Nanofocusing of mid-infrared electromagnetic waves on graphene monolayer Weibin Qiu, Xianhe Liu, Jing Zhao, Shuhong He, Yuhui Ma, Jia-Xian Wang, and Jiaoqing Pan Citation: Applied Physics Letters 104, 041109 (2014); doi: 10.1063/1.4863926 View online: http://dx.doi.org/10.1063/1.4863926 View Table of Contents: http://scitation.aip.org/content/aip/journal/apl/104/4?ver=pdfcov Published by the AIP Publishing Articles you may be interested in Approaching total absorption at near infrared in a large area monolayer graphene by critical coupling Appl. Phys. Lett. 105, 181105 (2014); 10.1063/1.4901181 Increase of the grating coupler bandwidth with a graphene overlay Appl. Phys. Lett. 104, 111109 (2014); 10.1063/1.4869219 Infrared spectroscopy of large scale single layer graphene on self assembled organic monolayer Appl. Phys. Lett. 104, 041904 (2014); 10.1063/1.4863416 Narrowband mid-infrared transmission filtering of a single layer dielectric grating Appl. Phys. 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Downloaded to IP: 159.226.228.14 On: Thu, 19 Mar 2015 06:21:03 APPLIED PHYSICS LETTERS 104, 041109 (2014) Nanofocusing of mid-infrared electromagnetic waves on graphene monolayer Weibin Qiu,1,2,a),b) Xianhe Liu,1,a) Jing Zhao,1 Shuhong He,1 Yuhui Ma,1 Jia-Xian Wang,1 and Jiaoqing Pan2 1 College of Information Science and Engineering, National Huaqiao University, Xiamen 361021, Fujian, China 2 Institute of Semiconductors, Chinese Academy of Science, 100083 Beijing, China (Received 23 September 2013; accepted 19 January 2014; published online 29 January 2014) Nanofocusing of mid-infrared (MIR) electromagnetic waves on graphene monolayer with gradient chemical potential is investigated with numerical simulation. On an isolated freestanding monolayer graphene sheet with spatially varied chemical potential, the focusing spot sizes of frequencies between 44 THz and 56 THz can reach around 1.6 nm and the intensity enhancement factors are between 2178 and 654. For 56 THz infrared, a group velocity as slow as 5 105 times of the light speed in vacuum is obtained at the focusing point. When the graphene sheet is placed on top of an aluminum oxide substrate, the focusing spot size of 56 THz infrared reduces to 1.1 nm and the intensity enhancement factor is still as high as 220. This structure offers an approach for focusing light in the MIR regime beyond the diffraction limit without complicated device geometry C 2014 AIP Publishing LLC. [http://dx.doi.org/10.1063/1.4863926] engineering. V Nanofocusing of electromagnetic (EM) waves in surface plasmon polariton (SPP) waveguide structures has attracted intensive attention due to its promising applications in the fields of sensing,1–3 tip-enhanced Raman spectroscopy,4 extreme ultraviolet (EUV) generation,5 and optical nonlinearity.6 Until now, various nanostructures, such as taped gaps,7 nanowedges,8 pyramids,9 and cones,10 have been demonstrated both theoretically and experimentally to achieve nanofocusing of EM waves. In many reported structures, the geometry is altered gradiently as the plasmon wave propagates and the EM field is enhanced as the group velocity slows down, achieving nanofocusing eventually.11–14 Though the nanofocusing of mid-infrared (MIR) or farinfrared (FIR) light is important for various applications, such as probing,15 spectroscopy,16 and chemical analysis,17 metals like gold and silver commonly used in the structures mentioned above are not ideal for MIR regime due to the poor field confinement and the intrinsic mismatch between MIR and the surface plasmon resonance frequencies of these metals.18,19 Graphene, a 2-dimentional (2D) material composed of a single carbon atom layer, has caught intensive interest due to its unique electronic band structure and promising applications in electronic and photonic devices,20–24 metametarials,25 optical cloaking,26 femtosecond lasers,27 nonlinear optics,28 and solar cells.29 Furthermore, SPP waves can propagate on graphene with supporting substrate30 and possess outstanding advantages, such as relatively low loss, high confinement, and most significantly, tunability of chemical potential.31 In this letter, we numerically analyze nanofocusing of MIR on a graphene monolayer, which has spatially gradient chemical potential without complicated device geometry. This would be an effective alternative to tapered waveguide structures that have more complicated geometry and higher cost in terms of fabrication. For analyzing the mechanism of nanofocusing, the system of interest shown in Fig. 1 is air-graphene-air configuration, where the one-atom thick graphene sheet is located in an XOZ plane. The SPP waves are launched at x ¼ 0 nm, propagating along positive x direction. It has been pointed out that as long as the thickness of the material becomes extremely small compared to the wavelength, the value of the thickness loses the meaning, i.e., different thicknesses yield similar propagation properties and are equivalent in terms of simulation.30,32 In our simulation, we treat the graphene monolayer as a 2D sheet with zero thickness. Thus, in the configuration, where the zero thickness graphene sheet is surrounded by air, graphene itself is the boundary. There is surface current density J ¼ rs E along graphene, where E is the electric field and rs is the surface conductivity of the graphene sheet. Since it is 2D current existing in the monolayer graphene sheet, there is obviously no current in y direction. The non-zero components of the EM field are Hz, Ex, Ey. The electrical field component perpendicular to the graphene sheet, Ey, is discontinuous and anti-phase, while Ex parallel a) FIG. 1. Schematic of a monolayer graphene sheet located in the XOZ plane. SPP waves are launched at x ¼ 0 nm and propagate along positive x direction. Weibin Qiu and Xianhe Liu contributed equally to this work. Author to whom correspondence should be addressed. Electronic addresses: wbqiu@hqu.edu.cn and wqiu@semi.ac.cn b) 0003-6951/2014/104(4)/041109/5/$30.00 104, 041109-1 C 2014 AIP Publishing LLC V This article is copyrighted as indicated in the article. Reuse of AIP content is subject to the terms at: http://scitation.aip.org/termsconditions. Downloaded to IP: 159.226.228.14 On: Thu, 19 Mar 2015 06:21:03 041109-2 Qiu et al. Appl. Phys. Lett. 104, 041109 (2014) to graphene is continuous and in-phase. Hz is also discontinuous due to the existence of the surface current. The dispersion relation of the SPP wave propagating along the graphene sheet surrounded by air is given by b ¼ k0 qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi 1 ð2=g0 rs Þ2 ; (1) where b is the complex propagation constant along graphene, k0 is the propagation wave number in free space, rs is the surface conductivity of graphene sheet, and g0 (377 X) is the impedance of the air.30,32 Note that we only consider transverse-magnetic surface waves.33 rs has the contributions from both interband electron transition and intraband electron-photon scattering, i.e., rs ¼ rinter þ rintra . rinter and rintra can be expressed as " # e2 2jlc j hðx þ is1 Þ ln (2) rinter ¼ i 4ph 2jlc j þ hðx þ is1 Þ and rintra e2 k B T lc lc þ 2ln exp þ1 ; ¼i 2 kB T p h ðx þ is1 Þ kB T (3) where s is momentum relaxation time, x is radian frequency, lc is chemical potential, T is temperature, h is the reduced Planck constant, and kB is the Boltzmann constant.26 In this letter, we choose the temperature to be 300 K and s ¼ 0:5 ps, which is conservative for practical graphene.26,34 It should be noted that the chemical potential lc can be modified locally by doping35,36 and biased gate voltage,37,38 which is the particular advantage of graphene over metals commonly used. In general, the complex wavenumber obtained from Eq. (1) can be expressed as the sum of the real part and the imaginary part b ¼ b0 þ ib00 , where b0 denotes the wavenumber, while b00 describes the loss property of SPP waves. Larger b0 implies shorter wavelength and stronger localization of EM waves. The wavenumber b0 and the group velocity of SPP waves on graphene sheet with spatially homogeneous lc are shown in Fig. 2(a) as a function of frequency f. Here, we define that for a certain chemical potential, the critical frequency fc is the frequency that gives equal real part and imaginary part of the complex wavenumber, i.e., b0 ¼ b00 . In other words, the SPP wave is fully damped. The curve of the inset of Fig. 2(b) shows critical frequency corresponding to different chemical potentials. As the frequency approaches the critical frequencyfc for a certain chemical potential, b0 increases drastically. Since 2p=b0 is the wavelength of the SPP wave and implies the spatial extension of EM waves, the confinement of the EM waves along graphene is very strong and nanofocusing effect is expected around this frequency fc . For example, the critical frequencies for chemical potentials of 0.12 eV and 0.40 eV are 48.1 THz and 160.9 THz, respectively. Furthermore, the group velocity vg becomes very low around the critical frequency. Ideally, if b0 goes to infinite as the frequency increases, zero group velocity of the SPP wave would be achieved and the wavelength FIG. 2. (a) The dispersion relation and group velocity of SPP waves propagating along freestanding graphene with homogeneous chemical potential. (b) The wavenumber and group velocity of SPP waves as a function of chemical potential. The inset in (b) shows the critical frequency as a function of chemical potential. The green regime indicates that SPP waves are allowed and the red regime indicates that SPP waves are fully damped or not supported. For each chemical potential, calculation is not performed for frequencies higher than its critical frequency. of the SPP wave would shrink to zero as well, which means that the EM field is concentrated on a singularity point on the graphene sheet. Of course, there is loss accompanying wave propagation and such ideal case is hardly achievable. Similar behavior will occur when the frequency is kept fixed and the chemical potential is gradually reduced, which means that the SPP wave of a certain frequency propagates along a graphene sheet with spatially decreasing gradient chemical potential. This scenario is indicated by the blue trajectory in the inset of Fig. 2(b). The green regime means b0 > b00 and the red regime means b0 < b00 or SPP waves are not supported. As the chemical potential decreases, b0 becomes larger, the confinement of the light field becomes stronger, and the group velocity slows down. Together with the slowing down of group velocity, the intensity accumulates and becomes increasingly higher, which is essentially a result of energy conservation.39 As the point follows the trajectory and approaches the red regime in the inset of Fig. 2(b), the chemical potential goes sufficiently low and the loss of the SPP waves becomes higher and higher at the same time. Therefore, nanofocusing effect actually depends on the competition between energy accumulation and loss during propagation. As long as the energy accumulation rate far exceeds energy loss rate, nanofocusing effect can be expected. Additionally, if the launched wave has several frequency components, different frequencies would be focused at different positions on a graphene sheet with appropriately designed chemical potential distribution. This article is copyrighted as indicated in the article. Reuse of AIP content is subject to the terms at: http://scitation.aip.org/termsconditions. Downloaded to IP: 159.226.228.14 On: Thu, 19 Mar 2015 06:21:03 041109-3 Qiu et al. Appl. Phys. Lett. 104, 041109 (2014) To numerically justify the discussion above, we conducted finite element method simulation using COMSOL Multiphysics Ver 4.3b to compute the light field of SPP waves propagating along a graphene monolayer with gradient chemical potential lc . The graphene sheet is in the XOZ plane at y ¼ 250 nm and SPP waves are launched at x ¼ 0 nm. The distribution of chemical potential lc over the graphene sheet is a function of position. In our simulation, it is defined to be lc ¼ lc0 ½1 expð0:015ðx 1000ÞÞ; (4) where lc0 ¼ 0:4 eV is the chemical potential at x ¼ 0 nm. The purpose of choosing this distribution is nothing more than having a spatially rapidly varied chemical potential. The frequencies of simulated SPP waves are 44, 47, 50, 53, and 56 THz. The corresponding wavelength in free space is 6.81 lm, 6.38 lm, 6.00 lm, 5.66 lm, and 5.35 lm. The evolution of jEj during propagation at y ¼ 250 nm, i.e., along the graphene sheet, is shown in Fig. 3(a) and the values have been normalized with the norm of electric field at the launching point jE0 j. The intensity enhancement factor R ¼ jEpeak j2 =jE0 j2 reaches 654 for 56 THz and even 2178 for 44 THz. The full width at half maximum (FWHM) of the focusing spot of 56 THz is 1.6 nm. It is obvious that other frequencies have spot size on the same order, which indicates that nanofocusing effect is achieved for different frequencies FIG. 3. (a) The evolution of electric field norm around the focusing spots along the graphene sheet at y ¼ 250 nm. The values are normalized by the electric field norm at the launching point. The inset shows how the chemical potential varies near the focusing spots. (b) The time averaged energy density distribution near the focusing spots. The values are normalized by the time averaged energy density at the launching point. If five frequencies are launched together, they will be focused at different positions. The inset in (b) is a magnification of the focusing spot of 44 THz. on the same structure. The five distinct focusing spots of the frequencies are clearly shown in Fig. 3(b), where the time averaged energy density of each frequency is normalized by the time averaged energy density at the launching point. Since the position of the focusing spot depends on the chemical potential distribution, it can be tuned by modifying the distribution of chemical potential. Meanwhile, the intensity enhancement factor R might be changed consequently as well. Passing the focusing spot, the SPP waves vanish due to EM loss.9 Before the SPP waves reach the focusing spot, the local chemical potential is far above hx=2, rinter has a small real part and the loss is dominated by intraband electronphoton scattering, thereby bringing very limited loss to the propagation of SPP waves. However, when the chemical potential continues decreasing and reaches around hx=2, the contribution of loss from interband electron transition indicated by Eq. (2) becomes more significant and eventually dwarfs the counterpart from intraband electron-photon scattering,26,27 rendering the SPP waves to vanish. In a way similar to defining critical frequency, the critical chemical potential lc for a certain frequency can be defined as the chemical potential that gives b0 ¼ b00 . It is worthwhile to point out that the position of the focusing point is determined by the location of the criticallc , while the size of the focusing point is fully controlled by how rapidly lc approaches the critical value. Practically, one should keep the chemical potential far above hx=2 to avoid propagation loss and then reduce it to the critical value as rapidly as possible at the desired position to achieve nanofocusing. Under the chemical potential distribution governed by Eq. (4), the group velocity remains almost unchanged before the chemical potential falls down rapidly. Take 56 THz as an example. At the FWHM of the focusing spot, the group velocity drastically slows down to 5 105 times the light speed in vacuum, effectively enabling energy accumulation in the vicinity of the focusing spot. From a practical point of view, graphene may be supported by a substrate rather than remain isolated in free space. We apply the same principle of nanofocusing to this case though the substrate can introduce quantitative difference to the dispersion relation. The jHj field loses the symmetry along y direction, albeit the jEj field keeps symmetric over the air and the substrate. According to eigen SPP mode analysis, the EM energy of SPP waves is dominated by electric field. The time averaged EM energy density is given by hwi ¼ ðl0 lr jHj2 þ e0 er jEj2 Þ=2. Thus, the energy stored in the substrate at the focusing point is approximately er;sub times that in the air above the graphene sheet. In order to demonstrate the ability of graphene sheet on a substrate to focus SPP waves, aluminum oxide film is used as the substrate in the simulation and 56 THz is the frequency as an example. The chemical potential distribution remains the same as the freestanding graphene case. Aluminum oxide sits below y ¼ 250 nm and the graphene sheet is still in the XOZ plane at y ¼ 250 nm. The refractive index of aluminum oxide is approximately 1.48 and the material absorption is negligible.40 Figure 4(a) reveals the |E| distribution of 56 THz MIR focused at x ¼ 971 nm with FWHM of 1.1 nm and the intensity enhancement factor R is around 220, showing that the mechanism of nanofocusing is still valid. Also as This article is copyrighted as indicated in the article. Reuse of AIP content is subject to the terms at: http://scitation.aip.org/termsconditions. Downloaded to IP: 159.226.228.14 On: Thu, 19 Mar 2015 06:21:03 041109-4 Qiu et al. Appl. Phys. Lett. 104, 041109 (2014) In summary, we proposed and numerically analyzed nanofocusing of MIR in monolayer graphene with gradient chemical potential distribution. Nanofocusing was dominated by the competition between energy accumulation and loss during propagation. Intensity enhancement factors obtained on isolated freestanding graphene were between 2178 and 654 for frequencies between 44 THz and 56 THz. For a graphene sheet resting on aluminum oxide substrate, the intensity enhancement factor could still reach 220 for 56 THz. The proposed structure was planar structure without any tapers, wedges, grooves, or cones, which were commonly studied in other literatures. This is an effective alternative to achieving nanofocusing of MIR without complicated and expensive device geometry engineering. Last but not least, the nanofocusing effect can be tuned by tailoring the chemical potential distribution and there would be a broad span of applications, including sensing, nanoimaging, single molecule detection, optical information process, and ultrahigh density optical storage. FIG. 4. (a) The electric field norm around the focusing spot of 56 THz light. The values are normalized by the electric field norm at the launching point. (b) The time averaged energy density distribution near the focusing spots. The value is normalized by the time averaged energy density at the launching point. Below y ¼ 250 nm is the aluminum oxide substrate with a refractive index of 1.48. The graphene sheet is in the plane of y ¼ 250 nm. The intensity enhancement factor is 220. Pronounced nanofocusing effect still occurs, though weaker than freestanding case. The authors are grateful to the support by the National Science and Technology Major Project under Grant No. 2011ZX02708, the National 863 Project under Grant No. 2012AA012203, the Opened Fund of the State Key Laboratory on Integrated Optoelectronics under Grant No. IOSKL2012KF12. 1 expected in Fig. 4(b), the time averaged energy density in the substrate is er;sub times as high as that in the air. Though the intensity enhancement factor R is now lower than 654 for the same frequency in the freestanding case, it is still considerable enhancement. The reason for the drop of intensity enhancement factor is that the existence of the substrate underneath changes the loss property of SPP waves. If low loss is desired for practical application purpose, low refractive index material is preferable. When it comes to fabricating a real structure, several other issues might also be taken into account. First, rough substrate surface usually introduce extra light scattering, thereby enhancing the attenuation of the SPP waves. It is favorable to use substrate with high surface quality. Second, if doping is used for realizing gradient chemical potential, a reasonably high doping level should be carefully chosen. Usually dopants may scatter electrons associated with SPP wave propagation and consequently reduce relaxation time s. It may not be recommended to have extremely high doping level. Third, if the chemical potential is controlled by a gate, the electrostatic design should meet two requirements simultaneously, effective control over the chemical potential and weak influence on the propagation of SPP waves. 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