Singlet-triplet transition rate enhancement inside hyperbolic metamaterials

TY - JOUR

T1 - Singlet-triplet transition rate enhancement inside hyperbolic metamaterials

AU - Roth, Diane Joane

AU - Ginzburg, Pavel

AU - Hirvonen, Liisa Maija

AU - Levitt, James Alan

AU - Nasir, Mazhar Ejaz

AU - Suhling, Klaus

AU - Richards, David Robert

AU - Podolskiy, Viktor

AU - Zayats, Anatoly

PY - 2019/9/1

Y1 - 2019/9/1

N2 - The spontaneous emission process is known to be largely affected by the surrounding electromagnetic environment of emitters, which manifests itself via the Purcell enhancement of decay rates. This phenomenon has been extensively investigated in the case of dipolar transitions in quantum systems, commonly delivering fast decay rates in comparison to forbidden transitions such as high-order multipolar transitions or spin-forbidden, singlet-triplet phosphorescence processes. Here, we demonstrate a decay rate enhancement of almost 2800-fold considering a Ruthenium-based phosphorescent emitter located inside a plasmonic hyperbolic metamaterial. The standard electromagnetic local density of states description, typically employed for the Purcell factor analysis of dipolar transitions, is unable to account for a photoluminescence enhancement of this magnitude, which is attributed to the interplay between the local density of states and strongly inhomogeneous electromagnetic fields inside the metamaterial. The large available range of spontaneous emission lifetimes reported here enables application of phosphorescent emitters in novel fast and efficient light-emitting sources, beneficial for optical communications, quantum information processing, spectroscopy or bio-imaging.

AB - The spontaneous emission process is known to be largely affected by the surrounding electromagnetic environment of emitters, which manifests itself via the Purcell enhancement of decay rates. This phenomenon has been extensively investigated in the case of dipolar transitions in quantum systems, commonly delivering fast decay rates in comparison to forbidden transitions such as high-order multipolar transitions or spin-forbidden, singlet-triplet phosphorescence processes. Here, we demonstrate a decay rate enhancement of almost 2800-fold considering a Ruthenium-based phosphorescent emitter located inside a plasmonic hyperbolic metamaterial. The standard electromagnetic local density of states description, typically employed for the Purcell factor analysis of dipolar transitions, is unable to account for a photoluminescence enhancement of this magnitude, which is attributed to the interplay between the local density of states and strongly inhomogeneous electromagnetic fields inside the metamaterial. The large available range of spontaneous emission lifetimes reported here enables application of phosphorescent emitters in novel fast and efficient light-emitting sources, beneficial for optical communications, quantum information processing, spectroscopy or bio-imaging.

KW - hyperbolic metamaterials

KW - phosphorescence

KW - ruthenium complexes

KW - singlet–triplet transitions

KW - time-correlated single photon counting

U2 - 10.1002/lpor.201900101

DO - 10.1002/lpor.201900101

M3 - Article

SN - 1863-8899

VL - 13

JO - Laser and Photonics Reviews

JF - Laser and Photonics Reviews

IS - 9

M1 - 1900101

ER -