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Functional Nanostructured Materials (including low-D carbon)
Circular Dichroism Control of Tungsten Diselenide (WSe2) Atomic Layers with Plasmonic Meta-Molecules Hsiang-Ting Lin, Chiao-Yun Chang, Pi Ju Cheng, Ming-Yang Li, Chia-Chin Cheng, Shu-Wei Chang, lance L. J. Li, Chih Wei Chu, Pei-Kuen Wei, and Min-Hsiung Shih ACS Appl. Mater. Interfaces, Just Accepted Manuscript • DOI: 10.1021/acsami.8b01472 • Publication Date (Web): 16 Apr 2018 Downloaded from http://pubs.acs.org on April 16, 2018
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ACS Applied Materials & Interfaces
Circular Dichroism Control of Tungsten Diselenide (WSe2) Atomic Layers with Plasmonic Meta-Molecules Hsiang-Ting Lin1,2, Chiao-Yun Chang1, Pi-Ju Cheng1, Ming-Yang Li1,3, Chia-Chin Cheng3, Shu-Wei Chang1,2, Lance L. J. Li,3 Chih-Wei Chu1, Pei-Kuen Wei1, and Min-Hsiung Shih1,2,4* 1
Research Center for Applied Sciences (RCAS), Academia Sinica, Taipei 11529, Taiwan
2
Department of Photonics and Institute of Electro-Optical Engineering, National Chiao Tung
University (NCTU), Hsinchu 30010, Taiwan 3
Physical Science and Engineering Division, King Abdullah University of Science and Technology (KAUST), Thuwal, 23955-6900, Kingdom of Saudi Arabia
4
Department of Photonics, National Sun Yat-sen University (NSYSU), Kaohsiung 80424, Taiwan
*E-mail address:
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Abstract Controlling circularly polarized states of light is critical to the development of functional devices for key and emerging applications such as display technology and quantum communication, and the compact circular polarization-tunable photon source is one critical element to realize the applications in the chip-scale integrated system. The atomic layers of transition metal dichalcogenide (TMDC) exhibit intrinsic circularly polarized emissions and are potential chiroptical materials for ultrathin circularly polarized photon sources. In this work, we demonstrated circularly polarized photon sources of TMDC with device thicknesses approximately 50 nm. Circularly polarized photoluminescence from atomic layers of tungsten diselenide (WSe2) was precisely controlled with chiral meta-molecules, and the optical chirality of WSe2 was enhanced more than 4 times by integrating with the meta-molecules. Both the enhanced and reversed circular dichroisms had been achieved. Through integrations of the novel gain material and plasmonic structure which are both low dimensional, a compact device capable of efficiently manipulating emissions of circularly polarized photon was realized. These ultrathin devices are suitable for important applications such as the optical information technology and chip-scale bio-sensing.
KEYWORDS: Two-dimensional materials, Transition metal dichalcogenides (TMDCs), WSe2, Surface plasmon, Metasurface, Chirality, Circular Dichroism
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ACS Applied Materials & Interfaces
INTRODUCTION Controlling circularly polarized states of light is critical to their usages in various areas including display technology,1,2 quantum-based optical information processing, and communication.3–5 The distinct behaviors in the emission and absorption of two circularly polarized lights are known as the circular dichroism (CD). The phenomena take place as the light transmits through specific media which respond differently to the field components in two circular polarization states, namely left-hand circularly polarized (LCP) and right-hand circularly polarized (RCP) states. In fact, the occurrences of such events usually indicate the optical chirality of media. Since many biological molecules and organic compounds exhibit CD, the circularly polarized radiation plays an increasingly important role not only in optics but also in the fields of chemistry, biomedicine, and elementary particle physics.6–11 Recently, it has been observed that atomic layers of transition metal dichalcogenides (TMDCs)12–41 exhibit unusual absorption and emission of circularly polarized lights.12,13 TMDCs are layered semiconductors formed by transition metal atoms (M) and halogen atoms (X) with a typical chemical formula of MX2. The thickness of each layer in TMDCs is less than 1 nm. In monolayer TMDCs, the M and X atoms are separately arranged in the respective hexagonal lattice structures. Their bandgaps around the Fermi level are direct and range in 1 to 2 eV.14–18 The direct bandgaps are located at the degenerate but inequivalent K points (also known as K valleys) in the Brillouin zone. Because their crystal structure comprises two types of atoms, the inversion symmetry is broken in monolayer TMDCs, and this makes the electron-hole pairs (excitons) in the two K valleys (denoted as K1 and K2) present in different states of electric polarizations (σ 3 ACS Paragon Plus Environment
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and σ ). As the circularly polarized light excites the monolayer TMDCs, the RCP and
LCP fields couple only to the σ and σ state transitions in bands at the K1 and K2 valleys, respectively, due to the angular-momentum conservation. Under such
circumstances, circularly dichroic photoluminescence (PL) could be triggered.19 Accessing different valley states through circularly polarized lights has been experimentally demonstrated with several TMDCs including molybdenum disulfide (MoS2),19–21 molybdenum diselenide (MoSe2),22 tungsten sulfide (WS2),23 and tungsten diselenide (WSe2).24–27 The phenomena of CD indicate that TMDCs are promising optical materials with a controllable optical chirality and may enable the generation of circularly polarized photons. However, the operation temperature and excitation photon energy need to be carefully controlled in order to induce observable CD in monolayer TMDCs. It had been shown that the CD of PL in monolayer MoS2 quickly diminished at a temperature more than 90 K due to the elevated intervalley scattering of carriers at the higher temperatures.19 Moreover, even in the presence of the selective coupling between circularly polarized photons and electron-hole pairs near K points, as the excitation photon energy increases and gets much higher than the direct bandgap, the degree of circular polarization of the emitted radiation would drop rapidly or simply vanish. Such trends had been observed in MoS2,19,21 MoSe2,22 and WSe2.27 To counteract these behaviors, several researchers have proposed various approaches to maintain the CD of PL in TMDCs. Such methods include the applications of an in-plane electric field,27,28 an out-of-plane magnetic field,29–33 and a localized magnetic field.34
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ACS Applied Materials & Interfaces
One means of controlling circularly polarized light is to apply a chiral plasmonic metasurface. Owing to the confinement of localized surface plasmon resonance (LSPR) modes in metallic nanostructures, plasmonic metasurfaces with chiral building blocks exhibit a strong optical chirality. The optical chirality has been achieved in various plasmonic metasurfaces including helical structures,42–43 coupled achiral38 or chiral plasmonic elements,42,45-46 , Tamm plasmonic structure47 and pseudo-chirality effects.48,49 In this way, a plasmonic chiral metasurface with at least one dimension in the nanoscale can be utilized to manipulate the degree of circular polarization of the luminescence. Combining TMDCs with plasmonic metasurfaces is beneficial for several reasons. First, as the plasmonic metasurface is directly fabricated on a monolayer TMDC, tightly confined LSPR modes of the meta-surface strongly interact with the carriers within the thin sheet material. Second, the geometry-dependent LSPR modes of plasmonic nanostructures in metasurfaces provide the wavelength tunability for emission windows of different materials. Third, the ultrathin atomic layer of TMDCs ( ,
(#) + =;2( ; >
#
#
(#)
= |&|+ ?|6( (%(#) )|+ ,
. = R, L,
(#)
+ |6( (%(#) )|+ , @, (5)
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(#) +
(#)
where ( ≡ =;2( ; > are the RCP and LCP intensities from dipole . In Eq. (5), the (#)
roles played by fractions ,
(#)
and ,
appear as the information of valleys while square
modului |6(( A%(#) B|+ of the matrix elments characterize the polarization effect of chiral (::)
MMs. In this way, the circular dichroism CD
of the CP-PL in the presence of the
MM can then be expressed as a weighted sum of the local counterpart (#)
(#)
(#)
(#)
(#)
(#)
CD (%(#) , , , , ) ≡ ( − )/( + ): (::) CD
=
(::)
(::)
(::)
− +
(::)
=