Exciton behavior under the influence of metal nanoparticle near fields: Significance of nonlocal effects

Harini Hapuarachchi, Sarath D. Gunapala, Qiaoliang Bao, Mark I. Stockman, Malin Premaratne

Research output: Contribution to journalArticleResearchpeer-review

Abstract

We analytically characterize the influence of a neighboring metal nanoparticle (MNP) on the behavioral trends of a quantum dot (QD) using a generalized nonlocal optical response (GNOR) method based approach, taking the MNP distance dependent modifications to the QD population relaxation and dephasing rates into account. The GNOR model is a recent generalization and an extension of the hydrodynamic Drude model (HDM), which goes beyond HDM by taking into account both the convection current and electron diffusion in the MNPs. It allows unified theoretical explanation of some experimentally observed plasmonic phenomena which otherwise would require ab initio analysis as the conventional local response approximation (LRA) fails to account for them. For example, it has been demonstrated in literature that the GNOR model captures size dependent resonance shifts of small MNPs which are unrevealed by the conventional LRA based methods, and it has proven to yield results displaying better agreement with the experimental observations for plasmonic experiments. Attempts to incorporate MNP nonlocal effects in the analytical characterization of vicinal excitons found in literature utilize the phenomenological hydrodynamic model and assume the absence of MNP interband effects. Moreover, they are only applicable to narrow parameter regions. In this paper we present a complete analytical characterization which overcomes these drawbacks and lends to the perusal of the system over wide continua of various parameters, enabling us to get an elevated view at a much lesser level of complexity compared to the conventional LRA based numerical methods or the conventional ab initio methods of accounting for the nonlocal effects. Our proposed GNOR based model predicts strong modifications to various QD properties such as population difference, absorption, MNP induced shifts to excitonic energy and Förster enhanced broadening, coherent plasmonic field enhancement, and quantum state purity, compared to the conventional LRA based predictions. Such modifications are prominent with small MNP radii, high QD dipole moments, small detunings (of the coherent external illumination from the bare excitonic resonance), and near parameter regions exhibiting plasmonic meta resonance (PMR)-like behavior. Moreover, our complete analytical characterization enables optimization of the large system parameter space for different applications, a luxury not fully offered by the methods currently available in literature.

Original languageEnglish
Article number115430
Number of pages14
JournalPhysical Review B
Volume98
Issue number11
DOIs
Publication statusPublished - 18 Sep 2018

Cite this

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title = "Exciton behavior under the influence of metal nanoparticle near fields: Significance of nonlocal effects",
abstract = "We analytically characterize the influence of a neighboring metal nanoparticle (MNP) on the behavioral trends of a quantum dot (QD) using a generalized nonlocal optical response (GNOR) method based approach, taking the MNP distance dependent modifications to the QD population relaxation and dephasing rates into account. The GNOR model is a recent generalization and an extension of the hydrodynamic Drude model (HDM), which goes beyond HDM by taking into account both the convection current and electron diffusion in the MNPs. It allows unified theoretical explanation of some experimentally observed plasmonic phenomena which otherwise would require ab initio analysis as the conventional local response approximation (LRA) fails to account for them. For example, it has been demonstrated in literature that the GNOR model captures size dependent resonance shifts of small MNPs which are unrevealed by the conventional LRA based methods, and it has proven to yield results displaying better agreement with the experimental observations for plasmonic experiments. Attempts to incorporate MNP nonlocal effects in the analytical characterization of vicinal excitons found in literature utilize the phenomenological hydrodynamic model and assume the absence of MNP interband effects. Moreover, they are only applicable to narrow parameter regions. In this paper we present a complete analytical characterization which overcomes these drawbacks and lends to the perusal of the system over wide continua of various parameters, enabling us to get an elevated view at a much lesser level of complexity compared to the conventional LRA based numerical methods or the conventional ab initio methods of accounting for the nonlocal effects. Our proposed GNOR based model predicts strong modifications to various QD properties such as population difference, absorption, MNP induced shifts to excitonic energy and F{\"o}rster enhanced broadening, coherent plasmonic field enhancement, and quantum state purity, compared to the conventional LRA based predictions. Such modifications are prominent with small MNP radii, high QD dipole moments, small detunings (of the coherent external illumination from the bare excitonic resonance), and near parameter regions exhibiting plasmonic meta resonance (PMR)-like behavior. Moreover, our complete analytical characterization enables optimization of the large system parameter space for different applications, a luxury not fully offered by the methods currently available in literature.",
author = "Harini Hapuarachchi and Gunapala, {Sarath D.} and Qiaoliang Bao and Stockman, {Mark I.} and Malin Premaratne",
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Exciton behavior under the influence of metal nanoparticle near fields : Significance of nonlocal effects. / Hapuarachchi, Harini; Gunapala, Sarath D.; Bao, Qiaoliang; Stockman, Mark I.; Premaratne, Malin.

In: Physical Review B, Vol. 98, No. 11, 115430, 18.09.2018.

Research output: Contribution to journalArticleResearchpeer-review

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T1 - Exciton behavior under the influence of metal nanoparticle near fields

T2 - Significance of nonlocal effects

AU - Hapuarachchi, Harini

AU - Gunapala, Sarath D.

AU - Bao, Qiaoliang

AU - Stockman, Mark I.

AU - Premaratne, Malin

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