• Opto-Electronic Advances
  • Vol. 5, Issue 7, 200097 (2022)
Peilong Hong1、*, Lei Xu2、*, and Mohsen Rahmani2
Author Affiliations
  • 1School of Optoelectronic Science and Engineering, University of Electronic Science and Technology of China (UESTC), Chengdu 611731, China
  • 2Advanced Optics & Photonics Laboratory, Department of Engineering, School of Science & Technology, Nottingham Trent University, Nottingham NG11 8NS, UK
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    DOI: 10.29026/oea.2022.200097 Cite this Article
    Peilong Hong, Lei Xu, Mohsen Rahmani. Dual bound states in the continuum enhanced second harmonic generation with transition metal dichalcogenides monolayer[J]. Opto-Electronic Advances, 2022, 5(7): 200097 Copy Citation Text show less

    Abstract

    The emergence of two dimensional (2D) materials has opened new possibilities for exhibiting second harmonic generation (SHG) at the nanoscale, due to their remarkable optical response related to stable excitons at room temperature. However, the ultimate atomic-scale interaction length with light makes the SHG of Transition Metal Dichalcogenides (TMDs) monolayers naturally weak. Here, we propose coupling a monolayer of TMDs with a photonic grating slab that works with doubly resonant bound states in the continuum (BIC). The BIC slabs are designed to exhibit a pair of BICs, resonant with both the fundamental wave (FW) and the second harmonic wave (SHW). Firstly, the spatial mode matching can be fulfilled by tilting FW's incident angle. We theoretically demonstrate that this strategy leads to more than four orders of magnitude enhancement of SHG efficiency than a sole monolayer of TMDs, under a pump light intensity of 0.1 GW/cm2. Moreover, we demonstrate that patterning the TMDs monolayer can further enhance the spatial overlap coefficient, which leads to an extra three orders of magnitude enhancement of SHG efficiency. These results demonstrate remarkable possibilities for enhancing SHG with nonlinear 2D materials, opening many opportunities for chip-based light sources, nanolasers, imaging, and biochemical sensing. The emergence of two dimensional (2D) materials has opened new possibilities for exhibiting second harmonic generation (SHG) at the nanoscale, due to their remarkable optical response related to stable excitons at room temperature. However, the ultimate atomic-scale interaction length with light makes the SHG of Transition Metal Dichalcogenides (TMDs) monolayers naturally weak. Here, we propose coupling a monolayer of TMDs with a photonic grating slab that works with doubly resonant bound states in the continuum (BIC). The BIC slabs are designed to exhibit a pair of BICs, resonant with both the fundamental wave (FW) and the second harmonic wave (SHW). Firstly, the spatial mode matching can be fulfilled by tilting FW's incident angle. We theoretically demonstrate that this strategy leads to more than four orders of magnitude enhancement of SHG efficiency than a sole monolayer of TMDs, under a pump light intensity of 0.1 GW/cm2. Moreover, we demonstrate that patterning the TMDs monolayer can further enhance the spatial overlap coefficient, which leads to an extra three orders of magnitude enhancement of SHG efficiency. These results demonstrate remarkable possibilities for enhancing SHG with nonlinear 2D materials, opening many opportunities for chip-based light sources, nanolasers, imaging, and biochemical sensing.

    Introduction

    Two-dimensional (2D) materials consist of a single layer of atoms of crystalline materials. Beyond graphene, the most famous 2D material, over 700 other 2D materials have been recently explored and introduced for a wide range of electrical, mechanical, thermal, and optical applications1. For optical applications, monolayers of transition metal dichalcogenides (TMDs) have attracted significant attention due to their direct bandgap, strong luminescence, and small Bohr radii. These characteristics enable a strong excitonic response at room temperature2, 3. Moreover, TMDs monolayers are inherently noncentrosymmetric, showing very high second-order nonlinear susceptibility4-9. However, because of the intrinsic atomic thickness, the conversion efficiency of the second harmonic generation (SHG) with TMDs monolayer is naturally low, bringing their practical applications into the bottleneck. To enhance the SHG efficiency of TMDs materials, their integration with various resonant nanostructures has appeared as a promising approach. One of the candidates is metallic nanostructure, whose free-electrons can couple with the incoming electromagnetic radiation to generate surface plasmons. Plasmonic nanostructures have been employed to enhance SHG with TMD monolayers10-12. However, high ohmic losses and low damage thresholds of plasmonic structures have limited the advances in this direction. Subsequently, dielectric nanostructures with high refractive indices were developed by using materials with low optical losses, and thereby have been used as an alternative platform to enhance SHG of TMDs monolayers13-17. Particularly, the recently explored bound state in the continuum (BIC)18, 19 in high-refractive-index materials has emerged as a promising playground for enhancing SHG with 2D nonlinear materials.

    A BIC can be understood as a state that coexists with the extended wave but does not radiate into the continuum space. It was initially proposed by von Neumann and Wigner in 1929, and recently has received significant interest in optics for both fundamental and practical reasons18-24. The BIC can support extremely high quality factors (theoretically infinite), leading to high confinement of electric field. An ideal BIC does not couple into free space but can be easily overcome by slightly changing structural parameters. It is also called quasi-BIC, thereby offering an unprecedented platform for nanophotonic research and applications. BICs or quasi-BICs have been employed for lasing25, 26, SHG27, 28, third harmonic generation29, nonlinear exciton-polariton effect30, nonlinear imaging31, etc. Recently, BIC has been employed for enhancing SHG via a heterostructured photonic slab. Such a slab was designed to exhibit BIC in the second harmonic wave (SHW), while the fundamental wave (FW) is resonant with a normal photonic bandgap cavity mode32. This design has demonstrated an enhanced SHG, compared with a homogeneous bulk nonlinear material33. It is worth noting that recent studies have also demonstrated that the BIC can significantly enhance SHG with TMDs monolayer34, 35. However, these studies have designed BIC to be resonant with FW.

    In this work, we propose a dual BICs scheme for enhancing SHG of integrated TMDs monolayer, i.e., matching both FW and SHW with a pair of BICs, concurrently. The BIC pair is achieved in a photonic grating slab and is classified as TE-type BIC (resonant with FW) and TM-type BIC (resonant with SHW). We chose GaP as the grating material since GaP is of high refractive index and negligible absorption in a broad spectral window covering near-infrared to the visible range. To match the modes spatially, which is crucial for enhancing SHG via the dual BICs scheme, we have considered the following two approaches. The first approach is to tilt the incident angle of FW when a homogeneous TMDs monolayer is placed on top of the grating slab. This strategy allows dual BICs scheme to enhance SHG, significantly. Second, we show that patterning the TMDs monolayer can even further reinforce the spatial overlap coefficient, which leads to extra enhancement of SHG. With these strategies together, we can enhance the system's SHG efficiency up to > 4 × 10 7 folds compared to a monolayer of TMDs with pump light of intensity 0.1 GW/cm2. We believe that our approaches offer new possibilities in practical applications with TMDs and other 2D nonlinear optical materials.

    Scheme and theoretical analysis

    To generate a pair of BICs, we consider a photonic grating slab as shown in Fig. 1(a). The cell length (lattice constant) is a, the grating strip's width is w, and the thickness of the grating is t. For this nanostructure, there are two kinds of BICs, i.e., the symmetry-protected BICs located at Γ (Kx= 0) and the destructive-interference induced BICs at off Γ (Kx≠0) position20-22. Here we consider a pair of symmetry-protected BICs, which are of different polarizations. One is the TE-type BIC with the electric field polarized along y direction, and the other is the TM-type BIC with the magnetic field polarized along y direction.

    Photonic grating slab with a pair of BICs for enhancing SHG. (a) Photonic grating slab that contains TE-type and TM-type BICs. (b) Spatial distribution of the electric field of TE and TM modes in a unit cell at Kx = 0, respectively. (c) Band structure of the target TE and TM modes of the photonic grating slab with thickness t = 0.37 ·a, respectively. (d) Kx dependent quality factor of the TE and TM modes shown in (c), respectively.

    Figure 1.Photonic grating slab with a pair of BICs for enhancing SHG. (a) Photonic grating slab that contains TE-type and TM-type BICs. (b) Spatial distribution of the electric field of TE and TM modes in a unit cell at Kx = 0, respectively. (c) Band structure of the target TE and TM modes of the photonic grating slab with thickness t = 0.37 ·a, respectively. (d) Kx dependent quality factor of the TE and TM modes shown in (c), respectively.

    The differently polarized BICs are explored due to the consideration of the second-order nonlinear susceptibility of the TMDs monolayer, which is4, 9

    χxxx(2)=χxyy(2)=χyxy(2)=χyyx(2)=χ(2),

    where x' corresponds to the armchair direction of the TMDs monolayer. In this work, we match the FW mode to be resonant with the TE-type BIC, and the SHW mode corresponds to the TM-type BIC. If the crystal axis of TMDs monolayer (x', y', z') is aligned with the grating slab axis (x, y, z), the effective nonlinear susceptibility χxyy(2)=χxyy(2) of the TMD monolayer plays the key role in the dual BICs scheme. In this situation, the armchair direction of the TMDs monolayer is along the x axis shown in Fig. 1(a). Consequently, χxyy(2) plays the key role in the scheme, and effective second-order polarizability is

    Px(2)(2ω,r)=ϵ0χxyy(2)Ey(ω,r)Ey(ω,r),

    where Ey(ω, r) represents the electric field of the FW.

    To make the pair of BICs meet the frequency matching condition for SHG, we fix cell length a = 677 nm and the width of grating strip w = 0.7a, and scan the thickness t of the grating. We chose GaP as the grating material, which is highly transparent in a broad spectral window from near-infrared to the visible regime. The target wavelength of FW (TE mode) and SHW (TM mode) are 1560 nm and 780 nm, respectively, and the corresponding refractive index of GaP is 3.05 for FW and 3.20 for SHW36, respectively. The full wave simulation was done with the COMSOL Multiphysics (See Supplemental information Section 1 for details). As an example shown in Fig. 1(c), when thickness t reaches 0.37a, the frequency of TE-type BIC is half of that of the TM-type BIC state at Kx≈0.16Ka, where Ka = 2π/a. Meanwhile, the quality factor of both TE and TM modes is also obtained, as shown in Fig. 1(d). We see that the quality factor of both TE and TM modes increases as the wave vector Kx decreases, and diverges to infinite at Kx= 0. This result confirms that the TE and TM type BICs appear at Kx = 0. Note that the diverging quality factor for BICs originates from that the leakage of the light field from the grating slab to free space is prohibited by the symmetry of the system. As can be seen from Fig. 1(b), the spatial distribution of BICs field in the slab is antisymmetric along x direction, which will eliminate the outcoupling of BICs into free space due to destructive interference. As a result, the light field is confined within the grating slab. Additionally, with Kx close to zero, the BIC is not ideal, but with a limited coupling rate to the free space. Nevertheless, a high quality factor can be reached within a near Kx = 0 regime.

    To clearly show how the SHG efficiency is enhanced in the dual BICs scheme, let us first recall the temporal coupled mode theory that describes SHG with a pair of resonant modes32, 37-39. Assuming that A and B are the amplitudes of the FW cavity mode and SHW cavity mode, respectively, and F is the amplitude of incident FW, then their mutual coupling can be described as38

    dAdt=(iω1γ1)A+g1Fiω1β1A*B,

    dBdt=(iω2γ2)Biω2β2A2,

    here ωjand γj(j = 1,2) mean the resonant angular frequency, and the dissipation rate of the cavity mode, respectively. gj demotes the coupling rate between the cavity mode and freely propagating FW in the continuum, and |g1|2=2γ1rad by considering the time reversal and energy conservation according to the temporal coupled mode theory. The last terms of both equations are energy transfer rates between the two cavity modes due to optical nonlinear interaction. The coupling coefficients β1=2β2*38, and β2 is expressed as

    β2=14TMDdrϵ0χxyy(2)E2x*E1yE1ydrϵ2|E1|2drϵ2|E2|2.

    Now, considering the undepleted pump approximation, the amplitude of SHW cavity modes can be derived as

    B=ω2β22ωω2iγ2g12F2(ωω1iγ1)2,

    then, the power of coupling-out SHW can be derived to be

    P2ω=2γ2rad|B|2=8γ2radω22|β2|2|2ωω2iγ2|2(γ1rad)2Pω2|ωω1iγ1|4.

    The relation Pω= |F|2 has been used in the derivation, where Pωdenotes the power of incident FW.

    By making the FW and SHW resonant with the pair of BICs, i.e., ω = ω1, and 2ω = ω2, we can derive for obtaining the result of dual BICs scheme as

    P2ωPω=64|χxyy(2)|2Q2Q12Pωε0λ3ωγ2radγ2(γ1rad)2γ12Z2ω,ωTMD.

    In the above equation, Z2ω,ωTMD is the dimensionless overlap coefficient of the paired BICs within the nonlinear 2D material region, expressed as

    Z2ω,ωTMD=|λ13TMDdrE2x*E1yE1ydrϵ1|E1|2drϵ2|E2|2|2.

    Note that ϵj(j = 1,2) is the relative dielectric function of the cavity material for the FW and SHW, respectively. From Eq. (8), we see that besides the well-known incident power Pωdependence, the SHG efficiency is proportional to the quality factors of the cavity mode Qj(j = 1,2), the ratio of radiative rate to the total dissipation rate of the two cavity modes γjrad/γj(j = 1,2), and the dimensionless overlap coefficient Z2ω,ωTMD. In the dual BICs scheme, the quality factors Qj(j = 1, 2) are optimized. There is no other dissipation channel for the cavities in an ideal situation, and γjrad/γj=1 (j = 1,2), then Z2ω,ωTMD is the only parameter that needs careful consideration. But in a real situation, absorption and scattering will cause additional dissipation, and then γjrad/γj (j = 1,2), together with Qjand Z2ω,ωTMD, will contribute to SHG.

    Simulation results and discussions

    Now we consider integrating TMDs monolayer onto the photonic grating slab. The selected TMDs monolayer is WS2 with thickness dWS2 = 0.618 nm, and its complex refractive index can be extracted from experimental data in the literature40, which is n˜TE=3.48+0.08i for FW (~1560 nm) and n˜TM=3.85+0.20i for SHW (~780 nm). A direct way is to place the WS2 monolayer on top of the grating slab as shown in the inset of Fig. 2(a). However, when we look close to the spatial mode structure of the BICs shown in Fig. 1(b), due to the symmetry-protected nature, the pair of BICs are of odd symmetry. As a result, the spatial overlap coefficient Z2ω,ωTMD will be zero at Kx = 0, since E2x(r) is odd symmetric while (E1y(ω, r))2 is even symmetric.

    Spatial overlap coefficient and SHG efficiency with a homogeneous WS2 on top of the photonic grating slab. (a) The Kx dependent spatial overlap coefficient Z2ω,ωTMD. (b) The Kx dependent SHG efficiency monitored at the reflected (top) and transmitted (bottom) side, respectively. The blue star is a reference point for showing the SHG efficiency with a freely-standing WS2 monolayer. The FW is incident from the top side of the grating, and the intensity of FW is set to be 0.1 GW/cm2.

    Figure 2.Spatial overlap coefficient and SHG efficiency with a homogeneous WS2 on top of the photonic grating slab. (a) The Kx dependent spatial overlap coefficient Z2ω,ωTMD. (b) The Kx dependent SHG efficiency monitored at the reflected (top) and transmitted (bottom) side, respectively. The blue star is a reference point for showing the SHG efficiency with a freely-standing WS2 monolayer. The FW is incident from the top side of the grating, and the intensity of FW is set to be 0.1 GW/cm2.

    To exploit double BICs for enhancing SHG, the zero spatial overlap case should be circumvented. This can be achieved by selecting quasi-BICs near Kx = 0 as the target cavity. Before evaluating the spatial overlap coefficient Z2ω,ωTMD between the paired quasi-BICs upon Kx, we need to find the doubly resonant condition at different Kx. To achieve this goal, we first simulated by scanning Kx and t, and obtained a set of interpolated curves with ωTE v.s.t and ωTM v.s. t at different Kx. With the set of curves, one can numerically get the value tm that makes ωTE = ωTM/2 at specific Kx, i.e., the doubly resonant condition. This result was further checked in a new full wave simulation with tm as the parameter. Through this procedure, we can get the structure parameter tm that makes the pair of quasi-BICs in resonances for enhancing SHG.

    With the eigenmode solution through full wave simulation at the doubly resonant condition, we calculate the dimensionless overlap coefficient at different Kx between the TE and TM type quasi-BICs. The result is shown in Fig. 2(a). As can be seen, Z2ω,ωTMD increases quickly when Kx leaves zero point, offering the possibility to enhance SHG in the dual BICs scheme.

    To confirm that the dual BICs scheme works in this case, the SHG efficiency P2ω/Pω is obtained by employing a full wave simulation under the undepleted pump approximation. In the simulation, a y-polarized FW is launched from the top side of the grating, and the incident angleθ is related to the wave vector Kxby Kx= ωTE/c0 sin(θ). The intensity of FW is set to be 0.1 GW/cm2. We monitor the power of SHW at the top and bottom sides at the same time. Since the structure is mirror-symmetric alongx direction, we did a simulation for Kxalong the positive direction, expecting that similar results can be obtained with Kx along the negative direction. The simulation result of SHG efficiency is shown in Fig. 2(b). As an example, the electric field distribution of FW and SHW at Kx = 0.01Ka are shown in the Supplemental information Section 2. From the result, we see that the SHG efficiency is quite low at Kx = 0, and is at the same order as that of freely standing WS2 monolayer (0.46 × 10−10 with freely standing WS2 with the same excitation intensity). This is expected since light does not couple into the BIC at this condition. However, SHG efficiency increases rapidly when leaving Kx = 0 point, and reaches a maximum value ~2 × 10−6 (> 4 × 104 times of that of freely standing WS2). After that, the SHG efficiency decreases slowly as the incident angle increases to Kx = 0.04Ka. This result clearly shows that the dual BICs scheme can work effectively for enhancing SHG with TMDs monolayer.

    To fully explore the potential of the dual BICs scheme, we propose to pattern the TMDs monolayer to avoid destructive interference for the dimensionless overlap coefficient shown in Eq. (9). We removed certain parts of the TMDs monolayer, and in each unit cell, only kept a strip TMDs monolayer of width 0.5w on top of the left-half grating strip, as shown in the inset of Fig. 3(a). In this way, Z2ω,ωTMD can be enlarged significantly. To confirm this result, we first find the doubly resonant condition at different Kx through the same procedure, as mentioned above. Then, we calculate the spatial overlap coefficient Z2ω,ωTMD at different Kx, and the result is shown in Fig. 3(a). Compared with the homogeneous case, Z2ω,ωTMD in the patterning case is increased up to ~100 times at Kx = ±0.01 Ka. This high overlap factor is expected to boost the SHG efficiency of WS2 monolayer further.

    Spatial overlap coefficient and SHG efficiency with a patterned WS2 on top of the photonic grating slab. (a) The Kx dependent spatial overlap coefficient Z2ω,ωTMD. (b) The Kx dependent SHG efficiency monitored at the reflected (top) and transmitted (bottom) side, respectively. The blue star is a reference point for showing the maximum SHG efficiency achieved in the case with homogeneous WS2 monolayer. The FW is incident from the top side of the grating, and the intensity of FW is set to be 0.1 GW/cm2.

    Figure 3.Spatial overlap coefficient and SHG efficiency with a patterned WS2 on top of the photonic grating slab. (a) The Kx dependent spatial overlap coefficient Z2ω,ωTMD. (b) The Kx dependent SHG efficiency monitored at the reflected (top) and transmitted (bottom) side, respectively. The blue star is a reference point for showing the maximum SHG efficiency achieved in the case with homogeneous WS2 monolayer. The FW is incident from the top side of the grating, and the intensity of FW is set to be 0.1 GW/cm2.

    To check the SHG enhancement, we did a full wave simulation to obtain the SHG efficiency by launching ay-polarized FW of 0.1 GW/cm2 from the top side. Again, we monitor the power of SHW at both the top and bottom sides of the photonic grating slab. The result of SHG efficiency is shown in Fig. 3(b), and the electric field distribution of FW and SHW at Kx = 0.01Ka are shown in the Supplemental information Section 3. From the result, we see that the SHG efficiency is significantly improved as compared to that with a homogeneous WS2 monolayer. The peak value of SHG efficiency reaches ~2 × 10−3 (> 4 × 107 times of that of freely standing WS2 monolayer) at a negative incident angle. At a positive incident angle, the enhancement factor is relatively lower, but the peak value still reaches ~2 × 10−4. This asymmetric behavior of SHG efficiency upon incident angle is related to mirror symmetry breaking by employing a patterned WS2 monolayer on top of the grating slab (see Supplemental information Section 4). It is precisely the same reason that enables light to be coupled in and out at Kx = 0, so that the SHG efficiency is significantly improved at Kx= 0, up to ~2 × 10−5.

    The SHG efficiency is limited by the intrinsic absorption of the WS2 monolayer both at the FW mode and the SHW mode. The intrinsic absorption of WS2 leads to the limited value of quality factor Qj (j = 1,2) (~24000 for TE-type BIC, and ~4800 for TM-type BIC in the pattering case). Therefore, the coupling coefficients ratio γjrad/γj (j = 1,2) contributes to the total SHG efficiency. To further enhance high SHG efficiency, one can consider spectrum range that is of low absorption, as well as 2D nonlinear materials of low absorption within the interested spectrum range. The finite size of a real 3D device will influence and lower the Q-factor due to the lattice perturbations at the edge breaking the coherence and leading to light scattering into free space. However, numerical investigation shows that a grating of several tens of unit cells can give rise to a high quality factor close to the theoretical one (Supplemental information Section 5). Besides, non-ideal fabrication of the photonic grating in practice could introduce scattering losses, which will affect the performance of BICs. Moreover, it would be interesting to extend the dual BICs scheme to other photonic systems for boosting SHG, and we have summarized the general procedure of designing the dual BICs scheme in Supplemental information Section 6.

    It has been found that the polarization of SHG signal can be changed by rotating the crystal orientation of TMDs monolayer41-43, due to the rich interference phenomena caused by the specific nonlinear susceptibility tensor of TMDs monolayer. Therefore, the polarization of the SHG signals in the dual BICs scheme should be related to the crystal orientation of the TMDs monolayer. We have investigated this effect by intentionally rotating the orientation of the TMDs monolayer, and the polarization-resolved SHG signal indeed shows an orientation angle dependence (See Supplemental information Section 7 for detailed description and results).

    Notably, GaP is a nonlinear optical material, and can exhibit SHG under appropriate condition44-46, which has been attracting a lot of attention in linear and nonlinear nano photonics recently47-49. However, here we consider GaP with its crystal axis corresponding to the axis (x, y, z) in Fig.1 (a), and therefore, due to its specific nonlinear susceptibility, GaP does not exhibit SHG under the incident y-polarized (TE-mode) pump light, and works only as a high refractive index linear material. In a relatively different configuration, i.e., rotating the polarization of pump light to 90 degrees against y axis and scanning the incident angle, GaP can exhibit SHG. In this configuration, the SHG efficiency of GaP is shown in the Supplemental information Section 8, and the maximum efficiency is achieved at a relatively large incident angle (>50 degrees), but is about 2 orders lower than that with homogeneous WS2 monolayer, and 5 orders lower than that with patterned WS2 monolayer.

    Conclusions

    In conclusion, we propose a dual BICs scheme to enhance SHG with TMDs monolayer. We have shown that a photonic grating slab can be designed to work in the dual BICs regime, i.e., the FW and SHW are resonant with the TE-type and TM-type BICs, respectively. To fully exploit the advantages of the dual BICs scheme, we have investigated strategies to overcome the limitation of zero overlap coefficient for SHG. With a homogeneous TMDs monolayer on top of the grating, we demonstrated that the spatial overlap coefficient increases as Kx. Subsequently, we managed to optimize SHG by tilting the incident angle of FW, giving rise to > 4 × 104 times enhancement at Kx ≈ ±0.01Ka, as compared to the free-standing situation. Moreover, we showed that patterning the TMDs monolayer can significantly improve the spatial mode overlap coefficient, further boosting the SHG in the dual BICs scheme. We showed that the maximum SHG efficiency at the patterning case is ~103 times larger than homogeneous TMDs monolayer at Kx≈ 0.01Ka. And in total, the SHG efficiency reached > 4 × 107 times enhancement compared with that with freely standing WS2 monolayer. These results offer new possibilities to enhance SHG in practical applications with TMDs monolayers, which opens new opportunities for nonlinear optics with atomic thin 2D materials.

    References

    Peilong Hong, Lei Xu, Mohsen Rahmani. Dual bound states in the continuum enhanced second harmonic generation with transition metal dichalcogenides monolayer[J]. Opto-Electronic Advances, 2022, 5(7): 200097
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