiencies
of larger fluorescent concentrator systems.
2.2
Opaline systems
The efficiency increase of 20% is already a great success since it shows that photonic structures reduce the escape cone
lo sses sign ificantly. However, the used filter is a multilayer system and therefore costly to produce. Three-dimensional
photonic structures are a potential alternative to the presented multilayer systems. A special three-dimensional photonic
structure is the opal. The opal has the advantage that it can be produced by a dip -coating process utilizing self-
organization of mono-disperse PMMA beads (Figure 6)
. This is a potentially low-cost process that could be applied on
32
large area concentrators.
Producing opaline films of high quality directly on the PMMA o f the fluorescent collector is difficult, since the PMMA
surface is hydrophobic. However, the surface can be made hydrophilic by an oxygen plasma treatment. An alternative
approach is producing the opaline film on a sacrifice layer and transferring the film to the fluorescent concentrator.
To investigate the effect of the opal on the collection efficiency of the fluorescent concentrator, an opaline film with
properties adapted to the BA241 material was produced on a glass substrate. The diameter of the PMMA beads was
256 nm and around 50 layers of beads were deposited on the glass. The reflection of the opal on the glass is shown in
Figure 7 in comparison to the absorption and fluorescence of the dye.
The sample was placed on top of a 2 cm x 2 cm sample of BA241 with one GaInP solar cell attached to one edge. Under
the bottom and around the free edges white PTFE reflectors were placed. The efficiency was determined with and
with out the opal on top. Without the photonic structure the efficiency was 3.3%, but dropped with the opal on top to
3.0%. The reasons for this drop are that for one there is more than 10% unwanted reflection in the absorption range of
th e dye, wh ich causes sev ere losses. This unwanted reflection is mostly caused by stacking faults that cause scattering.
Proc. of SPIE Vol. 7725 77250S-5
Second, the reflection peak in the emission region of the dye is not perfectly aligned to the emission spectrum. Moreover,
the reflection only peaks at around 70%. Therefo re not all the light emitted into the escape cone is reflected back into the
concentrator
The reflection can be increased with depositing opaline films with more layers of PMMA beads and by reducing the
stacking faults. A reduction of stacking fault would result in a reduction of the unwanted reflection as well. However,
increasing the number of layers makes a stacking fault-free assembly of the beads less likely. In consequence, progress in
th e preparation of the film is necessary, to make it technologically viable to deposit opaline photonic structures on large
area fluorescent concentrators.
Figure 6:
SEM image of an opaline film produced by the self-organization of mono-disperse PMMA beads. This film was
produced on a sacrifice layer so it could be transferred to a fluorescent concentrator later on.
Figure 7:
The reflection of an opaline film made of 256 nm PMMA beads in comparison to the absorption and emission of
the fluorescent concentrator. Up to now, the reflection peak of the photonic structure at the emission wavelengths of the
dye is not high enough to over-compensate the losses due to the reflection of the photonic structure in the absorption
range of the dye
2.3
Next steps
To successfully reduce escape cone losses of fluorescent concentrators with photonic structures in a commercial
application, the most important task is to find a low-cost process to produce high-quality structures. Furthermore, the
photonic structures shou ld be deposited d irectly on to the fluorescent concentrators. This reduces the number of
boundaries and therefore unwanted reflections. With an adequate design, the photonic structures can act as an
antireflection coating in the absorp tion range of the dye and as reflector for the emitted radiation at the same time. In this
configuration, reflection and escape cone losses are reduced simultaneously. But also even more radical photonic
concepts are possible, as we will discuss in the following section.
Proc. of SPIE Vol. 7725 77250S-6
3.
RESTRICTING THE ANGULAR EMISSION
We have seen before that photonic structures reduce the escape cone losses. However, even with a photonic structure,
light emitted into the escape cone is more frequently subject to loss events. Because it is emitted into a steep angle in
respect to the front surface, it has a very long effective path until it reaches a solar cell, and therefore suffers more from
path length dependent losses. Hence, it would be very beneficial to suppress emission into these unfavorable directions
completely. This shou ld as well be po ssible with the help of photo nic structures. Already the very first works on
and Yablonovitch
dealt with influencing emission with photonic structures. Many papers
photonic crystals of Bykov
33
34
discussed the possibilities subsequently
. For influencing the emission of the dye su ccessfully, it is necessary that the
35 -41
photonic structures are very close to the emission process or that the luminescent material is incorporated into the
photonic structures. For the fluorescent concentrator systems this means that one has to go from the macroscopic design
of the presented systems to a system design we denote “Nano-Fluko”.
Figure 8: Conceptual sketch of a “Nano-Fluko”. A very thin layer of luminescent material with thickness t in the range of
wavelength
of the emitted light is placed between two photonic structures, e.g. Bragg stacks. The photonic structures
transmit light in the absorption range of the luminescent material with an energy E
. They are reflective in the emission
1
region (E
) of the luminescent material. Because the layer with the luminescent material is so thin, the photonic
2
structures suppress the emission into unfavorable directions.
One possible realization of such a “Nano-Fluko” would be a very thin layer of luminescent material between two
photonic structures, e.g. Rugate filters or Bragg stack s (Figure 8). In such a configuration, the emission of the light
would b e restricted to a plane parallel to the photonic structure. Galli et al. showed that the emission of Er
can be
3+
strongly enhanced, if it is incorporated in a photonic crystal waveguide and that efficient waveguiding occurs
.
4 2, 43
Therefore there is first experimental evidence that such a system can work, and it is an interesting approach to apply this
concept to fluorescent concentrators.
Another realization could be a photonic crystal fiber doped with a luminescent material (Figure 9). However, to design
th e photonic structure around the fiber with the right spectral selectivity will be a deman ding task. On the other hand,
such a realization would enable very interesting application opportunities. For instance, the fibers could be woven into a
flexible fabric with the properties of a fluorescent concentrator.
Proc. of SPIE Vol. 7725 77250S-7
Figure 9: Alternative realization of a “Nano-Fluko”. The luminescent material is incorporated into a photonic crystal fiber. If
the photonic shell is designed with the right spectral selectivity, the fiber could accept light in the absorption range (E
)
1
of the luminescent material from all directions. Emission with energies (E
) would be restricted to the direction of the
2
fiber.
Probably a more realistic option is to incorporate the luminescent material d irectly into th e p ho tonic structure. This could
be done for example with an opaline film made from PMMA beads that incorporate much smaller luminescent
nanocrystals (Figure 10). If the optical band-gap in the emission range of the dye is incomplete, emission into certain
directions is allowed and effective light guiding occurs.
Figure 10: Sketch of “Nano-Fluko” realized by incorporation of the luminescent material directly into the photonic structure.
This could be done for example with an opaline film made from PMMA beads that incorporate much smaller
luminescent nanocrystals. If the optical band-gap in the emission range of the dye is incomplete, emission into certain
directions is allowed and effective light guiding occurs.
For all the suggested options for realization, several layers with the same dye will b e needed to achieve sufficient
absorption. As the guided light is constraint to very thin layers high intensities will occur in these layers. Because of
thermodynamical reasons, there is a limit for which concentration can be achieved with a fluorescent concentrator
depending on the Stokes Shift of the used dye
. One question is therefore, which system sizes can be achieved using
44
th is approach until th e thermodynamic limit reduces efficiency.
Furthermore, attaching solar cells to the thin layers is a challenge. Especially, because preferably different types of solar
cells are attached to layers with different dyes. In Figure 11 two different options are shown. One option is to produce
different types of solar cells on one chip, e.g. with a MOVPE-process from III-V semiconductors. Because the required
areas will be very small, this could be v iable from a commercial point of view as well. Preferably, contact fingers should
be aligned between the light guiding layers such that no reflections losses occur. An alternative option would be to
vertically cut through conventional tandem solar cells in a process comparable to that used for sliver cells
.
45
Proc. of SPIE Vol. 7725 77250S-8
Figure 11: Two options of how a “Nano-Fluko” system complete with solar cells could be realized. To achieve good
absorption several layers with luminescent materials must be stacked onto each other. The combination of different
materials ensures good utilization of the solar spectrum. On the right, the attachment of solar cells made from different
materials on one common substrate is shown. The contact fingers should be aligned with the photonic structures so no
shading losses occur. On the left, the option is shown to cut a standard tandem solar cell vertically, similar to the sliver
cell process and to attach such vertical cuts to the edges of a “Nano-Fluko”.
4.
SUMMARY
We have investigated, how the escape cone losses of fluorescent concentrators can be reduced with the help of photonic
structures. We showed that a 20% increase in collection efficiency could be achieved with a commercially available
multi-layer system. Opaline films might be a solution to produce photonic structures on large areas at low costs. For a
positive effect on the light collection efficiency, however, further progress in the production of the opaline films is
necessary. We presented different suggestions, of how path-length depend losses can be reduced by restricting the
angular emission range of the used dyes by incorporating these dyes into photonic structures.
ACKNOWLEDGEMENTS
The authors would like to thank Armin Bösch, Henning Helmers, and Elisabeth Schäffer for their support and the III-V
group at Fraunhofer ISE for the production of solar cells. The presented work was supported by the German Research
Foundation within the Nanosun (PAK88) project.
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Proc. of SPIE Vol. 7725 77250S-11
For example, at latitudes of 65 degrees the change in solar energy in summer & winter can vary by more than 25% as a result of the Earth's orbital variation. Because
changes in winter and summer tend to offset, the change in the annual average insolation at any given location is near zero, but the redistribution of energy between summer
and winter does strongly affect the intensity of seasonal cycles. Such changes associated with the redistribution of solar energy are considered a likely cause for the coming
and going of recent ice ages.