Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

arXiv:1603.09140 · Physical review. B./Physical review. B

Theoretical study of plasmonic lasing in junctions with many molecules

Yuan Zhang, Klaus Mølmer, Volkhard May

Published Jul 11, 2016• 5 citations
arXivHTMLPDF

Abstract

We calculate the quantum state of the plasmon field excited by an ensemble of molecular emitters, which are driven by exchange of electrons with metallic nanoparticle electrodes. Assuming identical emitters that are coupled collectively to the plasmon mode but are otherwise subject to independent relaxation channels, we show that symmetry constraints on the total system density matrix imply a drastic reduction in the numerical complexity. For ${N}_{\text{m}}$ three-level molecules, we may thus represent the density matrix by a number of terms scaling as $({N}_{\mathrm{m}}+8)!/(8!{N}_{\mathrm{m}}!)$ instead of ${9}^{{N}_{\text{m}}}$, and this allows exact simulations of up to ${N}_{\text{m}}=10$ molecules. Our simulations demonstrate that many emitters compensate strong plasmon damping and lead to the population of high plasmon number states as well as a narrowed emission, which indicates a transition from spontaneous emission to amplified spontaneous emission. For large ${N}_{\text{m}}$, our exact results are reproduced by an approximate approach based on the plasmon reduced density matrix. With this approach, we have extended the simulations to more than 100 molecules and shown that the plasmon number state population follows a Poisson-like distribution, which indicates the formation of a plasmon coherent state. This clearly indicates a transition from amplified spontaneous emission to lasing. An alternative approach based on nonlinear rate equations for the molecular state populations and the mean plasmon number also reproduce the main lasing characteristics of the system.

DOI
10.1103/physrevb.94.045412

Related papers

Spontaneous emission by an ensemble of dipoles coupled to a plasmonic nanoresonator

Jaylon Uzodinma, Nicholas E. Nelson, Qilin Dai +1 more

Spontaneous emission from ensembles of quantum emitters (QEs) such as atoms, molecules or semiconductor quantum dots can be greatly enhanced by cooperative effects arising from electromagnetic correlations. We describe a cooperative mechanism for emission of light by an ensemble of QEs based upon cooperative energy transfer from QEs to localized surface plasmons in metal-dielectric structures followed by plasmon radiation at a rate that scales with the ensemble size. For large QE ensembles saturating the plasmon mode volume, we derive universal, i.e. independent of local field distribution, expression for cooperative Purcell factor that can by far exceed the field enhancement limits for individual QE in a hot spot. We also derive radiated power spectrum that retains the plasmon resonance lineshape and, in contrast to common cooperative mechanisms, is insensitive to natural variations of QEs' emission frequencies.

Journal of Modern Optics•Jul 29, 2019•2 citations

Relaxation dynamics of a quantum emitter resonantly coupled to a coherent state of a localized surface plasmon

Khachatur Nerkararyan, Sergey I. Bozhevolnyi

We investigate the relaxation dynamics of a quantum dipole emitter (QDE), e.g., a molecule or quantum dot, located near a metal nanoparticle (MNP) exhibiting a dipolar localized surface plasmon (LSP) resonance at the frequency of the QDE radiative transition. A generic three-level QDE, which is pumped with an external laser pulse and thereby brought into an optically active excited state, is considered to be weakly coupled to the resonant LSP described by a coherent state. It is shown that, under the condition of the QDE-MNP characteristic relaxation time being much shorter than that of the QDE in free space but much longer than the LSP lifetime, the QDE relaxation dynamics can be described analytically and feature, in general, non-exponential decay with complicated transient behaviour. The main physical consequence of this relaxation process is that the emission, being largely determined by the MNP, comes out with a substantial delay. It is also shown that energy dissipation in the QDE-MNP system is relatively weak with the probability of the photon emission being ∼0.75, a number which, rather surprisingly, does not explicitly depend on the metal absorption characteristics. A large number of QDE-MNP system parameters in our analytical description open new possibilities for controlling quantum emitter dynamics.

Faraday Discussions•Oct 20, 2014•8 citations

A Review of Many-Body Interactions in Linear and Nonlinear Plasmonic Nanohybrids

Mahi R. Singh

In this review article, we discuss the many-body interactions in plasmonic nanohybrids made of an ensemble of quantum emitters and metallic nanoparticles. A theory of the linear and nonlinear optical emission intensity was developed by using the many-body quantum mechanical density matrix method. The ensemble of quantum emitters and metallic nanoparticles interact with each other via the dipole-dipole interaction. Surfaces plasmon polaritons are located near to the surface of the metallic nanoparticles. We showed that the nonlinear Kerr intensity enhances due to the weak dipole-dipole coupling limits. On the other hand, in the strong dipole-dipole coupling limit, the single peak in the Kerr intensity splits into two peaks. The splitting of the Kerr spectrum is due to the creation of dressed states in the plasmonic nanohybrids within the strong dipole-dipole interaction. Further, we found that the Kerr nonlinearity is also enhanced due to the interaction between the surface plasmon polaritons and excitons of the quantum emitters. Next, we predicted the spontaneous decay rates are enhanced due to the dipole-dipole coupling. The enhancement of the Kerr intensity due to the surface plasmon polaritons can be used to fabricate nanosensors. The splitting of one peak (ON) two peaks (OFF) can be used to fabricate the nanoswitches for nanotechnology and nanomedical applications.

Symmetry•Mar 9, 2021•10 citations

Cooperative effects in plasmonics: superfluorescence near metal nanostructures

Vitaliy N. Pustovit, Tigran V. Shahbazyan

We develop a theory of cooperative emission of light by an ensemble of emitters, such as fluorescing molecules or semiconductor quantum dots, located near a metal nanostructure supporting surface plasmon. The primary mechanism of cooperative emission in such systems is resonant energy transfer between emitters and plasmons rather than the Dicke radiative coupling between emitters. We identify two types of plasmonic coupling between the emitters, (i) plasmon-enhanced radiative coupling and (ii) plasmon-assisted nonradiative energy transfer, the competition between them governing the structure of system eigenstates. Specifically, when emitters are removed by more than several nm from the metal surface, the emission is dominated by three superradiant states with the same quantum yield as a single emitter, resulting in a drastic reduction of ensemble radiated energy, while at smaller distances cooperative behavior is destroyed by nonradiative transitions. The crossover between two regimes can be observed in distance dependence of ensemble quantum efficiency. Our numerical calculations incorporating direct and plasmon-assisted interactions between the emitters indicate that they do not destroy the plasmonic Dicke effect.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Aug 19, 2010•0 citations

Plasmon-mediated superradiance near metal nanostructures

Vitaliy N. Pustovit, Tigran V. Shahbazyan

We develop a theory of cooperative emission of light by an ensemble of emitters, such as fluorescing molecules or semiconductor quantum dots, located near a metal nanostructure supporting surface plasmon. The primary mechanism of cooperative emission in such systems is resonant energy transfer between emitters and plasmons rather than the Dicke radiative coupling between emitters. We identify two types of plasmonic coupling between the emitters, (i) plasmon-enhanced radiative coupling and (ii) plasmon-assisted nonradiative energy transfer, the competition between them governing the structure of system eigenstates. Specifically, when emitters are removed by more than several nanometers from the metal surface, the emission is dominated by three superradiant states with the same quantum yield as a single emitter, resulting in a drastic reduction of ensemble radiated energy, while at smaller distances cooperative behavior is destroyed by nonradiative transitions. The crossover between two regimes can be observed in distance dependence of ensemble quantum efficiency. Our numerical calculations incorporating direct and plasmon-assisted interactions between the emitters indicate that they do not destroy the plasmonic Dicke effect.

arXiv:1001.0422•Physical Review B•Aug 30, 2010•104 citations

Quantum-coherence-enhanced transient surface plasmon lasing

Pankaj Kumar Jha, Yuan Wang, Xuexin Ren +1 more

Abstract Quantum coherence and interference offer novel pathways to control light–matter interaction at the atomic scale, with enticing prospects in both fundamental and applied science. Here, we demonstrate coherent control over transient excitation of localized surface plasmon modes of a silver nanosphere adjacent to a quantum coherence medium composed of three-level quantum emitters, using a theoretical approach. We show that quantum interference enables more than two orders of magnitude enhancement in the surface plasmon field generated when the quantum emitters are driven coherently, in comparison to incoherent pumping. Furthermore, under optimal conditions, intense surface plasmon lasing can be induced without population inversion on the spasing transition. Our results open up the possibility of overcoming dissipative losses in plasmonic modes in the transient regime when steady-state population inversion is difficult to achieve due to fast relaxation rates and impractical pumping requirements.

Journal of Optics•Feb 15, 2017•12 citations
We calculate the quantum state of the plasmon field excited by an ensemble of molecular emitters, which are driven by exchange of electrons with metallic nanoparticle electrodes. Assuming identical emitters that are coupled collectively to the plasmon mode but are otherwise subject to independent relaxation channels, we show that symmetry constraints on the total system density matrix imply a drastic reduction in the numerical complexity. For Nm{N}_{\text{m}}Nm​ three-level molecules, we may thus represent the density matrix by a number of terms scaling as (Nm+8)!/(8!Nm!)({N}_{\mathrm{m}}+8)!/(8!{N}_{\mathrm{m}}!)(Nm​+8)!/(8!Nm​!) instead of 9Nm{9}^{{N}_{\text{m}}}9Nm​, and this allows exact simulations of up to Nm=10{N}_{\text{m}}=10Nm​=10 molecules. Our simulations demonstrate that many emitters compensate strong plasmon damping and lead to the population of high plasmon number states as well as a narrowed emission, which indicates a transition from spontaneous emission to amplified spontaneous emission. For large Nm{N}_{\text{m}}Nm​, our exact results are reproduced by an approximate approach based on the plasmon reduced density matrix. With this approach, we have extended the simulations to more than 100 molecules and shown that the plasmon number state population follows a Poisson-like distribution, which indicates the formation of a plasmon coherent state. This clearly indicates a transition from amplified spontaneous emission to lasing. An alternative approach based on nonlinear rate equations for the molecular state populations and the mean plasmon number also reproduce the main lasing characteristics of the system.
Spontaneous emission from ensembles of quantum emitters (QEs) such as atoms, molecules or semiconductor quantum dots can be greatly enhanced by cooperative effects arising from electromagnetic correlations. We describe a cooperative mechanism for emission of light by an ensemble of QEs based upon cooperative energy transfer from QEs to localized surface plasmons in metal-dielectric structures followed by plasmon radiation at a rate that scales with the ensemble size. For large QE ensembles saturating the plasmon mode volume, we derive universal, i.e. independent of local field distribution, expression for cooperative Purcell factor that can by far exceed the field enhancement limits for individual QE in a hot spot. We also derive radiated power spectrum that retains the plasmon resonance lineshape and, in contrast to common cooperative mechanisms, is insensitive to natural variations of QEs' emission frequencies.
We investigate the relaxation dynamics of a quantum dipole emitter (QDE), e.g., a molecule or quantum dot, located near a metal nanoparticle (MNP) exhibiting a dipolar localized surface plasmon (LSP) resonance at the frequency of the QDE radiative transition. A generic three-level QDE, which is pumped with an external laser pulse and thereby brought into an optically active excited state, is considered to be weakly coupled to the resonant LSP described by a coherent state. It is shown that, under the condition of the QDE-MNP characteristic relaxation time being much shorter than that of the QDE in free space but much longer than the LSP lifetime, the QDE relaxation dynamics can be described analytically and feature, in general, non-exponential decay with complicated transient behaviour. The main physical consequence of this relaxation process is that the emission, being largely determined by the MNP, comes out with a substantial delay. It is also shown that energy dissipation in the QDE-MNP system is relatively weak with the probability of the photon emission being ∼0.75, a number which, rather surprisingly, does not explicitly depend on the metal absorption characteristics. A large number of QDE-MNP system parameters in our analytical description open new possibilities for controlling quantum emitter dynamics.
In this review article, we discuss the many-body interactions in plasmonic nanohybrids made of an ensemble of quantum emitters and metallic nanoparticles. A theory of the linear and nonlinear optical emission intensity was developed by using the many-body quantum mechanical density matrix method. The ensemble of quantum emitters and metallic nanoparticles interact with each other via the dipole-dipole interaction. Surfaces plasmon polaritons are located near to the surface of the metallic nanoparticles. We showed that the nonlinear Kerr intensity enhances due to the weak dipole-dipole coupling limits. On the other hand, in the strong dipole-dipole coupling limit, the single peak in the Kerr intensity splits into two peaks. The splitting of the Kerr spectrum is due to the creation of dressed states in the plasmonic nanohybrids within the strong dipole-dipole interaction. Further, we found that the Kerr nonlinearity is also enhanced due to the interaction between the surface plasmon polaritons and excitons of the quantum emitters. Next, we predicted the spontaneous decay rates are enhanced due to the dipole-dipole coupling. The enhancement of the Kerr intensity due to the surface plasmon polaritons can be used to fabricate nanosensors. The splitting of one peak (ON) two peaks (OFF) can be used to fabricate the nanoswitches for nanotechnology and nanomedical applications.
We develop a theory of cooperative emission of light by an ensemble of emitters, such as fluorescing molecules or semiconductor quantum dots, located near a metal nanostructure supporting surface plasmon. The primary mechanism of cooperative emission in such systems is resonant energy transfer between emitters and plasmons rather than the Dicke radiative coupling between emitters. We identify two types of plasmonic coupling between the emitters, (i) plasmon-enhanced radiative coupling and (ii) plasmon-assisted nonradiative energy transfer, the competition between them governing the structure of system eigenstates. Specifically, when emitters are removed by more than several nm from the metal surface, the emission is dominated by three superradiant states with the same quantum yield as a single emitter, resulting in a drastic reduction of ensemble radiated energy, while at smaller distances cooperative behavior is destroyed by nonradiative transitions. The crossover between two regimes can be observed in distance dependence of ensemble quantum efficiency. Our numerical calculations incorporating direct and plasmon-assisted interactions between the emitters indicate that they do not destroy the plasmonic Dicke effect.
We develop a theory of cooperative emission of light by an ensemble of emitters, such as fluorescing molecules or semiconductor quantum dots, located near a metal nanostructure supporting surface plasmon. The primary mechanism of cooperative emission in such systems is resonant energy transfer between emitters and plasmons rather than the Dicke radiative coupling between emitters. We identify two types of plasmonic coupling between the emitters, (i) plasmon-enhanced radiative coupling and (ii) plasmon-assisted nonradiative energy transfer, the competition between them governing the structure of system eigenstates. Specifically, when emitters are removed by more than several nanometers from the metal surface, the emission is dominated by three superradiant states with the same quantum yield as a single emitter, resulting in a drastic reduction of ensemble radiated energy, while at smaller distances cooperative behavior is destroyed by nonradiative transitions. The crossover between two regimes can be observed in distance dependence of ensemble quantum efficiency. Our numerical calculations incorporating direct and plasmon-assisted interactions between the emitters indicate that they do not destroy the plasmonic Dicke effect.
Abstract Quantum coherence and interference offer novel pathways to control light–matter interaction at the atomic scale, with enticing prospects in both fundamental and applied science. Here, we demonstrate coherent control over transient excitation of localized surface plasmon modes of a silver nanosphere adjacent to a quantum coherence medium composed of three-level quantum emitters, using a theoretical approach. We show that quantum interference enables more than two orders of magnitude enhancement in the surface plasmon field generated when the quantum emitters are driven coherently, in comparison to incoherent pumping. Furthermore, under optimal conditions, intense surface plasmon lasing can be induced without population inversion on the spasing transition. Our results open up the possibility of overcoming dissipative losses in plasmonic modes in the transient regime when steady-state population inversion is difficult to achieve due to fast relaxation rates and impractical pumping requirements.