Influence of spatial dispersion on spectral tuning of phonon-polaritons

Beechem, Thomas E.; Saltonstall, Christopher B.; Gilbert, Tristan; Matson, Joseph; Ugwu, Fabian; Kasica, Richard; Bezares, Francisco J.; Valentine, Jason; Caldwell, Joshua D.

doi:10.1103/physrevb.100.205419

Influence of spatial dispersion on spectral tuning of phonon-polaritons

Journal Article · Wed Nov 20 00:00:00 EST 2019 · Physical Review B

DOI:https://doi.org/10.1103/physrevb.100.205419· OSTI ID:1760356

^[1]; Saltonstall, Christopher B. ^[2]; Gilbert, Tristan ^[3]; Matson, Joseph ^[3]; Ugwu, Fabian ^[3]; Kasica, Richard ^[4]; Bezares, Francisco J. ^[5]; Valentine, Jason ^[3]; Caldwell, Joshua D. ^[3]

Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies (CINT)
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Vanderbilt Univ., Nashville, TN (United States)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
Univ. of Puerto Rico, Cayey, PR (United States)

The field of nanophotonics has long sought to identify mechanisms to realize dynamical control of optical modes. In most approaches, the magnitude of tuning is dependent upon the degree to which the optical permittivity is malleable upon some material change, such as carrier concentration. Here, through a multiwavelength Raman spectroscopic examination of 4H-SiC nanopillars, momentum is identified as an alternative means to enhance spectral tunability of nanophotonic modes, owing to the spatial dispersion implicit in the infrared (IR) optical permittivity of polar semiconductors. Experimentally, this is deduced through the observation of a “forbidden” Raman mode at ≈ 780cm^-1 and the emergence of the surface-optical phonon polariton at ≈ 950 cm^-1, which evolved with intensities dependent upon the nanopillar diameter and the wavelength of the incident light. The evolution of these modes is accompanied by a redshift and spectral narrowing of the longitudinal-optical plasmon coupled (LOPC) mode exhibiting a similar wavelength and diameter dependence. Mie resonances, identified using ultraviolet-visible spectroscopy and excited by the visible laser excitation of the Raman experiment, acted to vary the momentum sampled during the Raman experiment leading to these spectral dependencies. Furthermore, this was deduced by fitting the Raman response accounting for both the presence of the surface phonon and the overdamped LOPC mode under the Lindhard-Mermin approximation. This fitting not only explains the Raman response, but also clearly exhibits the spatially disperse permittivity of the SiC, which is shown to have a momentum-dependent sensitivity to carrier concentration. Such sensitivity, in turn, highlights the potential of spatial dispersion as a means to accentuate the performance of active IR nanophotonic approaches employing phonon polaritons.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC04-94AL85000; NA0003525

OSTI ID:: 1760356

Report Number(s):: SAND--2020-12512J; 692003

Journal Information:: Physical Review B, Journal Name: Physical Review B Journal Issue: 20 Vol. 100; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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