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Title: Efficient Nonlinear Metasurface Based on Nonplanar Plasmonic Nanocavities

 [1]; ORCiD logo [2]; ORCiD logo [1]
  1. Department of Physics, Emory University, Atlanta, Georgia 30322, United States
  2. Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439, United States
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Argonne-Northwestern Solar Energy Research Center (ANSER)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
DOE Contract Number:
Resource Type:
Journal Article
Resource Relation:
Journal Name: ACS Photonics; Journal Volume: 4; Journal Issue: 5; Related Information: ANSER partners with Northwestern University (lead); Argonne National Laboratory; University of Chicago; University of Illinois, Urbana-Champaign; Yale University
Country of Publication:
United States
catalysis (homogeneous), catalysis (heterogeneous), solar (photovoltaic), solar (fuels), photosynthesis (natural and artificial), bio-inspired, hydrogen and fuel cells, electrodes - solar, defects, charge transport, spin dynamics, membrane, materials and chemistry by design, optics, synthesis (novel materials), synthesis (self-assembly)

Citation Formats

Wang, Feng, Martinson, Alex B. F., and Harutyunyan, Hayk. Efficient Nonlinear Metasurface Based on Nonplanar Plasmonic Nanocavities. United States: N. p., 2017. Web. doi:10.1021/acsphotonics.7b00094.
Wang, Feng, Martinson, Alex B. F., & Harutyunyan, Hayk. Efficient Nonlinear Metasurface Based on Nonplanar Plasmonic Nanocavities. United States. doi:10.1021/acsphotonics.7b00094.
Wang, Feng, Martinson, Alex B. F., and Harutyunyan, Hayk. Tue . "Efficient Nonlinear Metasurface Based on Nonplanar Plasmonic Nanocavities". United States. doi:10.1021/acsphotonics.7b00094.
title = {Efficient Nonlinear Metasurface Based on Nonplanar Plasmonic Nanocavities},
author = {Wang, Feng and Martinson, Alex B. F. and Harutyunyan, Hayk},
abstractNote = {},
doi = {10.1021/acsphotonics.7b00094},
journal = {ACS Photonics},
number = 5,
volume = 4,
place = {United States},
year = {Tue Apr 11 00:00:00 EDT 2017},
month = {Tue Apr 11 00:00:00 EDT 2017}
  • Since their discovery in the 1960s, nonlinear optical effects have revolutionized optical technologies and laser industry. Development of efficient nanoscale nonlinear sources will pave the way for new applications in photonic circuitry, quantum optics and biosensing. However, nonlinear signal generation at dimensions smaller than the wavelength of light brings new challenges. The fundamental difficulty of designing an efficient nonlinear source is that some of the contributing factors involved in nonlinear wave-mixing at the nanoscale are often hard to satisfy simultaneously. Here, we overcome these limitations by developing a new type of nonplanar plasmonic metasurfaces, which can greatly enhance the secondmore » harmonic generation (SHG) at visible frequencies and achieve conversion efficiency of ~6 × 10 -5 at a peak pump intensity of ~0.5 GW/cm 2. This is 4-5 orders of magnitude larger than the efficiencies observed for nonlinear thin films and doubly resonant plasmonic antennas. The proposed metasurface consists of an array of metal-dielectric-metal (MDM) nanocavities formed by conformally cross-linked nanowires separated by an ultrathin nonlinear material layer. The nonplanar MDM geometry minimizes the destructive interference of nonlinear emission into the far-field, provides strongly enhanced independently tunable resonances both for fundamental and harmonic frequencies, a good mutual overlap of the modes and a strong interaction with the nonlinear spacer. Lastly, our findings enable the development of efficient nanoscale single photon sources, integrated frequency converters, and other nonlinear devices.« less
  • Coherent superposition of light from subwavelength sources is an attractive prospect for the manipulation of the direction, shape and polarization of optical beams. This phenomenon constitutes the basis of phased arrays, commonly used at microwave and radio frequencies. Here we propose a new concept for phased-array sources at infrared frequencies based on metamaterial nanocavities coupled to a highly nonlinear semiconductor heterostructure. Optical pumping of the nanocavity induces a localized, phase-locked, nonlinear resonant polarization that acts as a source feed for a higher-order resonance of the nanocavity. Varying the nanocavity design enables the production of beams with arbitrary shape and polarization.more » As an example, we demonstrate two second harmonic phased-array sources that perform two optical functions at the second harmonic wavelength (~5 μm): a beam splitter and a polarizing beam splitter. As a result, proper design of the nanocavity and nonlinear heterostructure will enable such phased arrays to span most of the infrared spectrum.« less
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  • Single-walled carbon nanotubes (SWCNTs) are promising absorbers and emitters to enable novel photonic applications and devices but are also known to suffer from low optical quantum yields. Here we demonstrate SWCNT excitons coupled to plasmonic nanocavity arrays reaching deeply into the Purcell regime with Purcell factors (F P) up to F P = 180 (average F P = 57), Purcell-enhanced quantum yields of 62% (average 42%), and a photon emission rate of 15 MHz into the first lens. The cavity coupling is quasi-deterministic since the photophysical properties of every SWCNT are enhanced by at least one order of magnitude. Furthermore,more » the measured ultra-narrow exciton linewidth (18 ueV) reaches the radiative lifetime limit, which is promising towards generation of transform-limited single photons. Furthermore, to demonstrate utility beyond quantum light sources we show that nanocavity-coupled SWCNTs perform as single-molecule thermometers detecting plasmonically induced heat at cryogenic temperatures in a unique interplay of excitons, phonons, and plasmons at the nanoscale.« less