Coherent light-driven electron transport through polycyclic aromatic hydrocarbon: laser frequency, field intensity, and polarization angle dependence

Abstract

A laser field is a potential control tool for operating ultrafast electronic devices due to a wide variety of options such as field strength, frequency, and polarization. To investigate these variables upon electron transport through a single-molecule device, we simulate a phenyl-acetylene macrocycle (PAM) within a linear-polarized laser field using single-particle Green's functions combined with the non-Hermitian Floquet theory. In the absence of the laser field, the PAM behaves as a perfect insulator due to destructive quantum interference. In the weak-field regime, field-amplitude power laws for one-, two-, and three-photon assisted tunneling are evident in the computational results. The study reveals a range of experimentally feasible field strengths for the observation of picoampere current caused by photon assisted tunneling. In addition, we find that the light-driven current is proportional to the cosine square of the polarization angle, and molecular electronic structure is revealed by the current-frequency characteristics. The origin of these behaviors is established using non-Hermitian Floquet perturbation analysis. The computations show that PAM-based optoelectronic switches have robust large on-off switching ratios under weak-field operating conditions, which are not sensitive to asymmetric molecule-lead couplings.

Conductance and activation energy for electron transport in series and parallel intramolecular circuits

“…Electron transport through single molecules attracts general interest since a large diversity of molecules may provide novel applications for next generation electronics. [1][2][3][4] During the last two decades, molecules have been found that can act as passive components such as resistors 5,6 and active components such as transistors, [7][8][9] rectifiers, [10][11][12] and optoelectronic devices, [13][14][15][16] indicating that molecular electronics has the makings of a prototype for modern electronics. To further explore these prospects, integrating individual components together forming intramolecular circuits and logic gates is required.…”

Photoinduced Anomalous Coulomb Blockade and the Role of Triplet States in Electron Transport through an Irradiated Molecular Transistor

“…Coherent electron transport through irradiated molecular junctions has been investigated by several pioneering groups, ,− and photon-assisted tunnelling is considered a main contribution in the coherent limit. ,− Within the framework of Floquet-based methods accompanied by a tight-binding model, Tikhonov et al and Keller et al developed a scattering approach in which each Floquet state was treated as an independent transport channel. Lehmann et al derived the current formula from a reduced density matrix formalism in which the coherence between Floquet states was considered.…”

Exploring laser-driven quantum phenomena from a time-frequency analysis perspective: a comprehensive study

“…To explore the physical meaning of the shifting in Fig. 4(a)-(c), we analyze it using the Floquet method [53], which has been extensively used in chemical physics [54,55]. Details of the Floquet method can be found in Appendix B.…”