I. INTRODUCTION
Section:
ChooseTop of pageABSTRACTI. INTRODUCTION <<II. PREPARATION OF THE SA...III. EXPERIMENTAL RESULTSIV. THEORYV. SUMMARYSUPPLEMENTARY MATERIALREFERENCESSemiconductor microcavity containing quantum wells (QWs) is an example of an optical resonator with strong nonlinear effects. In the strong light–matter coupling regime, cavity photons mix with excitons, forming quasiparticles called exciton–polaritons (in short, polaritons). Polaritons, despite their photonic origin, strongly interact with each other via Coulomb interactions due to the excitonic component.
The optical bistability in microcavities in the strongly coupled regime can result from the bleaching of light–matter coupling, as theoretically predicted.2121. A. Tredicucci, Y. Chen, V. Pellegrini, M. Börger, and F. Bassani, “Optical bistability of semiconductor microcavities in the strong-coupling regime,” Phys. Rev. A 54, 3493–3498 (1996). https://doi.org/10.1103/physreva.54.3493 On the other hand, bistability more frequently results from the Kerr-type nonlinearity due to polariton–polariton interactions.1,2,22–241. A. Kavokin, J. J. Baumberg, G. Malpuech, and F. P. Laussy, Microcavities (Oxford University Press, 2017).2. I. Carusotto and C. Ciuti, “Quantum fluids of light,” Rev. Mod. Phys. 85, 299–366 (2013). https://doi.org/10.1103/revmodphys.85.29922. A. Baas, J. P. Karr, H. Eleuch, and E. Giacobino, “Optical bistability in semiconductor microcavities,” Phys. Rev. A 69, 023809 (2004). https://doi.org/10.1103/physreva.69.02380923. F. Claude, M. J. Jacquet, R. Usciati, I. Carusotto, E. Giacobino, A. Bramati, and Q. Glorieux, “High-resolution coherent probe spectroscopy of a polariton quantum fluid,” Phys. Rev. Lett. 129, 103601 (2022). https://doi.org/10.1103/physrevlett.129.10360124. N. A. Gippius, S. G. Tikhodeev, V. D. Kulakovskii, D. N. Krizhanovskii, and A. I. Tartakovskii, “Nonlinear dynamics of polariton scattering in semiconductor microcavity: Bistability vs stimulated scattering,” Europhys. Lett. 67, 997 (2004). https://doi.org/10.1209/epl/i2004-10133-6 It can be realized under various experimental conditions, typically with quasi-resonant pumping.22,23,2522. A. Baas, J. P. Karr, H. Eleuch, and E. Giacobino, “Optical bistability in semiconductor microcavities,” Phys. Rev. A 69, 023809 (2004). https://doi.org/10.1103/physreva.69.02380923. F. Claude, M. J. Jacquet, R. Usciati, I. Carusotto, E. Giacobino, A. Bramati, and Q. Glorieux, “High-resolution coherent probe spectroscopy of a polariton quantum fluid,” Phys. Rev. Lett. 129, 103601 (2022). https://doi.org/10.1103/physrevlett.129.10360125. E. A. Cotta and F. M. Matinaga, “Bistability double-crossing curve effect in a polariton-laser semiconductor microcavity,” Phys. Rev. B 76, 073308 (2007). https://doi.org/10.1103/physrevb.76.073308 Moreover, taking into account the polariton spin degree of freedom and polarization of incident light, a multistable behavior has been observed.26,2726. N. A. Gippius, I. A. Shelykh, D. D. Solnyshkov, S. S. Gavrilov, Y. G. Rubo, A. V. Kavokin, S. G. Tikhodeev, and G. Malpuech, “Polarization multistability of cavity polaritons,” Phys. Rev. Lett. 98, 236401 (2007). https://doi.org/10.1103/physrevlett.98.23640127. T. K. Paraïso, M. Wouters, Y. Léger, F. Morier-Genoud, and B. Deveaud-Plédran, “Multistability of a coherent spin ensemble in a semiconductor microcavity,” Nat. Mater. 9, 655–660 (2010). https://doi.org/10.1038/nmat2787 Additionally, the bi- or multistability of the polariton condensate can also be observed for the non-resonant excitation of the system.28–3028. L. Pickup, K. Kalinin, A. Askitopoulos, Z. Hatzopoulos, P. G. Savvidis, N. G. Berloff, and P. G. Lagoudakis, “Optical bistability under nonresonant excitation in spinor polariton condensates,” Phys. Rev. Lett. 120, 225301 (2018). https://doi.org/10.1103/physrevlett.120.22530129. Y. del Valle-Inclan Redondo, H. Sigurdsson, H. Ohadi, I. A. Shelykh, Y. G. Rubo, Z. Hatzopoulos, P. G. Savvidis, and J. J. Baumberg, “Observation of inversion, hysteresis, and collapse of spin in optically trapped polariton condensates,” Phys. Rev. B 99, 165311 (2019). https://doi.org/10.1103/physrevb.99.16531130. H. Sigurdsson, “Hysteresis in linearly polarized nonresonantly driven exciton–polariton condensates,” Phys. Rev. Res. 2, 023323 (2020). https://doi.org/10.1103/physrevresearch.2.023323Bistability has been widely studied because of the possible applications of this effect in optical logic circuits,31,3231. T. C. H. Liew, A. V. Kavokin, and I. A. Shelykh, “Optical circuits based on polariton neurons in semiconductor microcavities,” Phys. Rev. Lett. 101, 016402 (2008). https://doi.org/10.1103/PhysRevLett.101.01640232. T. C. H. Liew, A. V. Kavokin, T. Ostatnický, M. Kaliteevski, I. A. Shelykh, and R. A. Abram, “Exciton–polariton integrated circuits,” Phys. Rev. B 82, 033302 (2010). https://doi.org/10.1103/physrevb.82.033302 Ising-model simulators,33,3433. M. Foss-Feig, P. Niroula, J. T. Young, M. Hafezi, A. V. Gorshkov, R. M. Wilson, and M. F. Maghrebi, “Emergent equilibrium in many-body optical bistability,” Phys. Rev. A 95, 043826 (2017). https://doi.org/10.1103/physreva.95.04382634. O. Kyriienko, H. Sigurdsson, and T. C. H. Liew, “Probabilistic solving of NP-hard problems with bistable nonlinear optical networks,” Phys. Rev. B 99, 195301 (2019). https://doi.org/10.1103/physrevb.99.195301 optical switches,35,3635. I. A. Shelykh, T. C. H. Liew, and A. V. Kavokin, “Spin rings in semiconductor microcavities,” Phys. Rev. Lett. 100, 116401 (2008). https://doi.org/10.1103/physrevlett.100.11640136. H. Suchomel, S. Brodbeck, T. C. H. Liew, M. Amthor, M. Klaas, S. Klembt, M. Kamp, S. Höfling, and C. Schneider, “Prototype of a bistable polariton field-effect transistor switch,” Sci. Rep. 7, 5114 (2017). https://doi.org/10.1038/s41598-017-05277-1 or the construction of optical transistors.36,3736. H. Suchomel, S. Brodbeck, T. C. H. Liew, M. Amthor, M. Klaas, S. Klembt, M. Kamp, S. Höfling, and C. Schneider, “Prototype of a bistable polariton field-effect transistor switch,” Sci. Rep. 7, 5114 (2017). https://doi.org/10.1038/s41598-017-05277-137. D. Ballarini, M. De Giorgi, E. Cancellieri, R. Houdré, E. Giacobino, R. Cingolani, A. Bramati, G. Gigli, and D. Sanvitto, “All-optical polariton transistor,” Nat. Commun. 4, 1778 (2013). https://doi.org/10.1038/ncomms2734 The spin multistability of polaritons can be used to construct a complete architecture of photonic logic gates.3838. T. Espinosa-Ortega and T. C. H. Liew, “Complete architecture of integrated photonic circuits based on AND and NOT logic gates of exciton polaritons in semiconductor microcavities,” Phys. Rev. B 87, 195305 (2013). https://doi.org/10.1103/physrevb.87.195305In the majority of experiments performed in microcavities based on III–V semiconductors,22,3922. A. Baas, J. P. Karr, H. Eleuch, and E. Giacobino, “Optical bistability in semiconductor microcavities,” Phys. Rev. A 69, 023809 (2004). https://doi.org/10.1103/physreva.69.02380939. A. Baas, J.-P. Karr, M. Romanelli, A. Bramati, and E. Giacobino, “Optical bistability in semiconductor microcavities in the nondegenerate parametric oscillation regime: Analogy with the optical parametric oscillator,” Phys. Rev. B 70, 161307 (2004). https://doi.org/10.1103/physrevb.70.161307 bistability appears in the form of a hysteresis loop, when the structure is pumped by a laser with energy detuned slightly above the lower polariton mode. In such a configuration, the polariton energy blueshifts with an increase in the pump power and the system switches to a higher transmission state when the polariton energy becomes locked to the laser energy. With a subsequent reduction in the incident power, the system remains locked in the higher transmission state for a certain range of power before switching to the lower transmission state. This range of bistability corresponds to a hysteresis loop in the input–output characteristics. According to the description above, it results in a counterclockwise dependence in the diagram of the output power as a function of the input power.In this work, we describe the inverted type of bistability that we created in a CdTe-based microcavity. To show the novelty of our results, it is useful to compare the experimental input–output power characteristics measured at two different laser energies. Figure 1(a) illustrates the dispersion relation of polariton modes, with quasi-resonant laser energies marked with (1) and (2). When the energy of the laser is above the lower polariton mode energy, as in the case of (1), the measured input–output power characteristics are presented in Fig. 1(b). It exhibits a counterclockwise direction and qualitatively resembles the hysteresis loop reported previously in the literature.22,3922. A. Baas, J. P. Karr, H. Eleuch, and E. Giacobino, “Optical bistability in semiconductor microcavities,” Phys. Rev. A 69, 023809 (2004). https://doi.org/10.1103/physreva.69.02380939. A. Baas, J.-P. Karr, M. Romanelli, A. Bramati, and E. Giacobino, “Optical bistability in semiconductor microcavities in the nondegenerate parametric oscillation regime: Analogy with the optical parametric oscillator,” Phys. Rev. B 70, 161307 (2004). https://doi.org/10.1103/physrevb.70.161307 However, when the laser energy is below the lower polariton energy, as in the case of (2), the system develops another hysteresis loop, which exhibits an unexpected shape. This new type of optical bistability with an inverted (clockwise) hysteresis direction is shown in Fig. 1(c). As the input power is increased, the transmitted light intensity increases linearly. Furthermore, the system abruptly switches from the strong coupling regime to the weak coupling regime, which is observed as a sudden drop in the transmitted light intensity. As the excitation power is then reduced, the system remains in the weakly coupled state for a certain range of input power. This leads to the formation of a hysteresis loop with a clockwise direction, opposite to the optical bistability observed due to the Kerr-like nonlinearity.Moreover, from the point of view of applications, the measured input–output characteristics exhibit a behavior that is essential for the so-called optical limiters.40–4240. L. W. Tutt and T. F. Boggess, “A review of optical limiting mechanisms and devices using organics, fullerenes, semiconductors and other materials,” Prog. Quantum Electron. 17, 299–338 (1993). https://doi.org/10.1016/0079-6727(93)90004-s41. R. Gadhwal and A. Devi, “A review on the development of optical limiters from homogeneous to reflective 1-D photonic crystal structures,” Opt. Laser Technol. 141, 107144 (2021). https://doi.org/10.1016/j.optlastec.2021.10714442. R. Gadhwal, P. Kaushik, and A. Devi, “A review on 1D photonic crystal based reflective optical limiters,” Crit. Rev. Solid State Mater. Sci. 48, 93–111 (2023). https://doi.org/10.1080/10408436.2022.2041394 Optical limiting is an effect where the transmitted light intensity does not increase above a certain threshold pumping power. Optical limiters are useful elements in photonic systems that allow low light intensities to pass but simultaneously protect sensitive elements by blocking high laser intensities. Various physical effects can be used in optical limiters: multi-photon absorption,43–4543. J. H. Vella, J. H. Goldsmith, A. T. Browning, N. I. Limberopoulos, I. Vitebskiy, E. Makri, and T. Kottos, “Experimental realization of a reflective optical limiter,” Phys. Rev. Appl. 5, 064010 (2016). https://doi.org/10.1103/physrevapplied.5.06401044. E. Makri, H. Ramezani, T. Kottos, and I. Vitebskiy, “Concept of a reflective power limiter based on nonlinear localized modes,” Phys. Rev. A 89, 031802 (2014). https://doi.org/10.1103/physreva.89.03180245. G. S. He, L.-S. Tan, Q. Zheng, and P. N. Prasad, “Multiphoton absorbing materials: Molecular designs, characterizations, and applications,” Chem. Rev. 108, 1245–1330 (2008). https://doi.org/10.1021/cr050054x reverse saturated absorption,46,4746. J. W. Perry, K. Mansour, I.-Y. S. Lee, X.-L. Wu, P. V. Bedworth, C.-T. Chen, D. Ng, S. R. Marder, P. Miles, T. Wada, M. Tian, and H. Sasabe, “Organic optical limiter with a strong nonlinear absorptive response,” Science 273, 1533–1536 (1996). https://doi.org/10.1126/science.273.5281.153347. D. Dini, M. J. F. Calvete, and M. Hanack, “Nonlinear optical materials for the smart filtering of optical radiation,” Chem. Rev. 116, 13043–13233 (2016). https://doi.org/10.1021/acs.chemrev.6b00033 self-defocusing,4848. R. C. C. Leite, S. P. S. Porto, and T. C. Damen, “The thermal lens effect as a power-limiting device,” Appl. Phys. Lett. 10, 100–101 (1967). https://doi.org/10.1063/1.1754849 or nonlinear scattering.49,5049. L. Vivien, P. Lançon, D. Riehl, F. Hache, and E. Anglaret, “Carbon nanotubes for optical limiting,” Carbon 40, 1789–1797 (2002). https://doi.org/10.1016/s0008-6223(02)00046-550. D. J. Hagan, “Optical limiting,” in Handbook of Optics, Third Edition Volume IV: Optical Properties of Materials, Nonlinear Optics, Quantum Optics (Set), 3rd ed., edited by M. Bass, C. Decusatis, J. M. Enoch, V. Lakshminarayanan, G. Li, C. MacDonald, V. N. Mahajan, and E. Van Stryland (McGraw-Hill Education, 2009), Chap. 13. Optical limiting can be realized in a wide range of structures, such as photonic crystals,5151. S. Husaini, H. Teng, and V. M. Menon, “Enhanced nonlinear optical response of metal nanocomposite based photonic crystals,” Appl. Phys. Lett. 101, 111103 (2012). https://doi.org/10.1063/1.4751840 micro-ring resonators,5252. S. Yan, J. Dong, A. Zheng, and X. Zhang, “Chip-integrated optical power limiter based on an all-passive micro-ring resonator,” Sci. Rep. 4, 6676 (2014). https://doi.org/10.1038/srep06676 waveguides,53,5453. M. Heinrich, F. Eilenberger, R. Keil, F. Dreisow, E. Suran, F. Louradour, A. Tünnermann, T. Pertsch, S. Nolte, and A. Szameit, “Optical limiting and spectral stabilization in segmented photonic lattices,” Opt. Express 20, 27299–27310 (2012). https://doi.org/10.1364/oe.20.02729954. U. Kuhl, F. Mortessagne, E. Makri, I. Vitebskiy, and T. Kottos, “Waveguide photonic limiters based on topologically protected resonant modes,” Phys. Rev. B 95, 121409 (2017). https://doi.org/10.1103/physrevb.95.121409 microcavities,43,5543. J. H. Vella, J. H. Goldsmith, A. T. Browning, N. I. Limberopoulos, I. Vitebskiy, E. Makri, and T. Kottos, “Experimental realization of a reflective optical limiter,” Phys. Rev. Appl. 5, 064010 (2016). https://doi.org/10.1103/physrevapplied.5.06401055. A. A. Ryzhov, “Optical limiting performance of a GaAs/AlAs heterostructure microcavity in the near-infrared,” Appl. Opt. 56, 5811 (2017). https://doi.org/10.1364/ao.56.005811 or microcavities in the strong coupling regime.2,562. I. Carusotto and C. Ciuti, “Quantum fluids of light,” Rev. Mod. Phys. 85, 299–366 (2013). https://doi.org/10.1103/revmodphys.85.29956. D. Sanvitto and S. Kéna-Cohen, “The road towards polaritonic devices,” Nat. Mater. 15, 1061–1073 (2016). https://doi.org/10.1038/nmat4668This work is organized as follows: Sec. describes the preparation of the sample, with an emphasis on the exfoliation process of a CdTe-based microcavity from a GaAs substrate. The experimental results are presented in Sec. . These consist of the results from quasi-resonant transmission intensity studies at different energies of the incident laser and the angle-resolved luminescence as a function of excitation power. We theoretically explain all the effects in terms of suppression of strong coupling and polariton energy reduction and compare them with the case of Kerr-type interactions in Sec. .II. PREPARATION OF THE SAMPLE
Section:
ChooseTop of pageABSTRACTI. INTRODUCTIONII. PREPARATION OF THE SA... <<III. EXPERIMENTAL RESULTSIV. THEORYV. SUMMARYSUPPLEMENTARY MATERIALREFERENCESIn detail, the investigated semiconductor optical microcavity structure consisted of two Bragg mirrors (DBRs), each made of 20 pairs of alternating CdTe layers alloyed with magnesium and zinc. The 600 nm thick cavity between the DBRs was formed by a (Cd,Zn,Mg)Te layer. Within the cavity layer, 6 CdTe:Mn QWs were placed at the maxima of the electric field distribution.
III. EXPERIMENTAL RESULTS
Section:
ChooseTop of pageABSTRACTI. INTRODUCTIONII. PREPARATION OF THE SA...III. EXPERIMENTAL RESULTS <<IV. THEORYV. SUMMARYSUPPLEMENTARY MATERIALREFERENCESThe transmissive semiconductor microcavity obtained by the wet exfoliation process was located in a cryostat at a temperature of 4.5 K.
Measurements were performed to determine the dependence of the intensity of the light transmitted through the sample on the power of the incident laser beam. Such input–output optical power characteristics were collected at various energies of the laser, tuned in the spectral region of the lower polariton mode. A linearly polarized continuous wave laser beam from a tunable Ti:sapphire source was focused on the sample using a lens with a focal length f = 25.4 mm. The diameter of the laser spot on the sample was around 12 µm. The transmitted signal was collected with a 50× microscope objective with a numerical aperture of NA = 0.55. The incident and transmitted laser powers were simultaneously measured by two detectors: one placed before the cryostat and the second one behind the sample. The laser power was changed in the range from single microwatts to tens of milliwatts. The incident power was automatically adjusted in a continuous manner with the angle of a half-wave plate mounted on a programmable rotation stage before a linear polarizer.
The input–output power characteristics, measured for different laser energies, are shown in Fig. 3. Detuning is defined as the energy difference between the laser energy and the minimum of the lower polariton branch, δ = EP − ELP(k = 0). In the case of laser energy (1), at δ = 4.1 meV, a hysteresis loop was observed in the 30–40 mW input power range. While increasing the power of the incident laser, the system abruptly switched to a higher transmission state at around 38 mW. While reducing the incident optical power, the system switched to a lower transmission state at around 33 mW, forming a hysteresis loop with a counterclockwise direction. Although the observed input–output characteristics resemble the optical bistability originating from the Kerr-like nonlinearity of lower polaritons, in our system, it has a different origin. As will be discussed in detail in Sec. , here, it is a result of the energy crossing between the laser and the strongly redshifting upper polariton mode. As the laser energy is detuned closer to the lower polariton, this hysteresis loop shifts toward higher pumping powers.As the energy was decreased to approach the minimum of the lower polariton branch, the bistable behavior for the input power around 30 mW moved away from the measured range of pumping powers. Under these conditions, the system acts as an optical limiter. For laser detuning δ = 1.0 meV above the lower polariton mode, the transmitted light intensity increases almost linearly with the input power up to 7.5 mW. Then, the optical limiting occurs, with the transmitted power being almost independent of the excitation intensity. At δ = 0 meV, the range of linear input–output dependence increases to 10 mW. For higher pump intensities, the output power slightly decreases and saturates.
When the laser energy is tuned below the minimum of the lower polariton mode, a qualitatively different phenomenon emerges. We observe a new hysteresis loop with the direction inverted with respect to the common counterclockwise hysteresis. It has a triangular shape and stems from a cusp formed at the maximum of transmitted power. The appearance of a new type of hysteresis is the result of physical processes that will be discussed in detail alongside our theoretical model in Sec. . As the pumping power was increased, for δ = −1.0 meV, the transmitted laser power increased linearly up to 15.8 mW, when it abruptly switched to a lower transmission state. The switching is related to the transition of the system from the strong coupling to the weak coupling regime (Sec. ). With a further increase in the incident laser power, the transmitted light intensity slowly decreased. However, when the incident laser power was decreased, the system remained in a lower transmission state until 13.6 mW, completing the clockwise hysteresis loop. As the energy of the incident laser was tuned further down below the lower polariton mode [δ = −2.1 meV, (2)], the bistability range broadened and shifted to higher input powers.To better understand the observed phenomenon, the laser energy was adjusted to the minimum energy of the lower polariton mode, which corresponds to the appearance of the inverted hysteresis. The measured input–output characteristics in Fig. 4(a) show the switching between the strong and weak coupling at 18 mW, accompanied by a sudden drop in the transmitted light intensity. The experimental setup was then modified to allow for angle-resolved measurements by Fourier space imaging of the light emitted from the microcavity (for details, see the supplementary material). The weak luminescence from the microcavity was directed to the slit of the spectrometer, and the high intensity of transmitted laser light was cut out with a bandpass filter.The acquired polariton dispersion relations at different excitation powers are presented in Figs. 4(b)–4(d). In Fig. 4(b), which shows the dispersion relation for 6.79 mW input power, two modes of upper and lower polaritons are clearly visible. A Rabi splitting of 7 meV was obtained from the coupled oscillator model [see Eq. (A.1) in the Appendix] fitted to the measured angle-resolved spectra. The corresponding modes of the upper and lower polaritons are marked with the red lines, while the corresponding bare cavity photon and exciton energies are depicted with the black dashed lines. Similarly, in Fig. 4(c), which corresponds to the power just before the transition to the lower transmission state, both polariton modes can be seen. The coupling strength decreased to 3 meV, but the system remains in the strong coupling regime. In Fig. 4(d), for a power just above the transition (20.21 mW), only a single mode with a parabolic dispersion is visible. The system transitioned from the strong to weak coupling regime as the light–matter coupling strength decreased below the linewidth of polariton modes.To summarize the experimental results, the investigated exfoliated optical microcavity based on CdTe demonstrated a new type of optical bistability, where the energy of the incident laser was set below the minimum energy of the lower polariton mode. The intensity of the transmitted light formed a hysteresis loop with a clockwise direction. A decrease in the Rabi splitting in the cavity was observed when increasing the pumping power. The switching between the two bistable states was accompanied by the transition between the strong and weak coupling regimes. In addition, as for high excitation powers, the transmitted power decreased, the system can find application as an optical limiter.
V. SUMMARY
Section:
ChooseTop of pageABSTRACTI. INTRODUCTIONII. PREPARATION OF THE SA...III. EXPERIMENTAL RESULTSIV. THEORYV. SUMMARY <<SUPPLEMENTARY MATERIALREFERENCESTo summarize, the quasi-resonant laser transmission was investigated in an exfoliated II–VI semiconductor microcavity. With increasing laser power, the polariton modes exhibited suppression of the exciton–photon coupling strength, as evidenced by the angle-resolved measurements. For varying excitation power, the transmitted light intensity showed a bistable behavior with hysteresis loops. For the incident laser energy above the lower polariton mode, the hysteresis loop resembled the behavior reported in GaAs-based structures, where it originates from the lower polariton energy blueshift due to Kerr-like nonlinearities. Here, the bistability arose from the energy redshift of the upper polariton mode. Most importantly, when the laser energy was set below the lower polariton mode, the system exhibited a different kind of bistable behavior, showing a hysteresis loop with the opposite direction. As a function of increasing pumping power, the transmittance decreased sharply. We suggest that this transmittance blocking phenomenon can be used in an efficient optical limiter.
All the observed properties were taken into account in the theoretical analysis. Starting from the two-component model with the Kerr-like nonlinear term, the well-known hysteresis loop was observed for the system driven with a laser tuned at the energy above the lower polariton mode. However, contrary to the experimental results, hysteresis loops due to both upper and lower polaritons exhibited the same (counterclockwise) direction.
To explain the experimental results, the model was extended to take into account the polariton energy redshift and Rabi energy reduction. The simulated input–output characteristics changed significantly. Depending on the energy of the driving field, the hysteresis loops exhibited clockwise or counterclockwise directions, in full agreement with the experimental observations.
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