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Control of Physical and Chemical Processes with Nonlocal Metal− Dielectric Environments Vanessa N

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Control of Physical and Chemical Processes with Nonlocal Metal− Dielectric Environments Vanessa N Perspective Cite This: ACS Photonics 2019, 6, 3039−3056 pubs.acs.org/journal/apchd5 Control of Physical and Chemical Processes with Nonlocal Metal− Dielectric Environments Vanessa N. Peters,‡,# Srujana Prayakarao,# Samantha R. Koutsares, Carl E. Bonner, and Mikhail A. Noginov* Center for Materials Research, Norfolk State University, Norfolk, Virginia 23504, United States ABSTRACT: In this Perspective, we make the case that (meta) material platforms that were originally designed to control the propagation of light can affect scores of physical and chemical phenomena, which are often thought to lie outside of the traditional electrodynamics domain. We show that nonlocal metal-dielectric environments, which can be as simple as metal−dielectric interfaces, can control spontaneous and stimulated emission, Förster energy transfer, wetting contact angle, and rates of chemical reactions. The affected phenomena can occur in both strong and weak coupling regimes and the large coupling strength seems to enhance the effects of nonlocal environments. This intriguing field of study has experienced a rapid growth over the past decade and many exciting discoveries and applications are expected in the years to come. KEYWORDS: metamaterials, plasmonics, nonlocal metal−dielectric environment, weak and strong coupling regimes anipulation of light with dielectric media and metallic Hyperbolic Metamaterials, (ii) Control of Energy Transfer M surfaces is not limited to traditional large-scale optics, with Nonlocal Metal−Dielectric Environments, (iii) Long- like eyeglass lenses and looking glasses. Thus, metal−dielectric Range Wetting Transparency on Top of Layered Metal- interfaces and metallic nanostructures support a variety of Dielectric Substrates, and (iv) Control of Chemical Reactions propagating and localized surface plasmons (SPs): resonant in Weak and Strong Coupling Regimes. These phenomena are oscillations of free electron density coupled to electromagnetic unified by underlying concept of controlling material’s waves. Surface plasmons can confine and strengthen electric polarizability and dipole−dipole interactions with inhomoge- and magnetic fields oscillating at optical frequencies and neous metal/dielectric environments. The major results and enhance spontaneous emission and Raman scattering.1,2 On conclusions are summarized in section III (Summary). the other hand, the last two decades witnessed rapid Fundamental Concepts. Control of Spontaneous development of metamaterials: engineered materials comprised Emission with Electromagnetic Environments. Spontaneous of subwavelength inclusions with rationally designed shapes, emission is one of the most fundamental phenomena in physics 27 Downloaded via NORFOLK STATE UNIV on January 3, 2020 at 23:31:00 (UTC). sizes, compositions, and mutual orientations (commonly) and optics. Following the Fermi’s Golden Rule, its rate is embedded in a dielectric matrix.3−5 Nearly fantastic theoretical proportional to the density of final states−the number of predictions and experimental demonstrations of metamaterials modes per frequency interval dω and per volume (known as See https://pubs.acs.org/sharingguidelines for options on how to legitimately share published articles. range from a negative index of refraction to an invisibility Photonic Density of States, PDOS, or Local Density of States, 28 optical cloaking. Metamaterials can govern the rate,6−14 the LDOS), which is given by spectrum,15 and the directionality10,16 of spontaneous 23 23 emission. More recently, it has been shown that metamaterials pd()ωω= ω n /( π cd ) ω (1) and, more generally, a variety of nanoscopic metal−dielectric Here ω is the angular frequency, n is the refractive index, and c structures can control scores of physical phenomena, including 29 Förster energy transfer,17−19 van der Waals forces,20,21 and is the speed of light. It has been predicted by Purcell that the chemical reactions,22−26 which lie outside of a traditional rate of spontaneous emission, which otherwise is low, can be electrodynamics domain. The phenomena above are of increased by orders of magnitude if the emitter is placed in a particular interest to the present discussion. cavity with a large quality factor Q. The corresponding This Perspective is organized as follows. In section I of the spontaneous emission enhancement factor (known as the paper, following the introductory paragraph, we briefly review Purcell factor) is equal to several fundamental concepts, including spontaneous emission, energy transfer, light−matter interactions (in weak and strong Received: May 21, 2019 coupling regimes), van der Waals forces, and rates of chemical Revised: October 26, 2019 reactions. These processes are discussed in more detail in Accepted: November 12, 2019 section II, which includes (i) Control of Emission with Published: December 2, 2019 © 2019 American Chemical Society 3039 DOI: 10.1021/acsphotonics.9b00734 ACS Photonics 2019, 6, 3039−3056 ACS Photonics Perspective 32 f = 3/4QλπV (2) where λ is the wavelength and V is the volume of the cavity.29 Three decades later, Drexhage et al. have demonstrated30,31 that the spontaneous emission rate of an emitter (in the optical range) varies with the distance to a metallic mirror, following nodes and antinodes of a standing wave formed by a superposition of the incident and reflected light waves and the corresponding minima and maxima in the spatial Figure 2. Hyperboloid isofrequency dispersion surfaces for (a) εx = εy ε ε ε ε distribution of PDOS, Figure 1. Photonic density of states > 0 and z < 0 and (b) x = y < 0 and z > 0). Adopted with permission from ref 47. Copyright 2014 Springer. Förster Energy Transfer. Excited molecule can make a transition to a ground state by emitting a photon, as in the case of spontaneous emission.28 Among many other ways of giving away its energy (e.g., to molecular vibrations,49 phonons,50 plasmons,51,52 polaritons,53 etc.), it can transfer its excitation to a closely situated ground state molecule:54 the process of particular interest in this study, Figure 3. In general, if two Figure 3. Schematic of irreversible Förster donor−acceptor energy transfer showing absorption of light in donor, combination of radiative and nonradiative relaxation processes in the donor (WD), 3+ Figure 1. Fluorescence decay time of Eu in front of a silver mirror; donor−acceptor energy transfer (γDA), and the relaxation processes in solid line, calculation done at the quantum yield η∞ = 0.7; circles, the acceptor (WA). experiment. Adopted with permission from ref 30. Copyright 1970 Elsevier. molecules are coupled in some way (e.g., via Coulomb interactions), this can result in an energy transfer between and the rates of spontaneous emission can be strongly 54 modified by high-Q resonators,32,33 photonic band crys- them. This energy transfer can be reversible (oscillatory), tals,34−37 plasmonic structures,38−40 and other photonic when the coupling strength Ω is much larger than (i) the decay environments. However, in many cases, the singularity of rates (inverse longitudinal decay times) of both donor and ff acceptor (1/τd and 1/τa) and (ii) the rate of the phase PDOS is spectrally narrow, which limits its e ect on a broad- 54 band spontaneous emission. correlation decay (inverse transverse relaxation time, 1/T2 ). In the latter case, the splitting of the energy eigenvalues of the The Renaissance in control of spontaneous emission with 54 engineered photonic environments followed emergence of interacting molecules is expected (as discussed in section II). Alternatively, the energy transfer can be irreversible, when T metamaterials with hyperbolic dispersion−artificial nanostruc- 2 τ τ 54 “ ” tured materials, whose dielectric permittivities in orthogonal ≪ d ≪ a. Following ref 54, the term energy transfer directions have opposite signs41−47 resulting in hyperbolic should be reserved only for those cases, which involve isofrequency dispersion curves for extraordinary waves and substantial irreversibility and a relaxation process (to the broadband singularity of PDOS.10,12,48 ground state). However, this terminology is not uniformly The isofrequency dispersion surface, for extraordinary waves, followed by all authors. in a (loss-less) uniaxial hyperbolic metamaterial, is given by Förster developed the theory of energy transfer for molecules having broad spectra in a condensed medium.54−57 22 2 2 The theory is based on the perturbation model in adiabatic kkxy+ kz ω += approximation. The theory assumes that the energy transfer εεz x c (3) occurs owing to a dipole−dipole interaction between where εx = εy and εz are the dielectric permittivities in x, y, and molecules, which is so weak that it does not change the ji zy energy eigenvalues of the molecules. Förster has shown that, z directions, and kx,y,jz arez the wavevector components. The shapes of the dispersionk surfaces{ for (εx = εy > 0 and εz < 0) under such conditions, the probability of the energy transfer W and (εx = εy < 0 and εz > 0) are depicted in Figure 2a and b, can be expressed in terms of the integral of the overlap of the respectively. luminescence and absorption spectra of interacting molecules: Experimentally, enhancement of the rate of spontaneous 6 emission with hyperbolic metamaterials was first demonstrated 3 2 R0 W = χ in ref 6, followed by scores of related works exploring different 6 2 τ0R (4) morphologies and emitters.7−14 These studies are discussed in section II. where 3040 DOI: 10.1021/acsphotonics.9b00734 ACS Photonics 2019, 6, 3039−3056 ACS Photonics Perspective fl Figure 4. (a) Interaction of uctuating dipole p1 and induced dipole p2. (b) Interaction of two slabs, 1 and 2, when the gap between the slabs is filled with the medium M.20 (c) Same as in (a), in vicinity of the metallic mirror that produces image charges. (d) Same as in (b), in the presence of slab 3.21 Adopted with permission from ref 21. Copyright 2016 Nature. fl 6 3 η0 dν̅ In Figure 4a, uctuating the dipole in atom 1 induces the R0 = 5 44F()()νσν̅ ̅ 2(2π ) n ∫ ν (5) dipole in atom 2, and these two dipoles attract each other.
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