Nanotechnology for Next Generation Photovoltaics

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1 340 Nanotechnology for Next Generation Photovoltaics NARASIMHA RAO MAVILLA 1,2, CHETAN SINGH SOLANKI 1,3, JUZER VASI 1,2 * 1 National Centre for Photovoltaic Research & Education, IIT Bombay, Mumbai , India 2 Department of Electrical Engineering, IIT Bombay, Mumbai , India 3 Department of Energy Science & Engineering, IIT Bombay, Mumbai , India vasi@ee.iitb.ac.in Abstract The use of nanotechnology holds the promise of a new generation of photovoltaic devices can achieve better performance. This paper will focus mainly on the use of Si nanocrystals (Si-NC) in solar cells. The use of appropriately sized Si nanocrystals allows the tailoring of the band gap so as to harvest light of different wavelengths present in the solar spectrum, and thus create tandem multi-junction photovoltaic cells using only silicon and its oxides. A series of ultra-thin multilayered (ML) samples with alternating layers of Si-rich oxide (SRO) and SiO 2 were annealed to obtain Si-NCs in an oxide matrix. The structural properties including their optical band-gap tunability were studied. The optical band-gap estimated using Tauc analysis shows an increase from 1.45 ev to 2.5 ev, as the Si-NC size decreases from 10 nm to 2 nm, indicating the possibility of making an all-si tandem cell. Keywords : solar cell, tandem junction, silicon nanocrystal, 1. Introduction Energy is one of the key requirements for mankind, and harnessing it in a clean and effective way is a continuing quest. Solar photovoltaics has the potential for the generation of clean

2 341 renewable energy, especially in a country like India with its abundant sunshine. It is also particularly suitable for off-grid generation in remote and rural areas. Recognizing this potential, the Government of India launched the Jawaharlal Nehru National Solar Mission (JNNSM) in January It envisages the deployment of 20 GW of grid-connected solar power and 2 GW of off-grid solar power by the year 2022 in a phase-wise manner. Although solar cells have been in existence for over 50 years, for much of this time they have been bedeviled by high cost and/or low efficiency. As a consequence, though they found use in various niche applications, they could not compete with conventional energy sources until recently. During the last few years, the price of solar photovoltaic devices has dropped dramatically, and the holy grail of grid parity is in sight. At a scientific and technological level, new developments which use nanotechnology in solar cells hold the promise of a new generation of photovoltaic devices 1,2. These developments may lead to further improvements in performance and/or lower cost of solar cells, and thus may provide excellent examples of nanoscience and nanotechnology benefitting mankind. After a broad review of the use of nanotechnology in photovoltaics, this paper will focus on the use of Si nanocrystals (Si-NC) in solar cells. The ability to control properties of silicon crystals, such as the bandgap, as their size decreases provides flexibility in designing photovoltaic devices. The use of Si nanocrystals of different sizes can allow us to harvest light of different wavelengths present in the solar spectrum. Layers of such nanocrystals appropriately designed and inserted into a tandem solar cell, can in principle produce more efficient devices. A brief overview of tandem solar cells, including all-si tandem cells, will be presented. This will be followed by a description of the experimental work being done at the National Centre for Photovoltaic Research and Education (NCPRE) at IIT Bombay to realize Si-NCs by the deposition of multiple alternate nano-scale

3 342 layers of silicon dioxide (SiO2) and silicon-rich oxide (SRO) which is SiOx where x<2. The experimental work shows that by varying the thickness of the SRO layer, it is possible to get Si-NCs varying in size from about 2 to 10 nm, and whose bandgaps vary from 2.5 to 1.4 ev. 2. Use of Nano-sized Structures in Photovoltaics The resurgence of R&D in photovoltaics in recent years has included many inputs from nanoscience and nanotechnology. This section describes briefly a few of these Dye-Sensitized Solar Cells 3,4 The dye-sensitized solar cell (DSSC) uses an insulator (often TiO2) which is sensitized by a photosensitive molecular dye. Incoming photons excite electrons in the dye which are efficiently captured by the TiO2 and transported to the anode. On the other side, an electrolyte replenishes the electrons in the dye, and thus completes the flow of current through the cathode. In order to maximize the contact area between the TiO2 and the dye, it is advantageous to have the TiO2 in the form of nanoparticles or nanotubes. There is a considerable amount of ongoing research on the types of nanoparticles, nanotubes and nanowires used in DSSCs, using TiO2 as well as other materials such as ZnO. DSSCs have achieved fairly high efficiencies of about 10-12%, and have a major cost advantage over conventional semiconductor (eg silicon) solar cells. Some of the main drawbacks of DSSCs are the use of liquid electrolyte and dyes, long-term lifetime and degradation Semiconductor-Sensitized Solar Cells (SSSC) 5,6 The semiconductor-sensitized solar cell (SSSC) is similar to the DSSC, except that the dye is replaced by a semiconductor which acts as the photosensitive absorber. This semiconductor (such as CdS/PbS, CdSe, Sb2S3) is chosen to have a high absorption coefficient, and band edges well aligned to the TiO2

4 343 nanoparticles. The advantage of SSSCs is that it could be an allsolid-state cell; however efficiencies achieved so far are in the 4-5 % range Nanowire Solar Cells 7 Nanowire solar cells use p-n junctions in semiconductor nanowires rather than semiconductor wafers or thin films. The advantage of using nanowires arises out of the ability to use less quantity as well as lower quality of the semiconductor, enhanced light trapping, and the possibility to deposit such nanowires on a variety of cheap substrates. Nanowire solar cells have been made with a variety of semiconductors, including Si, Ge, CdTe, CdSe, ZnO, and GaAs, and have achieved efficiencies upto 10% Quantum Dot Tandem Solar Cells 8 In order to capture as much as possible of the solar spectrum, one can use several junctions in tandem made of materials with different energy bandgaps. Indeed, such tandem cells using materials like GaInP/GaInAs/Ge have achieved high efficiencies of greater than 40%. It would be convenient, however, to have tandem solar cells made of a single material (for example, silicon) and tune the bandgap by using quantum dots or nanocrystals of different sizes. This idea is the basis of the all-si nanocrystal tandem solar cell, which is described in more detail in the rest of this paper. 3. Si Nanocrystal Tandem Solar Cell 3.1. Overcoming the Shockley-Queisser limit The solar spectrum ranges from UV to IR. All wavelengths cannot be effectively captured by a semiconductor of a particular bandgap Eg. If Eg is too large, most of the photons will not be absorbed; if it is too small, the photons will be absorbed, but much of their energy will be lost by thermalization. p-n junctions utilizing semiconductors with Eg 1.5 ev give the highest

5 344 theoretical efficiency of about 31%; this is known as the Shockley- Queisser limit 9. Various methods have been suggested to overcome this fundamental limit. These include hot-carrier solar cells, multiple energy band solar cells and multi-junction tandem solar cells Multijunction Tandem Solar Cells The concept of a multijunction solar cell is simple: use several p-n junction solar cells in tandem, each with different bandgaps which capture efficiently different parts of the solar spectrum. However, realizing such a solar cell in practice is not straightforward. An example of a multijunction tandem solar cell is the GaInP/GaInAs/Ge solar cell which has achieved 41% efficiency. However, use of several materials poses a technology Fig. 1. Schematic picture of a 3-junction all-si tandem solar cell using two layers of Si QDs.

6 345 challenge, and such cells can be very expensive. It would be good if one could realize different bandgaps using only one material (for example, Si) whose bandgap is varied by using appropriate nanostructures. This is the idea behind the all-si multijunction tandem solar cell using different size nanocrystals or quantum dots (QDs) 8. This is shown in Fig. 1. Light comes in from the top, and the lowest wavelengths are first absorbed in the top cell, whereas the higher wavelengths go through and are absorbed in the middle and bottom cells. 4. Fabrication and Characterization of Si Nanocrystals 4.1. Fabrication of SiO2/SRO Multilayer Structures The creation of a structure like the one shown in Fig.1 requires one or more cells each containing several layers of Si nanocrystals embedded in an insulator matrix. In each cell, the size of the nanocrystals is different. There are many ways of realizing such multi-layers (ML). One of the best ways to do this is to deposit alternate thin (nano-scale) layers of SiO2 and a silicon-rich oxide (SRO, which is SiOx with x<2) 11. A high-temperature annealing step results in the excess silicon agglomerating together and finally crystallizing into Si nanocrystals separated by SiO2, as shown in Fig. 2, thus achieving the desired structure. The size of the nanocrystal is about the thickness of the original SRO layer. The deposition can be done by chemical vapour deposition (CVD). At IIT Bombay, we have used a variety of CVD techniques to achieve the ML structures, and have found that Inductively Coupled Plasma CVD (ICPCVD) gives excellent results. Advantages of ICPCVD over other CVD techniques like hot-wire CVD and conventional plasma-enhanced CVD include lower deposition temperatures, less hydrogen content, and better controllability of the process, because it is possible to control the ion flux and ion energy independently by two separate RF sources.

7 346 Fig. 2. Schematic representation of formation of Si nanocrystals from SRO layers by annealing. Initially amorphous silicon islands are formed, which later crystallize into QDs. We have made a variety of multilayer structures by ICPCVD. The SRO layer thicknesses can be well controlled by varying the deposition time. We have obtained structures with the SRO layer thickness varying from 2 nm to 10 nm; this would potentially give Si nanocrystals varying in size from approximately 2 to 10 nm. It is well known that because of quantum confinement, the ground state energies of electrons and holes are raised, thus increasing the effective bandgap in a nanocrystal compared to the bulk. Further, as can be easily understood from quantum-well analysis, the smaller the size of the nanocrystal, the larger the bandgap. Fig. 3 (a) and (b) show TEM pictures of our multilayer SiO2/SRO structures deposited by ICPCVD, and the formation of Si nanocrystals after annealing at 900 C Size and Bandgap characterization of Si nanocrystals We have done a detailed characterization of the samples by XPS, Raman spectroscopy and optical absorption. The XPS studies 12 on the silicon dioxide and SRO (SiOx) films show that for

8 347 silicon dioxide the x in SiOx is indeed very close to 2, whereas for the SRO it is ~ 0.5. Raman spectroscopy results 13 show that the deposited SiO2 and SRO are amorphous in nature, but after annealing, a clear signature of Si recrystallization emerges. We have estimated the size of the Si nanocrystals by using the Raman phonon confinement model. This shows the sizes to be wellcorrelated with the original SRO layer thickness, which is also confirmed independently by the TEM photos when available. (a) Fig. 3. TEM pictures of a 41-layer SiO2/SRO structure (a) before annealing and (b) after annealing. We have also measured bandgaps of the nanocrystals by measuring transmission, reflectance and hence absorption using a UV-Vis photospectrometer. A Tauc analysis of the absorption characteristics is shown in Fig. 4 for four multilayer samples. A summary of the results is given in Table 1, clearly indicating that the band gap increases as the nanocrystal size decreases. This establishes that using only silicon and its oxide, we can vary the bandgap and thus build tandem solar cells. The next steps in making the full solar cell will be to deposit 2 sub-cells of several multilayers on a silicon substrate, optimizing the number of layers as well as the separation of the nanocrystals in each subcell. (b)

9 348 Fig. 4. Tauc analysis of 4 multilayer samples having varying SRO layer thickness; (a) ML1=2 nm, (b) ML2=4 nm, (c) ML3=6 nm, (d) ML4=8 nm. Table 1. Summary of results of NC diameter and bandgap for 5 different multilayer samples. Sample ID SRO deposition time (s) Nominal SRO thickness (nm) Si NC dia (nm) (from Raman) Bandgap (ev) ML ML ML ML ML

10 Conclusions Photovoltaics is growing in importance as a source of clean, renewable energy. It presents an excellent application area for the use of nanoscience and nanotechnology, whereby performance and cost can both be benefitted by the judicious use of nanostructures. At the National Centre for Photovoltaic Research and Education (NCPRE) at IIT Bombay, we have ongoing research on several aspects of solar cells which use nanostructures. One of these, the Si quantum dot solar cell using nanocrystals of silicon embedded in a silicon dioxide matrix, has been described in some detail in this paper. Our results show that we can get excellent control of silicon nanocrystal size using multilayers deposited by ICPCVD, and that there is a significant variation in the absorption bandgap of these nanocrystals as their size is varied. This holds the promise for the realization of all-si multijunction solar cells, and this work is currently in progress at NCPRE. Acknowledgments The authors acknowledge funding received from the Ministry of New and Renewable Energy (MNRE) of the Government of India for the National Centre for Photovoltaic Research and education (NCPRE) at IIT Bombay, and also the use of facilities at the Centre of Excellence in Nanoelectronics (CEN) at IIT Bombay, which has been funded by the Department of Electronics and Information Technology (DEITY) of the Government of India. References 1. C. B. Honsberg, A. M. Barnett, D. Kirkpatrick (2006) Nanostructured solar cells for high efficiency photovoltaics. 4th World Conference on Photovoltaic Energy Conversion, Hawaii. 2. G. Zhang, S. Finefrock, D. Liang, G. Yadav, H. Yang, H. Fang and Y. Wu (2011) Semiconductor nanostructure-based photovoltaic solar cells. Nanoscale, 3,

11 B. O'Regan and M. Grätzel (1991) A Low-cost, High-efficiency Solar Cell Based on Dye-sensitized Colloidal TiO2 Films. Nature 353, M. Gratzel (2003) Dye-sensitized solar cells. Journal of Photochemistry and Photobiology C: Photochemistry Reviews, 4, G. Hodes and D. Cahen (2012) All-solid-state semiconductorsensitized nanoporous solar cells. Accounts of Chemical Research, 45, I. Mora-Sero and J. Bisquert (2012) Breakthroughs in the Development of Semiconductor-Sensitized Solar Cells. J. Phys. Chem. Lett. 1, E. C. Garnett, M. L. Brongersma, Y. Cui, and M. D. McGehee, (2011) Nanowire Solar Cells. Annu. Rev. Mater. Res. 4, E-C. Cho, S. Park, X. Hao, D. Song, G. Conibeer, S-C. Park, M.A. Green (2008) Silicon quantum dot/crystalline silicon solar cells, Nanotechnology W. Shockley and H. Queisser (1961) Detailed balance limit of efficiency of p-n junction solar cells. J. Appl. Phys. 32, M. A. Green (2000) Prospects for photovoltaic efficiency enhancement using low-dimensional structures. Nanotechnology 11, M. Zacharias, J. Heitmann, R. Scholz, U. Kahler, M. Schmidt, and J. BlaÌsing (2002) Size-controlled highly luminescent silicon nanocrystals: A SiO/SiO 2 superlattice approach. Applied Physics Letters, 80, N. R. Mavilla, H. K. Singh, C. S. Solanki, and J. Vasi (2012) Structural properties of ICPCVD fabricated SiO 2 /SiOx superlattice for use in beyond Shockley-Queisser-limit solar cells. 27th European Photovoltaic Solar Energy Conference (EUPVSEC), Frankfurt. 13. N. R. Mavilla, D. K. R. Rai, C. S. Solanki, and J. Vasi (2012) Optical bandgap tuning of ICPCVD-made silicon nanocrystals for next generation photovoltaics. 38th IEEE Photovoltaic Specialists Conference (PVSC), Austin, USA.

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