Spontaneous emission alteration in InGaAs/GaAs vertical cavity surface emitting laser (VCSEL) structures

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1 Semicond. Sci. Technol. 14 (1999) Printed in the UK PII: S (99) Spontaneous emission alteration in InGaAs/GaAs vertical cavity surface emitting laser (VCSEL) structures Yoshihiko Hanamaki, Hidefumi Akiyama and Yasuhiro Shiraki Research Centre for Advanced Science and Technology (RCAST), The University of Tokyo, Komaba, Meguro-ku, Tokyo , Japan Institute for Solid State Physics (ISSP), The University of Tokyo, Roppongi, Minato-ku, Tokyo , Japan Received 16 November 1998, in final form 14 April 1999, accepted for publication 2 June 1999 Abstract. The spontaneous emission from vertical-cavity surface-emitting laser (VCSEL) structures consisting of an In 0.2 Ga 0.8 As/GaAs quantum well and AlAs/GaAs distributed Bragg reflectors (DBRs) was systematically investigated as a function of reflectivity of DBRs, energy difference between the excitonic energy and the cavity mode and emission wavelength. Significant lifetime alteration, which was much more than that of the previous experimental results and the theoretical estimation based on the atomic dipole model, was observed when the reflectivity was changed. This was attributed to the cooperation between the microcavity effect and the carrier carrier scattering effect which is not considered in the atomic dipole model. The spontaneous emission lifetime of the VCSEL structure whose gain peak is not equal to the cavity mode was found to be changed depending on the energy difference between the excitonic energy and the cavity mode and the lifetime was the shortest when the excitonic energy was equal to the cavity mode. It was also observed that the spontaneous emission lifetime depends on the emission wavelength and was the shortest at the cavity mode, the reason for which has not been fully clarified yet. 1. Introduction Quantum wells (QWs) embedded in microcavity structures are attracting much attention both from fundamental interest and from applications to photonics devices [1 6]. In semiconductor microcavities, an ultimately high intensity optical field is obtained around QWs by using distributed Bragg reflectors (DBRs) composed of λ/4 multilayers. Reduction in the available photon mode in a direction perpendicular to the cavity results in an increase in the emission at allowed cavity modes. This may change the spontaneous emission characteristics. Experimental studies on the alteration of spontaneous emission characteristics have been carried out in various systems [7 13]. In the case of semiconductors, much attention has been concentrated on making use of the microcavity effect in semiconductor optical devices to improve device performance in several aspects such as extreme reduction of a threshold current for the onset of lasing, suppression of noise and low divergence of output beams. However, the fundamental physics of spontaneous emission in this system has not been fully clarified, and the reflectivity dependence, the interaction dependence between the excitonic energy and the cavity mode and the wavelength Present address: High Frequency and Optical Semiconductor Division, Mitsubishi Electronic Corporation, 4-1, Mizuhara, Itami-shi, Hyogo , Japan. dependence of the spontaneous emission have not been systematically examined yet. Semiconductor vertical-cavity surface-emitting laser (VCSEL) structures are suitable for investigating the characteristics of the spontaneous emission since precisely designed VCSEL structures with high quality are fabricated by recent crystal growth technology such as molecular beam epitaxy (MBE) and metal organic chemical vapour deposition (MOCVD). The reflectivity dependence of the spontaneous emission can be easily studied by changing AlAs/GaAs pairs of DBRs. The interaction between excitonic energy and cavity mode can be systematically changed by utilizing thermal characteristics of VCSEL structures. This is because the lasing wavelength of VCSELs is determined by the optical properties of mirrors and the cavity, and the gain spectrum and the cavity resonance mode shift to longer wavelength but with different rates with increasing temperature [14 17]. Preliminary experiments revealed that spontaneous emission lifetime alters depending on the reflectivity of DBR mirrors, which is much larger than the theoretical predictions [18]. In this paper, the reflectivity dependence of the spontaneous emission enhancement of VCSELs is systematically studied and the origin of the lifetime alteration is discussed. How the spontaneous emission depends on the interaction between the excitonic energy and the cavity mode is also /99/ $ IOP Publishing Ltd 797

2 Y Hanamaki et al (a) (b) Figure 1. (a) Schematic structure of the VCSEL fabricated to investigate the reflectivity dependence of the spontaneous emission lifetime. (b) Schematic structure of the VCSEL fabricated to investigate the dependence on the interaction between the excitonic energy and the cavity mode. The cavity mode of the VCSEL structure is not equal to the QW wavelength at room temperature. investigated by changing the temperature. Finally, the wavelength dependence of the spontaneous emission lifetime is examined. 2. Experiments The VCSEL structures studied were grown on (100) undoped GaAs substrates by an MBE apparatus (VG-80H system). The top and bottom DBRs consist of λ/4 AlAs/GaAs alternating layers. The λ-cavity consists of GaAs spacers and an In 0.2 Ga 0.8 As single QW at the centre of the cavity. In all experiments, the gain width of the In 0.2 Ga 0.8 As/GaAs QW at room temperature was designed to be broader than the cavity resonance mode and there was only one cavity mode within the gain width. X-ray diffraction measurement of AlAs/GaAs superlattices was performed to determine the growth rate of AlAs and GaAs before sample fabrication. First, in order to study the reflectivity dependence of the QW spontaneous emission, the pair number of quarterwave stacks of top and bottom DBRs was varied from five to 20. The VCSEL structure grown is schematically shown in figure 1(a). The calculated maximum reflectivities of VCSEL structures seen from the surface are 87.0%, 97.3%, 98.9% and 99.9% for 5, 10, 15 and 20 pairs, respectively [19] where the variation of absorption coefficient over the wavelength rate of interest was included. QWs consisting of a 65 Å thick In 0.2 Ga 0.8 As/GaAs well and 1343 Å GaAs barrier layers were fabricated between two sets of AlAs/GaAs DBR mirrors. The layer thicknesses of the AlAs (830 Å)/GaAs (696 Å) DBR were designed to be one quarter wavelength of the room temperature emission peak (970 nm) of the In 0.2 Ga 0.8 As/GaAs QW. After 3000 Å buffer layers of GaAs were deposited, the bottom DBR was grown at the growth temperature of 580 C with V/III ratio of 8 and the λ-cavity was grown by keeping the growth temperature at 520 Cto prevent indium desorption and segregation. Finally, the top DBR, identical to the bottom DBR, was grown. Next, in order to study the interaction between the excitonic energy and the cavity mode, a VCSEL structure schematically shown in figure 1(b) was fabricated. The wavelength of the cavity mode ( 930 nm) is about 55 nm shorter than the QW wavelength ( 985 nm) at room temperature. Since the temperature dependence of both wavelengths is different, tuning the interaction between the QW excitonic energy and the cavity mode is possible by changing the temperature. Sample preparation was done in the same way as mentioned above, but thicknesses of the In 0.2 Ga 0.8 As QW (70 Å) and AlAs (784 Å)/GaAs (652 Å) DBRs were slightly different. After the VCSEL structure was fabricated, these samples were characterized by reflectivity, photoluminescence (PL) and time-resolved PL (TRPL) measurements. The reflectivity measurements were performed using a quartz halogen light source and CdS photoelectric cell in the nm range with the resolution of 8 nm. For the PL spectrum measurements, excitation light with 860 nm from a continuous wave (CW) Ti:sapphire laser was used to excite the In 0.2 Ga 0.8 As/GaAs QW through the top DBR. Since the highreflectivity zone is away from the wavelength of the incident light, the reflection of the pump laser due to the top DBR is very small. The PL from the In 0.2 Ga 0.8 As/GaAs QW was detected normal to the sample surface and analysed by a standard lock-in amplifier system with a Hamamatsu R2658 photomultiplier with the resolution of 0.2 nm. The TRPL measurements were carried out using a time-correlated single-photon-counting system [20] with a Hamamatsu S1 photomultiplier. The VCSEL structures were photoexcited by a mode-locked Styrl 9M dye laser tuned at 860 nm, where the pulse width and repetition rate were 5 ps and 75.4 MHz, respectively. The carrier density is influenced by the reflectivity of the DBR and the absorption of GaAs layers. The measurement system resolution was 2 nm when reflectivity dependence and interaction dependence were measured, but was 0.5 nm when emission wavelength dependence was measured. 798

3 Spontaneous emission from InGaAs/GaAs VCSELs Figure 3. Luminescence intensity transient of VCSEL structures measured at the cavity mode at room temperature. Figure 2. (a) Reflectivity spectra and photoluminescence spectra (PL) of VCSEL structures with different numbers of AlAs/GaAs. (b) PL spectrum of a conventional single QW without DBRs as a reference. 3. Results and discussion 3.1. Reflectivity dependence of the spontaneous emission Figure 2 shows the measured reflectivity spectra of VCSEL structures with different numbers of AlAs/GaAs pairs at room temperature along with their PL spectra. A dip corresponding to the cavity mode is observed in the reflectivity spectrum around 970 nm in all samples. It is also seen in this figure that as the number of AlAs/GaAs pairs is increased, the highreflectivity zone becomes narrower and the linewidth of the dip also becomes narrower. The measured PL peaks with linewidths of 2 15 nm are observed to coincide with the cavity transmission peaks. The cavity length is designed so that the resonance mode wavelength becomes equal to the gain peak of the In 0.2 Ga 0.8 As/GaAs QW whose gain spectrum is represented by the PL spectrum of the reference In 0.2 Ga 0.8 As/GaAs QW without DBR grown under the same growth condition as shown at the bottom of figure 2. The PL peak of the 15-pair VCSEL structure is in a shorter wavelength region than the others, which comes from the misestimation of the growth rate of GaAs and/or AlAs during MBE growth. However, since the misestimation of the 15-pair VCSEL structure is only 4%, the gain peak of the 15-pair VCSEL structure is thought not to be significantly shifted from the wavelength of 970 nm. It is seen that the PL spectral shape of the five-pair VCSEL structure is almost equal to that of the reference QW, while a strong influence of the DBR reflectivity on the PL is observed in other VCSEL structures and the PL peak becomes sharper as the pair number of DBRs is increased. It should be mentioned that the spectral shape did not change when the excitation intensity was varied from 10 to 500 mw, indicating that the spontaneous emission was the dominant recombination process and the stimulated emission was negligibly small. Figure 3 shows the luminescence intensity transient of the VCSEL structures measured at their cavity mode. The decay time of the luminescence intensity of the five-pair VCSEL structure is the longest, 17 ns, which is almost equal to that of the reference QW sample without a DBR. In case of the conventional QW structure, the spontaneous emission lifetime seems to be very short, because it is influenced by the surface recombination. On the other hand, the spontaneous emission lifetime of the reference QW sample seems to be long. This is because in the reference sample block layers were inserted around the QW to keep the surface recombination effect. The decay time is clearly seen to become shorter with increasing number of AlAs/GaAs DBR pairs. The spontaneous emission lifetime of the 20-pair VCSEL structure is one-sixth that of the five-pair VCSEL structure. We may attribute this systematic decrease of the decay time to the alteration of the spontaneous emission lifetime due to the 799

4 Y Hanamaki et al Figure 4. Excitation power dependence of the inverse of the spontaneous emission lifetime (1/τ) of VCSEL structures. microcavity effect rather than the nonradiative recombination or the stimulated emission processes. Although similar experimental results have been reported for bulk GaAs [21], such a drastic alteration in the spontaneous emission lifetime has not been reported before. The excitation power dependence of the inverse spontaneous emission lifetime of VCSEL structures is shown in figure 4. It is seen that the inverse of the spontaneous emission lifetime of the VCSEL structures with higher reflectivity is always larger under any excitation power. Further, the spontaneous emission lifetime of each VCSEL structure does not significantly change between the average power of 40 and 90 mw. This indicates that the stimulated emission does not affect the experimental results and that the lifetime shortening comes from the microcavity effect. It is obvious that the abrupt change in the spontaneous emission lifetime of the 20-pair VCSEL structure above 100 mw is due to the stimulated emission. In order to confirm that the drastic alteration in the spontaneous emission lifetime is due to the high reflectivity of DBRs, the spontaneous emission lifetime of another reference VCSEL structure was also measured. It has the same structure as the 20 pairs, but the cavity length is shortened to have the cavity resonance at 930 nm. Since its resonance wavelength ( 930 nm) is far from its gain peak ( 970 nm), the interaction between the excitonic emission and the resonance mode should be small. The spontaneous emission lifetime of this off-resonant VCSEL structure at the resonance wavelength was 18 ns, comparable to those of VCSEL structures with low reflectivity or without DBRs and much longer than that of the on-resonant 20-pair VCSEL structure. Therefore, it can be concluded that the spontaneous emission lifetime change comes from the interaction between the excitonic energy and the cavity mode. We comment here on the spontaneous emission lifetime (9 ns) of the 15-pair VCSEL structure which is much larger than that of the 20-pair VCSEL structure. Since the overlap between the cavity resonance and the gain peak is not perfect due to the misestimation of growth rates, the microcavity effect is not significant compared to the 20-pair VCSEL structure. If this sample were well fabricated, the lifetime alteration would be smoother between 10 and 20 of the pair number. According to the theories of Ujihara or Yamanishi et al [22, 23] which are based on the atomic dipole model, the spontaneous emission lifetime can be altered only by 30% at the most by the microcavity effect and there are many reports supporting the estimation. However, since the spontaneous emission lifetime was altered by more than 30% in our experiments, it is reasonable to consider that the atomic dipole model cannot be applied to the interpretation of our experimental results. A theoretical explanation for the observed alteration has not been achieved yet. However, our present results are very consistent with the report by Jin et al [21] which proposes that carrier population kinetics in QW should be properly taken into account, and the spontaneous emission lifetime can be shortened by the Coulomb scattering effect. In order to confirm the drastic alteration of the spontaneous emission lifetime systematically, further experiments were done as shown below Dependence on the interaction between the excitonic energy and the cavity mode It was clarified in the preceding section that the spontaneous emission alteration comes from the interaction between the excitonic energy and the cavity mode. In this section, the interaction between the excitonic energy and the cavity mode was systematically changed by changing the measuring temperature. Figure 5 shows the PL spectra of the VCSEL structure schematically shown in figure 1(b) as a function of temperature. Both the QW peak (excitonic energy) and the cavity mode peak are observed, since the cavity mode is designed not to be equal to the QW wavelength except in a certain temperature range. Both peaks shift to shorter wavelengths with decreasing temperature. However, the QW peak shifts faster than the cavity mode peak and goes into the vicinity of cavity mode peak at K where the PL intensity of the cavity mode significantly increases, and finally comes to a shorter wavelength region than the cavity mode under 40 K. The emission enhancement at the cavity mode is obviously due to the increased interaction between the excitonic energy and the cavity mode. In figure 6, the peak wavelengths of two PL emissions are plotted as a function of temperature. Cavity mode and exciton shown in this figure correspond to peak and peak shown in figure 5, respectively. It is seen that the temperature dependence of the QW and the cavity mode is different and that the interaction between the excitonic energy and the cavity mode can be tuned continuously 800

5 Spontaneous emission from InGaAs/GaAs VCSELs Figure 5. PL spectra of the VCSEL structure schematically shown in figure 1(b) as a function of temperature. Peak and peak show the cavity mode and the excitonic peak, respectively. Figure 6. Two PL emission peaks as a function of temperature. by changing temperature. Weisbuch et al reported that semiconductor quantum microcavity with QWs as the active medium displays mode splitting in reflectivity curves when the QWs and the optical cavity are in resonance [1]. However, we could not observe the mode splitting in the PL spectra shown in figure 5 in the temperature range of K where the QW and the cavity mode are in resonance. Houdré et al reported that the amount of mode splitting is very small when the luminescence spectrum width is as the same as the mode splitting [24]. Therefore, the reason why the mode Figure 7. Temperature dependence of the inverse of the spontaneous emission lifetime. Black circles show the experimental results of the VCSEL sample and the broken line shows the experimental results of the normal QW. splitting was not able to be observed in this experiment even in resonance is thought to be that the excitonic luminescence peak width was as the same as the mode splitting; in other words, the experiment was done in the weakly coupled condition. Even in the weakly coupled condition, however, Heinzen et al reported that spontaneous emission alteration was observed in an atomic system [25]. Since the PL spectrum of the present semiconductor sample is seen to be drastically changed by the microcavity effect, the spontaneous emission is considered to be also altered and therefore, the spontaneous emission lifetime of the cavity mode was measured as a function of temperature. Figure 7 shows the temperature dependence of the inverse of the spontaneous emission lifetime. In this figure, the black circles show the experimental results of the sample with DBRs and the broken line shows the reference of the normal QW without DBRs. Although conventional QW monotonically decreases as the measuring temperature is decreased, the VCSEL structure shows a prominent peak in the temperature range of K. This clearly shows that the spontaneous emission lifetime alteration strongly depends on the interaction between the excitonic energy and the cavity mode. It is very interesting that lifetime alteration was observed even in the weakly coupled condition which is believed to hardly give rise to the microcavity effect Wavelength dependence of the spontaneous emission lifetime As already shown in figure 2, the PL intensities and their full-width at half-maximum (FWHM) are quite different between the conventional QW without a cavity and the 801

6 Y Hanamaki et al 4. Summary Figure 8. Wavelength dependence of the spontaneous emission lifetime of VCSELs. VCSEL structure with high reflectivity DBRs. Further, since the spontaneous emission at the cavity mode is enhanced and the others are suppressed by the microcavity effect, it is anticipated that the spontaneous emission lifetime is dependent on its emission wavelength. Therefore, in this section, the spontaneous emission lifetime which may be influenced by the microcavity effect was investigated as a function of the spontaneous emission wavelength. Figure 8 shows the wavelength dependence of the spontaneous emission lifetime. It is seen that the lifetime at the cavity mode ( nm) is the shortest and the lifetime becomes longer as the measurement wavelength is separated from the cavity mode. This result indicates that the PL spectral shape changes during the decay, which contradicts the result described in the previous section. This may be attributed to the wavelength resolution of the measurement system. In the previous experiment, the system resolution was lower than this experimental set-up ( 0.5 nm) and therefore the spectral change was probably not detected. In the present experiment, on the other hand, the system resolution is so high that emission wavelength dependence may be observed even though Coulomb scattering exists in this system. The details of the mechanism are not clarified yet. In shorter wavelength region than the cavity mode, the spontaneous emission lifetime is almost the same as the cavity mode s. This is because the spontaneous emission lifetime is governed by the relaxation process rather than the microcavity effect in this region. On the other hand, in the longer wavelength region, the spontaneous emission lifetime becomes longer. Since the photon energy is lower than the cavity mode, the spontaneous emission suppression may be remarkable. The spontaneous emission from vertical-cavity surfaceemitting laser (VCSEL) structures consisting of an In 0.2 Ga 0.8 As/GaAs quantum well and AlAs/GaAs distributed Bragg reflectors (DBRs) was systematically investigated as a function of reflectivity of DBRs, the energy difference between the excitonic energy and the cavity mode and the emission wavelength. The PL of VCSEL structures showed that the spontaneous emission is enhanced as the reflectivity of DBRs becomes higher, and the drastic decrease of the spontaneous emission lifetime was observed beyond the previously reported experimental results for QWs and the theoretical estimation based on the atomic dipole model. This can be attributed to cooperation between the microcavity effect and the carrier carrier scattering effect which is not considered in the atomic dipole model. In VCSEL structures whose gain peak is not equal to the cavity mode, it was clearly observed that the spontaneous emission lifetime strongly depends on the interaction between the excitonic energy and the cavity mode and the spontaneous emission lifetime was the shortest when the excitonic energy was equal to the cavity mode. Moreover, the spontaneous emission lifetime was found to depend on the emission wavelength and become the shortest at the cavity mode. The reason for this phenomenon, which is known for the atomic cavity, is not understood yet and more detailed studies are necessary. Acknowledgments The authors would like to thank Professor R Ito and Dr H Yaguchi for their valuable discussion. The authors are also very grateful to S Ohtake for his technical assistance. This work was in part supported by a Grant-in-Aid for Scientific Research on Priority Area Quantum Coherent Electronics from the Ministry of Education, Science and Culture. References [1] Weisbuch C, Nishioka M, Ishikawa A and Arakawa Y 1992 Phys. Rev. Lett [2] Yamamoto Y, Machinaga F, Machida S, Karlsson A, Jacobson J, Björk G and Mukai T 1993 J. Physique IV 3 39 [3] Young D B, Scott J W, Peters F H, Peters M G, Majewski M L, Thibeault B J, Corzine SWand Coldren L A 1993 IEEE J. Quantum Electron [4] Shtengel G, Temkin H, Uchida T, Kim M, Brusenbach P and Parson C 1994 Appl. Phys. Lett [5] Deppe D G and Lei C 1991 J. Appl. Phys [6] Baba T, Hamano T, Koyama F and Iga K 1991 IEEE J. Quantum Electron [7] Nishioka K, Tanaka K, Nakamura T, Lee Y and Yamanishi M 1993 Appl. Phys. Lett [8] Yamauchi T, Arakawa Y and Nishioka M 1991 Appl. Phys. Lett [9] Schubert E F, Vredenverg A M, Hunt N E, Wrong Y H, Becker P C, Poate J M, Jacobson D C, Feldman LCand Zydzik G J 1992 Appl. Phys. Lett

7 Spontaneous emission from InGaAs/GaAs VCSELs [10] Vredenberg A M, Hunt NEJ,Schubert E F, Jacobson D C, Poate J M and Zydzik G J 1993 Phys. Rev. Lett [11] Yamamoto Y, Machida S, Horikoshi Y, Igeta K and Björk G 1991 Opt. Commun [12] Hunt N E, Schubert E F, Kopf R F, Sivco D L, Cho AYand Zydzik G J 1993 Appl. Phys. Lett [13] Cao H, Jacobson J, Björk G, Pau S and Yamamto Y 1995 Appl. Phys. Lett [14] Lu B, Zhou P, Cheng J, Malloy K J and Zolper J C 1994 Appl. Phys. Lett [15] Tell B, Brown-Goebeler K F and Liibenguth R E 1993 IEEE Photon. Technol. Lett [16] Tell B, Brown-Goebeler K F, Liibenguth R E, Baez FMand Lee Y H 1992 Appl. Phys. Lett [17] Hasnain G, Tai K, Yang L, Wang Y H, Fischer G J, Wynn J D, Weir B, Dutta N K and Cho A Y 1991 IEEE J. Quantum Electron [18] Hanamaki Y, Kinoshita H, Akiyama H, Ogasawara N and Shiraki Y 1997 Phys. Rev. B 56 R4379 [19] Björk G and Nilsson O 1987 J. Lightwave Technol [20] Jeong H, Lee I I, Seo J C, Lee M, Kim D, Lee S J, Park S H and Kim U 1993 Solid State Commun [21] Jin R, Tobin M S, Leavitt R P, Gibbs H M, Khitorova G, Boggavarapu D, Lyngnes O, Lindmark E, Jahnke F and Koch S W 1996 Microcavities and Photonic Bandgaps: Physics and Application ed J J Rarity and C Weisbuch (Boston: Kluwer) pp [22] Ujihara K, Nakamura A, Manba O and Feng X-P 1991 Japan. J. Appl. Phys [23] Yamanishi M 1992 Japan. J. Appl. Phys [24] Houdré R, Stanley R P, Oesterle U, Ilegems M and Weisbuch C 1994 Phys. Rev. B [25] Heinzen D J, Childs J J, Thomas J E and Feld M S 1987 Phys. Rev. Lett

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