Hybrid quantum systems for enhanced nonlinear optical susceptibilities

Sullivan, Dennis M.; Mossman, Sean; Kuzyk, Mark G.

doi:10.1364/josab.33.00e143

Cited by 4 publications

(3 citation statements)

References 27 publications

(31 reference statements)

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“…A previous paper describes the accuracy of the FDTD method in determining the eigenstates of quantum wires [11]. A subsequent paper describes the determination of the hyperpolarizability of quantum wires in close proximity to an electric dipole [12]. In this paper we describe the simulation of a magnetic dipole formulated as a quantum loop as well as the FDTD implementation of the quantum magnet-ic dipole operator.…”

Section: Introductionmentioning

confidence: 99%

Three Dimensional Time Domain Simulationof the Quantum Magnetic Dipole

Houle¹,

Sullivan²,

Crowell³

et al. 2018

Int J Magnetics Electromagnetism

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A method is presented to simulate the magnetic response of a quantum toroid for the purpose of optimizing the nonlinear characteristics of an induced magnetic dipole. This is a true three-dimensional simulation based on the direct implementation of the time-dependent Schrödinger equation. We demonstrate that the expectation value the quantum magnetic dipole operator returns results consistent with a classical electron in a loop under the influence of a magnetic field.

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Section: Introductionmentioning

confidence: 99%

Three Dimensional Time Domain Simulationof the Quantum Magnetic Dipole

Houle¹,

Sullivan²,

Crowell³

et al. 2018

Int J Magnetics Electromagnetism

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“…The accuracy of this method in determining the eigenstates of quantum wires was previously described [14]. The FDTD method was used in the determination of the hyperpolarizability of quantum wires in close proximity to an electric dipole [15]. A method was also presented to simulate the magnetic response of a quantum toroid using the quantum magnetic dipole operator [16].…”

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confidence: 99%

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2018

Int J Magnetics Electromagnetism

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Materials with nonlinear properties have applications in optical switching [1], lasers, photovoltaic cells [2], imaging [2], cancer therapy [3,4], advanced computing [5,6], and communication technologies [7,8]. To improve applications, it is important to establish good methods and models to explore the optimization of nonlinear effects by increasing the nonlinear response. This work provides a way of calculating the nonlinear response of nanostructures. This helps in designing new systems without the need for doing difficult and time-consuming measurements.

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“…Nanostructures consisting of short metal rods with a side prong also meet these criteria and are of interest for future exploration. Finally, hybrid materials [31] point to design paradigms which could achieve the exact limits. These systems have spectra that scale linearly or faster with eigenstate number.…”

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confidence: 99%

Exact Fundamental Limits of the First and Second Hyperpolarizabilities

et al. 2017

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Nonlinear optical interactions of light with materials originate in the microscopic response of the molecular constituents to excitation by an optical field, and are expressed by the first (β) and second (γ) hyperpolarizabilities. Upper bounds to these quantities were derived seventeen years ago using approximate, truncated state models that violated completeness and unitarity, and far exceed those achieved by potential optimization of analytical systems. This letter determines the fundamental limits of the first and second hyperpolarizability tensors using Monte-Carlo sampling of energy spectra and transition moments constrained by the diagonal Thomas-Reiche-Kuhn (TRK) sum rules and filtered by the off-diagonal TRK sum rules. The upper bounds of β and γ are determined from these quantities by applying error-refined extrapolation to perfect compliance to the sum rules. The method yields the largest diagonal component of the hyperpolarizabilities for an arbitrary number of interacting electrons in any number of dimensions. The new method provides design insight to the synthetic chemist and nanophysicist for approaching the limits. This analysis also reveals that the special cases which lead to divergent nonlinearities in the many-state catastrophe are not physically realizable.PACS numbers: 42.65.An, 78.67.LtIntroduction-Nonlinear optics is the study of quantum systems with polarizations that are nonlinear functions of external electromagnetic fields. This letter solves the problem of determining the exact fundamental limits of nonlinear optics by delineating the first procedure for computing the first and second hyperpolarizabilities consistent with on-and off-diagonal quantum mechanical sum rules. In the process, we show that prior predictions of the limits using truncated sum rules are too high by nearly 30% for β[1, 2] and 40% for γ [2], that predictions of the many-state catastrophe [3] are spurious, and that predictions of the scaling of the hyperpolarizabilities with the strength of the ground-to-excited state transition moment are modified in a way that will direct molecular synthesists to make new design choices.The nonlinear optical response of a material is generated by the collective response of the basic elements comprising it. This letter concerns the maximum values of the nonlinear optical response of a molecular-scale structure, not a material. The nonlinear optics of an elemental structure is measured by the effect it has on the molecular polarization vector when perturbatively excited by an electric field E i , with i = x, y, z:

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Hybrid quantum systems for enhanced nonlinear optical susceptibilities

Cited by 4 publications

References 27 publications

Three Dimensional Time Domain Simulationof the Quantum Magnetic Dipole

Three Dimensional Time Domain Simulationof the Quantum Magnetic Dipole

Untitled

Exact Fundamental Limits of the First and Second Hyperpolarizabilities

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