PEDOT:PSS hybrid solar cells incorporated with silver plasmonic nanospheres

    Si/PEDOT:PSS hybrid solar cells incorporated with silver plasmonic nanospheres Lei Hong, Rusli, Xincai Wang, Hongyu Zheng, Jianxiong Wang, Hao Wang, HongYu Yu PII: DOI: Reference:

S0040-6090(15)01283-3 doi: 10.1016/j.tsf.2015.12.033 TSF 34902

To appear in:

Thin Solid Films

Received date: Revised date: Accepted date:

1 July 2015 25 November 2015 9 December 2015

Please cite this article as: Lei Hong, Rusli, Xincai Wang, Hongyu Zheng, Jianxiong Wang, Hao Wang, HongYu Yu, Si/PEDOT:PSS hybrid solar cells incorporated with silver plasmonic nanospheres, Thin Solid Films (2015), doi: 10.1016/j.tsf.2015.12.033

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ACCEPTED MANUSCRIPT Si/PEDOT:PSS hybrid solar cells incorporated with

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silver plasmonic nanospheres

HongYu Yu3 1

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Lei Hong, *1, 2 Rusli, 1 Xincai Wang,2 Hongyu Zheng,2 Jianxiong Wang,1Hao Wang,1

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Novitas, Nanoelectronics Centre of Excellence, School of Electrical and Electronic Engineering,

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Nanyang Technological University, 50 Nanyang Avenue, Singapore 2

Singapore Institute of Manufacturing Technology, A*STAR (Agency for Science, Technology

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and Research), 71 Nanyang Drive, Singapore 3

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South University of Science and Technology of China, Shenzhen, China

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Abstract

We study the incorporation of periodic silver nanospheres on planar hybrid

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Si/PEDOT:PSS solar cell for absorption enhancement based on the plasmonic effect. The impact of the periodicity and diameter of the silver nanospheres on the light absorption of the hybrid cell is systematically simulated using the finite element method. The light absorption is found to improve significantly in the presence of the silver nanospheres, achieving a maximum ultimate efficiency of 22.6 % when the periodicity is 600 nm and the nanospheres diameter to periodicity ratio is 0.45. This is 23.8% higher than that of the planar hybrid thin cell without the silver nanospheres. The physics behind the enhanced light absorption in the hybrid cell arising from the introduction of periodic silver nanospheres is also discussed.

*email addresses: [email protected] 1

ACCEPTED MANUSCRIPT I. INTRODUCTION

During the last decade, significant research effort has been dedicated towards Si nanostructures based solar cells [1-3]. The strong trapping of light by the nanostructures can substantially increase light absorption and improve cell performance.

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However, such nanostructures based solar cells are costly as their fabrication at nanoscale involves complicated processes such

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as photolithography, high temperature thermal diffusion, reactive ion etching, etc. This has prompted research on hybrid

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nanostructures based solar cells in recent years, such as the SiNWs/PEDOT:PSS solar cell, which leverages on the advantages of both Si nanostructures and organic materials that include high power conversion efficiency, low temperature and low cost simple solution based processes [4-6]. Currently, the highest efficiency reported for hybrid solar cell is based on a Si nanowire

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structure with a cell efficiency of 13.01% [6].

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The introduction of nanostructures can substantially increase light absorption and result in a higher short circuit current density. However, due to the large surface area introduced that is generally defective and promotes carriers recombination, the open circuit voltage and fill-factor are degraded, conceding the cell performance that is expected from the use of

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nanostructures [7]. Therefore, alternative approaches should be explored to improve the performance of hybrid solar cells

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without the use of Si nanostructures. We have previously demonstrated that it is possible to obtain hybrid solar cells with good performance without the use of nanostructures [8]. The cells were fabricated on planar Si substrate and have a high efficiency

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of 10.6 %, attributed to the high open circuit voltage arising from the good Si surface quality and passivation [8]. This approach is attractive as it eliminates the need of nanostructure and substantially simplifies the fabrication process.

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To further improve the efficiency of such planar hybrid cells without nanostructures for light trapping, one possible approach is to incorporate plasmonic silver (Ag) nanospheres (NS) to improve their light absorption. Incorporation of metallic plasmonic nanospheres into solar cells for light absorption enhancement has been demonstrated previously [9-11]. The sunlight can be effectively guided within the absorbing layer due to the collective oscillations of electrons at the surface of the metal nanospheres [12-14]. The improved light absorption is achieved through the following mechanisms: Firstly, when the plasmonic nanoparticles are placed at the interface between air and Si, they effectively trap the sunlight into the underlying Si material by forward scattering [15, 16]. It has been demonstrated that this scattering induced light absorption enhancement has a strong dependence on the shape and size of the plasmonic nanoparticles [9, 12]. Secondly, the plasmonic nanoparticles function as antennas to enhance the local field around the nanoparticles [15], and hence the incident light can be effectively trapped into this localized surface plasmon modes. This mechanism works well mainly for very small diameter nanoparticles of less than 20 nm, but is very useful for materials with short diffusion length [15]. Thirdly, by using a metallic grating at the

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ACCEPTED MANUSCRIPT back surface of Si, the incident light can be coupled into the surface plasmon modes induced at the interface between the Si thin film and the metal structure [15, 17]. For sunlight with frequency close to that for plasmonic resonance, the light is effectively guided and trapped within the structure. This mechanism is critical for the long wavelength sunlight, which

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generally has a small light absorption coefficient in Si [18]. Although the introduction of plasmonic nanoparticles can increase

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light absorption, it also induces light loss due to absorption within the nanoparticles themselves [15]. Therefore, a balance

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must be struck with a proper design of their shape, dimension and structure. Todate a number of such metal nanoparticles incorporated photovoltaic devices have been demonstrated experimentally. A 13% increment in the power conversion efficiency has been reported by incorporating monofunctional poly (ethylene glycol) (PEG)-capped gold nanoparticle into the

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PEDOT:PSS layer in organic solar cells [19]. The gold nanoparticle solution was added into the PEDOT:PSS and then spin coated onto the glass substrate for the formation of the organic solar cell. Kim et al. has introduced another method of

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depositing silver nanoparticle using the spin coating processing [20]. The silver nanoparticles solution was dropped onto the substrate followed by spinning coating. After that, a thin layer of SiO2 was deposited on top of the silver nanoparticles to passivate the surface. Chen et al. has reported a 23 % enhancement in the power conversion efficiency for thin film amorphous

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silicon solar cell incorporated with silver nanoparticles using a similar spin coating method [21]. A silver metal mesh film with

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ordered pores introduced at the back surface of Si has been reported by Wu et al [22]. Closed packed polystyrene particles were initially deposited, followed by the deposition of silver seeds in the voids of the polystyrene particles, and the subsequent

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removal of the polystyrene particles [22]. It is noted that all the above mentioned approaches are low cost and simple to implement, indicating a promising future on the application of plasmonic effect in solar cell for enhanced light absorption.

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Todate, the incorporation of plasmonic nanospheres into Si/PEDOT:PSS hybrid solar cell has not been reported.

In this paper, we report for the first time a detailed study on the incorporation of Ag NS into planar hybrid Si/PEDOT:PSS thin film solar cells to improve the light absorption using optical simulation based on the finite element method. In contrast to most other studies in this field where the Ag nanoparticles are in direct contact with the Si material, the plasmonic scattering would be very different in the case of hybrid Si/PEDOT:PSS solar cell, due to the presence of a layer of PEDOT:PSS located between the Ag nanoparticles and the Si material. There is optical absorption in the PEDOT:PSS across certain bands of the solar spectrum. However, the optical absorption does not lead to photocurrent generation because of the short diffusion length of the carriers in the PEDOT:PSS. As a result, the optimum design for the Ag nanoparticles would be very different for the Si/PEDOT:PSS hybrid cells as compared to the conventional Si solar cells . The effects of the diameter and the structural periodicity of the Ag NS on light absorption enhancement are systematically investigated to provide a design guideline for the fabrication of high performance hybrid Si/PEDOT:PSS solar cells. It is found that light absorption is

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ACCEPTED MANUSCRIPT maximized at a Ag diameter of 270 nm and periodicity of 600 nm, which gives rise to the highest ultimate efficiency of 22.6 %. This reflects an improvement of ~ 23.8% as compared with planar hybrid Si thin film cells without the Ag NS.

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II. SIMULATION METHODOLOGY

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The commercial software High Frequency Structure Simulator (HFSS) based on the finite element method has been used

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to simulate the light absorption of Ag NS incorporated planar hybrid Si/PEDOT:PSS solar cell [23]. Figure 1(a) shows the schematic of the thin film hybrid cell structure used in this study. The height H of the planar Si thin film is fixed at 2 m. As we have previously demonstrated that the optimal thickness for the PEDOT:PSS layer (T) ranges from 60 nm to 80 nm, we

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have chosen T = 60 nm in the simulation [8]. The cell structure is optimized for light absorption by varying the diameter (D) and periodicity (P) of the Ag NS. The incident light with wavelength () ranging from 300 nm to 1100 nm is normally incident

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on the surface of the hybrid Si solar cell. By solving the Maxwell’s equations from the interaction between the incident light and the hybrid thin film structure, the spatial distribution of the energy flux can be obtained, from which the light reflectance (R), transmittance (T) and absorption (A) within Si, PEDOT:PSS and Ag NSs can be deduced. The optical constants of Si, Ag

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and PEDOT:PSS used in our simulation are taken from the literature [24, 25]. To determine the optimized geometric

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configuration for absorption of sunlight, the ultimate efficiency () is calculated as follows by assuming an internal quantum

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efficiency of 100% [26] :





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Eg P( ) A( )

300 

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 P ( ) d  0

In the above, Eg is the band gap of Si, E is the photon energy, λ is the incident light wavelength, A(λ) is the absorption efficiency and P(λ) is the spectral irradiance of the standard AM1.5G solar spectrum.

III. RESULTS AND DISCUSSION

Figures 2 (a), (b) and (c) show the light absorption in Si (ASi), PEDOT:PSS (APEDOT:PSS) and Ag (AAg) respectively, while and Figs. 2 (d) and (e) display the overall reflectance and transmittance of the hybrid structure with a fixed D/P ratio of 0.5 and varying P from 300 to 800 nm. The corresponding results for a planar hybrid structure without Ag NS are also plotted for comparison. For the planar cell, ASi is high for 300 nm <  < 600 nm, and it reduces significantly at longer wavelengths. For the cell incorporated with Ag NS having small P of 300 nm, ASi is poor over the range 300 nm <  < 600 nm, and is even lower than the cell without Ag NS. As the Ag NS diameter of this cell is relatively small at 150 nm, therefore mainly the dipolar

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ACCEPTED MANUSCRIPT mode has been excited, resulting in enhanced AAg and weak induced scattering of sunlight. This can be seen from the strong AAg of 47 % at the resonance frequency of 400 nm and the larger overall reflectance in the same wavelength range. As P increases to 400 nm, there are two AAg absorption peaks at 370 nm and 450 nm, indicating that higher order modes have been

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excited. Hence, the light absorption within Ag NS is reduced while the scattering effect is enhanced over the range 300 nm <

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 < 600 nm. Consequently, the light reflection is reduced and ASi is increased compared to the structure with P = 300 nm.

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Nevertheless, the result is still not better than the cell without Ag NS. When P is further increased to 600 nm, the resonance frequencies for absorption in Ag NS and scattering are further separated apart, with the latter shifts towards the center of the solar spectrum, resulting in strong scattering of light for  around 600 nm - 800 nm. This is consistent with the fact that

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induced plasmon resonance will be broader and red-shifted as the dimension of the metal nanoparticle increases [12]. Consequently, ASi is strong for 600 nm <  < 800 nm as compared to the cell without Ag NS. It is also noted that ASi for  < ~

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500 nm is lower than that of the cell without Ag NS due to the absorption within the Ag NS. Therefore, by varying the diameter of the NS, the scattering and absorption induced by the Ag NS can occur at different parts of the solar spectrum. With

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a further increase of P to 800 nm, ASi is weakened for  < 800 nm. It is however improved for  > 800 nm, which indicates that the induced plasmon mode has shifted to longer wavelength range, leading to strong scattering of light over this part of the

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spectrum. Nevertheless, as the solar irradiance for  > 800 nm is low, the overall light absorption within Si will be degraded.

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As the absorption coefficient of PEDOT:PSS is large for longer wavelength light, consequently a high absorption within the PEDOT:PSS film is observed, as shown in Fig 2 (b). From the results obtained, it is found that the optimum structural

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periodicity for maximum absorption of sunlight occurs at around P = 600 nm.

Figure 3 shows the optical characteristics of the hybrid Si/PEDOT: PSS cell at the optimum P of 600 nm and varying D/P ratios. When D/P is small at 0.1, the light absorption in Si is similar to that of the planar cell. In this case, D = 60 nm which is very small and the Ag NS are far separated apart. Hence, the Ag NS can be considered as isolated from each other and it is difficult for them to interact effectively to induce a strong resonance. When the D/P ratio is increased to 0.3, marginal absorption enhancement in ASi is observed for  > 600 nm as compared with the cell with D/P = 0.1, due to induced resonance by the NS. With a further increase in the D/P ratio to 0.5, a higher absorption is achieved over the range 500 nm <  < 800 nm which is around the peak of solar spectrum, as compared to the cell with D/P = 0.3. In addition, due to the strong scattering induced, the light absorption in the PEDOT:PSS film is also increased, as can be seen from Fig. 3 (b). When the D/P ratio is increased to 0.7, ASi decreases significantly compared to the cell with D/P = 0.5 for  < 700 nm. This is attributed to the following two reasons. Firstly, due to a larger surface area being covered with Ag NS at this large D/P ratio, light reflection increases significantly due to a strong backward scattering, as confirmed from the results shown in Fig 3 (d) [27]. Secondly,

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ACCEPTED MANUSCRIPT the center of the Ag NS is further away from the underlying Si surface at larger D/P ratio, resulting in a lower percentage of light scattered into the underlying Si film. From the results obtained, it is found that the optimum D/P ratio for maximum absorption of sunlight occurs at a moderate range of D/P of about 0.5.

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To more comprehensively determine the effects of the structural parameters of the cells on sunlight absorption, the

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ultimate efficiency η of the cells incorporated with Ag NS of different diameters are calculated and plotted as a function of the

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D/P ratio, as shown in Fig. 4. For D/P  0.2, η is slightly over 18 % for all cells with different P, which is also comparable with that of the cell without Ag NS of 18.25 %. This indicates that at small D/P ratios, the Ag NS are effectively isolated and not able to induce strong plasmonic effect. Hence, there is negligible light absorption enhancement. When P is small at 300 nm

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and 400 nm, it is observed that η decreases with increasing D/P ratio, due to light being absorbed within the Ag NS. At larger P, η generally increases and reaches a peak, before it decreases with increasing D/P ratio. The optimal light absorption for cells

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with different P occurs within the range 0.4 < D/P < 0.5. In terms of varying P, it is also observed that η improves with P and peaks at P = 600 nm, before it decreases at large P. Therefore the optimum structure has P = 600 nm and D/P = 0.45, and

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achieved the highest η of 22.6 %.

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Figure 5 shows the light absorption of the hybrid Si/PEDOT:PSS cells incorporated with Ag NS on top as a function of the

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Si film thickness. It is clearly seen that, compared with the planar cell without the Ag NS, the light absorption is consistently higher over a wide range of Si film thickness from 500 nm to 8 µm. The improvement in light absorption though is noted to diminish with increasing Si film thickness, which is expected as thicker films are already intrinsically better in light absorption.

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Still, there is about 6% improvement observed for the thickest 8 µm Si film investigated, which attests to the usefulness of incorporating Ag NS even for thicker Si/PEDOT:PSS cell.

IV. CONCLUSIONS

In conclusion, we have conducted a systematic study of hybrid Si/PEDOT:PSS cell incorporated with silver nanospheres on top. The impact of varying the structural periodicity and silver nanosphere diameter on the light absorption of the hybrid cell is investigated. It is found that due to the strong scattering effect of the Ag NS, the light absorption is significantly increased. At the optimum structural periodicity of 600 nm and diameter/periodicity ratio of 0.45, the highest ultimate efficiency of 22.6% has been obtained, which is 23.8% higher than that of the hybrid cell without the Ag NS. Therefore, the simulation results revealed that the plasmonic effect arising from the silver nanospheres introduced is effective in enhancing the optical absorption of the hybrid Si/PEDOT:PSS cell to further improve its efficiency.

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ACCEPTED MANUSCRIPT ACKNOWLEDGMENT We acknowledge the financial support from the Economic Development Board of Singapore (EDB), the Ministry of Education

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(MOE) of Singapore Tier 2 Grant MOE2012-T2-1-104 and World Future Foundation (WFF).

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ACCEPTED MANUSCRIPT List of figure captions Figure 1: Schematics of the hybrid Si/PEDOT: PSS cell structure incorporated with Ag nanospheres on

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the top surface.

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Figure 2: Light absorption within (a) Si film, (b) PEDOT: PSS film and (c) Ag NS, and (d) reflectance and (e) transmittance of the hybrid Si/PEDOT: PSS cells with a fixed D/P ratio of 0.5.

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Figure 3: Light absorption within (a) Si film, (b) PEDOT: PSS film and (c) Ag NS, and (d) reflectance

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and (e) transmittance of the hybrid Si/PEDOT:PSS cells with a fixed P of 600 nm.

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function of the D/P ratio.

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Figure 4: (a) Ultimate efficiency of the hybrid Si/PEDOT: PSS cells with different diameters D as a

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Figure 5: (a) Absorption spectra and (b) ultimate efficiency of the hybrid Si/PEDOT: PSS cells with

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different Si thin film thicknesses.

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ACCEPTED MANUSCRIPT Highlights

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Model the light absorption of hybrid Si/PEDOT:PSS solar cell with Ag nanosphere The impact of Ag structural dimension on the light absorption is simulated The maximum ultimate efficiency of 22.6% is achieved

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