Supporting Information

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1 Supporting Information Cascade Signal Amplification Based on Copper Nanoparticle-Reported Rolling Circle Amplification for Ultrasensitive Electrochemical Detection of the Prostate Cancer Biomarker Ye Zhu a, Huijuan Wang b, Lin Wang c, Jing Zhu a, Wei Jiang a * a Key Laboratory of Colloid and Interface Chemistry of Education Ministry, School of Chemistry and Chemical Engineering, Shandong University, Jinan , China. b School of Pharmaceutical Sciences, Shandong University, Jinan , China. c Department of Radiation Oncology, Qilu Hospital, Shandong University, Jinan , China. Corresponding Author: * wjiang@sdu.edu.cn. Tel: Fax: S1

2 Table S1. Comparison of the Analytical Methods Using Poly(thymine)-templated CuNPs for Signal Generation. Templates for CuNPs Techniques target Linear range Detection limit Refs fluorescence S1 nuclease U/mL U/m L S1 Terminal deoxynucleotidyl transferase catalyzed fluorescence T4 PNK U/mL fluorescence T4 PNK U/mL 0.25 U/mL S U/mL S3 fluorescence Cu μm S4 (40 bases) fluorescence Hg nm 0.1 nm. S5 fluorescence H 2 O μm 0.55 μm. S6 (40 bases) glucose mm 0.05 mm fluorescence melamine mm 95 nm S7 fluorescence cysteine nm 12.5 nm S8 (25 bases) fluorescence N- acetylcysteine mm 50 nm S9 fluorescence streptavidin nm 0.1 nm S10 S2

3 fluorescence trypsin μm 1.75 nm S11 Terminal deoxynucleotidyl transferase catalyzed fluorescence DNA nm 98.2 pm S12 RCA product containing thousands of repeats electrochemical PSA fg/ml ( fm) fg/ml (0.59 am) This work Figure S1. TEM image of fifty-thymine sequence-templated CuNPs. S3

4 Figure S2. (A) DPSV responses of the method using aptamer-t50-templated CuNPs toward varying PSA concentrations (from a to k: 0, 0.01, 0.05, 0.1, 0.5, 1, 5, 10, 50, 100, and 500 ng/ml); (B) The corresponding calibration curve. Figure S3. (A) DPSV responses of the developed method toward spiked PSA in 10 6 times diluted serum samples (from a to m: 0, 0.005, 0.01, 0.05, 0.1, 0.5, 1, 5, 10, 50, 100, 500, and 1000 fg/ml PSA); (B) The corresponding calibration curve. REFERENCES (S1) Qing, Z.; He, X.; Qing, T.; Wang, K.; Shi, H.; He, D.; Zou, Z.; Yan, L.; Xu, F.; Ye, X.; Mao, Z. Poly(Thymine)-Templated Fluorescent Copper Nanoparticles for Ultrasensitive Label-Free Nuclease Assay and Its Inhibitors Screening. Anal. Chem. 2013, 85, S4

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6 (S11) Ou, L.-J.; Li, X.-Y.; Li, L.-J.; Liu, H.-W.; Sun, A.-M.; Liu, K.-J. A Sensitive Assay for Trypsin Using Poly(Thymine)-Templated Copper Nanoparticles as Fluorescent Probes. Analyst 2015, 140, (S12) Hu, W.; Ning, Y.; Kong, J.; Zhang, X. Formation of Copper Nanoparticles on Poly(Thymine) through Surface-Initiated Enzymatic Polymerization and Its Application for DNA Detection. Analyst 2015, 140, S6