| Nucleotide rectifying ratio with proposed sequencing protocol. a, The suggested protocol to distinguish between nucleotides by rectifying ratio (RR): interrupt a constant bias of-0.8 V with short square pulses of +0.8 V and during this alternating square pulse period ("PP") measure the rectifying ratio. The rectifying ratio is defined as the absolute value of the ratio of currents for negative and positive bias. b, Calculated RR for different nucleotides (dGMP-diamonds, dAMP-circles, dCMP-squares and dTMP-triangles) as a function of absolute value of applied bias. c, Transmission of dGMP as a function of energy at +0.2 V for two different molecule-electrode tilt angles. 

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... protocol is performed by interrupting the constant bias with short square pulses of +0.8 V to obtain an optimal RR, as depicted in Fig. 2a. The calculated rectifying ratio from the pulse period (PP) for all four nucleotides as a function of the absolute value of the constant bias is shown in Fig. 2b. It is evident that the nucleotides exhibit different rectification behaviours, which makes them distinct for sequencing. The most extreme differences in RR between the ...

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... protocol is performed by interrupting the constant bias with short square pulses of +0.8 V to obtain an optimal RR, as depicted in Fig. 2a. The calculated rectifying ratio from the pulse period (PP) for all four nucleotides as a function of the absolute value of the constant bias is shown in Fig. 2b. It is evident that the nucleotides exhibit different rectification behaviours, which makes them distinct for sequencing. The most extreme differences in RR between the different nucleotides are at a bias of 0.8 V, making that the optimal working point for the sequencing protocol. At this bias, RR is 1,000, 50, 1 and 0.3 for dAMP, ...

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... this bias, RR is 1,000, 50, 1 and 0.3 for dAMP, dGMP, dTMP and dCMP, respectively. While the transverse current amplitude is highly sensitive to mutual molecule-electrode orientation 15 (see Figure 2c), rectification strongly depends on nucleotide HOMO position with respect to E F and is less sensitive to orientation. Calculations for dGMP oriented at an angle of 30̊ with respect to the Y axis (tilted in the plane which contains the nucleotide base) at ±0.2 V bias show that while transmission is diminished (I rot0 /I rot30 =100) due to tilting, the position of HOMO with respect to E F remains the same (see Fig. 2b) implicating that RR will change only slightly. ...

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... respect to E F and is less sensitive to orientation. Calculations for dGMP oriented at an angle of 30̊ with respect to the Y axis (tilted in the plane which contains the nucleotide base) at ±0.2 V bias show that while transmission is diminished (I rot0 /I rot30 =100) due to tilting, the position of HOMO with respect to E F remains the same (see Fig. 2b) implicating that RR will change only slightly. Our results suggest that the rectifying ratio is robust to the effect of orientation (RR rot30 =6RR rot0 ) and we propose measuring RR of single-stranded ssDNA in a high- throughput sequencing tool. suggested protocol to distinguish between nucleotides by rectifying ratio (RR): interrupt ...

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... we discussed above, asymmetry in transport with respect to the sign of bias that enables rectification is pronounced, especially for dGMP (RR=10), even for bias as small as 50 mV (see Fig. 2b). As will be shown in the following, this significant asymmetry in transport is the consequence of strong pinning of molecular HOMO levels to the electrochemical potential of one of the electrodes, which can lead to HOMO either contributing to the current or not. This can result in significant ...

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... of nucleotide rotation (dGMP is given as an example) on transmission is shown in Figure S2. When dGMP is rotated by 30̊ peak transmission diminishes by nearly two orders of magnitude which directly reflects on the current. ...

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... the position of HOMO with respect to the Fermi energy remains the same, implying that the rectifying ratio will also be insensitive to molecular rotation. Figure S2.Electronic transmission of dGMP rotated by 30̊ around the Y axis (axis perpendicular to the plane that contains the nucleotide base, see inset).Top panel: transmission on logarithmic scale for dGMP (solid black line) and dGMProtated by30⁰ (dotted black line) at +0.2V. Bottom panel: transmission on logarithmic scale for dGMP (solid black line) and dGMProtated by30⁰ (dotted black line) at -0.2V. ...

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... we discussed above, asymmetry in transport with respect to the sign of bias that enables rectification is pronounced, especially for dGMP (RR=10), even for bias as small as 50 mV (see Fig. 2b). As will be shown in the following, this significant asymmetry in transport is the consequence of strong pinning of molecular HOMO levels to the electrochemical potential of one of the electrodes, which can lead to HOMO either contributing to the current or not. This can result in significant ...

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... of nucleotide rotation (dGMP is given as an example) on transmission is shown in Figure S2. When dGMP is rotated by 30̊ peak transmission diminishes by nearly two orders of magnitude which directly reflects on the current. However the position of HOMO with respect to the Fermi energy remains the same, implying that the rectifying ratio will also be insensitive to molecular rotation. Figure S2. Electronic transmission of dGMP rotated by 30̊ around the Y axis (axis perpendicular to the plane that contains the nucleotide base, see inset). Top panel: transmission on logarithmic scale for dGMP (solid black line) and dGMP rotated by 30⁰ (dotted black line) at +0.2V. Bottom panel: transmission on logarithmic scale for dGMP (solid black line) and dGMP rotated by 30⁰ (dotted black line) at ...

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... of nucleotide rotation (dGMP is given as an example) on transmission is shown in Figure S2. When dGMP is rotated by 30̊ peak transmission diminishes by nearly two orders of magnitude which directly reflects on the current. However the position of HOMO with respect to the Fermi energy remains the same, implying that the rectifying ratio will also be insensitive to molecular rotation. Figure S2. Electronic transmission of dGMP rotated by 30̊ around the Y axis (axis perpendicular to the plane that contains the nucleotide base, see inset). Top panel: transmission on logarithmic scale for dGMP (solid black line) and dGMP rotated by 30⁰ (dotted black line) at +0.2V. Bottom panel: transmission on logarithmic scale for dGMP (solid black line) and dGMP rotated by 30⁰ (dotted black line) at ...

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... our proposed sequencing protocol, constant negative bias is applied to the electrodes to keep the phosphosugar group facing the left electrode, as depicted in the right panel of Fig. 1. The protocol is performed by interrupting the constant bias with short square pulses of +0.8 V to obtain an optimal RR, as depicted in Fig. 2a. The calculated rectifying ratio from the pulse period (PP) for all four nucleotides as a function of the absolute value of the constant bias is shown in Fig. 2b. It is evident that the nucleotides exhibit different rectification behaviours, which makes them distinct for sequencing. The most extreme differences in RR between the different nucleotides are at a bias of 0.8 V, making that the optimal working point for the sequencing protocol. At this bias, RR is 1000, 50, 1 and 0.3 for dAMP, dGMP, dTMP and dCMP, respectively. While the transverse current amplitude is highly sensitive to mutual molecule- electrode orientation 15 (see Figure 2c), rectification strongly depends on nucleotide HOMO position with respect to E F and is less sensitive to orientation. Calculations for dGMP oriented at an angle of 30̊ with respect to the Y axis (tilted in the plane which contains the nucleotide base) at ±0.2 V bias show that while transmission is diminished (I rot0 /I rot30 =100) due to tilting, the position of HOMO with respect to E F remains the same (see Fig. 2b) implicating that RR will change only slightly. Our results suggest that the rectifying ratio is robust to the effect of orientation (RR rot30 =6RR rot0 ) and we propose measuring RR of single-stranded ssDNA in a high- throughput sequencing tool. ...

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... our proposed sequencing protocol, constant negative bias is applied to the electrodes to keep the phosphosugar group facing the left electrode, as depicted in the right panel of Fig. 1. The protocol is performed by interrupting the constant bias with short square pulses of +0.8 V to obtain an optimal RR, as depicted in Fig. 2a. The calculated rectifying ratio from the pulse period (PP) for all four nucleotides as a function of the absolute value of the constant bias is shown in Fig. 2b. It is evident that the nucleotides exhibit different rectification behaviours, which makes them distinct for sequencing. The most extreme differences in RR between the different nucleotides are at a bias of 0.8 V, making that the optimal working point for the sequencing protocol. At this bias, RR is 1000, 50, 1 and 0.3 for dAMP, dGMP, dTMP and dCMP, respectively. While the transverse current amplitude is highly sensitive to mutual molecule- electrode orientation 15 (see Figure 2c), rectification strongly depends on nucleotide HOMO position with respect to E F and is less sensitive to orientation. Calculations for dGMP oriented at an angle of 30̊ with respect to the Y axis (tilted in the plane which contains the nucleotide base) at ±0.2 V bias show that while transmission is diminished (I rot0 /I rot30 =100) due to tilting, the position of HOMO with respect to E F remains the same (see Fig. 2b) implicating that RR will change only slightly. Our results suggest that the rectifying ratio is robust to the effect of orientation (RR rot30 =6RR rot0 ) and we propose measuring RR of single-stranded ssDNA in a high- throughput sequencing tool. ...

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... our proposed sequencing protocol, constant negative bias is applied to the electrodes to keep the phosphosugar group facing the left electrode, as depicted in the right panel of Fig. 1. The protocol is performed by interrupting the constant bias with short square pulses of +0.8 V to obtain an optimal RR, as depicted in Fig. 2a. The calculated rectifying ratio from the pulse period (PP) for all four nucleotides as a function of the absolute value of the constant bias is shown in Fig. 2b. It is evident that the nucleotides exhibit different rectification behaviours, which makes them distinct for sequencing. The most extreme differences in RR between the different nucleotides are at a bias of 0.8 V, making that the optimal working point for the sequencing protocol. At this bias, RR is 1000, 50, 1 and 0.3 for dAMP, dGMP, dTMP and dCMP, respectively. While the transverse current amplitude is highly sensitive to mutual molecule- electrode orientation 15 (see Figure 2c), rectification strongly depends on nucleotide HOMO position with respect to E F and is less sensitive to orientation. Calculations for dGMP oriented at an angle of 30̊ with respect to the Y axis (tilted in the plane which contains the nucleotide base) at ±0.2 V bias show that while transmission is diminished (I rot0 /I rot30 =100) due to tilting, the position of HOMO with respect to E F remains the same (see Fig. 2b) implicating that RR will change only slightly. Our results suggest that the rectifying ratio is robust to the effect of orientation (RR rot30 =6RR rot0 ) and we propose measuring RR of single-stranded ssDNA in a high- throughput sequencing tool. ...

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... our proposed sequencing protocol, constant negative bias is applied to the electrodes to keep the phosphosugar group facing the left electrode, as depicted in the right panel of Fig. 1. The protocol is performed by interrupting the constant bias with short square pulses of +0.8 V to obtain an optimal RR, as depicted in Fig. 2a. The calculated rectifying ratio from the pulse period (PP) for all four nucleotides as a function of the absolute value of the constant bias is shown in Fig. 2b. It is evident that the nucleotides exhibit different rectification behaviours, which makes them distinct for sequencing. The most extreme differences in RR between the different nucleotides are at a bias of 0.8 V, making that the optimal working point for the sequencing protocol. At this bias, RR is 1000, 50, 1 and 0.3 for dAMP, dGMP, dTMP and dCMP, respectively. While the transverse current amplitude is highly sensitive to mutual molecule- electrode orientation 15 (see Figure 2c), rectification strongly depends on nucleotide HOMO position with respect to E F and is less sensitive to orientation. Calculations for dGMP oriented at an angle of 30̊ with respect to the Y axis (tilted in the plane which contains the nucleotide base) at ±0.2 V bias show that while transmission is diminished (I rot0 /I rot30 =100) due to tilting, the position of HOMO with respect to E F remains the same (see Fig. 2b) implicating that RR will change only slightly. Our results suggest that the rectifying ratio is robust to the effect of orientation (RR rot30 =6RR rot0 ) and we propose measuring RR of single-stranded ssDNA in a high- throughput sequencing tool. ...