Quantum Dot Sensitized Solar Cells (QDSSCs)

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 Contents

1. Introduction

2. History of DSSCs

3. Quantum Dot Semiconductor Solar Cells (QDSSCs)

4. Working Principle of a QDSSCs

5. Fabrication techniques
5.1. Doctor blading
5.2. Screen printing
5.3. Other methods

6. Preparation of Quantum Dot sensitizing layer

6.1. In-situ methods
6.2. Ex-Situ methods

7. Further development of QDSSCs

7.1. Sensitizer Materials
7.2. Triple junction
7.3. Redox electrolyte
7.4. Counter electrode
7.5.Other methods

8. Types of QDSSCs

9. Advantages

10. Disadvantages

11. Conclusion

12. References

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 1. Introduction
As the modern world requires alternating energy sources with the
rapid depletion of fossil fuels and the imminent threats of global warming,
several technologies are currently working on developing a reliable, cost-
effective, and environmental-friendly energy source. Many renewable
energy sources such as wind energy, tidal energy, hydro-electrical and
geothermal energies are currently being used as alternative sources of
energy and the generation of energy by the direct conversion of sunlight
into electricity using photovoltaic (PV) cells has been one of the most
promising among them. But the greatest challenges when developing new
types of advanced materials have been the development of new materials,
which are robust and inexpensive and have the desired electrical and
optical properties while giving the capability of ease of fabrication,
higher efficiencies to the PVs. Since the first generation, silicon-based PV
cells have been dominating the solar energy industry because of the
robustness and the cheaper price of silicon. But all the silicon-based PV
cells are currently limited to an efficiency of 33.7% and it hugely affects
the amount of energy that can be supplied to the current demand. The
Shockley−Queisser limit, which is the thermodynamic limit of light
conversion efficiency is also at around 32.9% for a cell of the single
junction. Due to such reasons, solar energy still haven been able to use as
the primary source of energy rather than used as an additional supply.

Solar power used as additional supply to main power line

To overcome this limitation many attempts are being carried out resulting
in the advancement of the third and fourth generation of solar cells. Some

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of those advancements are the solar cell family of photoelectrochemical
solar cells (PESC). They include technologies such as dye-sensitized
solar cells (DSSCs) and quantum dot (QD)- sensitized solar cells
(QDSSCs). Those technologies are currently showing promising
advancements in the terms of high conversion efficiency and low-cost
fabrication. Among those two, QDSSC has the most attention as the
quantum dot technology has many advantages when used as sensitizers
such as their large absorption coefficient, absorption spectrum tunability,
hot electron injection, multiplication, etc. With those advantages, those
solar cells have been able to achieve higher efficiencies such as 44.7%.

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 2. History of DSSCs
The first DSSC was introduced in 1991 along with optically active
sensitizing material. When considering the making of DSSCs, they
consist of two electrodes, a sensitized photo-anode, and a counter
electrode with appropriate electrolyte. A transparent conductive substrate,
usually Fluorine doped tin oxide – FTO or Indium doped tin oxide – ITO
or PET-ITO, is used for making the sensitized photo-anode by depositing
a wide bandgap semiconductor material over it. Then an optically active
sensitized dye layer is deposited over it. The dye-based on Ru was used to
achieve higher efficiencies and lower costs. Along with liquid electrolytes
based on iodide-triiodide (I -–I3-), platinum (Pt) is used as a common
counter electrode in DSSC. DSSC is usually preferable over conventional
p-n junction solar cells because that they do not require very pure and
defect-free semiconductors. But their efficiencies are limited due to some
reasons such as absorption spectrum performance of the dye, breakdown
of the dye, and the low thermal and long-term stability.

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 3. Quantum dot semiconductor solar cells (QDSSCs)
So after some time, the dye was replaced by quantum dots, which
are light-absorbing materials. Hence the design of QDSSC was
introduced. These QDs consist of some unique characteristics related to
optoelectronics such as size-dependent tunable energy band gap, carrier
multiplication, etc. And to increase the overall performance of solar cells,
those unique characteristics are optimized. Also, the QDSSC is capable of
absorbing a wide range of solar radiation wavelengths from UV to
infrared.

QDSSC structure

QDSSC is widely used in the field of photovoltaic (PV)s in different

configurations. Those are designed based on the form of QD Schottky
junction solar cell, QD hetero-junction solar cell, QD hybrid polymer
solar cell, QD sensitized solar cell (QDSSC), QD & Dye co-sensitized
solar cell, QD rainbow solar cell, etc. QDSSCs have surpassed the other
forms and have emerged as a promising technology in the field of PVs.

When considering the making of DSSCs, they consist of two electrodes, a

sensitized photo-anode, and a counter electrode with appropriate
electrolyte. And the sensitized photo-anode is made by depositing a wide
band-gap semiconductor over a transparent conductive substrate
(Fluorine doped tin oxide – FTO or Indium doped tin oxide – ITO or
PET-ITO) and then depositing a layer of optically active sensitized dye
over it. Platinum (Pt) is a common counter electrode in DSSC, using an
iodide-triiodide (I –I3) based liquid electrolyte. Although DSSCs are
preferable to conventional p-n junction solar cells in that they do not
require a very pure and defect-free semiconductor, their efficiency is
restricted due to dye absorption spectrum performance, dye breakdown,
and low thermal and long-term stability.

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 4. Working principles
Most of the QDSSCs includes wide-band-gap semiconductor
which is usually TiO2, Semiconductor nanocrystals that have narrow
bandgaps, a redox electrolyte solution along a counter electrode. The
electrons are injected into the wide-bandgap semiconductor conduction
band when the semiconductor nanocrystals are excited. Then the
electrons are diffuse to the front contact and the holes are sent to the
electrolyte for the process of regeneration occurs at the counter electrode.

To excite and form electron and hole pairs, the QDs must be irradiated
with sunlight having energy equal to its bandgap energy. Different
chemical processes occur during charge separation and transit

Here, the letters e and h stand for electron and hole, respectively.

Following the above process, the transportation of chargers at wide

bandgap (WBG) SC/QD interface as follows.

Here, Red and Ox denote the reduction and oxidation of electrolytes

respectively. Also, the size of the QD is the parameter that determines the
separation of charges at the WBG SC/QD interface. The reduction of the
size of QD results in the improvement of electron transport.

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Working of (a) DSSC and (b) QDSSC

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 5. Fabrication techniques

When it comes to the fabrication technologies of QDSSC, many

improvements have been done to improve solar cell performance. And
the most popular synthesis methods which are being used for QDSSC for
semiconductors thin-film coated electrodes, QD layer deposition, and
counter electrode preparation are as follows.
For the preparation of semiconductor coated electrode, many thin film
deposition techniques such as doctor blading, screen printing, etc. Are
being used. They create a layer of wide bandgap semiconductor, usually
TiO2, ZnO, and SnO2, over a conductive substrate mainly FTO or ITO
glass.

5.1. Doctor blading

In doctor blading an appropriate ratio of an organic binder such as
ethylcellulose, a surfactant, usually terpineol, a solvent such as ethanol, is
used to create a thick and viscous paste of evenly dispersed nanocrystals
of semiconductor. This paste is then applied to a specific portion of the
substrate’s conducting surface. This specific area is usually marked with
scotch tape or a mask. Then a sharp blade is used to create a
homogeneous coating of semiconductors by distributing the paste over
the electrode. Drying of the thin film process is done at the ambient
temperature before using the high temperature for the annealing process.
The quality of the thin film is determined by the composition of the paste,
speed and the angle of the blade, and the annealing temperature, etc. Also
masking using multilayer scotch tape helps to regulate the thickness of
the thin films.

5.2. Screen printing

But in screen printing, a huge amount of thin films of the same quality
can be produced at the same time. It is mainly used in the commercial
fabrication of conventional silicon solar cells. In the most basic type of
screen printing technique, a mask with a mesh type structure is used on
the conductive surface of the substrate. Using the same way as in the
doctor blade method, a paste is made and pasted on the mesh of the mask
to fill the open areas of the mesh. Then a machine-operated squeegee is
dragged across the substrate to force the paste through the open areas of
the mesh. Then the mask is removed after ejecting the remaining paste off
the electrode’s surface. Here also drying and the annealing process is
done similar to the doctor blade method.

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 5.3. Other methods
As for the other methods, spluttering, spray pyrolysis, electro-spinning,
and atomic layer deposition are used to get the varied structural and
morphological qualities while improving the thin film quality. Sometimes
a combination of two techniques is used in instances such as the
fabrication of one-dimensional nanostructures, such as nanorods and
nanotubes. Usually, spin coating or sputtering techniques deposit the seed
layer on the substrate while hydrothermal techniques to assist in growing
one-dimensional nanostructures on semiconductors are used on such
occasions.
Usually, screen printing is the most suited process to fabricate
photoanode with mesoporous spherical shape while spin coating or spray
pyrolysis is used for seed layer deposition. The hydrothermal process is
most suited for processes such as creating vertical one-dimensional or
hierarchical structures.

QDSSC fabrication techniques (a) doctor blading, (b) spin coating, (c)
CBD, (d) SILAR, (e) molecular linker attachment and, (f) electrophoretic
techniques

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 6. Preparation of QD sensitizing layer
And in the preparation of the QD sensitizing layer, there are two methods
used namely in-situ method or the ex-situ methods to deposit the QD
layer on a semiconductor coated electrode. In-situ methods are often used
as a manufacturing process in QDSSC technologies as they are simple
and low cost. Which makes them an ideal choice for large-scale
manufacturing. There are two processes which mainly used in in-situ QD
deposition namely, chemical bath deposition (CBD) and sequential ionic
layer absorption and reaction (SILAR).
6.1. In-situ methods

The CBD process is a simple, repeatable, and cost-effective

method for producing high-quality compounds semiconductor metal
halides, and chalcogenide thin films. This method can be used on both
metallic and non-metallic substrates. Due to past researches, the CBD
process is now able to generate films with good structural, optical, and
electrical characteristics similar to those generated by other advanced thin
film deposition methods. In this method, desired chemicals are
precipitated slowly by using their ions in a reaction bath solution.

The sequential ionic layer absorption and reaction method is mostly used
for thin film deposition of large-area thin films because of its economical,
easy, and convenient capabilities. It primarily depends on processes of
absorption and reaction of ions from solutions. Also to avoid
homogeneous precipitation in the solution, washing with deionized water
in between each immersion is done.

The growth mechanism consists of three main phases. First, the

compound’s most strongly adsorbed ions which have been grown by the
substrate while immersed in a solution of one of its cationic precursors
were specifically adsorbed. Then the excess solution which still adheres
to the substrate is water rinsed. And finally, chemical reactions occur
between the adsorbed cations and anions. Factors such as optimization of
precursor concentrations, pH of the solutions, adsorption, reaction and
washing times, etc. determine the quality of the thin films.

6.2. Ex-situ methods

When depositing ex-situ grown QDs, the size and the form of the
monodisperse QDs are adjusted by synthesizing using organic capping
ligands. After the production, the QDs are removed from the additional

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organic ligands. Next, they are dissolved in an organic solvent and then
connected the TiO2 electrodes. In order to address the issue of not
bonding between the layers of QDs and mesoporous TiO2, mercapto-
carboxylic acid is used as a bifunctional molecular linker. In the dipping
process of electrode in mercapto-carboxylic acid ligands, the change in
surface of TiO2 occurs. This process is known as the dip coating. This
allows the carboxylic acid groups to be bonded with TiO2 surface. Then
this modified TiO2 electrode is submerged in the QDs solution which
allows the QDs to diffuse into the pores and the binding the QDs with
TiO2 surface is done by the mercapto groups using partial ligand
exchange.
Another method of depositing particles on TiO2 surface is the
electrophoretic QD deposition process.

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 7. Further development of QDSSCs
High performance QDSSCs are being developed with a significant
progress in the recent years. Increasing the efficiencies of light to electric
power conversion have been a main focus on those researches. Increase
of efficiencies about 5-7 % have been achieved by some researchers.
When compared to DSSCs, this is a giant leap forward. But in order to
achieve such efficiencies while implementing them commercially, further
research and developments have to be done. There are some important
areas that need to be considered when developing the QDSSCs further.
Those areas mainly consist of materials and interfaces needed for
QDSSCs.

Main interfaces or the material of QDSSC

7.1.Sensitizer Materials
When it comes to the semiconductor sensitizer materials in QDSSCs,
most widely used materials are CdS and CdSe. That is due to the reasons
such as their harvesting ability sun’s spectrum’s several regions and their
good charge separation properties. This is the process of hole removal
with the use of electron injection into wide band gap oxide and redox

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electrolyte. Based on the numerous studies done in recent years, the
possibility of using sensitizer materials such as QD sensitizers have been
improved rapidly. It has resulted a rapid growth of QDSSC conversion
related efficiencies too. When getting a high power conversion efficiency
(PCE) using QDSSCs, some aspects needs to be considered. One of the
requirement is efficiently absorbing the incoming light source. For this,
the photosensitizer or the QD required to have a good absorption
coefficient and a band gap energy. Although the QDSSCs can produce a
large open - circuit voltage when using the QDs with a high band gap
energy but, their light absorption is not enough to excite required amount
of electron due to the small range of light with short wavelengths can
excite the QD electrons. And when using the low band gap energy QDs,
they can absorb a good range of light wavelengths which able to excite
the electrons, but they have a low open - circuit voltages.

Due to that, many researchers have been invested in finding a optimum

trade off value between these two qualities. Although it has found that the
optimum value for this is about 1.4eV calculated in theories, but in
practical approaches, many variables affect this value and have been hard
to predict accurately.

Many research efforts have been done, in order to develop an optimum

photosensitizer and they have explored material such as, CdS, CdSe,
CdTe, PbS, Ag2S, InAs, Bi2S3, CuInS2, different combinations of CdS,
CdSe, CdTe, PbS, Ag2S, InAs, Bi2S3, CuInS2. But most commonly used
ones are the mixtures of Cds and CdSe.

7.2. Triple junction

When it comes to the triple junction, the mechanisms of charge transfer
process occurs between nanostructured TiO2, the sensitizing QDs, and the
aqueous polysulfide electrolyte. They produce complex interfaces which
enables the charge transfer processes which heavily affects the overall
performance of QDSSCs. Charge injection and recombination processes
and modifying the photocurrent and photovoltage of the solar cell are
mainly impacted by the energy level distribution of the materials which
forms the triple junction. There are numerous ways to tune the band
edges of TiO2 with regard to the redox electrolyte in QDSSCs, as they
can in conventional DSSCs. This is often done by the alteration of pH
levels of the solution which finally result in change of the surface
environment of the TiO2, or modification of electrolyte by injecting
additives, or attaching molecular dipoles.

Recombination losses are also can be reduced in the triple junction. This

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is done by the use of semiconductor quantum rods (QR). The
semiconductor quantum rods are used to replace the QD particles which
are typically used at the TiO2/QDs/electrolyte triple junction. By this
method, the photogenerated charges are efficiently separated by the
rodlike particles which have a high aspect ratio. Because of that the holes
diffuse to one end of the particle while the electrons diffuse to the other.

7.3. Redox electrolyte

When it comes to the redox electrolyte, one of the primary problems in
the field of QDSSCs have been the creation of an effective electrolyte
solution of rapidly transferring electrons to regenerate oxidized QD
sensitizers. Also this solution should maintain a long term stability in
usual working conditions. In ordinary DSSCs the I-/I3- redox couple is
used and it is well known for its good performance. But when it used with
the QDSSCs, the inorganic semiconductor QDs are heavily corroded by
the iodine. This results in deterioration of the photoactive electrode
function rapidly. So the polysulfide redox couple which is in aqueous
solution is used instead. And by far it has been the most favoured
electrolyte for the cells of this types. The polysulfide electrolyte usually
results in high oxidized QD regeneration rates but it also has a low cell
Voc when compared to a standard DSSC. The energy difference between
the fermi level and the electrolyte redox potential is taken to determine
the Voc of a QDSSC. So the highest theoretical solar cell Voc which can
be achieved is highly restricted by the negative redox potentials by its
intrinsic polysulfide characteristics. So the current researches on
developing new forms of liquid electrolytes have been to overcome such
restrictions. But this should be done retaining the stability of the QDs as
well as increasing the Voc by having a higher positive redox potential

7.4. Counter electrode

When focussing on the counter electrode, the best performance of
QDSSCs can be get by discharging electrons quickly at the counter
electrode. As the polysulfide electrolyte was used to improve the
photoanode stability in liquid junction QDSSCs, they also result in lower
power conversion efficiencies when compared with DSSCs. Also Pt is
used as a counter electrode because of the highly catalytic behaviour over
a wide range of reactions regarding electrochemical processes, such as
the reduction of I-/I3- redox couple in DSSCs. But the problem with
platinum counter electrodes is the lower performance when they are used
with polysulfied electrolyte. Because of such problems, development of
alternative counter electrodes have been a focus in may researches. There
have been researches on developing such counter electrode material
which can efficiently catalyze the polysulfied reaction process while also

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being able to be stable in electrolyte solution. CoS, Cu2S are such counter
electrodes which discovered to be able to have a greater catalytic
characteristics than platinum.

7.5. Other methods

Other than the above mentioned, the active layer thickness is also a
parameter which can impact the overall performance of a solar cell. In
QD deposition, a photoanode which is too thin will not be able to provide
enough specific area for the process of deposition. Also a photoanode
which is too thick will not be able to transport electrons effectively. The
increase of the wide band gap semiconductor thin film depth also result in
the decrease of amount of deposited QDs. So when the thickness rises of
the thin film, the QD size will also grow. So the active layer thickness can
be optimized. Some experiments have demonstrated that a solar cell with
optimum thickness of 10 micrometers of TiO2 thin film have a highest
efficiency of 3.26%. Also a higher efficiency of 4.09% have been
achieved in a porous ZnO nanostructure CDS/CdSe QDSSC combined
with CuS counter electrode by altering the duration of the QD deposition.

Conducting oxide is also modified in several ways. When it comes to the

conducting oxide, it act as a supporting stage to the photoanode. Due to
that, it is very essential component which can significantly affect on
power conversion efficiency of QDSSCs. These conducting oxide surves
two important functions. It helps electrons by giving them smooth
pathways so that the photogenerated are efficiently transferred. The also
act as a surface area for light absorption and it helps to increase the
absorption because of their expanded surface area. There have been many
researches done because of the conducting oxides importance to the
QDSSCs. Most often used QDSSC conducting oxides are the TiO2 and
ZnO but there have been many attempts to develop other types of
conducting oxides. Some of them have used BaTiO3 and WO3 but due to
the fact that TiO2 and ZnO have a higher electron mobility, they are still
considered the most promising electrodes for solar cells.
The light absorption increases with the load of the photosentizers.
Because of that, the amount of photosensitizers which are loaded on the
photoanode should be kept maximum. Nanostructured conducting oxides
have a larger surfaces area so they are being used to achieve this need.
There are several types of nanostructures used when manufacturing
QDSSCs such as, nano - rods, particles, wires, tubes and sheets.
Combining between those structures are also done such as nanowires of
1D and sheets of 2D have combined to create a hierarchial 3D structure.
But reduction of PCE due to too complicated structures have restricted
the full use of the nano structures currently.

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Nano particles and nano tubes structures

17
 8. Types of QDSSCs

According to the type of QDs used, there are several types of QDSSCs
available.

Schottky QDSSC:
Thin film solar cells which uses the QDs as their principle absorber were
first introduced in 2005. Extraction of electrons and holes in
manufacturing was done using electron affinity between Transparent
Conductive Oxide (TCO) and the reflecting black contact (e.g. Mg).
These type of cells used PbS quantum dots along with an organic polymer.
This is used to absorb photons and generated exciton seperated by
conduction band offsets.

Depleted Heterojunction QDSSC:

Illumination development at the non rectified side and generation of
excessive electron trap states are the main two limitations of Schottky
QDSSCs. But when using a depleted hetrojunction a heavily doped n -
type metal oxide is introduced to p - n hetrojunction. And the p - type
junction is usually a thin film of thickness to 50 to 400 nm. They are
usually made of heavily doped metal oxides or Gold paired with
reflective metal, and illumination of hetrojunction is then done by WBG
semiconductor and transparent substrate in order to overcome the
drawback of Schottky QDSSC by resulting close junction
photogeneration.

Bulk-Heterojunction QDSSC:
In the depletion process of hetrojunction QDSSCs, minority carrier
transport is a serious problem that may be minimized using the bulk
heterojunction approach. The CQD thin film and the wide band gap
semiconductor produce an interpenetrating layer in this arrangement. It is
referred to as bulk heterojunction since it is a 3D structure, similar to
organic photovoltaic. Infiltration of structured electrons are permitted for
the CQDs because they cause more prominent depletion area. More
absorbing CQDs can improve both absorption and carrier collection at the
same time

Bulk-Nano Heterojunction QDSSC:

Bulk nano hetrojunction QDSSCs use one active bulk material such as
CdTe and one quantum confined material such as CdSe as p type and n
type semiconductor materials. Then those material both p type and n type

18
are combined with a solution phase mixture and get interpenetrated. So
this type of solar cells shows currents of both bulk and nano phases and
proven to be better than the previous ones.

Multiple-Junction QDSSC:
To get efficiencies higher than about 31%, multiple junction of QD solar
cell materials have been used instead of single junction QD solar cell
materials. By this method, different band gap materials for junction by
changing the size of the QDs can be achieved.

Different types of QDSSCs

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 9. Advantages of QDSSCs
As the QDSSCs still need to be optimized in order to have them available
in commercial use, they have many advantages and some disadvantages
when using. When considering about the advantages and benefits of using
QDSSCs, they have a good power to weight ratio which enables the
miniaturization. QDs are made of inorganic matamaterials, which have
dramatically improved optoelectronic capabilities at the quantum
confined scale. Electrons in QDs are easily stimulated because of the
narrow band gap of QDs. This is not the case when using dyes. They have
a higher resistance to photobleaching than dyes [46]. Most notably, every
single QD can be tuned in terms of band gaps, and many junction cells
can be created. Tunability in band gap can allow access to the whole
colour spectrum area by simply altering the size of the dot.Because the
synthesis of these QDs is simple and inexpensive, the cost of fabricating a
single solar cell is predicted to be affordable to the general public.
They also have a higher efficiencies and current studies suggest that they
can be further optimized. They also have a smaller mass and require less
space compared to other cells, and they are said to have a good
adaptability. Because of their versatility, they can be used in entire
structures such as windows rather than only using as rooftops.

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 10. Disadvantages of QDSSCs

And the drawbacks of quantum dot solar cells as follows. Surface

passivated QD production is a difficult operation since it necessitates the
selection of a suitable ligand/capping agent that can really fulfill the
surface dangling bonds while avoiding surface trap states. The CdSe
material which is used in QDSSC are extremely toxic and hazardous in
nature. Such as Cadmium is dangerous for human health and the
environment. So they need to be handled with care and this may
complicate things when QDSSCs are implemented in residential
structures. Another drawback is that they degrades faster in wet and UV
environments.

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 11. Conclusion

Quantum dot-sensitized solar cells (QDSSCs) have been the focus of

much study in the domains of materials science and physical chemistry in
recent years. QDSSC has the potential to replace all current renewable
green energy gathering systems. However, a few crucial characteristics
must be determined, particularly in terms of the synthesis of green, stable,
and long-lasting QDs. The conversion efficiency of QDSSCs have also
increased dramatically over the years. At first they were at less than 1%
but after the recent developments, they have been able to achieve
efficiencies about 6%. This is mainly because of the increase in
knowledge related to physical mechanisms which are being occurred
during the cells operation. Construction of complex solutions for different
failures in the system has made them improved in many ways. Many
realistic performances are currently being achieved by the researchers
such as recent discovery on doped PbS sensitized solar cell with current
densities with 30 mA/cm2 looks promising. As a result, the next big step
in QDSSC performance will be to increase the Voc of the cells
significantly, either by replacing the conventional polysulfide with a new
type of liquid redox electrolyte or by using appropriate solid hole
conductors, as has been successfully demonstrated in perovskite-based
solar cells.

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