Polaritonic Probe of an Emergent 2D Dipole Interface

Daniel J. Rizzo; Jin Zhang; Bjarke S. Jessen; Francesco L. Ruta; Matthew Cothrine; Jiaqiang Yan; David G. Mandrus; Stephen E. Nagler; Takashi Taniguchi; Kenji Watanabe; Michael M. Fogler; Abhay N. Pasupathy; Andrew J. Millis; Angel Rubio; James C. Hone; Cory R. Dean; D. N. Basov

doi:10.1021/acs.nanolett.3c01611

Polaritonic Probe of an Emergent 2D Dipole Interface

Daniel J. Rizzo, Jin Zhang, Bjarke S. Jessen, Francesco L. Ruta, Matthew Cothrine, Jiaqiang Yan, David G. Mandrus, Stephen E. Nagler, Takashi Taniguchi, Kenji Watanabe, Michael M. Fogler, Abhay N. Pasupathy, Andrew J. Millis, Angel Rubio, James C. Hone, Cory R. Dean, D. N. Basov

Correlated Electron Materials

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4 Scopus citations

Abstract

The use of work-function-mediated charge transfer has recently emerged as a reliable route toward nanoscale electrostatic control of individual atomic layers. Using α-RuCl₃ as a 2D electron acceptor, we are able to induce emergent nano-optical behavior in hexagonal boron nitride (hBN) that arises due to interlayer charge polarization. Using scattering-type scanning near-field optical microscopy (s-SNOM), we find that a thin layer of α-RuCl₃ adjacent to an hBN slab reduces the propagation length of hBN phonon polaritons (PhPs) in significant excess of what can be attributed to intrinsic optical losses. Concomitant nano-optical spectroscopy experiments reveal a novel resonance that aligns energetically with the region of excess PhP losses. These experimental observations are elucidated by first-principles density-functional theory and near-field model calculations, which show that the formation of a large interfacial dipole suppresses out-of-plane PhP propagation. Our results demonstrate the potential utility of charge-transfer heterostructures for tailoring optoelectronic properties of 2D insulators.

Original language	English
Pages (from-to)	8426-8435
Number of pages	10
Journal	Nano Letters
Volume	23
Issue number	18
DOIs	https://doi.org/10.1021/acs.nanolett.3c01611
State	Published - Sep 27 2023

Funding

Research at Columbia University was supported as part of the Energy Frontier Research Center on Programmable Quantum Materials funded by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), under award no. DE-SC0019443. J.Z. and A.R. were supported by the Cluster of Excellence “Advanced Imaging of Matter” (AIM) EXC 2056-390715994, funding by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under RTG 2247, Grupos Consolidados (IT1249-19) and SFB925 “Light induced dynamics and control of correlated quantum systems”. J.Z. and A.R. would like to acknowledge Nicolas Tancogne-Dejean and Lede Xian for fruitful discussions and also acknowledge support by the Max Planck Institute─New York City Center for Non-Equilibrium Quantum Phenomena. The Flatiron Institute is a division of the Simons Foundation. J.Z. acknowledges funding received from the European Union Horizon 2020 research and innovation program under Marie Sklodowska-Curie Grant Agreement 886291 (PeSD-NeSL). K.W. and T.T. acknowledge support from the JSPS KAKENHI (Grant Numbers 20H00354, 21H05233, and 23H02052) and World Premier International Research Center Initiative (WPI), MEXT, Japan. J.Q.Y. was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. S.E.N. received support from the Quantum Science Center (QSC), a National Quantum Information Science Research Center of the U.S. Department of Energy (DOE). D.G.M. acknowledges support from the Gordon and Betty Moore Foundation’s EPiQS Initiative, Grant GBMF906.

Keywords

charge transfer
heterostructures
phonon polaritons
scanning near-field optical microscopy (SNOM)
two-dimensional (2D) materials
α-RuCl

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10.1021/acs.nanolett.3c01611

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Rizzo, D. J., Zhang, J., Jessen, B. S., Ruta, F. L., Cothrine, M., Yan, J., Mandrus, D. G., Nagler, S. E., Taniguchi, T., Watanabe, K., Fogler, M. M., Pasupathy, A. N., Millis, A. J., Rubio, A., Hone, J. C., Dean, C. R., & Basov, D. N. (2023). Polaritonic Probe of an Emergent 2D Dipole Interface. Nano Letters, 23(18), 8426-8435. https://doi.org/10.1021/acs.nanolett.3c01611

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abstract = "The use of work-function-mediated charge transfer has recently emerged as a reliable route toward nanoscale electrostatic control of individual atomic layers. Using α-RuCl3 as a 2D electron acceptor, we are able to induce emergent nano-optical behavior in hexagonal boron nitride (hBN) that arises due to interlayer charge polarization. Using scattering-type scanning near-field optical microscopy (s-SNOM), we find that a thin layer of α-RuCl3 adjacent to an hBN slab reduces the propagation length of hBN phonon polaritons (PhPs) in significant excess of what can be attributed to intrinsic optical losses. Concomitant nano-optical spectroscopy experiments reveal a novel resonance that aligns energetically with the region of excess PhP losses. These experimental observations are elucidated by first-principles density-functional theory and near-field model calculations, which show that the formation of a large interfacial dipole suppresses out-of-plane PhP propagation. Our results demonstrate the potential utility of charge-transfer heterostructures for tailoring optoelectronic properties of 2D insulators.",

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AU - Rizzo, Daniel J.

AU - Zhang, Jin

AU - Jessen, Bjarke S.

AU - Ruta, Francesco L.

AU - Cothrine, Matthew

AU - Yan, Jiaqiang

AU - Mandrus, David G.

AU - Nagler, Stephen E.

AU - Taniguchi, Takashi

AU - Watanabe, Kenji

AU - Fogler, Michael M.

AU - Pasupathy, Abhay N.

AU - Millis, Andrew J.

AU - Rubio, Angel

AU - Hone, James C.

AU - Dean, Cory R.

AU - Basov, D. N.

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N2 - The use of work-function-mediated charge transfer has recently emerged as a reliable route toward nanoscale electrostatic control of individual atomic layers. Using α-RuCl3 as a 2D electron acceptor, we are able to induce emergent nano-optical behavior in hexagonal boron nitride (hBN) that arises due to interlayer charge polarization. Using scattering-type scanning near-field optical microscopy (s-SNOM), we find that a thin layer of α-RuCl3 adjacent to an hBN slab reduces the propagation length of hBN phonon polaritons (PhPs) in significant excess of what can be attributed to intrinsic optical losses. Concomitant nano-optical spectroscopy experiments reveal a novel resonance that aligns energetically with the region of excess PhP losses. These experimental observations are elucidated by first-principles density-functional theory and near-field model calculations, which show that the formation of a large interfacial dipole suppresses out-of-plane PhP propagation. Our results demonstrate the potential utility of charge-transfer heterostructures for tailoring optoelectronic properties of 2D insulators.

AB - The use of work-function-mediated charge transfer has recently emerged as a reliable route toward nanoscale electrostatic control of individual atomic layers. Using α-RuCl3 as a 2D electron acceptor, we are able to induce emergent nano-optical behavior in hexagonal boron nitride (hBN) that arises due to interlayer charge polarization. Using scattering-type scanning near-field optical microscopy (s-SNOM), we find that a thin layer of α-RuCl3 adjacent to an hBN slab reduces the propagation length of hBN phonon polaritons (PhPs) in significant excess of what can be attributed to intrinsic optical losses. Concomitant nano-optical spectroscopy experiments reveal a novel resonance that aligns energetically with the region of excess PhP losses. These experimental observations are elucidated by first-principles density-functional theory and near-field model calculations, which show that the formation of a large interfacial dipole suppresses out-of-plane PhP propagation. Our results demonstrate the potential utility of charge-transfer heterostructures for tailoring optoelectronic properties of 2D insulators.

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Polaritonic Probe of an Emergent 2D Dipole Interface

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