Distance-Dependent Plasmon-Enhanced Fluorescence of Upconversion Nanoparticles using Polyelectrolyte Multilayers as Tunable Spacers Ai Ling Feng a,b , Min Li You a,b , Limei Tian c, Srikanth Singamaneni c, Ming Liu d, Zhenfeng Duan e, Tian Jian Lu b, Feng Xu a,b, Min Lin a,b,e # a The Key Laboratory of Biomedical Information Engineering, Ministry of Education, School of Life Science and Technology, Xi'an Jiaotong University, Xi’an 710049, P.R. China b Bioinspired Engineering and Biomechanics Center (BEBC), Xi’an Jiaotong University, Xi’an 710049, P.R. China c Department of Mechanical Engineering and Materials Science, Institute of Materials Science and Engineering, Washington University in St. Louis, St Louis, MO 63130, USA d Electronic Materials Research Laboratory, Key Laboratory of the Ministry of Education & International Center for Dielectric Research, Xi'an Jiaotong University, Xi'an 710049, P.R. China e Center for Sarcoma and Connective Tissue Oncology, Massachusetts General Hospital, Harvard Medical School, MA 02114, USA # Corresponding author: minlin@mail.xjtu.edu.cn Figure S1 nanoparticles. Size distribution histogram of as-prepared upconversion Figure S2 Representative TEM image of UCNPs-PAA. There were no obvious change in morphology and size as compared with as-prepared UCNPs in Figure 2. Figure S3 Energy level diagram illustrating the luminescence mechanism of NaYF4:Yb,Er upconversion nanoparticles with the excitation of NIR laser. Figure S4 Size distribution histogram (length, diameter and aspect ratio) of different AuNRs. (a-c) AuNRs-980; (d-f) AuNRs-915; (g-i) AuNRs-735. Figure S5 UV-Vis-NIR extinction spectrum of AuNRs-980, AuNRs-915 and AuNRs-735 in solution. Figure S6 Simulated results of electric fields surrounding the surface of two AuNRs at the polymer surface with different relative positions. Electric fields distribution with side-by-side of two AuNRs with aspect ratios of: (a) 7.6 (AuNRs-980); (c) 6.3 (AuNRs-915); (e) 4.5 (AuNRs-735) and head-to-head of two AuNRs with aspect ratios of: (b) 7.6 (AuNRs-980); (d) 6.3 (AuNRs-915); (f) 4.5 (AuNRs-735) are shown. Figure S7 Simulated results of electric fields surrounding the surface of individual AuNRs at the polymer surface. The graph from AuNRs with different aspect ratios of: (a) 7.6 (AuNRs-980); (b) 6.3 (AuNRs-915); (c) 4.5 (AuNRs-735) are shown. Figure S8 Correlation of different aspect ratios of the AuNRs to the electric field intensity. Table S1 LSPR wavelength of AuNRs with different aspect ratios. LSPR Wavelength LSPR Wavelength Nomenclature Blue-shift (nm) in Solution (nm) on Silicon (nm) AuNRs-980 1075 980 95 AuNRs-915 1010 915 95 AuNRs-735 830 735 95 Table S2 Statistical analysis of size distribution for AuNRs with different aspect ratios. AuNRs-980 Parameters AuNRs-915 AuNRs-735 Length Diameter Aspect Length Diameter Aspect Length Diameter Aspect (nm) (nm) Ratio (nm) (nm) Ratio (nm) (nm) Ratio Mean 105.5 14.1 7.6 86.6 14.0 6.3 64.4 14.7 4.5 Max 196.0 22.5 15.5 124.5 17.9 9.0 85.7 19.8 7.3 Min 62.7 10.3 2.9 64.9 9.0 3.9 40.9 10.2 2.7 SD 20.2 1.7 1.9 10.7 1.5 1.0 7.3 1.8 0.8