Supporting Information Surface plasmon modes guided by Ga-doped ZnO layers bounded by different dielectrics Wasanthamala Badalawa 1, Hiroaki Matsui 1, Akifumi Ikehata2 and Hitoshi Tabata 1, 3 1 Department of Electrical Engineering and Information Systems, University of Tokyo, Bunkyo-ku, Tokyo 113-8656, Japan. 2 Analytical Science Division Nondestructive Evaluation Laboratory, National Food Research Institute, Tsukuba, Ibaraki 305-8642, Japan. 3 Department of Bioengineering, University of Tokyo, Bunkyo-ku, Tokyo 113-8656, Japan. 1) Lattice parameters and crystallinity of ZnO: Ga layers ZnO: Ga (7%) layers were grown on glass substrates (BK-7) using a pulsed layer ablation at 260oC in an O2 atmosphere at 10-4 Pa. Lattice parameters and crystallinity were evaluated by x-ray diffraction (XRD). Figures S1 show the 2/ patterns of the (0002) plane of 218-nm, 107-nm and 41-nm-thick layers, revealing that all layers were polycrystalline with a preferential orientation along the c-axis direction. c-axis lattice length slightly increased with decreasing layer thickness. Full-width half-maximum (FWHM) values of 218-nm, 107-nm, and 41-nm-thick layers were 0.31o, 0.30o and 0.37o, respectively. Lattice parameters and crystallinity of 218 nm-thick layer were similar to those of 107-nm and 41-nm-thick layers. 1000000 (0002) 100000 100000 10000 k WL c = 5.221Å 10000 (0002) t = 218nm 100 100 35 35 2 (degree) 40 40 (c) 100000 c = 5.227Å k (0002) c = 5.233Å 10000 WL 1000 1000 30 30 1000000 (b) Intensity (a.u.) (a) Intensity (a.u.) Intensity (a.u.) 1000000 k WL 1000 t = 107nm 30 30 35 2 (degree) 35 40 40 100 t = 41nm 30 30 35 35 2 (degree) 4040 Figure S1. 2 diffraction patterns of the (0002) plane for the ZnO: Ga layers with different layer thicknesses (t): (a) 218 nm, (b) 107 nm, and (c) 41 nm. 2) The complex dielectric functions of ZnO: Ga layers Figure S2 (a) shows the complex dielectric functions ( = 1 +i2) of ZnO: Ga layer (218-nm thickness) calculated using “Lorentz oscillator and Drude model” from experimental results of absolute transmission and reflection measurements, as measured in frequency range from 4,000 to 10,000cm-1. On the other hand, the complex dielectric functions of 107-nm-thick and 42-nm-thick layers were obtained by angle-dependent Ellipsometers (M-2000UI) in frequency range from 5,882 to 40,816 cm-1. The dielectric functions of all layers showed same behavior. The plasma frequency, (p), defined by 1(p) = 0 were ( 7776 cm-1 ), ( 7501 cm-1 ), and ( 7639 cm-1 ) at 218-nm, 107-nm and 41-nm-thick layers, respectively. These p values are dependent on electron density (ne) on the 66 (a) t = 218nm -12 -126 6 4000 are the permittivity of free space and the high-frequency represents the screened plasma frequency. The energy-loss 00 10000 20000 30000 40000 100 1 (0) =7502cm-1 33 50 50 -12 -12 6 64000 6000 00 100006 6 8000 = 41nm (c) t 10000 20000 0 100 30000 0 10000 20000 30000 40000 40000 100 00 1 (0) =7639cm-1 33 1 -6-6 50 50 00 10000 -12 -12 4000 10 1 Energy loss 0 2 -6 -6 0 function of Au is comparably small in NIR frequencies. 00 6 100006 8000 100 NIR frequencies. As shown in Fig. S2(d), ZnO:Ga has its maximum energy-loss position in NIR and this peak (b) t = 107nm 50 2 functions (-Im -1) of Au and ZnO:Ga are also compared in 6000 1 dielectric constant, respectively. Furthermore, the energy-loss 2 1 (0) =7776cm-1 3 -6 -6 bulk dielectric function and is the effective mass. 0 and ∞ 100 00 1 basis of the Drude model; p ne / 0 , where () is the 2 66 6000 0 -1 100.1 (d)10000 8000 20000 30000 0 40000 ZnO: Ga -2 100.01 Au -3 10 0.001 4000 4 6 Wave number 8000 8 10 (103 cm-1) Figure S2. Complex dielectric functions ( = 1+i2) of ZnO: Ga layers having different layer thicknesses: (a) 218 nm, (b) 107 nm, and (c) 41 nm. Black and red lines indicate 1 and 2, respectively. (d) Comparison of energy loss function (-Im ) of Au and Ga doped ZnO in NIR, red and black lines represent ZnO:Ga and Au respectively . 3) SPR spectra and Dispersion relation Figures S3 (a, c) show angle- and frequency-dependent SPR reflectivity spectra at room temperature for 180-nm, 162-nm, and 141-nm-thick layers as a function of the incident angle () from 45o (black line) to 75o (pink line) in 5o increments, respectively. A frequency position of SPR reflectivity shifted to higher frequencies with increasing ., as expected SPR behavior. 10000 20000 30000 40000 These results were similar to the SPR reflectivity of 218 nm-thick layers [Fig. 1(a) in the text], relating to a symmetric SP mode (s-mode) excited on the air-ZnO interface. Figure S3 (d) shows the dispersion relation (-kx curve) of the 180-nm, 162-nm and 141-nm-thick layers, as obtained from the SPR reflectivity in Figs. S3 (a, c). These results support a cutoff thickness of the s-mode (135 nm). ZnO:Ga 180nm Rp/Rs ratio 1 (b) t = 162nm 0.5 0 1 1 (a) t = 180 nm (c) t = 141nm 0.5 0.5 = 45o = 75o 4 6 kx (104 cm-1) 8 0 4000 4 kx 6000 6 (104 cm-1) 0 8000 4 8 4000 6000 6 kx (104 cm-1) 8000 8 Frequency (103 cm-1) 7000 7 6 6000 5 5000 4 4000 (d) c c/nglass ZNO_180NM2 ZNO_141NM2 ZNO_162NM2 180nm 162nm 141nm 2.5300003.5 40000 4.550000 6.5 60000 7.5 kx (104 cm-1) Figure S3. Angle- and frequency-dependent SPR reflectivity (Rp/Rs) of ZnO: Ga layers with different thicknesses (t): (a) 180 nm, (b) 162 nm, and (c) 141 nm. Incident angle () varies from 45o (black line) to 75o (pink line) in 5o increments. (d) Dispersion relation (-kx curve) of ZnO: Ga layers of different thicknesses; 180 nm (black dots), 162 nm (blue dots) and 141 nm (red dots). c and c/nglass represent light lines of air and glass, respectively. nglass is the refractive index of glass.