The defect states in atomically thin layers of transition metal dichalcogenides are promising candidates for single photon emission. However, the brightness of such quantum emission is often weak and is accompanied by undesirable effects such as spectral diffusion and strong background emission. By placing a monolayer directly on a rough gold substrate, here, we show a selective enhancement of sharp defect-bound exciton peaks, coupled with a suppressed spectral diffusion and strong quenching of background luminescence. By combining the experimental data with detailed electromagnetic simulations, we reveal that such selective luminescence enhancement originates from a combination of the Purcell effect and a wavelength dependent increment of the excitation electric field at the tips of tall rough features, coupled with a localized strain-induced exciton funneling effect. Notably, insertion of a thin hexagonal boron nitride sandwich layer between and the Au film results in a strong enhancement of the background luminescence, obscuring the sharp defect peaks. The findings demonstrate a simple strategy of using monolayer supported by a patterned metal film that offers a possibility of achieving quantum light sources with high purity, high brightness, and suppressed spectral diffusion.
REFERENCES
1.
D.
Browne
, S.
Bose
, F.
Mintert
, and M. S.
Kim
, “From quantum optics to quantum technologies
,” Prog. Quantum Electron.
54
, 2
–18
(2017
). 2.
A.
Beveratos
, A.
Villing
, J. P.
Poizat
, P.
Grangier
, R.
Brouri
, and T.
Gacoin
, “Single photon quantum cryptography
,” Phys. Rev. Lett.
89
(18
), 187901
(2002
). 3.
V.
Giovannetti
, S.
Lloyd
, and L.
MacCone
, “Advances in quantum metrology
,” Nat. Photonics
5
, 222
–229
(2011
). 4.
K. R.
Motes
, J. P.
Olson
, E. J.
Rabeaux
, J. P.
Dowling
, S. J.
Olson
, and P. P.
Rohde
, “Linear optical quantum metrology with single photons: Exploiting spontaneously generated entanglement to beat the shot-noise limit
,” Phys. Rev. Lett.
114
(17
), 170802
(2015
). 5.
I.
Aharonovich
, D.
Englund
, and M.
Toth
, “Solid-state single-photon emitters
,” Nat. Photonics
10
(10
), 631
–641
(2016
). 6.
M.
Koperski
, K.
Nogajewski
, A.
Arora
, J.
Marcus
, P.
Kossacki
, and M.
Potemski
, “Single photon emitters in exfoliated structures
,” Nat. Nanotechnol.
10
(6
), 503
–506
(2014
). 7.
A.
Srivastava
, M.
Sidler
, A. V.
Allain
, D. S.
Lembke
, A.
Kis
, and A.
Imamoglu
, “Optically active quantum dots in monolayer
,” Nat. Nanotechnol.
10
(6
), 491
–496
(2014
). 8.
C.
Chakraborty
, L.
Kinnischtzke
, K. M.
Goodfellow
, R.
Beams
, and A. N.
Vamivakas
, “Voltage-controlled quantum light from an atomically thin semiconductor
,” Nat. Nanotechnol.
10
(6
), 507
–511
(2015
). 9.
P.
Tonndorf
, R.
Schmidt
, R.
Schneider
, J.
Kern
, M.
Buscema
, G. A.
Steele
, A.
Castellanos-Gomez
, H. S. J.
van der Zant
, S.
Michaelis de Vasconcellos
, and R.
Bratschitsch
, “Single-photon emission from localized excitons in an atomically thin semiconductor
,” Optica
2
(4
), 347
(2015
). 10.
Y. M.
He
, G.
Clark
, J. R.
Schaibley
, Y.
He
, M. C.
Chen
, Y. J.
Wei
, X.
Ding
, Q.
Zhang
, W.
Yao
, X.
Xu
, C. Y.
Lu
, and J. W.
Pan
, “Single quantum emitters in monolayer semiconductors
,” Nat. Nanotechnol.
10
(6
), 497
–502
(2015
). 11.
C.
Palacios-Berraquero
, M.
Barbone
, D. M.
Kara
, X.
Chen
, I.
Goykhman
, D.
Yoon
, A. K.
Ott
, J.
Beitner
, K.
Watanabe
, T.
Taniguchi
, A. C.
Ferrari
, and M.
Atatüre
, “Atomically thin quantum light-emitting diodes
,” Nat. Commun.
7
, 12978
(2016
). 12.
G.
Clark
, J. R.
Schaibley
, J.
Ross
, T.
Taniguchi
, K.
Watanabe
, J. R.
Hendrickson
, S.
Mou
, W.
Yao
, and X.
Xu
, “Single defect light-emitting diode in a van der Waals heterostructure
,” Nano Lett.
16
(6
), 3944
–3948
(2016
). 13.
S.
Zhao
, J.
Lavie
, L.
Rondin
, L.
Orcin-Chaix
, C.
Diederichs
, P.
Roussignol
, Y.
Chassagneux
, C.
Voisin
, K.
Müllen
, A.
Narita
, S.
Campidelli
, and J. S.
Lauret
, “Single photon emission from graphene quantum dots at room temperature
,” Nat. Commun.
9
(1
), 3470
(2018
). 14.
T. T.
Tran
, K.
Bray
, M. J.
Ford
, M.
Toth
, and I.
Aharonovich
, “Quantum emission from hexagonal boron nitride monolayers
,” Nat. Nanotechnol.
11
(1
), 37
–41
(2016
). 15.
T. T.
Tran
, C.
Elbadawi
, D.
Totonjian
, C. J.
Lobo
, G.
Grosso
, H.
Moon
, D. R.
Englund
, M. J.
Ford
, I.
Aharonovich
, and M.
Toth
, “Robust multicolor single photon emission from point defects in hexagonal boron nitride
,” ACS Nano
10
(8
), 7331
–7338
(2016
). 16.
G.
Grosso
, H.
Moon
, B.
Lienhard
, S.
Ali
, D. K.
Efetov
, M. M.
Furchi
, P.
Jarillo-Herrero
, M. J.
Ford
, I.
Aharonovich
, and D.
Englund
, “Tunable and high-purity room temperature single-photon emission from atomic defects in hexagonal boron nitride
,” Nat. Commun.
8
(1
), 705
(2017
). 17.
R.
Bourrellier
, S.
Meuret
, A.
Tararan
, O.
Stéphan
, M.
Kociak
, L. H.
Tizei
, and A.
Zobelli
, “Bright UV single photon emission at point defects in h-BN
,” Nano Lett.
16
(7
), 4317
–4321
(2016
). 18.
J.
Ziegler
, R.
Klaiss
, A.
Blaikie
, D.
Miller
, V. R.
Horowitz
, and B. J.
Alemán
, “Deterministic quantum emitter formation in hexagonal boron nitride via controlled edge creation
,” Nano Lett.
19
(3
), 2121
–2127
(2019
). 19.
Y. J.
Zheng
, Y.
Chen
, Y. L.
Huang
, P. K.
Gogoi
, M.-Y.
Li
, L.-J.
Li
, P. E.
Trevisanutto
, Q.
Wang
, S. J.
Pennycook
, A. T. S.
Wee
, and S. Y.
Quek
, “Point defects and localized excitons in 2D
,” ACS Nano
13
(5
), 6050
–6059
(2019
). 20.
M.
Abdi
, J. P.
Chou
, A.
Gali
, and M. B.
Plenio
, “Color centers in hexagonal boron nitride monolayers: A group theory and ab initio analysis
,” ACS Photonics
5
(5
), 1967
–1976
(2018
). 21.
P.
Tonndorf
, O.
Del Pozo-Zamudio
, N.
Gruhler
, J.
Kern
, R.
Schmidt
, A. I.
Dmitriev
, A. P.
Bakhtinov
, A. I.
Tartakovskii
, W.
Pernice
, S.
Michaelis De Vasconcellos
, and R.
Bratschitsch
, “On-chip waveguide coupling of a layered semiconductor single-photon source
,” Nano Lett.
17
(9
), 5446
–5451
(2017
). 22.
M.
Blauth
, M.
Jürgensen
, G.
Vest
, O.
Hartwig
, M.
Prechtl
, J.
Cerne
, J. J.
Finley
, and M.
Kaniber
, “Coupling single photons from discrete quantum emitters in to lithographically defined plasmonic slot waveguides
,” Nano Lett.
18
(11
), 6812
–6819
(2018
). 23.
J.
Huang
, T. B.
Hoang
, and M. H.
Mikkelsen
, “Probing the origin of excitonic states in monolayer
,” Sci. Rep.
6
, 22414
(2016
). 24.
A.
Branny
, S.
Kumar
, R.
Proux
, and B. D.
Gerardot
, “Deterministic strain-induced arrays of quantum emitters in a two-dimensional semiconductor
,” Nat. Commun.
8
, 15053
(2017
). 25.
C.
Palacios-Berraquero
, D. M.
Kara
, A. R.
Montblanch
, M.
Barbone
, P.
Latawiec
, D.
Yoon
, A. K.
Ott
, M.
Loncar
, A. C.
Ferrari
, and M.
Atatüre
, “Large-scale quantum-emitter arrays in atomically thin semiconductors
,” Nat. Commun.
8
, 15093
(2017
). 26.
A. D.
Johnson
, F.
Cheng
, Y.
Tsai
, and C. K.
Shih
, “Giant enhancement of defect-bound exciton luminescence and suppression of band-edge luminescence in monolayer -Ag plasmonic hybrid structures
,” Nano Lett.
17
(7
), 4317
–4322
(2017
). 27.
L. N.
Tripathi
, O.
Iff
, S.
Betzold
, Ł.
Dusanowski
, M.
Emmerling
, K.
Moon
, Y. J.
Lee
, S. H.
Kwon
, S.
Höfling
, and C.
Schneider
, “Spontaneous emission enhancement in strain-induced monolayer-based quantum light sources on metallic surfaces
,” ACS Photonics
5
, 1919
–1926
(2018
). 28.
T.
Cai
, J. H.
Kim
, Z.
Yang
, S.
Dutta
, S.
Aghaeimeibodi
, and E.
Waks
, “Radiative enhancement of single quantum emitters in monolayers using site-controlled metallic nanopillars
,” ACS Photonics
5
, 3466
–3471
(2018
). 29.
Y.
Luo
, G. D.
Shepard
, J. V.
Ardelean
, D. A.
Rhodes
, B.
Kim
, K.
Barmak
, J. C.
Hone
, and S.
Strauf
, “Deterministic coupling of site-controlled quantum emitters in monolayer to plasmonic nanocavities
,” Nat. Nanotechnol.
13
, 1137
–1142
(2018
). 30.
Y.
Luo
, N.
Liu
, X.
Li
, J. C.
Hone
, and S.
Strauf
, “Single photon emission in up 160 K by quantum yield control
,” 2D Mater.
6
, 035017
(2019
). 31.
O.
Iff
, N.
Lundt
, S.
Betzold
, L. N.
Tripathi
, M.
Emmerling
, S.
Tongay
, Y. J.
Lee
, S.-H.
Kwon
, S.
Höfling
, and C.
Schneider
, “Deterministic coupling of quantum emitters in monolayers to plasmonic nanocavities
,” Opt. Express
26
, 25944
–25951
(2018
). 32.
A.
Castellanos-Gomez
, M.
Buscema
, R.
Molenaar
, V.
Singh
, L.
Janssen
, H. S.
Van Der Zant
, and G. A.
Steele
, “Deterministic transfer of two-dimensional materials by all-dry viscoelastic stamping
,” 2D Mater.
1
, 011002
(2014
). 33.
W.
Zhao
, Z.
Ghorannevis
, K. K.
Amara
, J. R.
Pang
, M.
Toh
, X.
Zhang
, C.
Kloc
, P. H.
Tan
, and G.
Eda
, “Lattice dynamics in mono- and few-layer sheets of and
,” Nanoscale
5
(20
), 9677
–9683
(2013
). 34.
M. M.
Ugeda
, A. J.
Bradley
, S. F.
Shi
, F. H.
Da Jornada
, Y.
Zhang
, D. Y.
Qiu
, W.
Ruan
, S. K.
Mo
, Z.
Hussain
, Z. X.
Shen
, F.
Wang
, S. G.
Louie
, and M. F.
Crommie
, “Giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor
,” Nat. Mater.
13
, 1091
–1095
(2014
). 35.
A.
Chernikov
, T. C.
Berkelbach
, H. M.
Hill
, A.
Rigosi
, Y.
Li
, O. B.
Aslan
, D. R.
Reichman
, M. S.
Hybertsen
, and T. F.
Heinz
, “Exciton binding energy and nonhydrogenic Rydberg series in monolayer
,” Phys. Rev. Lett.
113
(7
), 076802
(2014
). 36.
G.
Gupta
, S.
Kallatt
, and K.
Majumdar
, “Direct observation of giant binding energy modulation of exciton complexes in monolayer
,” Phys. Rev. B
96
(8
), 081403
(2017
). 37.
T.
Schmidt
, K.
Lischka
, and W.
Zulehner
, “Excitation-power dependence of the near-band-edge photoluminescence of semiconductors
,” Phys. Rev. B
45
(16
), 8989
–8994
(1992
). 38.
E. M.
Purcell
, H. C.
Torrey
, and R. V.
Pound
, “Resonance absorption by nuclear magnetic moments in a solid
,” Phys. Rev.
69
, 37
(1946
). 39.
R. R.
Chance
, A.
Prock
, and R.
Silbey
, “Lifetime of an emitting molecule near a partially reflecting surface
,” J. Chem. Phys.
60
(7
), 2744
–2748
(1974
). 40.
R. R.
Chance
, A.
Prock
, and R.
Silbey
, Molecular Fluorescence and Energy Transfer Near Interfaces
(John Wiley & Sons, Ltd.
, 2007
), pp. 1
–65
.41.
R. R.
Chance
, A.
Prock
, and R.
Silbey
, “Comments on the classical theory of energy transfer
,” J. Chem. Phys.
62
, 2245
–2253
(1975
). 42.
P. F.
Liao
and A.
Wokaun
, “Lightning rod effect in surface enhanced Raman scattering
,” J. Chem. Phys.
76
(1
), 751
–752
(1982
). 43.
P.
Bharadwaj
, B.
Deutsch
, and L.
Novotny
, “Optical antennas
,” Adv. Opt. Photonics
1
(3
), 438
(2009
). 44.
L.
Novotny
, B.
Hecht
, L.
Novotny
, and B.
Hecht
, “Propagation and focusing of optical fields,” in Principles of Nano-Optics (Cambridge University Press, Cambridge, 2012), pp. 45–85.45.
Z.
Wang
, Z.
Dong
, Y.
Gu
, Y. H.
Chang
, L.
Zhang
, L. J.
Li
, W.
Zhao
, G.
Eda
, W.
Zhang
, G.
Grinblat
, S. A.
Maier
, J. K.
Yang
, C. W.
Qiu
, and A. T.
Wee
, “Giant photoluminescence enhancement in tungsten-diselenide-gold plasmonic hybrid structures
,” Nat. Commun.
7
, 11283
(2016
). 46.
S.
Kumar
, A.
Kaczmarczyk
, and B. D.
Gerardot
, “Strain-induced spatial and spectral isolation of quantum emitters in mono- and bilayer
,” Nano Lett.
15
(11
), 7567
–7573
(2015
). 47.
L.
Besombes
, K.
Kheng
, L.
Marsal
, and H.
Mariette
, “Few-particle effects in single CdTe quantum dots
,” Phys. Rev. B
65
(12
), 121314
(2002
). 48.
M.
Holmes
, S.
Kako
, K.
Choi
, M.
Arita
, and Y.
Arakawa
, “Spectral diffusion and its influence on the emission linewidths of site-controlled GaN nanowire quantum dots
,” Phys. Rev. B
92
(11
), 115447
(2015
). 49.
J.
Seufert
, R.
Weigand
, G.
Bacher
, T.
Kümmell
, A.
Forchel
, K.
Leonardi
, and D.
Hommel
, “Spectral diffusion of the exciton transition in a single self-organized quantum dot
,” Appl. Phys. Lett.
76
(14
), 1872
–1874
(2000
). 50.
H. Y.
Jeong
, U. J.
Kim
, H.
Kim
, G. H.
Han
, H.
Lee
, M. S.
Kim
, Y.
Jin
, T. H.
Ly
, S. Y.
Lee
, Y. G.
Roh
, W. J.
Joo
, S. W.
Hwang
, Y.
Park
, and Y. H.
Lee
, “Optical gain in via coupling with nanostructured substrate: Fabry-Perot interference and plasmonic excitation
,” ACS Nano
10
, 8192
–8198
(2016
). 51.
H.
Xu
, “Enhanced light-matter interaction of a monolayer with a gold mirror layer
,” RSC Adv.
7
(37
), 23109
–23113
(2017
). 52.
J. T.
Liu
, T. B.
Wang
, X. J.
Li
, and N. H.
Liu
, “Enhanced absorption of monolayer with resonant back reflector
,” J. Appl. Phys.
115
, 193511
(2014
). © 2020 Author(s).
2020
Author(s)
You do not currently have access to this content.
