arXiv subjects

Maxim Sukharev

Publications and source records attributed to Maxim Sukharev.

At least 55 records · Page 3Linked to original sources

arXiv2017

Molecular Plasmonics: strong coupling at the low molecular density limit

We study the strong coupling between the molecular excited state and the plasmonic modes of silver hole arrays with a resonant frequency very close to the asymptotic line of the plasmonic dispersion relation, at the nonlinear regime. We demonstrate that the strong coupling regime can be achieved between the two sub-systems at low molecular densities with negligible damping of the electromagnetic field. Our results are supported by rigorous numerical simulations showing that the strong coupling is observed when the molecular transition lies within the nonlinear regime of the dispersion relation rather than the linear regime.

cond-mat.mes-hall↗

arXiv2016

Molecular plasmonics: the role of ro-vibrational molecular states in exciton-plasmon materials under strong coupling conditions

We extend the model of exciton-plasmon materials to include a ro-vibrational structure of molecules using wave-packet propagations on electronic potential energy surfaces. The new model replaces conventional two-level emitters with more complex molecules allowing to examine the influence of alignment and vibrational dynamics on strong coupling with surface plasmon-polaritons. We apply the model to a hybrid system comprising a thin layer of molecules placed on top of a periodic array of slits. Rigorous simulations are performed for two types of molecular systems described by vibrational bound-bound and bound-continuum electronic transitions. Calculations reveal new features in transmission, reflection and absorption spectra including the observation of significantly higher values of the Rabi splitting and vibrational patterns clearly seen in the corresponding spectra. We also examine the influence of anisotropic initial conditions on optical properties of hybrid materials demonstrating that the optical response of the system is significantly affected by an initial pre-alignment of the molecules. Our work demonstrates that pre-aligned molecules could serve as an efficient probe for the sub-diffraction characterization of the near-field near metal interfaces.

cond-mat.mes-hall↗

arXiv2016

Plasmonic opals: observation of a collective molecular exciton mode beyond the strong coupling

Achieving and controlling strong light-matter interactions in many-body systems is of paramount importance both for fundamental understanding and potential applications. In this paper we demonstrate both experimentally and theoretically how to manipulate strong coupling between the Bragg-plasmon mode supported by a organo-metallic array and molecular excitons in the form of J-aggregates dispersed on the hybrid structure. We observe experimentally the transition from a conventional strong coupling regime exhibiting the usual upper and lower polaritonic branches to a more complex regime, where a third nondispersive mode is seen, as the concentration of J-aggregates is increased. The numerical simulations confirm the presence of the third resonance. We attribute its physical nature to collective molecule-molecule interactions leading to the collective electromagnetic response. A simple analytical model is proposed to explain the physics of the third mode. The nonlinear dependence on molecular parameters followed from the model are confirmed in a set of rigorous numerical studies. It is shown that at the energy of the collective mode molecules oscillate completely out of phase with the incident radiation acting as an effective thin metal layer.

cond-mat.mes-hall↗

arXiv2016

Photon echo in exciton-plasmon nanomaterials: a time-dependent signature of strong coupling

We investigate the dynamics of photon echo exhibited by exciton-plasmon systems under strong coupling conditions. Using a self-consistent model based on coupled Maxwell-Bloch equations we investigate femtosecond time dynamics of ensembles of interacting molecules optically coupled to surface plasmon supporting materials. It is shown that observed photon echoes under two pulse pump-probe sequence are highly dependent on various material parameters such as molecular concentration and periodicity. Simulations of photon echoes in exciton-plasmon materials reveal a unique signature of the strong exciton-plasmon coupling, namely a double-peak structure in spectra of recorded echo signals. This phenomenon is shown to be related to hybrid states (upper and lower polaritons) in exciton-plasmon systems under strong coupling conditions. It is also demonstrated that the double-peak echo is highly sensitive to mild deviations of the coupling from resonant conditions making it a great tool for ultrafast probes.

cond-mat.mes-hall↗

arXiv2016

Non-Hermitian wave packet approximation for coupled two-level systems in weak and intense fields

We introduce an accurate non-Hermitian Schrödinger-type approximation of Bloch optical equations for two-level systems. This approximation provides a complete description of the excitation, relaxation and decoherence dynamics in both weak and strong laser fields. In this approach, it is sufficient to propagate the wave function of the quantum system instead of the density matrix, providing that relaxation and dephasing are taken into account via automatically-adjusted time-dependent gain and decay rates. The developed formalism is applied to the problem of scattering and absorption of electromagnetic radiation by a thin layer comprised of interacting two-level emitters.

quant-ph↗

arXiv2016

Plasmon transmission through excitonic subwavelength gaps

We study the transfer of electromagnetic energy across a subwavelength gap separating two co-axial metal nanorodes. The absence of spacer in the gap separating the rods the system exhibits the strong coupling between longitudinal plasmons in the two rods. The nature and magnitude of this coupling is studied by varying various geometrical parameters. When the length of one rod is varied this mode spectrum exhibits the familiar anti-crossing behavior that depends on the coupling strength determined by the gap width. As a function of frequency the transmission is dominated by a splitted longitudinal plasmon peak. The two hybrid modes are the dipole-like "bonding" mode characterized by a peak intensity in the gap, and a quadrupole-like "antibonding" mode whose amplitude vanishes at the gap center. When off-resonant $2-$level emitters are placed in the gap, almost no effect on the frequency dependent transmission is observed. In contrast, when the molecular system is resonant with the plasmonic lineshape, the transmission is strongly modified, showing characteristics of strong exciton-plasmon coupling, modifying mostly the transmission near the lower frequency "bonding" plasmon mode. The presence of resonant molecules in the gap affects not only the molecule-field interaction but also the spatial distribution of the field intensity and the electromagnetic energy flux across the junction.

physics.optics↗

arXiv2015

Surface plasmon-polaritons in periodic arrays of V-grooves strongly coupled to quantum emitters

We investigate the optical response of a system consisting of periodic silver V-grooves interacting with quantum emitters. Two surface plasmon-polariton resonances are identified in the reflection spectrum of bare silver grooves, with the intensity of one resonance being localized near the bottom of the groove and that of the other resonance being distributed throughout the entire groove. The linear response of the hybrid silver-emitter system is thoroughly analyzed by considering the coupling between surface plasmon polaritons and emitters as the geometry of the grooves and the spatial distribution of emitters within the grooves are varied. The nonlinear response of the system is also considered by pumping the emitters with a short, high-intensity pulse. By changing the duration or the intensity of the pump, the population of emitters in the ground state at the end of the pump is varied, and it is found (upon probing with a short pulse) that an increase in the fraction of emitters in the ground state corresponds to an increase in Rabi splitting. Spatial variations in the ground state population throughout the emitter region are shown to be a result of field retardation.

physics.optics↗

arXiv2015

Linear and nonlinear optics of hybrid plasmon-exciton nanomaterials in the presence of overlapping resonances

We consider a hybrid plasmon-exciton system comprised of a resonant molecular subsystem and three Au wires supporting a dipole mode which can be coupled to a dark mode in controllable fashion by variation of a symmetry parameter. The physics of such a system under strong coupling conditions is examined in detail. It is shown that if two wires supporting the dark mode are covered with molecular layers the system exhibits four resonant modes for a strong coupling regime due to asymmetry and lifted degeneracy of the molecular state in this case, while upon having molecular aggregates covering the top wire with dipolar mode, three resonant modes appear. Pump-probe simulations are performed to scrutinize the quantum dynamics and find possible ways to control plasmon-exciton materials. It is demonstrated that one can design hybrid nanomaterials with highly pronounced Fano-type resonances when excited by femtosecond lasers.

physics.optics↗

arXiv2015

Theory of Dipole Induced Electromagnetic Transparency

A detailed theory describing linear optics of vapors comprised of interacting multi-level quantum emitters is proposed. It is shown both by direct integration of Maxwell-Bloch equations and using a simple analytical model that at large densities narrow transparency windows appear in otherwise completely opaque spectra. The existence of such windows is attributed to overlapping resonances. This effect, first introduced for three-level systems in [R. Puthumpally-Joseph, M. Sukharev, O. Atabek and E. Charron, Phys. Rev. Lett. 113, 163603 (2014)], is due to strongly enhanced dipole-dipole interactions at high emitters' densities. The presented theory extends this effect to the case of multilevel systems. The theory is applied to the D1 transitions of interacting Rb-85 atoms. It is shown that at high atomic densities, Rb-85 atoms can behave as three-level emitters exhibiting all the properties of dipole induced electromagnetic transparency. Applications including slow light and laser pulse shaping are also proposed.

physics.optics↗

arXiv2014

Coherent Phase Control of Internal Conversion in Pyrazine

Shaped ultrafast laser pulses were used to study and control the ionization dynamics of electronically excited pyrazine in a pump and probe experiment. For pump pulses created without feedback from the product signal, the ion growth curve (the parent ion signal as a function of pump/probe delay) was described quantitatively by the classical rate equations for internal conversion of the $S_2$ and $S_1$ states. Very different, non-classical behavior was observed when a genetic algorithm (GA) was used to minimize the ion signal at some pre-determined target time, T. Two qualitatively different control mechanisms were identified for early (T$<1.5$ ps) and late (T$>1.5$ ps) target times. In the former case, the ion signal was largely suppressed for $t 1.5$ ps the ion growth curve followed the classical rate equations for $t<T$, while for $t \gg T$ the quantum yield for the GA-optimized pulse was much smaller than for a TL pulse. We interpret the first type of behavior as an indication that the wave packet produced by the pump laser is localized in a region of the $S_2$ potential energy surface where the vertical ionization energy exceeds the probe photon energy, whereas the second type of behavior may be described by a reduced absorption cross section for $S_0 \rightarrow S_2$ followed by incoherent decay of the excited molecules.

physics.atom-ph↗

arXiv2014

Dipole-Induced Electromagnetic Transparency

We determine the optical response of a thin and dense layer of interacting quantum emitters. We show that in such a dense system, the Lorentz redshift and the associated interaction broadening can be used to control the transmission and reflection spectra. In the presence of overlapping resonances, a Dipole-Induced Electromagnetic Transparency (DIET) regime, similar to Electromagnetically Induced Transparency (EIT), may be achieved. DIET relies on destructive interference between the electromagnetic waves emitted by quantum emitters. Carefully tuning material parameters allows to achieve narrow transmission windows in otherwise completely opaque media. We analyze in details this coherent and collective effect using a generalized Lorentz model and show how it can be controlled. Several potential applications of the phenomenon, such as slow light, are proposed.

quant-ph↗

arXiv2014

Control of optical properties of hybrid materials with chirped femtosecond laser pulses under strong coupling conditions

The interaction of chirped femtosecond laser pulses with hybrid materials - materials comprised of plasmon sustaining structures and resonant molecules - is scrutinized using a self-consistent model of coupled Maxwell-Bloch equations. The optical properties of such systems are examined with the example of periodic sinusoidal gratings. It is shown that under strong coupling conditions one can control light transmission using chirped pulses in a spatiotemporal manner. The temporal origin of control relies on chirps non-symmetric in time while the space control is achieved via spatial localization of electromagnetic energy due to plasmon resonances.

physics.optics↗

arXiv2013

Numerical calculations of radiative and non-radiative relaxation of molecules near metal particles

The dependence of the radiative emission and the non-radiative (energy transfer to the metal) relaxation rates of a molecule near a small metal particle on the molecule-to-particle distance and on the molecular orientation is calculated using a numerical solution of the Maxwell equations for a model that described the metal as a dispersive dielectric particle and the molecule as an oscillating point dipole. The emission rate is obtained by evaluating the total oscillating dipole in the system, while the non-radiative rate is inferred from the rate of heat production on the particle. For the distance dependence of the non-radiative rate we find, in agreement with experimental observations, marked deviation from the prediction of the standard theory of fluorescence resonance energy transfer (FRET). In departure from previous interpretations, we find that electromagnetic retardation is the main source of this deviation at large molecule-particle separations. The radiative emission rate reflects the total dipole induced in the molecule- particle system, and its behavior as function of distance and orientation stems mostly from the magnitude of the oscillating polarization on the metal particle (which, at resonance, is strongly affected by plasmon excitation), and from the way this polarization combines with the molecular dipole to form the total system dipole.

cond-mat.mes-hall↗

arXiv2013

Ultrafast Energy Transfer Between Molecular Assemblies and Surface Plasmons in the Strong Coupling Regime

The nonlinear optical dynamics of nano-materials comprised of plasmons interacting with quantum emitters is investigated by a self-consistent model based on the coupled Maxwell-Liouville-von Neumann equations. It is shown that ultra-short resonant laser pulses significantly modify the optical properties of such hybrid systems. It is further demonstrated that the energy transfer between interacting molecules and plasmons occurs on a femtosecond time scale and can be controlled with both material and laser parameters.

cond-mat.mes-hall↗

arXiv2013

Non-Hermitian wave packet approximation of Bloch optical equations

We introduce a non-Hermitian approximation of Bloch optical equations. This approximation provides a complete description of the excitation, relaxation and decoherence dynamics of ensembles of coupled quantum systems in weak laser fields, taking into account collective effects and dephasing. In the proposed method one propagates the wave function of the system instead of a complete density matrix. Relaxation and dephasing are taken into account via automatically-adjusted time-dependent gain and decay rates. As an application, we compute the numerical wave packet solution of a time-dependent non-Hermitian Schrodinger equation describing the interaction of electromagnetic radiation with a quantum nano-structure and compare the calculated transmission, reflection, and absorption spectra with those obtained from the numerical solution of the Liouville- von-Neumann equation. It is shown that the proposed wave packet scheme is significantly faster than the propagation of the full density matrix while maintaining small error. We provide the key ingredients for easy-to-use implementation of the proposed scheme and identify the limits and error scaling of this approximation.

cond-mat.mes-hall↗

arXiv2012

Molecular nanoplasmonics: self-consistent electrodynamics in current carrying junctions

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.

cond-mat.mes-hall↗

arXiv2012

Stimulated Raman Adiabatic Passage (STIRAP) as a Route to Achieving Optical Control in Plasmonics

Optical properties of ensembles of three-level quantum emitters coupled to plasmonic systems are investigated employing a self-consistent model. It is shown that stimulated Raman adiabatic passage (STIRAP) technique can be successfully adopted to control optical properties of hybrid materials with collective effects present and playing an important role in light-matter interactions. We consider a core-shell nanowire comprised of a silver core and a shell of coupled quantum emitters and utilize STIRAP scheme to control scattering efficiency of such a system in a frequency and spatial dependent manner. After the STIRAP induced population transfer to the final state takes place, the core-shell nanowire exhibits two sets of Rabi splittings with Fano lineshapes indicating strong interactions between two different atomic transitions driven by plasmon near-fields.

cond-mat.mes-hall↗

arXiv2012

Collective Plasmonic-Molecular Modes in the Strong Coupling Regime

We demonstrate strong coupling between molecular excited states and surface plasmon modes of a slit array in a thin metal film. The coupling manifests itself as an anti-crossing behavior of the two newly formed polaritons. As the coupling strength grows, a new mode emerges, which is attributed to long range molecular interactions mediated by the plasmonic field. The new, molecular-like mode repels the polariton states, and leads to an opening of energy gaps both below and above the asymptotic free molecule energy.

cond-mat.mes-hall↗