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JOURNAL OF APPLIED PHYSICS

VOLUME 89, NUMBER 4

15 FEBRUARY 2001

Quantum dot solar cells


V. Aroutiounian, S. Petrosyan,a) and A. Khachatryan
Department of Physics of Semiconductors, Yerevan State University, Yerevan, 375049, Armenia

K. Touryanb)
National Renewable Energy Laboratory, Golden, Colorado 80401

Received 25 August 2000; accepted for publication 14 November 2000 The quantum dot solar cell concept is proposed as a scheme for increased solar cell efciency. A theoretical model is presented for a practical p i n quantum dot solar cell, based on the self-organized InAs/GaAs system. The advantages of using the quantum dot in the active region for photon absorption in the long-wavelength part of the spectrum, leading to cell efciency, is discussed. 2001 American Institute of Physics. DOI: 10.1063/1.1339210

I. INTRODUCTION

Recently several design schemes have been proposed to increase the power conversion efciency of photovoltaic devices. By using two or more p n solar cell junctions, tandem cells made of different semiconductors, a multiheterojunction design yields a better match to the solar spectrum than a single-junction cell and may provide the efciency of conversion greater than 50%.1 In fact, two-junction solar cells, reported in Ref. 2, have been fabricated using GaAs and InP semiconductor alloys, providing the highest power conversion efciency of 30.2% for AM 1.5 spectra. Such high efciency, which is very close to the theoretical limit,3 has been achieved in the structure with optimized band gaps and with good current and lattice matching. Taking into account the recent advances in different optoelectronic devices, particularly in semiconductor lasers,4 attained by the molecular-beam epitaxy and metalorganic chemical deposition growth techniques, it would also seem appropriate to consider whether a low dimensional such as quantum dot p i n structure could provide a new approach to the high-efciency solar cell problem. The quantum well QW p i n solar cell was the rst low-dimensional structure proposed by Barnham and Duggan5 as an alternative to conventional tandem approaches to higher conversion efciency. The proper application of the multi-QW systems in the development of solar cells can potentially increase their efciency. In GaAs/Alx Ga1 x As p i n structure with inserted QWs, Paxman et al.6 have observed a signicant enhancement in the short-circuit current and energy conversion efciency in comparison with control samples that are identical in all respects except that they do not have QWs. The QW solar cell is based on the principle that, by suitable choice of various widths and depths of QWs, the absorption can take place at the different quantum energy levels, thereby reducing thermalization losses. In the QW solar cells the photocurrent and output voltage can be individually optimized, because the absorption edge and spectral characteristics can
a b

be tailored by the width and depth of QWs, while the output voltage is still primarily determined by wider band gap bulk material. Here we propose a concept of a device, namely the quantum dot QD solar cell, which provides direction to the high-efciency solar cell problem. A theoretical model is presented for a practical p i n QD solar cell built on the base of the self-organized InAs/GaAs system.4 We will study the advantages of the use of QDs in the active region for photon absorption in the long-wavelength part of the spectrum and increase the power conversion efciency.
II. MODEL

Electronic mail: stpetros@server.physdep.r.am Electronic mail: ken touryan@nrel.gov 2268

The model proposed is based on a p i n cell structure Fig. 1 a whose energy band diagram, shown in Fig. 1 b , includes multiquantum-dot layers in the intrinsic region of the structure to enhance the photocurrent. The effective band gap for absorption E eff will be determined by the lowest conned states of QDs. Note the InAs/GaAs system can cover a range of band gaps that is of particular importance for solar cells.4 The internal quantum efciency for the collection of charge carriers photoexcited in the QD can be enhanced using, for example, the phenomena of the resonant tunneling. High-density array of QDs can be fabricated using the well known stacking technique in the Stranski Krastanow growth mode.7 Usually, the strain elds of the lower QDs layer extended into the barrier material cause the vertical alignment of QDs. Due to the strong vertical coupling between QDs, electronic states can acquire a wire-like character.8 Therefore, high internal quantum efciency for the collection of carriers photoexcited in the QDs can occur as a result of channeling the electrons and holes through the coupling between aligned QDs. This effect allows one to separate and inject the generated electrons and holes in QDs, into adjacent p and n regions with high efciency. By changing the deposition mode the intermediate-layer thickness and the repetition number of island layer one can tune the size and shape of the InAs islands and thus the quantized energy levels to control the light absorption spectrum. Usually as a result of multiple-layer stacking the island density decreases monotonically with the number of periods of the
2001 American Institute of Physics

0021-8979/2001/89(4)/2268/4/$18.00

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J. Appl. Phys., Vol. 89, No. 4, 15 February 2001

Aroutiounian et al.

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black body curve, corresponding to a temperature of 5760 K. Hence, the spectral distribution of the solar ux incident on the cell surface under the condition 1 Sun, 1.5 AM can be written as9 F 3.5 1021
4

exp

hc kT 1

photon , cm2s m

where h is the Placks constant, c is the velocity of light, k is the Boltzmanns constant, and T 1 5760 K. 11 The excess electron density n(z) in the p-type layer satises the following equation: d2 n z dz 2 n z Ln G p ,z Dn 0, 3

where L n and D n are the electron diffusion length and diffusion constant, respectively. The boundary conditions for Eq. 3 represent the requirements of vanishing the excess electron density at the edge of the depletion range n(z p ) 0 and that surface recombination absorbs the current at the front surface (z 0) of the p layer with surface recombination velocity S n Dn
FIG. 1. a Schematic structure of QD solar cell. b Energy-band diagram of p i n QD solar cell, showing the p -type layer (0 z z p ), intrinsic layer with QDs (z p z z p z i ) and n -type layer (z p z i z z p z i z n ). Depletion layers in p and n layers are neglected.

d n dz

Sn n 0 .
z 0

Equation 3 can be solved analytically for the photogenerated electron current density at z z p . Finally, we have jn eF exp 1 R z pa n Ln sinh an an
2

multilayers and tends to saturation. The mean size of buried islands and their homogenization increases as the number of periods increases.7 Typically the dot size is around 10 nm and dot area densities range between 2 1010 and 1011 cm 2. The dot layers are separated by 510 nm barrier layers, the number of periods of InAs/GaAs multilayers9 can be more than 100 and therefore the real dot density in the active i region can be 1017 cm 3. Our model for the calculation of the power conversion efciency will include realistic estimates for the light absorption, photocurrent generation in pand n-type GaAs regions and InAs/GaAs QDs i-region, as well as the surface and bulk minority-carrier recombination and junction generation-recombination currents.
III. PHOTOCURRENT

bn an cosh zp Ln 5

bn an zp Ln ,

1 b na n

where e is the absolute value of the electronic charge, n cosh(zp /Ln) bn sinh(zp /Ln) 1, b n S n L n /D n , and a n( ) ( )L n . The total photocurrent collected by p type is equal to
p Jn
1

jn

d ,

We calculate the photocurrent by solving the minority carrier transport equation at room temperature in uniform p-type and n-type GaAs eldless regions. In the p-type layer, extending from the exposed surface at z 0 to the edge of the depletion region at z z p , the distribution of minority carriers is governed by the standard equations for electron current density and electron continuity. For the incident light of wavelength and ux F( ) the electronhole generation rate at a depth z, is equal to Gp ,z 1 R F exp z . 1

is where R( ) is the surface reection coefcient and the light absorption coefcient of GaAs.10 For further calculations, we use the model of solar spectrum described by a

where 1 0.9 m is the GaAs absorption cut-off wavelength. The current collected from the n-type region is determined in a similar manner. To write the generation term we have to take into account the attenuation of the light through the p-type and intrinsic region of the GaAs containing QDs made of InAs. The InAs on GaAs QD system usually shows an absorption in the range of 1.11.4 eV.4 Carrier connement in a QD quantizes their energy spectrum into a series of discrete levels, which is reected in the absorption spectra. Usually the absorption edge is shifted to higher energies due to strong connement effect and -like peaks are produced in the spectrum corresponding to different holeelectron level transitions.4 But due to a typical dot size uctuation of 10%, the absorption spectrum usually is inhomogeneously broadened. For the calculations, we will use the experimental

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J. Appl. Phys., Vol. 89, No. 4, 15 February 2001

Aroutiounian et al.

data for the absorption spectra of the InAs/GaAs QD ensemble.4 Because the absorption band of QDs does not overlap with the absorption band of barrier material of GaAs, we can present the photocarrier generation rate in QDs inside the i region as GD ,z F exp 1 R
D D

z zp ,

where D ( ) is the QDs ensemble absorption coefcient. Then the photocurrent collected from the QDs is equal to jD e
zp zi zp

current losses may be expected to rise with increasing i-layer width. In this case the proper calculation of the short-circuit current, and hence overall efciency, for the QD cell requires a detailed treatment of electronic band structure, carrier emission, capture, and recombination mechanisms in the multilayer QD region. However, note that due to the competition between the light absorption and recombination losses in the i region should there be an optimum number of QD layers for best response. But these questions are beyond the scope of this article and will be discussed elsewhere.

GD

,z dz.

8
IV. EFFICIENCY CALCULATIONS

There is also some photocurrent generation in the GaAs barrier regions within the i region jB e
zp zi zp

Using the standard superposition model of solar cell, the current density can be presented as J J sc J 0 exp eV/kT 1 , 14

GB

,z dz.

To write the generation rate in the barrier region we shall take into account that only the fraction (1 V D n D ) of i region is occupied by the GaAs barrier region GB ,z F exp exp 1 R z p 1 n DV D 1 n DV D z zp . 10

where J 0 is the reverse saturation current of the junction. The reverse saturation current is formed by the minority carriers that are generated at the depletion layer edges ( j s1 ) and in the interior of the i region ( j s2 ) due to thermal excitation. Such a current is controlled by the band gap of GaAs E gB and average band gap of the i region E eff 1 n D V D E gB n D V D E gD , connement energy. 15

where E gD is the band gap of QDs, which has to be taken as E g InAs Detailed balance between the incident and emitted radiation in thermal equilibrium give the following expression for the thermal generation current in the i region:12,13 j s2 A eff exp E eff . v kT 16

Here V D is the single QD volume and n D is the QDs volume density. For an intrinsic region, being free of the traps, the built-in electric eld sweeps the carrier across the depletion region and through the QDs channels. Therefore, the net photocurrent generated by light of given and collected from i region is equal to ji jD jB . 11

Total photocurrent collected from the i region is equal to Ji e


1

jB

2 1

jD

12

2 Here v is the ideality factor, A eff e 4 n2kT/c2h3 Eeff, and n is the average refractive index of the i region. The other dark current component j s1 has the usual form

where the integral is extended over the absorption wavelength interval of the QD and GaAs regions. If we allow some recombination losses for the intrinsic region then we must scale down the photocurrent.6 Therefore, we can write the short-circuit current density of the cell as
p J sc f i J n J n J i , p

j s1 A exp where A eN c N V

E gB
v kT

17

Dp N DL p

Dn . N AL n

18

13

where the transport factor f i represents the mean probability of an electron or hole crossing the i region without capturing and recombination. We have presented here only a general overview of photocurrent generation in a device. Therefore, we assumed the effective diffusion-drift length of carriers to be larger than the i-layer width so that most of photocarriers generated in quasinatural regions and inside the i region are swept out by the junction eld without suffering recombination losses ( f i 1). For an intrinsic region with a larger thickness the recombination processes governed in practice by background impurity levels limit the maximum number of QD layers and

Here N c and N V are the effective density of state in GaAs, N D and N A are the donor and acceptor concentration in the n-type and p-type regions, correspondingly. We can now calculate the cell power conversion efciency at the maximum power point. Finally, we have V optJ opt P0 kT J e t opt 1 / P 0 , t J e opt sc 0 19

where P 0 116 mW/cm2 is the incident solar ux for 1 sun, AM 1.5 condition and t opt has to be dened from the equation e t opt 1 t opt 1 J sc . J0 20

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J. Appl. Phys., Vol. 89, No. 4, 15 February 2001 TABLE I. The parameters used in calculations. Unit of measure cm s cm s m m cm2 s cm2 s cm3 cm 3 eV eV cm cm m m m fi
1

Aroutiounian et al.

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Parameters surface recombination velocity for electrons (S n ) surface recombination velocity for hole (S p ) diffusion length of electrons (L n ) diffusion length of hole (L p ) diffusion constant of electrons (D n ) diffusion constant of hole (D p ) volume of QD (V D ) volume density of QDs (n D ) surface reection coefcient R( ) band gap of GaAs (E gB ) band gap of QDs (E gD ) acceptor concentration (N A ) donor concentration (N D ) p-region length (z p ) i-region length (z i ) n-region length (z n ) transport factor

Value 6 103 6 10 2 3 200 10 1.77 1.7 0.1 1.4 0.95 1.4 1.7 0.8 3 2 1
3

35.1 mA/cm2 and V oc 0.753 V. Accordingly, in the rst case the cell efciency is expected to be 25%, while 19.5%. without QDs it is equal to
V. CONCLUSION

1 1

10 1017

18

The concept of QD solar cell has been described. It has been observed from the computed data that the conversion efciency of p i n structure can be signicantly increased by insertion of self-organized QD multilayers into the intrinsic region. This concept may also be useful for the fabrication of high efciency tandem solar cells.
ACKNOWLEDGMENTS

3 3

1018 1017

Investigations were carried out in the framework of the IPP AAX-8-17660-01 and ISTC A-322 grants.
A. Bennett and L. C. Olsen, Conf. Rec. IEEE Photovoltaic Spec. Conf. 13, 868 1978 . 2 T. Takamoto, E. Ikeda, H. Kurita, and M. Ohmari, Appl. Phys. Lett. 70, 381 1997 . 3 W. P. Vecchi, Sol. Energy 22, 383 1979 . 4 D. Bimberg, M. Grundmann, and N. Ledentsov, Quantum Dot Heterostructures Wiley, New York, 1999 . 5 K. W. J. Barnham and G. Duggan, J. Appl. Phys. 67, 3490 1990 . 6 M. Paxman et al., J. Appl. Phys. 74, 614 1993 . 7 Y. Nakata and Y. Sugiyama, in Semiconductors and Semimetals, Vol. 60, edited by M. Sugaware Academic, New York, 1999 , Chap. 2. 8 A. A. Darhuber et al., Appl. Phys. Lett. 70, 955 1997 . 9 J. C. Gonzalez et al., Appl. Phys. Lett. 76, 3400 2000 . 10 T. S. Moss and T. D. F. Hawkins, Infrared Phys. 1, 111 1962 . 11 S. Wieder, An Introduction to Solar Energy for Scientists and Engineering Wiley, New York, 1982 . 12 H. Kiess and W. Rehwald, Sol. Energy Mater. Sol. Cells 38, 45 1995 . 13 C. H. Henry, J. Appl. Phys. 51, 4494 1980 .
1

The physical constants used in our calculations are presented in Table I. The calculations show that the inclusion of the QDs in the intrinsic region does indeed enhance short-circuit current without signicant losses in the open-circuit voltage and results in signicantly improved cell efciency. Thus, the InAs/GaAs p i n solar cell, with 3 m width of i layer and the ideality factor v 1.2, can generate the photocurrent density J sc 45.17 mA/cm2 and open-circuit voltage V oc 0.746 V. Without the QDs the same structure has J sc

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