Towards 3D Electromagnetic Metamaterials in the THz Range B. D. F. Casse, H. O. Moser, M. Bahou, P. D. Gu, L. K. Jian, J. R. Kong, S. B. Mahmood and L. Wen Singapore Synchrotron Light Source (SSLS), National University of Singapore (NUS), 5 Research Link, Singapore 117603. Abstract. SSLS has been using its lithography-based micro/nanofabrication facility LiMiNT (Lithography for Micro and Nanotechnology) and its infrared spectro/microscopy facility ISMI to develop and characterize the first electromagnetic metamaterials having their spectral response in the THz range. Derived from Pendry’s nested-split-ring resonator design, these structures require micro/nanofabrication in order to have resonances in the THz range. They exhibit a negative refractive index and hold promise of sub-diffraction limit imaging. Besides the reduction of the size of the resonating structures to extend the spectral range towards the visible, outstanding issues include the production of high-aspect-ratio resonators that are sensitive for the magnetic field in any direction (3D sensitivity) and the capability to produce copious amounts of the electromagnetic metamaterials with a good yield. In this paper, we shall report on first results of 3D EM3 structures made by inclined exposures. Keywords: Electromagnetic Metamaterials, EM3, THz, Left-Handed Materials, 3D structures, Microfabrication, LIGA PACS: 42.70.Qs, 41.20.Jb, 73.20.Mf, 78.20.Ci

INTRODUCTION Electromagnetic Metamaterials (EM3 ) refer to artificially engineered structures having simultaneously negative permittivity ε and permeability µ . EM3 represent a new class of composite materials capable of exhibiting a negative index of refraction and possessing “superlenses” properties [1]. The significant achievements, from a micro/nanofabrication point of view of EM3 , are: 1) theoretical investigation of left-handed materials and prediction of their exotic properties by Veselago in 1967 [2]; 2) Pendry’s recipes for manufacturing εeff < 0 [3] and µeff < 0 [4] by a combination of wire arrays and split-ring resonators (SRRs) respectively; 3) EM3 operating in the GHz range; 4) the first microfabricated EM3 operating in the THz range [5]; 5) negative µ square split rings in the THz range [6]; 6) the first nanofabricated negative µ materials operating around 100 THz [7] and various EM3 structures beyond the 100 THz regime [8] [9] [10] [11]. EM3 structures produced so far in the terahertz range have been mostly two-dimensional (2D), and are therefore highly anisotropic. By anisotropy, it is inferred that the response of the system depends on the direction of illumination. For instance the split ring resonators behave as an LC circuit when incoming electromagnetic radiation has magnetic field components polarized parallel to the rings’ axis. Gay-Balmaz and Martin [12] were among the first to propose more three-dimensional (3D) EM3 by assembling planar EM3 structures such that they offer full coupling for the incident electric and magnetic fields in two or three orthogonal directions. Although this is seemingly the most logical way of obtaining isotropic structures, the technique of assembling planar unit cells becomes highly impractical when it comes to µm-size structures and below. Recently, we proposed schemes [8] [13] to produce more isotropic structures, within the same matrix, via tilted X-ray exposures that were introduced in the LIGA1 process years ago [14] [15] [16]. In this paper, we present first results of microfabrication of nearly 3D EM3 structures for the THz range. For the sake of rapid prototyping we limit ourselves to the fabrication of µeff < 0 rings as the implementation of the additional rod structure is obvious.

EXTRUDING THE 2-D PENDRY’S NESTED RINGS TO PRODUCE 3D STRUCTURES The split ring resonator of Sir John Pendry [4] shown in figure 1 forms the backbone of practically all metamaterials. It is designed to have a very strong magnetic response and potentially one that can lead to a negative effective

1

LIGA stands for the German words: LIthographie (Lithography), Galvanoformung (Electroplating) and Abformung (Molding)

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Plan view of a split ring showing geometric parameter definitions (left). Periodic arrangement the split rings (right).

permeability. The idea of achieving a magnetic response from conductors comes from the basic definition of a magnetic dipole moment m. Z 1 m= r × j dV (1) 2 where j is the current density. From the definition in (1), we can see that a magnetic response can be obtained if local currents can be induced to circulate in loops. Now if one introduces a resonance into the element, a negative effective permeability can be achieved at resonance because of the phase shift between exciting and resonating fields. The split ring resonator can be viewed as an LC circuit where a time-varying magnetic field applied parallel to the axis of the rings induces an emf in the plane of the element, driving currents within the ‘split rings’. The lower and upper limit of the frequency interval over which µeff < 0 was calculated from Pendry’s analytical formula [4] s 3dc20 1 ν0 ν0 = (2) < νmp = p 2π π 2 r3 1 − π r2 /ab where c0 is the speed of light in vacuo. In X-ray deep lithography, the angle of incidence can be varied to obtain inclined exposures as shown in figure 2 (left). The stack could even be rotated either continuously or to different positions between exposures. This tilting, rotating and even wobbling was proposed several years ago [14] [15]. By exploiting the full potential of LIGA, we can produce EM3 structures in which the axes of the SRRs would cover two (or even three) intersecting or perpendicular directions so that the incident field can always couple efficiently to the SRRs as shown in figure 2 (right). For structures inclined at an angle θ ◦ to the normal, an incident beam would always have a component H sin θ along the rings’ axis. The planar case corresponds to θ = 0 ◦ .

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FIGURE 2. Double angle X-ray exposures [1=+θ , 2=−θ to the normal] to produce 3D inclined SRR structures within the same matrix (left). For structures inclined at an angle θ ◦ to the normal, an incident beam would always have a component H sin θ along the rings’ axis (right).

MICROFABRICATION OF THE 3D EM3 STRUCTURES To produce the X-ray mask for the inclined EM3 structures, a two-stage lithography process has been developed: The first stage consisted of generating an intermediate optical mask by direct laser writing. The optical mask is made up of 0.09 inch soda lime glass covered with a first layer of 800 Å thick chromium and followed by a 0.5 µm thick AZ 1518 resist on top of the Cr layer. An AutoCAD design file containing split rings (with parameters r = 15 µm, c = 15 µm, d = 10 µm, g = 10 µm) was generated in 2 × 2 cm2 arrays and transferred into the AZ 1518 photoresist using direct laser writing with the DWL 66 2 . The DWL 66 is equipped with a 20 mW HeCd laser of 442 nm wavelength. The 20 mm write-head, allowing minimum feature sizes of 4 µm, was used in a double pass exposure. The positive photoresist was then developed in the AZ 400K developer followed by an immersion of the optical mask in a chromium etch for 2 minutes. The second stage consisted of producing a graphite mask with a gold absorber. SU8 2025 was spin coated onto a graphite wafer such that a thickness of 20 µm was achieved. Pattern transfer from the optical mask to the graphite mask was done by deep UV exposure using a Karl Suss MA8 contact UV mask aligner. A gentle oxygen plasma etch was applied to the graphite mask to remove residual resist in the developed areas. The graphite mask was brought into a gold electroplating bath in order to obtain nested split rings on the graphite membrane. Electroplating was carried out at a current density of 0.1 A/dm2 and temperature of 55 ◦ C. In order to produce EM3 materials for transmission experiments, the rings have to be embedded in a material that features high transparency in the relevant THz frequency range. SU8 2100 was chosen because of it’s good transparency in the far infrared region, short exposure time even for thick SU8 samples, and sufficient ruggedness to survive mechanical handling. SU8 2100 was spin coated onto a 4 inch silicon wafer, which had been sputtered with 40 nm of titanium and 100 nm of gold on top of the Ti layer, until a thickness of 200 µm was achieved. X-ray exposures were performed at angles of ± 10 ◦ , ± 30 ◦ and ± 45 ◦ to the normal of the mask-substrate stack to show the expected deterioration of the mask contrast at higher incidence angles. A secondary slit-type absorber was used, on alternate rings columns to prevent exposing open areas twice. i.e., the slits exposed odd columns of rings to the X-rays and blocked even ones for the first exposure, and vice versa for the second exposure. The final step was to postbake the SU8, resist development, descumming, and nickel electroplating at 0.4 A/dm2 . The SU8 chips were then peeled off the silicon wafer by stressing the plating and cleaving the back side of the wafer. Mask

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FIGURE 3. Cross section of resist template at 30 ◦ (left) exposure to the normal [scale bar 100 µm]. Lacking mask contrast prevents the formation of good structures. Qualitative dose deposition profile for various irradiation inclinations (right).

At 45 ◦ exposures the rings are deformed. This is due to the fact that light cannot penetrate the small inner ring gap (d = 10 µm) at this angle and thus does not cross link the areas in between the rings. At 30 ◦ to the normal (shown in figure 3 (left)), we are at the limit where light can penetrate the nested rings gap. The top part of the template looks acceptable but examining the cross section of the structure reveals that the bottom part has some deformations. The ideal dose profile is rectangular (corresponding to perpendicular irradiation) as shown in figure 3 (right). At 10 ◦ , the profile becomes trapezoidal, while at 30 ◦ , the dose profile is triangular. To obtain the best inclined structure, a 10 ◦ inclination was chosen, in order to have a dose profile as close as possible to the ideal one. Figure 4 (left) shows the cross section of a resist template that has been exposed at 10 ◦ to the normal. For this configuration, we observe a well-defined structure with straight sidewalls. A clean double angle exposures at ± 10 ◦

2

DWL 66 is a registered trademark of Heidelberg Instruments Mikrotechnik GmbH, Germany

to the normal is shown in figure 4 (right).

FIGURE 4. Cross section of resist template at 10 ◦ exposure to the normal (left). Double angle exposures at ± 10 ◦ to the normal (right). [Scale bar 100 µm].

CONCLUSION We have produced nearly three-dimensional (3D) split ring resonators (SRRs), within the same resist matrix using the LIGA process. By making the structures more isotropic, we remove the H polarization constraint placed on the impinging electromagnetic waves by the media. Basic geometry indicates that such 3D nested rings could lead to an improvement of the coupling of the H vector and thus ease future implementations of the latter in real-life applications. To produce inclined structures facing each other in the matrix of the SU8 2100 negative resist, a secondary slit-type absorber was used which prevents exposing the same areas twice. The slits are not necessary if we were dealing with a positive resist (e.g. PMMA), but the known drawback of PMMA is the long exposure time for high-aspect-ratio structures. Work is under way in SSLS to characterize the 3D composite structures by means of infrared spectroscopy.

ACKNOWLEDGMENTS The authors would like to thank Joe Wing Lee for his contribution to the microtechnology processes. This work was performed at the Singapore Synchrotron Light Source (SSLS) under A*STAR/MOE RP3979908M, A*STAR 0121050038, and NUS Core Support C-380-003-003-001 grants.

REFERENCES 1. 2. 3. 4. 5. 6. 7. 8. 9. 10. 11. 12. 13. 14. 15. 16.

J. B. Pendry, Phys. Rev. Lett. 85, 3966 (2000). V. G. Veselago, Sov. Phys. Usp. 10, 509 (1968). J. B. Pendry, A. J. Holden, W. J. Stewart, and I. Youngs, Phys. Rev. Lett. 76, 4773 (1996). J. B. Pendry, A. J. Holden, D. J. Robbins, and W. J. Stewart, IEEE Trans. Microwave Theory Tech. 47, 2075 (1999). H. O. Moser, B. D. F. Casse, O. Wilhelmi, and B. T. Saw, Phys. Rev. Lett. 94, 063901 (2005). T. J. Yen, W. J. Padilla, N. Fang, D. C. Vier, D. R. Smith, J. B. Pendry, D. N. Basov, and X. Zhang, Science 303, 1494 (2004). S. Linden, C. Enkrich, M. Wegener, J. Zhou, T. Koschny, and C. M. Soukoulis, Science 306, 1351 (2004). H. O. Moser, B. D. F. Casse, O. Wilhelmi, and B. T. Saw, “Electromagnetic Metamaterials over the whole THz range — achievements and perspectives, Proceedings of the ICMAT 2005 Symposium R (Electromagnetic Materials),” World Scientific, Singapore, 2005, pp. 55–58, ISBN 981-256-411-X(pbk). B. D. F. Casse, H. O. Moser, O. Wilhelmi, and B. T. Saw, “Micro- and Nano-Fabrication of Electromagnetic Metamaterials for the Terahertz range, Proceedings of the ICMAT 2005 Symposium R (Electromagnetic Materials),” World Scientific, Singapore, 2005, pp. 18–25, ISBN 981-256-411-X(pbk). B. D. F. Casse, H. O. Moser, M. Bahou, L. K. Jian, and P. D. Gu, in press for IEEE Transactions on Nanotechnology (2006). S. Zhang, W. Fan, N. C. Panoiu, K. J. Malloy, R. M. Osgood, and S. R. J. Brueck, Phys. Rev. Lett. 95, 137404 (2005). P. Gay-Balmaz, and O. J. F. Martin, J. Appl. Phys. 81, 939–941 (2002). B. D. F. Casse, H. O. Moser, L. K. Jian, M. Bahou, O. Wilhelmi, B. T. Saw, and P. D. Gu, Journal of Physics: Conference Series 34, 885–890 (2006). H. O. Moser, W. Ehrfeld, M. Lacher, and H. Lehr, “Fabrication of Three-dimensional Microdevices from Metals, Plastics and Ceramics,” Institut des Microtechniques de Franche-Compté, Besançon, France, 1992. W. Bacher, P. Bley, and H. O. Moser, Optoelectronics Interconnects and Packaging, SPIE Critical Reviews of Optical Science and Technology CR62, 442–460 (1996). G. Feiertag, W. Ehrfeld, H. Freimuth, H. L. H. Kolle, M. Schmidt, M. M. Sigalas, C. M. Soukoulis, G. Kiriakidis, T. Pedersen, J. Kuhl, and W. Koenig, Appl. Phys. Lett. 71, 1441 (1997).

Towards 3D Electromagnetic Metamaterials in the THz ...

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