Spectrally Tunable Infrared Plasmonic F,Sn:In2O3 Nanocrystal Cubes

Shin Hum Cho^a, Kevin M. Roccapriore^b, Chandriker Kavir Dass^c, Sandeep Ghosh^a, Junho Choi^d, Jungchul Noh^a, Lauren C. Reimnitz^a, Sungyeon Heo^e, Kihoon Kim^a, Karen Xie^a, Brian A. Korgel^a, Xiaoqin Li^d, Joshua R. Hendrickson^c, Jordan A. Hachtel^b, Delia J. Milliron^a

^aMcKetta Department of Chemical Engineering, University of Texas at Austin, 200 E. Dean Keeton St, Austin, TX, 78712, United States

^bCenter for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, EE. UU., Oak Ridge, United States

^cSensors Directorate, Air Force Research Laboratory, Wright-Patterson AFB, United States

^dDepartment of Physics, Center for Complex Quantum Systems, University of Texas at Austin, United States

^eDepartment of Electrical Engineering, Princeton University, Department of Electrical Engineering, Princeton University, Princeton, NJ 08544, United States

Online Meetups
Proceedings of Online Meetup: Shape-Controlled Nanocrystals: Synthesis, Characterization Methods and Applications (ShapeNC)

Online, Spain, 2020 May 7th - 7th

Organizer: Iwan Moreels

Poster, Shin Hum Cho, 002
Publication date: 6th May 2020

ePoster:

A synthetic challenge in faceted metal oxide nanocrystals (NCs) is realizing tunable localized surface plasmon resonance (LSPR) near-field response in the infrared (IR) [1]. Cube-shaped nanoparticles of noble metals exhibit LSPR spectral tunability limited to visible spectral range. Here, we describe the colloidal synthesis of fluorine, tin codoped indium oxide (F,Sn:In₂O₃) NC cubes with tunable IR range LSPR for around 10 nm particle sizes [2]. Free carrier concentration is tuned through controlled Sn dopant incorporation, where Sn is an aliovalent n-type dopant in the In₂O₃ lattice. F shapes the NC morphology into cubes by functioning as a surfactant on the {100} crystallographic facets [3].

Cube shaped F,Sn:In₂O₃ NCs exhibit narrow, shape-dependent multimodal LSPR due to corner, edge, and face centered modes. Monolayer NC arrays are fabricated through a liquid-air interface assembly, further demonstrating tunable LSPR response as NC film nanocavities that can heighten near-field enhancement (NFE). The tunable F,Sn:In₂O₃ NC near-field is coupled with PbS quantum dots, via the Purcell effect. The detuning frequency between the nanocavity and exciton is varied, resulting in IR near-field dependent enhanced exciton lifetime decay. LSPR near-field tunability is directly visualized through IR range scanning transmission electron microscopy-electron energy loss spectroscopy (STEM-EELS). STEM-EELS mapping of the spatially confined near-field in the F,Sn:In₂O₃ NC array interparticle gap demonstrates elevated NFE tunability in the arrays.

References:

[1] A. Agrawal, S. H. Cho, O. Zandi, S. Ghosh, R. W. Johns, and D. J. Milliron, “Localized surface plasmon resonance in semiconductor nanocrystals,” Chem. Rev. 118, (2018), 3121.

[2] Cho, S. H.; Roccapriore K. M.; Dass C. K.; Ghosh, S.; Choi, J.; Noh, J.; Reimnitz, L. C.; Heo, S.; Kim, K.; Xie, K.; Korgel, B. A; Li, X.; Hendrickson, J. R.; Hachtel, J. A; and Milliron, D. J.; “Spectrally Tunable Infrared Plasmonic F,Sn:In2O3 Nanocrystal Cubes,” J. Chem. Phys., 152 (2020), 014709.

[3] Cho, S. H.; Ghosh, S.; Berkson, Z. J.; Hachtel, J. A.; Shi, J.; Zhao, X.; Reimnitz, L. C.; Dahlman, C. J.; Ho, Y.; Yang, A.; et al. Syntheses of Colloidal F:In2O3 Cubes: Fluorine-Induced Faceting and Infrared Plasmonic Response. Chem. Mater. (2019), 31, 7, 2661–2676.

Acknowledgements:

S.H.C., S.G., L.C.R., S.H., K.K., J.C., J.N., B.A.K., X.L., D.J.M. acknowledge support from the National Science Foundation (NSF, CHE-1609656, CBET-1704634, NASCENT, an NSF ERC EEC-1160494, and CDCM, an NSF MRSEC DMR-1720595), the Welch Foundation (F-1848, F-1464, and F-1662), Fulbright Program (IIE-15151071). This work utilized the SAXS instrument acquired under an NSF MRI grant (CBET-1624659). Some microscopy research was performed as part of a user proposal at Oak Ridge National Laboratory (ORNL) the Center for Nanophase Materials Sciences (CNMS), a U.S. Department of Energy, Office of Science User Facility (J.A.H.), and by U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division (K.M.R.). This research was conducted, in part, using instrumentation within ORNL’s Materials Characterization Core provided by UT-Battelle, LLC, under contract No. DE-AC05-00OR22725 with the DOE, and sponsored by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the U.S. Department of Energy. C.K.D. and J.H. acknowledge support from the Air Force Office of Scientific Research under contract number FA9550-15RYCOR159.

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