Sub-wavelength nanostructured systems with tunable electromagnetic properties, such as hyperbolic metamaterials (HMMs), provide a useful platform to tailor spontaneous emission processes. Here, we investigate a system comprising Eu3+(NO3)3·6H2O nanocrystals on an HMM structure featuring a hexagonal array of Ag nanowires in a porous Al2O3 matrix. The HMM-coupled Eu3+ ions exhibit up to a 2.4 fold increase in their decay rate, accompanied by an enhancement of the emission rate of the 5D0 → 7F2 transition. Using finite-difference time-domain modeling, we corroborate these observations with the increase in the photonic density of states seen by the Eu3+ ions in the proximity of the HMM. Our results indicate that HMMs can serve as a valuable tool to control the emission from weak transitions and, hence, hint at a route toward more practical applications of rare-earth ions in nanoscale optoelectronics and quantum devices.
References
1.
R.
Yano
, M.
Mitsunaga
, and N.
Uesugi
, “Ultralong optical dephasing time in Eu3+:Y2SiO5
,” Opt. Lett
16
, 1884
(1991
).2.
H.
De Riedmatten
, M.
Afzelius
, M. U.
Staudt
, C.
Simon
, and N. A.
Gisin
, “Solid-state light-matter interface at the single-photon level
,” Nature
456
, 773
(2008
).3.
C.
Clausen
, I.
Usmani
, F.
Bussiøres
, N.
Sangouard
, M.
Afzelius
, H.
de Riedmatten
, and N.
Gisin
, “Quantum storage of photonic entanglement in a crystal
,” Nature
469
, 508
–511
(2011
).4.
E.
Saglamyurek
, N.
Sinclair
, J.
Jin
, J. A.
Slater
, D.
Oblak
, F.
Bussières
, M.
George
, R.
Ricken
, W.
Sohler
, and W.
Tittel
, “Broadband waveguide quantum memory for entangled photons
,” Nature
469
, 512
–515
(2011
).5.
R. L.
Ahlefeldt
, M. J.
Pearce
, M. R.
Hush
, and M. J.
Sellars
, “Quantum processing with ensembles of rare-earth ions in a stoichiometric crystal
,” Phys. Rev. A
101
, 012309
(2020
).6.
M.
Zhong
, M. P.
Hedges
, R. L.
Ahlefeldt
, J. G.
Bartholomew
, S. E.
Beavan
, S. M.
Wittig
, J. J.
Longdell
, and M. J.
Sellars
, “Optically addressable nuclear spins in a solid with a six-hour coherence time
,” Nature
517
, 177
(2015
).7.
P.
Siyushev
, K.
Xia
, R.
Reuter
, M.
Jamali
, N.
Zhao
, N.
Yang
, C.
Duan
, N.
Kukharchyk
, A. D.
Wieck
, R.
Kolesov
, and J.
Wrachtrup
, “Coherent properties of single rare-earth spin qubits
,” Nat. Commun.
5
, 3895
(2014
).8.
D.
Serrano
, C.
Deshmukh
, S.
Liu
, A.
Tallaire
, A.
Ferrier
, H.
de Riedmatten
, and P.
Goldner
, “Coherent optical and spin spectroscopy of nanoscale Pr3+:Y2O3
,” Phys. Rev. B
100
, 144304
(2019
).9.
A. M.
Dibos
, M.
Raha
, C. M.
Phenicie
, and J. D.
Thompson
, “Atomic source of single photons in the telecom band
,” Phys. Rev. Lett.
120
(24
), 243601
(2018
).10.
B.
Casabone
, J.
Benedikter
, T.
Hummer
, F.
Oehl
, K.
de Oliveira Lima
, T. W.
Hansch
, A.
Ferrier
, P.
Goldner
, H.
de Riedmatten
, and D.
Hunger
, “Cavity-enhanced spectroscopy of a few-ion ensemble in Eu3+:Y2O3
,” New J. Phys.
20
, 095006
(2018
).11.
T.
Zhong
, J. M.
Kindem
, J. G.
Bartholomew
, J.
Rochman
, I.
Craiciu
, E.
Miyazono
, M.
Bettinelli
, E.
Cavalli
, V.
Verma
, S. W.
Nam
, F.
Marsili
, M. D.
Shaw
, A. D.
Beyer
, and A.
Faraon
, “Nanophotonic rare-earth quantum memory with optically controlled retrieval
,” Science
357
(6358
), 1392
(2017
).12.
P.
Huo
, S.
Zhang
, Y.
Liang
, Y.
Lu
, and T.
Xu
, “Hyperbolic metamaterials and metasurfaces: Fundamentals and applications
,” Adv. Opt. Mater.
7
, 1801616
(2019
).13.
H. N.
Krishnamoorthy
, Z.
Jacob
, E.
Narimanov
, I.
Kretzschmar
, and V. M.
Menon
, “Topological transitions in metamaterials
,” Science
336
(6078
), 205
–209
(2012
).14.
Z.
Jacob
, I. I.
Smolyaninov
, and E. E.
Narimanov
, “Broadband Purcell effect: Radiative decay engineering with metamaterials
,” Appl. Phys. Lett.
100
(18
), 181105
(2012
).15.
Z.
Jacob
, J.-Y.
Kim
, G. V.
Naik
, A.
Boltasseva
, E. E.
Narimanov
, and V. M.
Shalaev
, “Engineering photonic density of states using metamaterials
,” Appl. Phys. B
100
(1
), 215
(2010
).16.
D.
Lu
, L.
Ferrari
, J. J.
Kan
, E. E.
Fullerton
, and Z.
Liu
, “Optimization of nanopatterned multilayer hyperbolic metamaterials for spontaneous light emission enhancement
,” Phys. Status Solidi A
215
(24
), 1800263
(2018
).17.
C.
Indukuri
, R. K.
Yadav
, and J. K.
Basu
, “Broadband room temperature strong coupling between quantum dots and metamaterials
,” Nanoscale
9
(32
), 11418
(2017
).18.
M. D.
Chambers
, P. A.
Rousseve
, and D. R.
Clarke
, “Decay pathway and high-temperature luminescence of Eu3+ in Ca2Gd8Si6O26
,” J. Lumin.
129
, 263
(2009
).19.
A. K.
Singh
, K. P.
O'Donnell
, P. R.
Edwards
, D.
Cameron
, K.
Lorenz
, M. J.
Kappers
, M.
Bockowski
, M.
Yamaga
, and R.
Prakash
, “Luminescence of Eu3+ in GaN(Mg, Eu): Transitions from the 5D1 level
,” Appl. Phys. Lett.
111
, 241105
(2017
).20.
F. T.
Rabouw
, P.
Tim Prins
, and D. J.
Norris
, “Europium-doped NaYF4 nanocrystals as probes for the electric and magnetic local density of optical states throughout the visible spectral range
,” Nano Lett.
16
, 7254
(2016
).21.
K.
Binnemans
, “Interpretation of europium (III) spectra
,” Coord. Chem. Rev.
295
, 1
(2015
).22.
E.
Moret
, J. G.
Bunzli
, and K. J.
Schenk
, “Structural and luminescence study of europium and terbium nitrate hexahydrates
,” Inorg. Chim. Acta
178
, 83
(1990
).23.
P.
Shekhar
, J.
Atkinson
, and Z.
Jacob
, “Hyperbolic metamaterials: Fundamentals and applications
,” Nano Convergence
1
(1
), 14
(2014
).24.
T.
Tumkur
, G.
Zhu
, P.
Black
, Y. A.
Barnakov
, C. E.
Bonner
, and M. A.
Noginov
, “Control of spontaneous emission in a volume of functionalized hyperbolic metamaterial
,” Appl. Phys. Lett.
99
(15
), 151115
(2011
).25.
C.
Cortes
, W.
Newman
, S.
Molesky
, and Z.
Jacob
, “Quantum nanophotonics using hyperbolic metamaterials
,” J. Optics
14
, 063001
(2012
).26.
A. N.
Poddubny
, P. A.
Belov
, P.
Ginzburg
, A. V.
Zayats
, and Y. S.
Kivshar
, “Microscopic model of Purcell enhancement in hyperbolic metamaterials
,” Phys. Rev. B
86
(3
), 035148
(2012
).27.
A. N.
Poddubny
, P. A.
Belov
, and Y. S.
Kivshar
, “Spontaneous radiation of a finite-size dipole emitter in hyperbolic media
,” Phys. Rev. A
84
(2
), 023807
(2011
).© 2021 Author(s).
2021
Author(s)
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