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The concentration of light on extreme-subwavelength scales provided by plasmons in conducting media enables strong extrinsic light-matter interactions required for optical sensing [1], quantum photonic [2], and nonlinear optical [3] technologies. While significant research has been devoted to the interaction of atoms and molecules with the enhanced linear optical fields generated by plasmonic nanostructures and their ability to enhance spontaneous emission from quantum emitters, light-matter coupling of the near fields produced by nonlinear optical processes in hybrid systems remains relatively unexplored [4]. Here we propose to utilize near fields generated by the plasmon-assisted nonlinear optical response of nanostructured graphene to resonantly couple the 2D layer with proximal quantum emitters operating in the near infrared [5]. Although graphene plasmon resonances are typically limited to the infrared and terahertz frequencies, below those of long-lived optical excitations in robust solid-state quantum light sources and many biologically interesting molecules, we show that electrically tuning the third harmonic of a localized plasmon in a graphene nanoisland to resonate with an electronic excitation in a few-level atomic system can enable graphene plasmon-mediated energy transfer and coherent control of quantum states. In the present scheme, emitter and plasmon resonances are nondegenerate, circumventing strong enhancement of spontaneous emission that arises in the linear coupling scheme. The combination of an intrinsically large nonlinear response and intense in-plane electric field enhancement associated with localized electrically-tunable plasmons renders graphene an ideal material platform for nonlinear near field coupling [5], although this principle could be straightforwardly applied to other plasmonic materials, opening a wide range of applications in sensing and quantum nano-optics.
[1] J. N. Anker, W. P. Hall, O. Lyandres, N. C. Shah, J. Zhao, and R. P. Van Duyne, Nat. Mater. 7, 442 (2008).
[2] M. S. Tame, K. R. McEnery, Ş. K. Özdemir, J. Lee, S. A. Maier, and M. S. Kim, Nat. Phys. 9, 329 (2013).
[3] M. Kauranen and A. V. Zayats, Nat. Photon. 6, 737 (2012).
[4] B. Metzger, M. Hentschel, and H. Giessen, Nano Lett. 17, 1931 (2017).
[5] J. D. Cox and F. J. García de Abajo, Phys. Rev. Lett. 121, 257403 (2018).
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