APPLIED PHYSICS LETTERS

VOLUME 76, NUMBER 15

10 APRIL 2000

Spontaneous polarization effects in wurtzite GaNAlGaN quantum wells and comparison with experiment
Seoung-Hwan Park
Department of Physics, Catholic University of Taegu-Hyosung, Hayang, Kyeongbuk, Korea

Shun-Lien Chuanga)
Department of Electrical and Computer Engineering, University of Illinois at Urbana-Champaign, 1406 West Green Street, Illinois 61801

Received 6 December 1999; accepted for publication 12 February 2000 Electronic and optical properties of wurtzite GaN/AlGaN quantum well QW structures with the spontaneous SP and piezoelectric PZ polarizations are investigated. Although the PZ eld in the well is zero where there is no strain if the QW structures are grown on a thick GaN layer, there may still exist a strong eld in the well due to the difference between the SP polarizations in the well and barrier regions. It is shown that the transition energies have signicant dependence on both the well and the barrier widths and the many-body optical gain is reduced largely due to the SP polarization. In particular, in the case of a QW structure with a large well width, the reduction of the optical gain is dominant due to larger spatial separation between the electron and hole wave functions. These results suggest that a QW structure with a thin well width below 30 is desirable for QW lasers. We show that the theoretical transition energies agree very well with the experimental results for several Al compositions and barrier widths. The estimated SP polarization constant for AlN is about 0.040 C/m2, which is smaller than the value ( 0.081 C/m2) predicted by previous theory. 2000 American Institute of Physics. S0003-69510001915-X

Group III nitrides such as GaN, AlN, and InN have attracted considerable interest for applications in high-power electronic and optoelectronic devices. The wurtzite WZ GaN-based structure grown along the c axis is found to have large strain-induced piezoelectric PZ elds.1,2 Bernardini et al.3 also pointed out that, in addition to the high PZ polarization, a large spontaneous SP polarization is expected to be present in WZ GaN-based semiconductors. Experimentally, several reports indicate that there exist giant electric elds even in unstrained GaN QWs: the high carrier density at the GaN/AlGaN interfaces,4 the red-shift of the photoluminescence PL transition energy, and the dramatical increase of the carrier lifetime,5 due to the PZ and SP polarizations. In addition, Leroux et al.6 observed the blue-shift of the PL transition energy with decreasing barrier width and attributed it to the SP polarization. Recent theoretical study7 also showed that the valence band structures and the overlap integral of the electron and hole wave functions of GaN/ AlGaN quantum-well structures are affected signicantly by both the SP polarization and PZ elds for 0001 wurtzite structures. These results suggest that the understanding of the role of the SP polarization in WZ semiconductors is very important in order to give a guideline on sample growth and device design issues. In this letter, we investigate electronic and optical properties of 0001-oriented WZ GaN/AlGaN QW structures with the SP and PZ polarization effects. These results are compared with those of the at-band FB model without SP and PZ polarizations. Also, the theoretical transition energies are compared with experimental results5,6 from PL measurea

ments. We consider a GaN/AlGaN multiquantum well MQW structure with the tensile-strained AlGaN barriers and the unstrained GaN wells assuming that the MQW structure is grown on a thick GaN substrate layer. The selfconsistent SC band structures and wave functions are ob dinger equation for electrons, the tained by solving the Schro block-diagonalized 3 3 Hamiltonian for holes, and Poissons equation iteratively.810 The optical gain spectra are calculated by the non-Markovian gain model with manybody effects under the spontaneous emission transformation method.11,12 The electric elds in the well and barrier due to the SP and PZ polarizations along the 0001-direction for 0001oriented WZ structure can be estimated from the periodic boundary condition for a superlattice structure as follows:2,7
w Fz b w w Pb S P P PZ P S P P PZ

w b L w / L b
Lw w F , Lb z

, 1

b Fz

where superscripts w and b represent the well and barrier, and L and are the layer thickness and the static dielectric constant, respectively. Although Eq. 1 applies to the superlattice structure, it can provide a good approximation to the MQW structure. The strain-induced piezoelectric polarization P iPZ ( i w , b ) is given by1
i i i P iPZ 2 d 31 C 11 C 12

i 2 2 C 13 i C 33

i ,

Electronic mail: s-chuang@uiuc.edu 1981

where d 31 is the piezoelectric constants, b ( a s a e )/ a e , and a s and a e are the lattice constants of the substrate and
2000 American Institute of Physics

0003-6951/2000/76(15)/1981/3/$17.00

1982

Appl. Phys. Lett., Vol. 76, No. 15, 10 April 2000

S.-H. Park and S.-L. Chuang

FIG. 2. a Calculated C1HH1 PL transition energies as a function of the well width and comparison with experimental data for several Al compositions and barrier widths at T 10 K and b the theorerical transition energy of GaN/Alx Ga1 x N QW structures as a function of the barrier width at T 10 K. FIG. 1. Potential proles and the electron and hole wave functions C1 and HH1 at the zone center for the self-consistent SC model solid curves with the SP and PZ polarization of a GaN/Al0.2Ga0.8N QW structure with a well width of a 30 and b 60 , respectively. The barrier width is set to 70 . The dashed curves are for the at-band FB model.

the epilayer materials. SP polarization constants calculated by Bernardini et al.3 are used in the calculation except for the comparison with experiment, which are 0.029 and 0.081 C/m2 for GaN and AlN, respectively. Figure 1 shows the potential proles and the wave functions C1 and HH1 at zone center for the SC model with the SP and PZ polarization of a GaN/Al0.2Ga0.8N QW structures with well widths of a 30 and b 60 , respectively. Here, the barrier width is set to 70 . The SC solutions are obtained at the surface carrier density of N 2 D 2 1012 cm2 and the dashed line corresponds to potential proles for the FB model without the SP and PZ polarization. The AlGaN barrier is under 0.484% tensile strain, and we assume that the layers have the Gaor A1 face. For the Ga face, the SP polarization is pointing towards the substrate because the SP polarization for GaN and AlN is found to be negative.4 Thus, the alignment of the PZ and SP polarization is parallel in the case of tensile strain. Potential proles show that there exists a large internal eld in the well due to the difference of the SP polarization between the well and barrier although the PZ eld in the QW is zero for the case that the well strain is zero. The estimated eld in the well is 1.55 and 1.14 MV/cm for L w 30 and 60 , respectively. The FB model shows symmetric electron and hole wave functions with respect to the center of the well. On the other hand, the SC model shows asymmetric electron and hole wave functions. Figure 2 show a the calculated C1HH1 PL transition energies as a function of the well width and comparison with experimental data for several Al compositions and barrier widths at T 10 K and b the theorerical transition energy of GaN/Alx Ga1 x N QW structures as a function of the barrier width. The experimental data were taken from Refs. 5 and 6. For comparison with the experiment data the SP polarization constant for AlN is used as a tting parameter. To compare with the measured PL energies, the C1HH1 band edge transition energies are red-shifted by 35 meV, to take into account the exitonic binding energy (25 5 meV) and the PL Stokes shift 0-20 meV.6 It is observed that the transition energy decreases with the well width and its decreasing rate

increases with Al composition. For a GaN/AlGaN QW with Al0.24 and L w 30 , although the well is narrow, its transition energy is signicantly lower than the exitonic band gap 3.478 eV of GaN. This is attributed to the large internal eld in the well due to the SP and PZ polarizations. The theoretical energies show very good agreement with the experimental results for several Al compositions and barrier widths. The estimated SP polarization constant for AlN is about 0.040 C/m2, which is lower than value ( 0.081 C/m2) calculated by the theory. So far, there have been a few reports that the SP polarization eld estimated from the theory3 appears to be too large to explain experimental data. For example, Leroux et al.6 reported the SP polarization constant ranging from 0.036 to 0.051 C/m2 for AlN from tting with the experiment. Suzuki and Iizuka13 also pointed out that the SP polarization eld calculated from the theory appears to be too large to explain the experiment related to the intersubband transition. Further theoretical and experimental studies are necessary to determine the exact SP polarization constant. Figure 2b also shows that the transition energies depend on both the well and the barrier widths. The barrier width depedence of the transition energy is dominant in the case of GaN/AlGaN QWs with a large well width. This is due to the fact that in the case of the QW with the larger well width, the geometric factor 1/( w b L w / L b ) of Eq. 1 decreases more rapidly with increasing barrier width. The QWs

FIG. 3. a Many-body optical gain-well width product as a function of the surface carrier density. The dashed curves correspond to the results for the FB model without the SP and PZ polarization. b The normalized optical matrix elements for the C1HH1 using the self-consistent SC model solid and the at-band FB model dashed as a function of the in-plane wavevector k for a GaN/Al0.2Ga0.8N QW structure with well widths of 30 and 50 .

Appl. Phys. Lett., Vol. 76, No. 15, 10 April 2000

S.-H. Park and S.-L. Chuang

1983

FIG. 4. a Many-body gain spectra multiplied by the well width gain-well width product of a GaN/Al0.2Ga0.8N well with L w 30 and 50 and b the peak gain energy, the quasi-Fermi energy separation F , and the band-gap renormalization BGR as a function of carrier density of a GaN/Al0.2Ga0.8N QW with L w 30 .

are grown on a thick GaN layer, therefore, the strain in the GaN quantum wells is zero and the AlGaN barriers have a tensile strain, as conrmed by x-ray measurements.5,6 If the well is under a compressive strain for a different type of substrate layer growth,14 it will have a PZ polarization in addition to the SP polarization and Eq. 1 with the corresponding polarization elds should be used. When the AlGaN barriers are unstrained and GaN wells are compressively strained, we expect from Eq. 1 that there is an equivalent electric eld in the well to that of the structure with an unstrained GaN wells and tensile strained AlGaN barriers with the same magnitude of the strain value. Figure 3a shows the many-body optical gain-well width product as a function of the surface carrier density for a GaN/Al0.2Ga0.8N QW structure with well widths of 30 and 50 . The dashed curves correspond to the results for the FB model without the SP and PZ polarizations. Here, optical gain from a single QW is plotted for simplicity. It is observed that the gain of the SC model is signicantly reduced compared to that of the FB model. In particular, in the case of L w 50 , its decrease is much larger than that for L w 30 . This is caused mainly by the decrease of the opticalmatrix element due to the spatial separation of the electron and hole wave functions as shown in Fig. 3b, where we plot the normalized optical matrix elements for the rst conduction to heavy-hole C1HH1 band transition for the FB and SC models, as a function of the in-plane wave vector k . The optical matrix elements corresponding to the C1HH1 transition at the zone center using the SC model are about 0.0645 and 0.006 for L w 30 and 50 , respectively. In the FB model, on the other hand, the normalized optical matrix elements for the C1-HH1 transitions are 0.241 and 0.247 for L w 30 and 50 , respectively. The matrix elements decrease signicantly with the inclusion of the SP and PZ polarization effects. The reduction for L w 50 is much larger than that for L w 30 . This is attributed to a larger spatial separation between the conduction and valence wave functions in the case of a large well width. These results also explain partially why, in most GaN-based laser devices demonstrated to date, the active QW thickness is usually chosen to be less than 3 nm.15 Figure 4 shows a many-body gain spectra multiplied by the well width of a GaN/Al0.2Ga0.8N QW with L w 30

and 50 and b the peak gain energy, the quasi-Fermi energy separation F , and the band-gap renormalization BGR as a function of carrier density of a GaN/Al0.2Ga0.8N QW with L w 30 . The many-body optical gain spectra are calculated at N 2 D 20 1012 cm2. The SC model shows that its peak gain is largely reduced and its peak energy is red-shifted compared to the FB model. These effects are dominant in the case of QW with a thick well width. Also, the peak energy ( E h ) as a function of the surface carrier density shows a blue-shift with increasing surface carrier density for both the SC and FB model. This means that the band lling effect ( F ) is dominant although the BGR gives a red-shift with increasing carrier density. It is observed that the the SC model has a faster blue-shift than the FB model due to the increase of the screening eld with the sheet carrier density. The sum of the quasi-Fermi energy separation F and the BGR shows a blue-shift with increasing carrier density. However, the SC model shows that the peak energy of the optical gain spectra is red-shifted compared to the FB model. In summary, we have investigated electronic and optical properties with SP and PZ polarizations for 0001-oriented WZ GaN/AlGaN QW structures. There exists a strong eld in the well due to the difference of the SP polarization between the wells and the barriers although the PZ eld in the wells is zero. This results in a signicant reduction of the many-body optical gain, which is mainly originated from the decrease of the optical-matrix element due to the spatial separation of the electron and hole wave functions. The theoretical band-edge transition energies with eld effects are in reasonable agreement with the experimental results. Also, the peak energy ( E h ) as a function of surface carrier density shows a blue-shift due to the band lling effect. S.-H.P. was supported by University Research Program supported by Ministry of Information & Communication in South Korea.
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