Abstract:We consider a biased molecular junction subjected to external time-dependent electromagnetic field. We discuss local field formation due to both surface plasmon-polariton excitations in the contacts and the molecular response. Employing realistic parameters we demonstrate that such self-consistent treatment is crucial for proper description of the junction transport characteristics.
“…At close proximity the possibility of electron tunneling between metal structures can considerably change the physics of the system and should be taken into account. [21,22,218] Similarly, electron transfer can strongly affect metal-molecule interaction at short distances and overshadows the effect of exciton-plasmon coupling. Indeed, plasmon-induced hot electron chemistry -processes in which following plasmon excitation electrons are exchanged between the metal ix When the molecule sits directly on the metal surface energy and electron transfer to the metal provide other efficient relaxation routes with relaxation times possibly of similar order.…”
This review provides a brief introduction to the physics of coupled exciton-plasmon systems, the theoretical description and experimental manifestation of such phenomena, followed by an account of the state-of-the-art methodology for the numerical simulations of such phenomena and supplemented by a number of FORTRAN codes, by which the interested reader can introduce himself/herself to the practice of such simulations. Applications to CW light scattering as well as transient response and relaxation are described. Particular attention is given to so-called strong coupling limit, where the hybrid exciton-plasmon nature of the system response is strongly expressed. While traditional descriptions of such phenomena usually rely on analysis of the electromagnetic response of inhomogeneous dielectric environments that individually support plasmon and exciton excitations, here we explore also the consequences of a more detailed description of the molecular environment in terms of its quantum density matrix (applied in a mean field approximation level). Such a description makes it possible to account for characteristics that cannot be described by the dielectric response model: the effects of dephasing on the molecular response on one hand, and nonlinear response on the other. It also highlights the still missing important ingredients in the numerical approach, in particular its limitation to a classical description of the radiation field and its reliance on a mean field description of the many-body molecular system. We end our review with an outlook to the near future, where these limitations will be addressed and new novel applications of the numerical approach will be pursued.
“…At close proximity the possibility of electron tunneling between metal structures can considerably change the physics of the system and should be taken into account. [21,22,218] Similarly, electron transfer can strongly affect metal-molecule interaction at short distances and overshadows the effect of exciton-plasmon coupling. Indeed, plasmon-induced hot electron chemistry -processes in which following plasmon excitation electrons are exchanged between the metal ix When the molecule sits directly on the metal surface energy and electron transfer to the metal provide other efficient relaxation routes with relaxation times possibly of similar order.…”
This review provides a brief introduction to the physics of coupled exciton-plasmon systems, the theoretical description and experimental manifestation of such phenomena, followed by an account of the state-of-the-art methodology for the numerical simulations of such phenomena and supplemented by a number of FORTRAN codes, by which the interested reader can introduce himself/herself to the practice of such simulations. Applications to CW light scattering as well as transient response and relaxation are described. Particular attention is given to so-called strong coupling limit, where the hybrid exciton-plasmon nature of the system response is strongly expressed. While traditional descriptions of such phenomena usually rely on analysis of the electromagnetic response of inhomogeneous dielectric environments that individually support plasmon and exciton excitations, here we explore also the consequences of a more detailed description of the molecular environment in terms of its quantum density matrix (applied in a mean field approximation level). Such a description makes it possible to account for characteristics that cannot be described by the dielectric response model: the effects of dephasing on the molecular response on one hand, and nonlinear response on the other. It also highlights the still missing important ingredients in the numerical approach, in particular its limitation to a classical description of the radiation field and its reliance on a mean field description of the many-body molecular system. We end our review with an outlook to the near future, where these limitations will be addressed and new novel applications of the numerical approach will be pursued.
“…[http://dx.doi.org/10.1063/1.4804544] Molecular plasmonics (a.k.a. nanopolaritonics), [1][2][3][4] a new field investigating the interaction between molecules and surface plasmons, requires modeling of a large number of electrons coupled to an electromagnetic field. Time dependent density functional theory (TDDFT) has been widely used to study quantum effects in plasmonics [5][6][7] that are missing in conventional classical electrodynamics models.…”
A discrete interaction model/quantum mechanical method for simulating surface-enhanced Raman spectroscopy The Journal of Chemical Physics 136, 214103 (2012); https://doi.org/10.1063/1.4722755 A discrete interaction model/quantum mechanical method to describe the interaction of metal nanoparticles and molecular absorption
In this work we consider a current carrying two level quantum dot(QD) that is
coupled to a single mode phonon bath. Using self-consistent Hartree-Fock
approximation, we obtain the I-V curve of QD. By considering the linear
response of our system to an incoming classical light, we see that depending on
the parametric regime, the system could have weak or strong light absorption or
may even show lasing. This lasing occurs at high enough bias voltages and is
explained by a population inversion considering side bands, while the total
electron population in the higher level is less than the lower one. The
frequency at which we have the most significant lasing depends on the level
spacing and phonon frequency and not on the electron-phonon coupling strength
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