Aiming at the issues of controlling the translocation speed of DNA through a solid-state nanopore and enlarging the signal-to-noise ratio of ionic current modulation, which are challenges for the application of nanopo...Aiming at the issues of controlling the translocation speed of DNA through a solid-state nanopore and enlarging the signal-to-noise ratio of ionic current modulation, which are challenges for the application of nanopore technology in DNA detection, salt concentration gradients are applied across the nanopore to investigate their influence on the DNA translocation time and signal-to-noise ratio. Experimental data demonstrates that, in symmetric concentration conditions, both the current blockade and dwell time for A-DNA translocation through a solid-state nanopore increase along with potassium chloride concentration. When the concentration in the trans chamber is decreased from 1 to 0.1 mol/L, keeping the concentration of the cis chamber at 1 mol/L, the normalized current blockade is found to be increased by one order. The increased dwell time and enhanced signal-to-noise ratio are achieved with salt gradients across the nanopore, which can improve the sensitivity when detecting DNA samples.展开更多
DNA and its conformational transition can be used to design nanometer-scale structures, nano-tweezers and nanomechanical devices. Experiments and molecular simulations have been used to study the concentration effect ...DNA and its conformational transition can be used to design nanometer-scale structures, nano-tweezers and nanomechanical devices. Experiments and molecular simulations have been used to study the concentration effect on the A-DNA→B-DNA conformational transition, but a systematical investigation on counterion effect on the dynamics of this transition has not been reported up to now. In present work, restrained and unrestrained molecular dynamics （MD） simulations have been performed to characterize the stability of DNA conformations and the dynamics of A-DNA→B-DNA transitions in aqueous solutions with different alkali metal counterions. The DNA duplex d（CGCGAATTCGCG）2, coion Cl- and counterions Li＋, Na＋, K＋, Rb＋ and Cs~ as well as water molecule were considered using the PARM99 force field in the AMBER8 package. It was found that B-form DNA is more stable than A-form DNA in aqueous electrolyte solutions with different alkali metal counterions. In- creasing KCI concentration in solution hinders the A-DNA^B-DNA transition and the transition times for different alkali metal counterions conform to neither the simple sequence related to naked ion size nor to hydrated diameter, but an apparently abnormal sequence of K＋ 〈 Rb＋ 〈 Cs＋ 〈 Na＋ 〈 Li＋. This abnormal sequence can be well understood in terms of an electrostatic model based on the effective cation diameters and the modified mean-spherical approximation （MMSA）. The present results provide valuable information for the design of DNA-based nanomaterials and nanodevices.展开更多
基金The National Natural Science Foundation of China(No.51435003,51375092)Fundamental Research Funds for the Central Universities+1 种基金the Innovative Project for Graduate Students of Jiangsu Province(No.KYLX_0100)the Scientific Research Foundation of Graduate School of Southeast University(No.YBJJ1540)
文摘Aiming at the issues of controlling the translocation speed of DNA through a solid-state nanopore and enlarging the signal-to-noise ratio of ionic current modulation, which are challenges for the application of nanopore technology in DNA detection, salt concentration gradients are applied across the nanopore to investigate their influence on the DNA translocation time and signal-to-noise ratio. Experimental data demonstrates that, in symmetric concentration conditions, both the current blockade and dwell time for A-DNA translocation through a solid-state nanopore increase along with potassium chloride concentration. When the concentration in the trans chamber is decreased from 1 to 0.1 mol/L, keeping the concentration of the cis chamber at 1 mol/L, the normalized current blockade is found to be increased by one order. The increased dwell time and enhanced signal-to-noise ratio are achieved with salt gradients across the nanopore, which can improve the sensitivity when detecting DNA samples.
基金supported by the National Natural Science Foundation of China(21176132 and 20876083)Specialized Research Fund for the Doctoral Program of Higher Education(20100002110024)
文摘DNA and its conformational transition can be used to design nanometer-scale structures, nano-tweezers and nanomechanical devices. Experiments and molecular simulations have been used to study the concentration effect on the A-DNA→B-DNA conformational transition, but a systematical investigation on counterion effect on the dynamics of this transition has not been reported up to now. In present work, restrained and unrestrained molecular dynamics （MD） simulations have been performed to characterize the stability of DNA conformations and the dynamics of A-DNA→B-DNA transitions in aqueous solutions with different alkali metal counterions. The DNA duplex d（CGCGAATTCGCG）2, coion Cl- and counterions Li＋, Na＋, K＋, Rb＋ and Cs~ as well as water molecule were considered using the PARM99 force field in the AMBER8 package. It was found that B-form DNA is more stable than A-form DNA in aqueous electrolyte solutions with different alkali metal counterions. In- creasing KCI concentration in solution hinders the A-DNA^B-DNA transition and the transition times for different alkali metal counterions conform to neither the simple sequence related to naked ion size nor to hydrated diameter, but an apparently abnormal sequence of K＋ 〈 Rb＋ 〈 Cs＋ 〈 Na＋ 〈 Li＋. This abnormal sequence can be well understood in terms of an electrostatic model based on the effective cation diameters and the modified mean-spherical approximation （MMSA）. The present results provide valuable information for the design of DNA-based nanomaterials and nanodevices.
