ISSN 1995-0780, Nanotechnologies in Russia, 2009, Vol. 4, Nos. 34, pp. 237243. Pleiades Publishing, Ltd., 2009.

. Original Russian Text S.A. Gavrilov, A.A. Dronov, V.I. Shevyakov, A.N. Belov, E.A. Poltoratskii, 2009, published in Rossiiskie nanotekhnologii, 2009, Vol. 4, Nos. 34.

EXPERIMENT

Ways to Increase the Efficiency of Solar Cells with Extremely Thin Absorption Layers
S. A. Gavrilova, A. A. Dronova, V. I. Shevyakova, A. N. Belova, and E. A. Poltoratskiib
Moscow Institute of Electronic Engineering (Technological University), proezd 4806 5, Zelenograd, Moscow, 124498 Russia b Lukin Scientic Research Institute of Physical Problems, Zelenograd, Moscow, Russia e-mail: pcfme@miee.ru AbstractThe effect of design parameters, electrical properties, and technological modes of formation on the efciency of the photoelectrical conversion of solar cells with extremely thin absorbing layers based on the SnO2:F/TiO2/In2S3/InxPb1 xS/CuSCN is investigated. It is shown that both a decrease in resistance due to an increase in roughness and a decrease in the average grain size of the TiO2 lms is attained with deposition using the solgel method under conditions of increased humidity. The use of Ni as the contact metal to a planarizing CuSCN layer provides the reduced value of the transient resistance. The optimization of the sequential resistance of the TiO2 lm and contact resistance to the CuSCN layer provided an increase in the efciency of photoelectric converters by a factor of more than four. The structures of solar cells formed in optimal technological modes showed the following characteristics: Jsc = 9 mA/cm2, Uoc = 720 mV, and they had an efciency of 2.9%. DOI: 10.1134/S1995078009030112
a

INTRODUCTION Energy storage, production, and conversion are some of the main directions in the development of science and technology; in these elds, considerable economic growth is expected thanks to the introduction of nanotechnologies. This is realistic as long as conditions of mass production at low prime cost of production and extended availability of the developed technologies are provided. The creation of photoelectric converters based on nanocrystalline titanium oxide is a striking example of incorporating nanotechnological designs in mass production [1]. Thanks to the low prime cost of their production and their unique massdimensional characteristics, such solar cells built on exible substrates have become the foundation for creating portable charging devices. The increase in the cost of conventional energy sources and the outlined decit of silicon wafers, which are conventionally the basis for solar cells, are a problem for the developers of photoelectric converters trying to produce technologies that can be alternatives to silicon technology. The record efciencies of solar cells based on IIIV heterostructures do not allow for their mass production because of high production expenses and the necessity of large initial investments needed to form the production infrastructure. In both cases the reason for the high prime cost of electrical energy, which is produced by the direct transformation of the optical energy to electric, is the high technological expense for materials of single-crystal substrates [2]. One way to solve this problem is by developing thinlm elements on lower-cost carriers such as metal and polymer ribbons [3]. Among the thin-lm elements, the

structures designed based on nanocrystalline oxides occupy a special place. In them, the effective spatial separation of charge carriers is realized in the nanometer-scale absorption layers, while the high values of the photocurrent are achieved due to the developed surface. This concept is shown in industrial samples by the example of the Grtzel batteries [4]. However, the presence of liquid between the electrodes considerably decreases the range of the working temperatures of devices. Replacing liquid with gel electrolytes [5] still did not allow one to attain protable levels of efciency, which should exceed the current prime cost of building by 56%. This work is devoted to developing a design for a solar cell with an extremely thin absorption layer (SCETAL) in which the electrolyte is absent and all functional layers are solid. The concept of solid-state SCETALs was suggested in [6] and was called an eta cell (extremely thin absorber cell). In these structures materials characterized by a high defectiveness are used, which considerably increases the recombination rate in the carrier bulk. The efciency of eta-cells increases as the thickness of the layer that absorbs the light decreases to sizes comparable with the diffusion length of charge carriers; i.e., for highly defective lms, they decrease to several tens of nanometers. However, this leads to a decrease in the number of absorbed photons per time unit in the active layer. This problem is solved thanks to the use of transparent conducting porous matrices based on titanium dioxide or zinc oxide nanocrystals with electrontype conduction. These matrices increase the effective area of heterojunctions by two orders of magnitude and substantially decrease the optical losses thanks to a

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6 5 4 3 2 1

hv
Fig. 1. Transverse section of the thin-lm structure of the photoelectric converter based on the SnO2:F/FiO2/In2S3/InxPb1 xS/CuSCN structure.

decrease in the reecting ability and the multiple refraction in the porous structure. The eta-cell concept was developed by several European research groups in France and Germany [79]. The authors of these studies used TiO2 deposited by the solgel method or electrochemically deposited ZnO lamentous nanocrystals as the n-type transparent electrode, which is called an electron acceptor. To form the absorbing layer, electrochemical or chemical absorption from aqueous solutions was used. The maximum efciency attained in these works was no higher than 1.5%. The lower-than-excepted efciency was a consequence of the fact that the chemical and electrochemical deposition methods did not provide a conform coating of the nanostructured carrier by the material of the absorbing layer. To solve this problem, we used the method of molecular layering (ML), the principles of which were developed in the mid-1960s under the direction of Aleskovskii [10]. The main idea of the ML method consists of providing conditions for irreversible chemical reactions between the functional groups on the surface of solid and externally supplied reagent molecules. Growing the layers of the specied thickness is done by the multiple alternate treatment of the surface of the deposited material, which provides the formation of functional groups of active atoms on the surface which are able to react with new portions of reagents. There is a method of achieving chemical assembly from solutions called the method of ion layering (IL) [11, 12]. In English-speaking literature, this method is called successive ion layer adsorption and reaction (SILAR). The formation of semiconductor compounds by the method of molecular layering is a cyclic process which involves four stages, namely, the adsorption of cations from the cation precursor solution; the removal of physically adsorbed complexes by washing in water; the chemisorption of anions from the anionic precursor solution, which is accompanied by the reaction of the formation of the chemical compound; and the removal of the reaction products by washing in water. The thickness of the

lm formed during such deposition is controlled by the amount of layering cycles. The eta cell involves a transparent substrate with a conductive coating, a nanostructured electron acceptor, an ultrathin absorbing layer, and a hole acceptor. The selection of materials for such a structure is performed based on the band energy diagram of the multilayered heterostructure, which contains a built-in electric eld providing the separation of photogenerated electrons and holes. Our previous investigations showed that in the SnO2:F/TiO2/In2S3/InxPb1 xS/CuSCN system, in which the electron acceptor is TiO2, the role of the absorbing layer is played by the In2S3/InxPb1 xS heterostructure; the hole acceptor is CuSCN, providing the highly efcient separation of charge carriers [13, 14]. In this work we present the results of investigations which substantiate the necessity of further optimizing the constructive parameters, the electrical properties, and the technological modes of formation of functional SCETAL (eta cell) layers based on the SnO2:F/TiO2/In2S3/InxPb1 xS/CuSCN heterostructure. EXPERIMENTAL Figure 1 represents the structure of the transverse section of eta cells studied in the present work. We used energy-saving architecture glass (layer 1) with a lm of conducting SnO2:F deposited (layer 2) on the surface as substrates for the formation of eta cells. Prior to the deposition of the rst TiO2 layer, the substrates were subjected to special liquidchemical treatment, which provided the removal of organic and inorganic pollutions from the surface. The deposition of TiO2 (layer 3) was performed by the method of controllable immersion of the vertically arranged substrate in a 10% (vol. fraction) solution of titanium(IV) isopropoxide Ti(OC3H7)4 in isopropanol CH3CH(OH)CH3. Vibrationless immersion with a rate of 120 mm/min was performed using a KSV LMX2 automated complex (KSV Instruments Ltd., Finland) for the layer-by-layer deposition of the lms by the
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WAYS TO INCREASE THE EFFICIENCY OF SOLAR CELLS Table 1. Parameters of the electron structure of materials entering the composition of the eta cells under study Semiconductor SnO2 : F TiO2 InOxS1 x x=0 x = 0.07 x = 0.14 InOxS1 x :Pb CuSCN Conduction type n+ n n Electron afnity, eV Work function, eV 4.7 4.3 4.65 4.25 3.85 3.3 1.9 4.7 5.2 4.7 4.7 4.7 4.7 5.3 Band gap, eV 3.9 3.2 2.1 2.5 2.9 1.8 3.4 Reference [15] [4] [15]

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p p+

[16] [6]

immersion method. Films with different microstructures were obtained by varying the relative humidity of the surrounding atmosphere in the deposition chamber. Dust particles can ingress on the deposited surface during the deposition. Therefore, deposition was performed in two stages with obligatory intermediate annealing in air at 450C for 20 min. The intermediate annealing provided the decomposition of the dust material under the effect of high temperature. The repeated deposition provided the healing of transparent pores formed in the TiO2 lm in the course of the preceding annealing. In the course of the subsequent annealing at 450C for 1 h, oxide with an anatase crystal structure was formed. Of all the polymorphs of TiO2, it has the highest electron diffusivity [4]. The In2S3 buffer layer (layer 4), which provides low recombination losses, was deposited by the IL method from solutions of 10 mM InCl3 and 10 mM Na2S (20 IL cycles). The absorbing InxPb1 xS layer (layer 5) was obtained similarly from the solution of the cation precursor containing 9 mM InCl3 and 1 mM Pb(CH3COO)2 (30 IL cycles). Then the annealing was performed at 150C for 1800 s in air. The p-type contact (acceptor of holes) was formed on a specially developed installation that lls in the space between the nanocrystals with the degenerate CuSCN semiconductor (layer 6). For this purpose, the substrate was placed on a mobile stage heated to 80C and 0.07 M of CuSCN solution in propylsulde was supplied using a special dosing unit. At the nal stage, metal contacts to the SnO2:F and CuSCN layer were formed by thermal evaporation in a vacuum (layer 7). To reveal the correlation of conductivity of the basic TiO2 layer with the technological modes of its deposition, local metal contacts were formed on the oxide surface and the reduced electrical resistance (/cm2) between the local metal contact and SnO2:F lm was determined. Using atomic force microscopy (an SZM-Solver 4R microscope was used), the surface morphology of the TiO2 lms was investigated in a semicontact mode and the average surface roughness was determined on area 1 1 m in size.
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To investigate the IV characteristics, the variable load resistance rated in a range of 01 M was connected immediately to the contacts of photoelectric converters. During the measurements, the samples were illuminated from the substrate side by an optical source with an emission power of 100 mW/cm2. Based on the measured IV characteristics, we determined the open-circuit voltage Uoc, the density of the short-circuit current Jsc, and the maximum value of the specic output power Pm as the multiplication of the current by the voltage. The established Pm determines the efciency of the solar cell according to the known relation Pm -, = ----Ps where Ps is the specic power of the incident solar radiation equal to approximately 100 mW/cm2. In determining the characteristics of solar cells, the lling factor FF of the currentvoltage characteristic is important. It is determined by the following formula: Pm FF = -------------- . J sc U oc The values of Uoc, Jsc, and FF allow one to completely characterize the parameters of solar cells. To determine the parameters of ohmic contacts of metal to CuSCN, we used the method of the Kelvin resistor [15]. This method allows one to determine the transient resistance of the contact with one measurement; it is independent of the geometric sizes of other contacts, other than the measuring one; and it provides increased accuracy in determining the specic transient resistance of contacts. RESULTS AND DISCUSSION Based on the known data on the electronic properties of the materials used in this work (Table 1), we constructed a schematic of the mutual arrangement of the edges of the bands of the allowed states and the Fermi levels (Fig. 2). In constructing the diagram, we used the
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CuSCN

3.4 eV 1.8 eV

Fig. 2. Energy characteristics of the layers entering the composition of the SnO2:F/TiO2/In2S3/InxPb1 xS/CuSCN structure.

solar cell and contact resistances at the boundaries of heterojunctions. Taking into account that SnO2:F and CuSCN are the degenerate semiconductors and the thicknesses of the layers of In2S3 and InxPb1 xS are smaller than the diffusion length of charge carriers [13], we can expect that TiO2 mostly contributes to the series resistance. According to existing notions, the charge transport in TiO2 is performed via diffusion [18, 19]. The electron transport is performed through the defect states, which are conditioned by the presence of atomic vacancies of oxygen in the near-surface layers [20, 21]. Consequently, nanocrystalline lms with large specic surface areas possess the best conductivity [20]. The way TiO2 with the solgel deposition is formed is described by the following sequential reactions TiOR + H2O TiOH + ROH, TiOR + TiOH TiOTi + ROH, TiOH + TiOH TiOTi + H2O, where R are the C3H7 groups with the use of titanium tetraisopropoxyde as the precursor. From the general theory of kinetics of chemical reactions, the rate of such process increases as the concentration of titanium tetraisopropoxide and water vapor pressure in the surrounding medium increase during the synthesis of the lms by the method of pulling the substrate from the melt. The hydrolysis rate determines the microstructure of deposited lms. To obtain highly dispersed systems, it is necessary to achieve high supersaturation with a limited growth rate of forming particles [22]. In the course of pulling the substrate from the solution, a meniscus is formed in the region of the solution air interface. The thickness of the meniscus and, consequently, the amount of titanium isopropoxyde on the surface unit are determined by the kinetics of wetting and decrease as the pulling rate decreases. The concentration supersaturation in such a process is provided due to the evaporation of the solvent (isopropanol) and adsorption of water vapors. It is evident that high supersaturation by water molecules can be provided thanks to an increase in the humidity of the atmosphere in the deposition installation. The decrease in the growth rate of the already-formed nuclei is achieved due to the depletion of the liquid layer during precipitation. Table 2 represents the values of structural parameters and the reduced electrical resistance of the TiO2 layer obtained at different humidity values of the atmosphere under conditions of an identical deposition rate of 120 mm/min. The values of efciency of photoelectric converters created with the use of the corresponding TiO2 layers are also presented here. We used Ni as the contact metal to CuSCN. Using the AFM (Fig. 3) it was established that, as humidity increases, the roughness of the lms increases
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data on the location of energy levels of InOxS1 x at x = 0.07 based on the data on the oxygen content in the lms obtained in [13]. The presented band diagram indicates that the electrons and holes, which are generated during the irradiation, will move with a high probability preferentially towards SnO2:F and CuSCN, respectively. It is known that the efciency of actual solar cells depends on the recombination at the boundaries of junctions and the sequential and shunt resistances of the element [16, 17]. The currentvoltage characteristic of the solar cell is described by the equation q ( U J Rs ) U JR J = J 0 exp -------------------------- 1 + ------------------s J L , kT Rp (1)

where J0 is the saturation current, Rs is the series resistance, and Rp is the shunt resistance. It follows from Eq. (1) that the efciency decreases with an increase in recombination losses (which can be judged by the value of J0). Up to now, no exact data are available on the distribution of the electric eld at the boundaries of heterojunctions under consideration. Therefore, from this viewpoint, it is rather difcult to judge the main channels of recombination losses in the structure. However, we can evaluate the power losses in the eta cell based on evaluations of the magnitude of the series resistance of the layers. According to Eq. (1), Rs most strongly affects the shape of the IV characteristic at large currents and high bias voltages, while the effect of Rp manifests itself at low voltages, where the current owing across the junction is small compared with the shunt current. Power losses exist in any actual solar cell, because Rs > 0 and Rp < . To provide little power loss, it is necessary to decrease Rs and increase Rp. In this case, series resistance plays the decisive role in the operation of the solar cell. The value of Rs for the eta cell is formed by the resistances of the layers entering the composition of the

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and the average size of the crystallites constituting the lm decreases. As expected, the resistance of the TiO2 lms decreases as the humidity increases. The decrease in the resistance of the TiO2 lms increases the efciency of the eta cell. As noted above, the contribution to the series resistance of actual solar cells is also introduced by the ohmic contacts to the planarizing layer of the hole acceptor. This quantity also affects the output power of the solar cells and, nally, the efciency value. In the literature there are almost no data on selecting materials for building ohmic contacts to the planarizing layer of the hole acceptor based on CuSCN and on the values of the transient resistance of ohmic contacts of various metals to it. The qualitative characteristics of the ohmic contacts are the transient resistance Rc and specic transient resistance c.
(a) nm 100 80 60 40 20 500 nm (b) 0 nm 12 10 8 6 4 2 500 nm 0

Table 2. Values of the reduced resistance of the TiO2 layer Formation mode of TiO2 1 2 60 25 150 46 1.2 3 80 110 80 2.32.4 2.9

Relative humidity in a chamber, % 30 Roughness, nm 10 Average grain size, nm 250 1213 Reduced resistance of the TiO2 layer, /cm2 , % 0.95

We built test structures of solar cells in which In, Cu, Au, and Ni were used as contact materials to the planarizing CuSCN layer. All samples were formed based on titanium oxide deposited at the highest atmospheric humidity. Table 3 represents the measured average values of resistivity of ohmic contacts, open-circuit voltages, densities of the short-circuit current, lling factor, and efciency of the corresponding eta cells.

Fig. 3. Two-dimensional AFM images of the surface and transverse section of the TiO2 layer deposited at various humidity values of the surrounding medium: (a) 30%, (b) 80%. NANOTECHNOLOGIES IN RUSSIA Vol. 4 Nos. 34 2009

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Table 3. Results of the measurements of the test-structure characteristics of solar cells Material of the ohmic contact with the planarizing layer In Cu Au Ni Characteristics of the eta cell L , cm2 0.70.8 0.4 0.1 0.050.07 Uoc , mV 550 600 680 720 Jsc , mA/cm2 4 5 8 9 FF, rel. units 0.3 0.35 0.4 0.45 , % 0.7 1.1 2.2 2.9

It follows from the obtained data that the value of the transient resistance of ohmic contacts to the CuSCN-based planarizing layer of hole acceptor decreases as the work function of the used metals increases. This can be explained by the fact that CuSCN is a degenerate ion p-type semiconductor, and the classic Schottky formation theory of the potential barrier in the metalsemiconductor compound is valid for it. The height of the energy barrier qb is determined by the following expression in this case [23]: q b = E g q ( m ), (2) where m is the work function of the metal, and Eg and are the band gap and electron affinity of the semiconductor. It is known that when metal contacts the semiconductor, the transient resistance increases exponentially as the values of qb increase [23]. According to the data presented in Table 1, the band gap of CuSCN equals 3.4 eV and the electron afnity is 1.9 eV. The values of the work function for In, Cu, Au, and Ni are 4.2, 4.3, 5.2, and 5.3 eV, respectively; according to expression (2), the potential barrier height for them is 1.1, 1.0, 0.1, and 0 eV, respectively. The decrease in contact resistance alongside the increasing potential barrier height between the metal and CuSCN explains the increase in the lling factor of the IV characteristic of the eta cell. Along with this, a simultaneous increase in the values of Uoc and Jsc is observed. These quantities are associated with each other by the following equation at JL J0 [18]: J sc JL kT kT U oc = ----- ln ---- + 1 ----- ln ----- . J 0 q J0 q (3)

recombination losses decrease when there is a decrease in the barrier height at the metalsemiconductor interface. A simultaneous increase in the values of FF, Uoc, and Jsc leads to a substantial increase in efciency , which is determined by the expression U oc J sc = FF ----------------- . Ps CONCLUSIONS The performed investigations showed that the functioning of eta cells follows the main regularities established for conventional photoelectric converters. The performed optimization of only two parameters, like the series resistance of the TiO2 lm and the contact resistance to the CuSCN layer, provided increasing efciency by a factor of more than four. The planned directions of the further developments, specifically, an increase in the region of the surface of heterojunctions due to the use of methods of directed control over the morphology of TiO2 and the optimization of the electronic and optical properties of chalcogenide semiconductors, should allow it to attain a level of > 5%, which, according to experts, is the protability threshold for this type of solar cell. ACKNOWLEDGMENTS This work was performed in the context of the Federal Target Program Investigating and Developing Priority Directions of the Development of Russian Scientic and Technological Complex for 20072012, SC no. 02.513.11.3151. REFERENCES
1. www.G24i.com. 2. Basic Research Needs for Solar Energy Utilization: Report of the Basic Research Sciences Workshop on Solar Energy Utilization, Argonne National Laboratory, Argonne, IL, United States, 2005 (Argonne National Laboratory, Argonne, 2005). 3. K. L. Chopra, P. D. Paulson, and V. Dutta, Thin-Film Solar Cells: An Overview, Prog. Photovoltaics 12, 69 92 (2004).
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Because all the studied eta cell structures were identically built, except for the selection of the material for the ohmic contact, the photocurrent density for them should remain almost invariable. Consequently, the increase in Uoc and Jsc is associated with a decrease in J0. This decrease is easily explained by the consideration of the generationrecombination processes in the depleted CuSCN region. According to the Shockley theory, at rst approximation, J0 ~ W, where W is the width of the space-charge region [23]. In turn, W ~ (qb)1/2. Consequently, the width of the space-charge region and

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