We report a novel strategy to control and construct sequential assembly of DNA functionalized gold nanoparticles(AuNPs)from a single solution.We systematically investigated the temperature-dependent kinetics of DNA-li...We report a novel strategy to control and construct sequential assembly of DNA functionalized gold nanoparticles(AuNPs)from a single solution.We systematically investigated the temperature-dependent kinetics of DNA-linked AuNP assembly.A sharp kinetic transition in the assembly process,strongly dependent on temperature,was identified.As the temperature increased,the assembly rate rose continuously until it reached a critical kinetic temperature(T_(crit)).Beyond this point,the assembly rate sharply decreased to near zero within a narrow temperature window of 2–3℃.This sharp kinetic transition is advantageous for designing highly specific detection systems.We leveraged the transition to control the assembly of AuNPs functionalized with DNA strands that differ by single-base mismatches.Using AuNPs of different sizes,we demonstrated the sequential assembly of AuNPs functionalized with perfectly matched DNA strands,followed by assembly of AuNPs with DNA containing a single-base mismatch,and finally assembly of AuNPs with DNA containing two-base mismatches.We also first assembled AuNPs functionalized with DNA containing two-base mismatches at a lower temperature,followed by assembling AuNPs with DNA containing a single-base mismatch at a higher temperature.Both approaches of controlled sequential assembly are useful for bottom-up assembly applications to form desirable nanostructures.展开更多
基金supported by the Canadian Institutes for Health Research,the Natural Sciences and Engineering Research Council of Canada,and the Canada Research Chairs program.
文摘We report a novel strategy to control and construct sequential assembly of DNA functionalized gold nanoparticles(AuNPs)from a single solution.We systematically investigated the temperature-dependent kinetics of DNA-linked AuNP assembly.A sharp kinetic transition in the assembly process,strongly dependent on temperature,was identified.As the temperature increased,the assembly rate rose continuously until it reached a critical kinetic temperature(T_(crit)).Beyond this point,the assembly rate sharply decreased to near zero within a narrow temperature window of 2–3℃.This sharp kinetic transition is advantageous for designing highly specific detection systems.We leveraged the transition to control the assembly of AuNPs functionalized with DNA strands that differ by single-base mismatches.Using AuNPs of different sizes,we demonstrated the sequential assembly of AuNPs functionalized with perfectly matched DNA strands,followed by assembly of AuNPs with DNA containing a single-base mismatch,and finally assembly of AuNPs with DNA containing two-base mismatches.We also first assembled AuNPs functionalized with DNA containing two-base mismatches at a lower temperature,followed by assembling AuNPs with DNA containing a single-base mismatch at a higher temperature.Both approaches of controlled sequential assembly are useful for bottom-up assembly applications to form desirable nanostructures.