Spectrally tunable infrared plasmonic F,Sn:In2O3 nanocrystal cubes

Cho, Shin Hum; Roccapriore, Kevin M.; Dass, Chandriker Kavir; Ghosh, Sandeep; Choi, Junho; Noh, Jungchul; Reimnitz, Lauren C.; Heo, Sungyeon; Kim, Ki-Hoon; Xie, Karen; Korgel, Brian A.; Li, Xiaoqin; Hendrickson, Joshua R.; Hachtel, Jordan A.; Milliron, Delia J.

doi:10.1063/1.5139050

Cited by 43 publications

(75 citation statements)

References 104 publications

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“…[ 31,32 ] Nowadays, improvements in analytical microscopy techniques provide potential for the detection and spatial mapping of IR excitations such as IR plasmons [ 33 ] and phonons [ 34 ] using sub‐nanometer electron probes and sub‐10 meV energy resolution. [ 35 ] This allows TCOs to be explored at higher energy resolutions, as recently presented with doped In 2 O 3 nanoparticles [ 36 ] and films. [ 37 ] Alternatively, the combination of beam monochromation with modest energy resolution (≈50 meV) and post‐acquisition deconvolution methods has improved the effective energy resolution down to 10 meV, and has been successfully applied to studies of near‐IR plasmons in metals.…”

Section: Introductionmentioning

confidence: 99%

Tunable Infrared Plasmon Response of Lithographic Sn‐doped Indium Oxide Nanostructures

Kapetanovic

Bicket

Lazar

et al. 2020

Advanced Optical Materials

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Transparent conductive oxides (TCOs) have strong potential for plasmonic applications. Given their easily tunable properties and low energy response, significant challenges in the controlled fabrication and precise characterization of TCOs must be better understood before this potential can be realized. Here, the mid‐ to near‐infrared plasmonic response of Sn‐doped In2O3 (ITO) nanostructures is presented, fabricated top‐down using electron beam lithography and radio‐frequency sputtering. These equilateral ITO triangles of different side lengths are imaged at high spatial and energy resolution with monochromated electron energy loss spectroscopy (EELS) in a scanning transmission electron microscope. Applying the Richardson–Lucy (RL) deconvolution algorithm to experimental EELS spectra reveals localized surface plasmon (LSP) excitations between 150 and 550 meV and a 730 meV bulk plasmon. This very‐low‐energy response to an electron beam is compared with boundary element method simulations of nanostructures. These simulations use the dielectric functions of continuous thin films of the same materials, characterized by ellipsometry, 4‐point probe, and Hall effect tests. Additionally, upon rapid thermal annealing of ITO, blue‐shifts in LSP energy, and longer LSP lifetimes are examined as a consequence of an amorphous‐to‐polycrystalline transformation and an increase in the free carrier density.

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Section: Introductionmentioning

confidence: 99%

Tunable Infrared Plasmon Response of Lithographic Sn‐doped Indium Oxide Nanostructures

Kapetanovic

Bicket

Lazar

et al. 2020

Advanced Optical Materials

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“…As compared to noble metal plasmonic nanoparticles with visible range LSPR located near the intraband transition loss region, doped metal oxide IR LSPR is far from the band edge loss. [19,20] This class of doped metal oxide nanocrystal with plasmon resonance located in the IR gifts a spectrally ideal particle pixel element for EELS analysis as the electron energy loss will be purely plasmonic, eliminating further complexity of intraband or band edge losses in ML analysis. Critically, while the selfassembled structures are nominally periodic, the colloidal synthesis process introduces a high degree of localized disorder in the particle size and shape variation, missing particles (defects), and holes, cracks, and edges in the self-assembled films.…”

Section: Resultsmentioning

confidence: 99%

“…Monolayer nanocrystal arrays were deposited onto a SiN TEM grid via Teflon trough liquid–air interface self‐assembly. [ 20 ] Native surface ligands were removed from the nanocrystal assembled array by TEM grid Ar plasma cleaning for 15 min.…”

Section: Methodsmentioning

confidence: 99%

Predictability of Localized Plasmonic Responses in Nanoparticle Assemblies

Roccapriore

Ziatdinov

Cho

et al. 2021

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Design of nanoscale structures with desired optical properties is a key task for nanophotonics. Here, the correlative relationship between local nanoparticle geometries and their plasmonic responses is established using encoder‐decoder neural networks. In the im2spec network, the relationship between local particle geometries and local spectra is established via encoding the observed geometries to a small number of latent variables and subsequently decoding into plasmonic spectra; in the spec2im network, the relationship is reversed. Surprisingly, these reduced descriptions allow high‐veracity predictions of local responses based on geometries for fixed compositions and surface chemical states. Analysis of the latent space distributions and the corresponding decoded and closest (in latent space) encoded images yields insight into the generative mechanisms of plasmonic interactions in the nanoparticle arrays. Ultimately, this approach creates a path toward determining configurations that yield the spectrum closest to the desired one, paving the way for stochastic design of nanoplasmonic structures.

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“…The material being studied is a self-assembled monolayer of chemically synthesized F,Sn:In 2 O 3 semiconductor nanoparticles with a typical dimension of 10 nm. These nanoparticles offer an ideal platform for spectrally tuning plasmonic responses based on electron donation from Sn and F dopants [38] that are spectrally far from the inter-band transition. Therefore, plasmon modes can be unambiguously identified.…”

Section: Methodsmentioning

confidence: 99%

“…Spectral tunability in metal nanoparticles is generally accomplished via particle size and shape tuning, however it is also possible to tune plasmon resonances by adjusting the number of conduction electrons in the material, for example by doping. [38] Here, we instead altered the concentration of conduction electrons in the material by using the electron beam, and also have the ability to modify the shape; thus, this work presents two nanoscale methods for tuning the resonant frequencies.…”

Section: Complex Structuresmentioning

confidence: 99%

Sculpting the Plasmonic Responses of Nanoparticles by Directed Electron Beam Irradiation

Roccapriore

Cho

Lupini

et al. 2021

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an excellent environment for exploration of fundamental physical and chemical pheno mena due to their extreme degrees of tunability. [5][6][7] As a result, they have been applied in a variety of fields ranging from nanophotonics, quantum optics, catalysis, medicine, mechanical or optical coatings, to surface enhanced Raman spectroscopy. [8][9][10][11][12][13] Nanoparticles on their own or in fewparticle clusters exhibit properties not found in the bulk due to a large ratio of surface area to volume; however, controlled ordering of nanoparticles assemblies allows development of new functionalities, leading to concepts such as single molecule sensing, [14] artificial molecules, [15] and molecular imaging. [16] This in turn leads to the dual challenge of preparation of nanoparticle assemblies with desired geometries and exploration of their functionalities of interest. An enormous variety of methods exist for nanoparticle synthesis including chemical synthesis and physical vapor deposition. [17][18][19][20][21][22] Electron beam lithography (EBL), focused ion beam (FIB) milling, and laser-induced dewetting methods can be used for control over material positioning and growth to some degree, but resulting particle sizes are currently too large for applications requiring particles with less than about 20 nm as the critical dimension. Colloidal self-assembly of nanocrystals is a chemical growth alternative that allows for high packing density and high-quality nanoparticle ordering for particle sizes below 10 nm and has been thoroughly reviewed, [23] but in general, the particle chemistry, stoichiometry, morphology, and relative position largely cannot be locally modified after the assembly process, which hinders opportunities to explore phenomena that depend on these traits.Perhaps the best way to extend the correlations between structure and properties is through a combination of these methods via controllable modification of synthesized plasmonic material. Intentionally modifying the plasmonic structures dynamically after synthesis has largely not been explored. Direct-write techniques such as EBL and FIB have high degrees of precision, and can be used for patterning down to the ≈1 nm level with an aberration corrected beam in specific geometries. [24] An even higher-precision alternative is the electron beam of the scanning transmission electron microscope Spatial confinement of matter in functional nanostructures has propelled these systems to the forefront of nanoscience, both as a playground for exotic physics and quantum phenomena and in multiple applications including plasmonics, optoelectronics, and sensing. In parallel, the emergence of monochromated electron energy loss spectroscopy (EELS) has enabled exploration of local nanoplasmonic functionalities within single nanoparticles and the collective response of nanoparticle assemblies, providing deep insight into associated mechanisms. However, modern synthesis processes for plasmonic nanostructures are often limited in the types of accessible geometry, and mat...

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Spectrally tunable infrared plasmonic F,Sn:In2O3 nanocrystal cubes

Cited by 43 publications

References 104 publications

Tunable Infrared Plasmon Response of Lithographic Sn‐doped Indium Oxide Nanostructures

Tunable Infrared Plasmon Response of Lithographic Sn‐doped Indium Oxide Nanostructures

Predictability of Localized Plasmonic Responses in Nanoparticle Assemblies

Sculpting the Plasmonic Responses of Nanoparticles by Directed Electron Beam Irradiation

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