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Linking Plasma Formation in Grapes To Microwave Resonances of Aqueous Dimers
Linking Plasma Formation in Grapes To Microwave Resonances of Aqueous Dimers
Edited by Catherine J. Murphy, University of Illinois at Urbana–Champaign, Urbana, IL, and approved January 9, 2019 (received for review October 25, 2018)
The sparking of cut grape hemispheres in a household microwave In this article, we present methods for studying Mie reso-
oven has been a poorly explained Internet parlor trick for over nances in absorbing dielectrics in the microwave regime. With
two decades. By expanding this phenomenon to whole spheri- thermographic studies, we offer a low-tech method for exper-
cal dimers of various grape-sized fruit and hydrogel water beads, imentally measuring internal and evanescent near-field elec-
we demonstrate that the formation of plasma is due to elec- tromagnetic concentrations with subwavelength resolution. We
tromagnetic hotspots arising from the cooperative interaction combine these methods with finite-element simulations to show
of Mie resonances in the individual spheres. The large dielec- progressions from isolated resonances to coupled-resonator
tric constant of water at the relevant gigahertz frequencies supermodes in aqueous dimers. The hotspots formed represent
can be used to form systems that mimic surface plasmon reso- superfocusing on the order of λ0 /100. With these tools, we pro-
nances that are typically reserved for nanoscale metallic objects. vide a detailed description and explanation of plasma formation
The absorptive properties of water furthermore act to homoge- from fruit dimers in a microwave oven, as well as opening a
nize higher-mode profiles and to preferentially select evanescent sandbox for the study of nanocluster photonics using absorbing
field concentrations such as the axial hotspot. Thus, beyond dielectrics.
providing an explanation for a popular-science phenomenon,
we outline a method to experimentally model subwavelength The Formation of Plasma from Aqueous Dimers
field patterns using thermal imaging in macroscopic dielectric The “grape plasma” phenomenon is currently restricted in the
systems. lay media to grape hemispheres, usually connected by a strip of
skin. Naturally, previous explanations for the phenomenon have
microwave photonics | dielectric resonators | plasma ionization | invariably involved the roles of the skin and of the open wet sur-
hydrogels | morphology-dependent resonances face in forming the plasma. However, we find that neither of
these components are essential to the formation of the plasma.
The phenomenon is exemplified in Fig. 1A and Movie S1. A close
APPLIED PHYSICAL
through the microwave-oven door, demonstrating that the plasma is initi- ulation parameters, including thermal coupling, can be found in
ated by K and Na species in the grapes and by Na in the NaCl-soaked water
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SI Appendix.
beads. The distinct spectrum of plasma from aluminum foil is shown for
comparison.
With thermal imaging, sparking is no longer desired, as it may coefficient∗ (17). When simulating a reduced absorption coef-
add spurious heating effects. Consequently, thermal-mapping ficient, the Q factor of the dimers is boosted, and a menagerie
experiments use lower irradiation times, and hydrogel beads are of complicated electromagnetic field modes are found inside
hydrated with deionized water and not soaked in a saline solu- the simulated beads, consistent with other reports for dielec-
tion. This allows us to measure the effect of bead size and sepa- tric spheres (12). However, when the full absorptive behavior of
ration on field-intensity maps in the system (Figs. 2 and 3). Live water dimers is included, the wide array of modes found at lower
in situ thermal imaging shows qualitatively very similar struc- absorption washes out, leaving relatively weak radially symmet-
ture to postirradiation imaging, as shown in Movie S5. Studying ric internal modes and an emergent hotspot localized to the
larger water beads, we note a well-defined central mode present proximal point of contact.
in isolated spheres (Fig. 2B). This in itself is clear evidence of This behavior can be seen in Fig. 4, in which simulated field
constructive interference, and therefore of a low-Q resonant patterns in grape-sized and larger dimers are shown, both for
cavity: With a penetration depth of ≈1.5 cm—smaller than the the full dielectric behavior of water and for reduced-absorption
radius of the large beads—a simple model of absorption would objects of equivalent index of refraction. With lower absorption,
be expected to yield a thermal pattern that is hotter near the sur- hotspot resonances are sharp, and there is a large difference
face, becoming less hot toward the center of the object as the in mode strength between beads with small size differences.
microwave radiation is attenuated. The fact that water spheres of For example, simulated 9.5-mm-radius beads display an intense
various sizes routinely yield the inverted pattern of a hot middle hotspot that is absent in 10-mm beads (Fig. 4 A and B). In
is thus evidence of optical resonance in isolated aqueous spheres. the absorptive case, the mode strength remains more con-
Moreover, when we control the orb separation within a dimer, stant across a large size range. This indicates that formation of
we see a clear progression of mode structure from isolated res- hotspots with absorption is a consequence of the broadening
onators to a bonding mode with a concentrated hotspot, as shown of the mode structure. The broadening results in more acces-
in Fig. 3. We also observe that larger beads can simultaneously sible intense hotspot-like modes, as well as homogenizing and
accommodate a supermode hotspot near the point of contact and suppressing higher-order internal modes. In a broad range of
a well-defined mode in their center (Fig. 2A). This is consistent simulated sizes and separations, we find that absorptive dimers
with simulations (Fig. 2C), and in both cases, the internal modes support a bright hotspot at the point of contact, even when no
become less marked as the central hotspot becomes stronger. hotspot is found in simulations of negligibly absorbing equivalent
As can be seen in Fig. 2C, central modes with little evanescent dimers.
character also interact, moving slightly toward each other along There are also trends with bead geometries. Generally, smaller
the dimer axis. beads at close dimer proximity favor a single hotspot between
the two spheres. As beads are separated or increased in size,
The Effects of Absorption internal central modes better coexist with the dimer hotspot and
A key finding arising from our experiments and simulations become more apparent (Fig. 4C). The washing out of modes with
is that similar field patterns persist across a wide range of increased absorption is exemplified by a broadening of resonance
dimer sizes. This is explained by the attendant absorption arising
from the high imaginary component of the complex dielec-
* Explicitly,
the√complex
tric constant of water. At 2.45 GHz and 20 ◦ C, ˜ = 1 + i2 ≈ p index of refraction is related to the complex susceptibility via
ñ = n + ik = ˜ = 1 + i2 , where n is typically referred to as the index of refraction
79 + i10, with 1 most directly contributing to the index of and k, which is responsible for absorption, is referred to as the extinction coefficient.
refraction, and 2 most directly contributing to the absorption At 20 ◦ C, we have n = 8.9 and k = 0.56.
APPLIED PHYSICAL
peaks, as can be seen in Fig. 5, which presents total integrated in Fig. 6 A and E, the hotspot appears to be most intense midgap
SCIENCES
EM energy as a function of dimer bead size. As expected from between the beads, rather than at their surface. This behavior
a lower-Q resonator, an increase in absorption broadens the res- contrasts with simulations that show stronger evanescent fields
onances and decreases their intensity in the bulk. This behavior near the surface when a significant gap is present (Fig. 3F). Thus,
thus supports the experimental observations that a microwave- it is possible that thermal contact between the paper and the sur-
induced hotspot is observed across a wide range of grape and face of the objects prevents a hotspot from being recorded on
hydrogel dimer sizes. the shims closest to each surface. Nonetheless, simulations show
The functional dependence of the complex dielectric constant significant field focusing spanning even significant gaps, which is
on temperature, frequency, and salinity provides an important confirmed with the thermal-paper experiments. We us two sim-
avenue for future research. For example, at 2.5 GHz, the absorp- ilar geometries to demonstrate this: First, as shown in Fig. 6
tive properties of water change more rapidly than does the index A and B, we can keep the dimer in contact by wrapping both
of refraction between the temperatures of 0 ◦ C and 60 ◦ C (17).
Thus, details of resonant mode structure, including localized
hotspots, may result in dynamic runaway or self-tuning processes
arising from local absorptive heating. Such complex behavior
may be observable with in situ live thermal videography (such
as Movie S5). It is entirely possible that the dimer hotspot
leads to localized heating that dramatically reduces absorption
near the gap, but not in the bulk, yielding a positive feedback
for hotspot intensification. The universality of the resonance
behavior means that detailed thermographic observations of field
dynamics in centimeter-scale aqueous structures can uniquely
inform nanophotonic scattering processes that cannot at present
be resolved at optical wavelengths.
spheres together in a thermal paper band and then using a num- Surface Geometry and Hollow Quail Eggs
ber of thermal-paper shims between the two spheres to form a Because the hotspot is observed for such a wide range of sizes
fixed-length gap. We see a clear progression of intensity, with and shapes, concerns may remain that the effect has an ori-
the highest intensity in the midgap shim. We can also individu- gin in the surface geometry and conductivity. While preexisting
ally wrap each bead in thermal paper (Fig. 6 C and D) and record notions that the dimer is acting as a conducting short antenna
the same progression, confirming high field strength through the are difficult to overturn definitively, we conduct an experiment
entire gap (Fig. 6E). that appears to preclude a “surface-only”-based explanation: We
Much of the interest in nanoplasmonics lies in the ability repeat the thermal-paper experiments with dimers of small quail
to create highly confined or intricately structured electromag- eggs (minor axis diameter ≈ 24 mm). The eggs are individually
netic concentrations in subwavelength regions. Whether such wrapped in single-layer bands of thermal paper and placed in
hotspots are used for direct optical processing or surface pat- contact along their minor axis. After confirming that unmodi-
terning or are used to probe/excite volumes that are too small fied eggs display a hotspot at the point of contact, the eggs are
to access with typical diffractive approaches, the ability to con- evacuated through a hole at their apex and rebanded. Empty
fine light to particular subwavelength regions in exclusion of egg dimers do not reproduce the hotspot and, with longer irra-
other nearby regions is of high technological interest. The opti- diation, eventually display stochastic surface heating. When the
cal writing demonstrated by the grape dimer on the thermal eggs are refilled with water and rebanded, the dimer hotspot
paper in the air gap represents a demonstration of resolution is reproduced (SI Appendix, Fig. S3). Visually, of course, it is
better than λ0 /80. With controlled excitation—in terms of flu- impossible to discern whether the eggs are empty or filled with
ence, time, and polarization—considerably smaller features will water, but a clear identification can be made from how they inter-
be achievable. While millimeter-sized thermal writing is not in act with microwave radiation. Thus, we eliminate surface effects
itself a scientific advance, the demonstration of such control such as conductivity as significant contributors to the formation
with microwave radiation in an absorbing dielectric is unex- of plasma from grapes in the microwave oven.
pected. The identified usefulness of absorbing dielectrics in
this work broadens the range of potentially useful materials. Summary
More important, however, are the implications to nanophotonic Through a combination of videography, FEM simulations, IR
technologies at the visible and UV wavelength scales, were semi- thermal imaging, and thermal-paper sectioning, we have shown
transparent high-index natural dielectrics or metamaterials to be that the popular-science phenomenon of forming plasma with
discovered. grapes in a household microwave oven is explained by MDR
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