ABSTRACT
Scanning tunneling microscope (STM)-induced luminescence provides an ideal platform for electrical generation and the atomic-scale manipulation of nonclassical states of light. However, despite its extreme importance in quantum technologies, squeezed light emission with reduced quantum fluctuations has hitherto not been demonstrated in such a platform. Here, we theoretically predict that the emitted light from the plasmon mode can be squeezed in an STM single molecular junction subject to an external laser drive. Going beyond the traditional paradigm that generates squeezing with the quadratic interaction of photons, our prediction explores the molecular coherence involved in an anharmonic energy spectrum of a coupled plasmon-molecule-exciton system. Furthermore, we show that, by selectively exciting the energy ladder, the squeezed plasmon can show either sub- or super-Poissonian statistical properties. We also demonstrate that, following the same principle, the molecular excitonic mode can be squeezed simultaneously.
ABSTRACT
The photon blockade induced by optical nonlinearity has been widely used to generate single-photon emission under optical driving in quantum optics. However, the same approach is difficult to achieve in electrically driven molecular junctions. Here we propose a scheme for tuning photon statistics via Fano-like interference effect in a system consisting of two molecules within one optical cavity. Under electrical pumping, a transition from photon bunching to antibunching takes place as a manifestation of the Fano-like interference. This effect persists even in the presence of the dipole-dipole interaction between molecules based on the parameters extracted from the experiments. Our proposal can be realized in current-carrying scanning tunneling microscope junctions.
ABSTRACT
We study vibrational statistics in current-carrying model molecular junctions using a master equation approach. In particular, we concentrate on the validity of using an effective temperature T_{eff} to characterize the nonequilibrium steady state of a vibrational mode. We identify cases in which a single T_{eff} cannot fully describe one vibrational state. In such cases, the probability distribution among different vibrational states does not follow the Boltzmann type. Consequently, the actual entropy (free energy) of the vibrational mode is lower (higher) than the corresponding thermal value given by T_{eff}, indicating extra work can be extracted from these states. Our results will be useful for the study of a nonthermal vibrational state in the thermodynamics of nanoscale systems, and its usage in nanoscale heat engines.
ABSTRACT
The coupling between molecular exciton and gap plasmons plays a key role in single molecular electroluminescence induced by a scanning tunneling microscope (STM). But it has been difficult to clarify the complex experimental phenomena. By employing the nonequilibrium Green's function method, we propose a general theoretical model to understand the light emission spectrum of single molecule and gap plasmons from an energy transport point of view. The coherent interaction between gap plasmons and molecular exciton leads to a prominent Fano resonance in the emission spectrum. We analyze the dependence of the Fano line shape on the system parameters, based on which we provide a unified account of several recent experimental observations. Moreover, we highlight the effect of the tip-molecule electronic coupling on the spectrum.