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arXiv 0906.4640cond-mat.mes-hallcond-mat.mtrl-sci
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脉冲偏压控制的分子开关

Molecular switch controlled by pulsed bias voltages

Velimir Meded, Alexei Bagrets, Andreas Arnold, Ferdinand Evers

摘要:

在最近的实验中观察到,BPDN-DT(联吡啶-二硝基-低聚亚苯基-亚乙炔基-二硫醇)的电流-电压特性(IV)可以通过在偏置电压V_bias中施加脉冲以非常受控的方式在“开”和“关”迹线之间切换。我们计算了极化子的形成能,以检验一个经常持有的信念,即极化子的形成可以解释所观察到的双稳态。我们的结果与这种机制不一致。相反,我们提出了一个构象重定向。该分子携带与V_bias耦合的固有偶极矩。斜变V_bias在偶极上施加力,该力可以将分子从基态(“关”)重新定向(“旋转”)到亚稳态构型(“开”)并返回。通过详细的电子结构计算,我们确定了一个特定的路径,通过分子的构象相空间的旋转。我们表明,这条路径具有足够高的障碍,以抑制热不稳定性,但仍然可以切换的结稳定的电压范围内的分子。理论IV定性地再现了关键的实验观察。我们提出,如何电导切换的替代机制可以实验验证。

英文摘要:

It was observed in recent experiments that the current-voltage characteristics (IV) of BPDN-DT (bipyridyl- dinitro- oligophenylene- ethynylene- dithiol) can be switched in a very controlled manner between "on" and "off" traces by applying a pulse in a bias voltage, V_bias. We have calculated the polaron formation energies to check a frequently held belief, namely, that the polaron formation can explain the observed bistability. Our results are not consistent with such a mechanism. Instead, we propose a conformational reorientation. The molecule carries an intrinsic dipole moment which couples to V_bias. Ramping V_bias exerts a force on the dipole that can reorient ("rotate") the molecule from the ground state ("off") into a metastable configuration ("on") and back. By elaborated electronic structure calculations, we identify a specific path for this rotation through the molecule's conformational phase space. We show that this path has sufficiently high barriers to inhibit thermal instability but still the molecule can be switched in the voltage range of the junction stability. The theoretical IVs reproduce qualitatively the key experimental observations. We propose, how the alternative mechanism of conductance switching can be experimentally verified.

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