TY - JOUR
T1 - Coherent light-driven electron transport through polycyclic aromatic hydrocarbon
T2 - Laser frequency, field intensity, and polarization angle dependence
AU - Hsu, Liang Yan
AU - Rabitz, Herschel
N1 - Publisher Copyright:
© the Owner Societies 2015.
PY - 2015/8/28
Y1 - 2015/8/28
N2 - 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.
AB - 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.
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U2 - 10.1039/c5cp02663f
DO - 10.1039/c5cp02663f
M3 - Article
C2 - 26204437
AN - SCOPUS:84938674728
SN - 1463-9076
VL - 17
SP - 20617
EP - 20629
JO - Physical Chemistry Chemical Physics
JF - Physical Chemistry Chemical Physics
IS - 32
ER -