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1.
Nano Lett ; 20(7): 5127-5132, 2020 Jul 08.
Artigo em Inglês | MEDLINE | ID: mdl-32497434

RESUMO

Metasurface lenses provide an ultrathin platform in which to focus light, but weak light-matter interactions limit their dynamic tunability. Here we design submicron-thick, ultrahigh quality factor (high-Q) metalenses that enable dynamic modulation of the focal length and intensity. Using full-field simulations, we show that quality factors exceeding 5000 can be generated by including subtle, periodic perturbations within the constituent Si nanoantennas. Such high-Q resonances enable lens modulation based on the nonlinear Kerr effect, with focal lengths varying from 4 to 6.5 µm and focal intensities decreasing by half as input intensity increases from 0.1 to 1 mW/µm2. We also show how multiple high-Q resonances can be embedded in the lens response through judicious placement of the perturbations. Our high-Q lens design, with quality factors 2 orders of magnitude higher than existing lens designs, provides a foundation for reconfigurable, multiplexed, and hyperspectral metasurface imaging platforms.

2.
Nat Mater ; 19(5): 534-539, 2020 May.
Artigo em Inglês | MEDLINE | ID: mdl-32094492

RESUMO

Defects in hexagonal boron nitride (hBN) exhibit high-brightness, room-temperature quantum emission, but their large spectral variability and unknown local structure challenge their technological utility. Here, we directly correlate hBN quantum emission with local strain using a combination of photoluminescence (PL), cathodoluminescence (CL) and nanobeam electron diffraction. Across 40 emitters, we observe zero phonon lines (ZPLs) in PL and CL ranging from 540 to 720 nm. CL mapping reveals that multiple defects and distinct defect species located within an optically diffraction-limited region can each contribute to the observed PL spectra. Local strain maps indicate that strain is not required to activate the emitters and is not solely responsible for the observed ZPL spectral range. Instead, at least four distinct defect classes are responsible for the observed emission range, and all four classes are stable upon both optical and electron illumination. Our results provide a foundation for future atomic-scale optical characterization of colour centres.

3.
Acc Chem Res ; 53(3): 588-598, 2020 03 17.
Artigo em Inglês | MEDLINE | ID: mdl-31913015

RESUMO

Chirality in Nature can be found across all length scales, from the subatomic to the galactic. At the molecular scale, the spatial dissymmetry in the atomic arrangements of pairs of mirror-image molecules, known as enantiomers, gives rise to fascinating and often critical differences in chemical and physical properties. With increasing hierarchical complexity, protein function, cell communication, and organism health rely on enantioselective interactions between molecules with selective handedness. For example, neurodegenerative and neuropsychiatric disorders including Alzheimer's and Parkinson's diseases have been linked to distortion of chiral-molecular structure. Moreover, d-amino acids have become increasingly recognized as potential biomarkers, necessitating comprehensive analytical methods for diagnosis that are capable of distinguishing l- from d-forms and quantifying trace concentrations of d-amino acids. Correspondingly, many pharmaceuticals and agrochemicals consist of chiral molecules that target particular enantioselective pathways. Yet, despite the importance of molecular chirality, it remains challenging to sense and to separate chiral compounds. Chiral-optical spectroscopies are designed to analyze the purity of chiral samples, but they are often insensitive to the trace enantiomeric excess that might be present in a patient sample, such as blood, urine, or sputum, or pharmaceutical product. Similarly, existing separation schemes to enable enantiopure solutions of chiral products are inefficient or costly. Consequently, most pharmaceuticals or agrochemicals are sold as racemic mixtures, with reduced efficacy and potential deleterious impacts.Recent advances in nanophotonics lay the foundation toward highly sensitive and efficient chiral detection and separation methods. In this Account, we highlight our group's effort to leverage nanoscale chiral light-matter interactions to detect, characterize, and separate enantiomers, potentially down to the single molecule level. Notably, certain resonant nanostructures can significantly enhance circular dichroism for improved chiral sensing and spectroscopy as well as high-yield enantioselective photochemistry. We first describe how achiral metallic and dielectric nanostructures can be utilized to increase the local optical chirality density by engineering the coupling between electric and magnetic optical resonances. While plasmonic nanoparticles locally enhance the optical chirality density, high-index dielectric nanoparticles can enable large-volume and uniform-sign enhancements in the optical chirality density. By overlapping these electric and magnetic resonances, local chiral fields can be enhanced by several orders of magnitude. We show how these design rules can enable high-yield enantioselective photochemistry and project a 2000-fold improvement in the yield of a photoionization reaction. Next, we discuss how optical forces can enable selective manipulation and separation of enantiomers. We describe the design of low-power enantioselective optical tweezers with the ability to trap sub-10 nm dielectric particles. We also characterize their chiral-optical forces with high spatial and force resolution using combined optical and atomic force microscopy. These optical tweezers exhibit an enantioselective optical force contrast exceeding 10 pN, enabling selective attraction or repulsion of enantiomers based on the illumination polarization. Finally, we discuss future challenges and opportunities spanning fundamental research to technology translation. Disease detection in the clinic as well as pharmaceutical and agrochemical industrial applications requiring large-scale, high-throughput production will gain particular benefit from the simplicity and relative low cost that nanophotonic platforms promise.

4.
J Am Chem Soc ; 141(42): 16997-17005, 2019 Oct 23.
Artigo em Inglês | MEDLINE | ID: mdl-31592655

RESUMO

Upconverting nanoparticles provide valuable benefits as optical probes for bioimaging and Förster resonant energy transfer (FRET) due to their high signal-to-noise ratio, photostability, and biocompatibility; yet, making nanoparticles small yields a significant decay in brightness due to increased surface quenching. Approaches to improve the brightness of UCNPs exist but often require increased nanoparticle size. Here we present a unique core-shell-shell nanoparticle architecture for small (sub-20 nm), bright upconversion with several key features: (1) maximal sensitizer concentration in the core for high near-infrared absorption, (2) efficient energy transfer between core and interior shell for strong emission, and (3) emitter localization near the nanoparticle surface for efficient FRET. This architecture consists of ß-NaYbF4 (core) @NaY0.8-xErxGd0.2F4 (interior shell) @NaY0.8Gd0.2F4 (exterior shell), where sensitizer and emitter ions are partitioned into core and interior shell, respectively. Emitter concentration is varied (x = 1, 2, 5, 10, 20, 50, and 80%) to investigate influence on single particle brightness, upconversion quantum yield, decay lifetimes, and FRET coupling. We compare these seven samples with the field-standard core-shell architecture of ß-NaY0.58Gd0.2Yb0.2Er0.02F4 (core) @NaY0.8Gd0.2F4 (shell), with sensitizer and emitter ions codoped in the core. At a single particle level, the core-shell-shell design was up to 2-fold brighter than the standard core-shell design. Further, by coupling a fluorescent dye to the surface of the two different architectures, we demonstrated up to 8-fold improved emission enhancement with the core-shell-shell compared to the core-shell design. We show how, given proper consideration for emitter concentration, we can design a unique nanoparticle architecture to yield comparable or improved brightness and FRET coupling within a small volume.

5.
Science ; 365(6460): 1475-1478, 2019 09 27.
Artigo em Inglês | MEDLINE | ID: mdl-31604278

RESUMO

Plasmon-coupled circular dichroism has emerged as a promising approach for ultrasensitive detection of biomolecular conformations through coupling between molecular chirality and surface plasmons. Chiral nanoparticle assemblies without chiral molecules present also have large optical activities. We apply single-particle circular differential scattering spectroscopy coupled with electron imaging and simulations to identify both structural chirality of plasmonic aggregates and plasmon-coupled circular dichroism induced by chiral proteins. We establish that both chiral aggregates and just a few proteins in interparticle gaps of achiral assemblies are responsible for the ensemble signal, but single nanoparticles do not contribute. We furthermore find that the protein plays two roles: It transfers chirality to both chiral and achiral plasmonic substrates, and it is also responsible for the chiral three-dimensional assembly of nanorods. Understanding these underlying factors paves the way toward sensing the chirality of single biomolecules.


Assuntos
Dicroísmo Circular , Nanotubos/química , Conformação Proteica , Soroalbumina Bovina/química , Microscopia Crioeletrônica , Ouro , Microscopia Eletrônica de Varredura , Microscopia Eletrônica de Transmissão , Análise Espectral Raman
6.
ACS Cent Sci ; 5(7): 1211-1222, 2019 Jul 24.
Artigo em Inglês | MEDLINE | ID: mdl-31403071

RESUMO

Upconverting nanoparticles (UCNPs) are promising tools for background-free imaging and sensing. However, their usefulness for in vivo applications depends on their biocompatibility, which we define by their optical performance in biological environments and their toxicity in living organisms. For UCNPs with a ratiometric color response to mechanical stress, consistent emission intensity and color are desired for the particles under nonmechanical stimuli. Here, we test the biocompatibility and mechanosensitivity of α-NaYF4:Yb,Er@NaLuF4 nanoparticles. First, we ligand-strip these particles to render them dispersible in aqueous media. Then, we characterize their mechanosensitivity (∼30% in the red-to-green spectral ratio per GPa), which is nearly 3-fold greater than those coated in oleic acid. We next design a suite of ex vivo and in vivo tests to investigate their structural and optical properties under several biorelevant conditions: over time in various buffers types, as a function of pH, and in vivo along the digestive tract of Caenorhabditis elegans worms. Finally, to ensure that the particles do not perturb biological function in C. elegans, we assess the chronic toxicity of nanoparticle ingestion using a reproductive brood assay. In these ways, we determine that mechanosensitive UCNPs are biocompatible, i.e., optically robust and nontoxic, for use as in vivo sensors to study animal digestion.

7.
Nat Commun ; 10(1): 3297, 2019 Jul 24.
Artigo em Inglês | MEDLINE | ID: mdl-31341164

RESUMO

Time reversal symmetry stands as a fundamental restriction on the vast majority of optical systems and devices. The reciprocal nature of Maxwell's equations in linear, time-invariant media adds complexity and scale to photonic diodes, isolators, circulators and also sets fundamental efficiency limits on optical energy conversion. Though many theoretical proposals and low frequency demonstrations of nonreciprocity exist, Faraday rotation remains the only known nonreciprocal mechanism that persists down to the atomic scale. Here, we present photon-spin-polarized stimulated Raman scattering as a new nonreciprocal optical phenomenon which has, in principle, no lower size limit. Exploiting this process, we numerically demonstrate nanoscale nonreciprocal transmission of free-space beams at near-infrared frequencies with a 250 nm thick silicon metasurface as well as a fully-subwavelength plasmonic gap nanoantenna. In revealing all-optical spin-splitting, our results provide a foundation for compact nonreciprocal communication and computing technologies, from nanoscale optical isolators and full-duplex nanoantennas to topologically-protected networks.

8.
Nano Lett ; 19(6): 3878-3885, 2019 06 12.
Artigo em Inglês | MEDLINE | ID: mdl-31056918

RESUMO

The optical efficiency of lanthanide-based upconversion is intricately related to the crystalline host lattice. Different crystal fields interacting with the electron clouds of the lanthanides can significantly affect transition probabilities between the energy levels. Here, we investigate six distinct alkaline-earth rare-earth fluoride host materials (M1- xLn xF2+x, MLnF) for infrared-to-visible upconversion, focusing on nanoparticles of CaYF, CaLuF, SrYF, SrLuF, BaYF, and BaLuF doped with Yb3+ and Er3+. We first synthesize ∼5 nm upconverting cores of each material via a thermal decomposition method. Then we introduce a dropwise hot-injection method to grow optically inert MYF shell layers around the active cores. Five distinct shell thicknesses are considered for each host material, resulting in 36 unique, monodisperse upconverting nanomaterials each with size below ∼15 nm. The upconversion quantum yield (UCQY) is measured for all core/shell nanoparticles as a function of shell thickness and compared with hexagonal (ß-phase) NaGdF4, a traditional upconverting host lattice. While the UCQY of core nanoparticles is below the detection limit (<10-5%), it increases by 4 to 5 orders of magnitude as the shell thickness approaches 4-6 nm. The UCQY values of our cubic MLnF nanoparticles meet or exceed the ß-NaGdF4 reference sample. Across all core/shell samples, SrLuF nanoparticles are the most efficient, with UCQY values of 0.53% at 80 W/cm2 for cubic nanoparticles with ∼11 nm edge length. This efficiency is 5 times higher than our ß-NaGdF4 reference material with comparable core size and shell thickness. Our work demonstrates efficient and bright upconversion in ultrasmall alkaline-earth-based nanoparticles, with applications spanning biological imaging and optical sensing.

9.
Nat Nanotechnol ; 14(5): 420-425, 2019 05.
Artigo em Inglês | MEDLINE | ID: mdl-30833691

RESUMO

Electron microscopy has been instrumental in our understanding of complex biological systems. Although electron microscopy reveals cellular morphology with nanoscale resolution, it does not provide information on the location of different types of proteins. An electron-microscopy-based bioimaging technology capable of localizing individual proteins and resolving protein-protein interactions with respect to cellular ultrastructure would provide important insights into the molecular biology of a cell. Here, we synthesize small lanthanide-doped nanoparticles and measure the absolute photon emission rate of individual nanoparticles resulting from a given electron excitation flux (cathodoluminescence). Our results suggest that the optimization of nanoparticle composition, synthesis protocols and electron imaging conditions can lead to sub-20-nm nanolabels that would enable high signal-to-noise localization of individual biomolecules within a cellular context. In ensemble measurements, these labels exhibit narrow spectra of nine distinct colours, so the imaging of biomolecules in a multicolour electron microscopy modality may be possible.


Assuntos
Corantes Fluorescentes/química , Microscopia Eletrônica de Transmissão , Nanopartículas/química
10.
Nat Commun ; 9(1): 4658, 2018 11 07.
Artigo em Inglês | MEDLINE | ID: mdl-30405133

RESUMO

Plasmonic nanoparticle catalysts offer improved light absorption and carrier transport compared to traditional photocatalysts. However, it remains unclear how plasmonic excitation affects multi-step reaction kinetics and promotes site-selectivity. Here, we visualize a plasmon-induced reaction at the sub-nanoparticle level in-situ and in real-time. Using an environmental transmission electron microscope combined with light excitation, we study the photocatalytic dehydrogenation of individual palladium nanocubes coupled to gold nanoparticles with sub-2 nanometer spatial resolution. We find that plasmons increase the rate of distinct reaction steps with unique time constants; enable reaction nucleation at specific sites closest to the electromagnetic hot spots; and appear to open a new reaction pathway that is not observed without illumination. These effects are explained by plasmon-mediated population of excited-state hybridized palladium-hydrogen orbitals. Our results help elucidate the role of plasmons in light-driven photochemical transformations, en-route to design of site-selective and product-specific photocatalysts.

11.
Nano Lett ; 18(9): 5357-5363, 2018 09 12.
Artigo em Inglês | MEDLINE | ID: mdl-30148640

RESUMO

Surface faceting in nanoparticles can profoundly impact the rate and selectivity of chemical transformations. However, the precise role of surface termination can be challenging to elucidate because many measurements are performed on ensembles of particles and do not have sufficient spatial resolution to observe reactions at the single and subparticle level. Here, we investigate solute intercalation in individual palladium hydride nanoparticles with distinct surface terminations. Using a combination of diffraction, electron energy loss spectroscopy, and dark-field contrast in an environmental transmission electron microscope (TEM), we compare the thermodynamics and directly visualize the kinetics of 40-70 nm {100}-terminated cubes and {111}-terminated octahedra with approximately 2 nm spatial resolution. Despite their distinct surface terminations, both particle morphologies nucleate the new phase at the tips of the particle. However, whereas the hydrogenated phase-front must rotate from [111] to [100] to propagate in cubes, the phase-front can propagate along the [100], [11̅0], and [111] directions in octahedra. Once the phase-front is established, the interface propagates linearly with time and is rate-limited by surface-to-subsurface diffusion and/or the atomic rearrangements needed to accommodate lattice strain. Following nucleation, both particle morphologies take approximately the same time to reach equilibrium, hydrogenating at similar pressures and without equilibrium phase coexistence. Our results highlight the importance of low-coordination number sites and strain, more so than surface faceting, in governing solute-driven reactions.

12.
Nano Lett ; 18(7): 4454-4459, 2018 07 11.
Artigo em Inglês | MEDLINE | ID: mdl-29927609

RESUMO

Lanthanide-doped nanoparticles are an emerging class of optical sensors, exhibiting sharp emission peaks, high signal-to-noise ratio, photostability, and a ratiometric color response to stress. The same centrosymmetric crystal field environment that allows for high mechanosensitivity in the cubic-phase (α), however, contributes to low upconversion quantum yield (UCQY). In this work, we engineer brighter mechanosensitive upconverters using a core-shell geometry. Sub-25 nm α-NaYF4:Yb,Er cores are shelled with an optically inert surface passivation layer of ∼4.5 nm thickness. Using different shell materials, including NaGdF4, NaYF4, and NaLuF4, we study how compressive to tensile strain influences the nanoparticles' imaging and sensing properties. All core-shell nanoparticles exhibit enhanced UCQY, up to 0.14% at 150 W/cm2, which rivals the efficiency of unshelled hexagonal-phase (ß) nanoparticles. Additionally, strain at the core-shell interface can tune mechanosensitivity. In particular, the compressive Gd shell results in the largest color response from yellow-green to orange or, quantitatively, a change in the red to green ratio of 12.2 ± 1.2% per GPa. For all samples, the ratiometric readouts are consistent over three pressure cycles from ambient to 5 GPa. Therefore, heteroepitaxial shelling significantly improves signal brightness without compromising the core's mechano-sensing capabilities and further, promotes core-shell cubic-phase nanoparticles as upcoming in vivo and in situ optical sensors.

13.
Nat Nanotechnol ; 13(5): 434, 2018 05.
Artigo em Inglês | MEDLINE | ID: mdl-29728664
14.
Nat Commun ; 9(1): 1775, 2018 05 02.
Artigo em Inglês | MEDLINE | ID: mdl-29720644

RESUMO

Nanorods are promising components of energy and information storage devices that rely on solute-driven phase transformations, due to their large surface-to-volume ratio and ability to accommodate strain. Here we investigate the hydrogen-induced phase transition in individual penta-twinned palladium nanorods of varying aspect ratios with ~3 nm spatial resolution to understand the correlation between nanorod structure and thermodynamics. We find that the hydrogenated phase preferentially nucleates at the rod tips, progressing along the length of the nanorods with increasing hydrogen pressure. While nucleation pressure is nearly constant for all lengths, the number of phase boundaries is length-dependent, with stable phase coexistence always occurring for rods longer than 55 nm. Moreover, such coexistence occurs within individual crystallites of the nanorods and is accompanied by defect formation, as supported by in situ electron microscopy and elastic energy calculations. These results highlight the effect of particle shape and dimension on thermodynamics, informing nanorod design for improved device cyclability.

15.
Nano Lett ; 18(4): 2689-2695, 2018 04 11.
Artigo em Inglês | MEDLINE | ID: mdl-29589449

RESUMO

We demonstrate a facile method to improve upconversion quantum yields in Yb,Er-based nanoparticles via emission dye-sensitization. Using the commercially available dye ATTO 542, chosen for its high radiative rate and significant spectral overlap with the green emission of Er3+, we decorate the surfaces of sub-25 nm hexagonal-phase Na(Y/Gd/Lu)0.8F4:Yb0.18Er0.02 upconverting nanoparticles with varying dye concentrations. Upconversion photoluminescence and absorption spectroscopy provide experimental confirmation of energy transfer to and emission from the dye molecules. Upconversion quantum yield is observed to increase with dye sensitization, with the highest enhancement measured for the smallest particles investigated (10.9 nm in diameter); specifically, these dye-decorated particles are more than 2× brighter than are unmodified, organic-soluble nanoparticles and more than 10× brighter than are water-soluble nanoparticles. We also observe 3× lifetime reductions with dye adsorption, confirming the quantum yield enhancement to result from the high radiative rate of the dye. The approach detailed in this work is widely implementable, renders the nanoparticles water-soluble, and most significantly improves sub-15 nm nanoparticles, making our method especially attractive for biological imaging applications.

16.
Adv Mater ; 30(7)2018 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-29315902

RESUMO

Chameleons are masters of light, expertly changing their color, pattern, and reflectivity in response to their environment. Engineered materials that share this tunability can be transformative, enabling active camouflage, tunable holograms, and novel colorimetric medical sensors. While progress has been made in creating artificial chameleon skin, existing schemes often require external power, are not continuously tunable, and may prove too stiff or bulky for applications. Here, a chemically tunable, large-area metamaterial is demonstrated that accesses a wide range of colors and refractive indices. An ordered monolayer of nanoresonators is fabricated, then its optical response is dynamically tuned by infiltrating its polymer substrate with solvents. The material shows a strong magnetic response with a dependence on resonator spacing that leads to a highly tunable effective permittivity, permeability, and refractive index spanning negative and positive values. The unity-order index tuning exceeds that of traditional electro-optic and photochromic materials and is robust to cycling, providing a path toward programmable optical elements and responsive light routing.

17.
Nano Lett ; 18(2): 1104-1109, 2018 02 14.
Artigo em Inglês | MEDLINE | ID: mdl-29369641

RESUMO

Metasurfaces enable almost complete control of light through ultrathin, subwavelength surfaces by locally and abruptly altering the scattered phase. To date, however, all metasurfaces obey time-reversal symmetry, meaning that forward and backward traveling waves will trace identical paths when being reflected, refracted, or diffracted. Here, we use full-field calculations to design a passive metasurface for nonreciprocal transmission of both direct and anomalously refracted near-infrared light over nanoscale optical path lengths. The metasurface consists of a 100 nm-thick, periodically patterned Si slab. Owing to the high-quality-factor resonances of the metasurface and the inherent Kerr nonlinearities of Si, this structure acts as an optical diode for free-space optical signals. This structure also exhibits nonreciprocal anomalous refraction with appropriate patterning to form a phase gradient metasurface. Compared to existing schemes for breaking time-reversal symmetry, our platform enables subwavelength nonreciprocity for arbitrary free-space optical inputs and provides a straightforward path to experimental realization. The concept is also generalizable to other metasurface functions, providing a foundation for one-way lensing and holography.

18.
Nat Nanotechnol ; 12(11): 1055-1059, 2017 11.
Artigo em Inglês | MEDLINE | ID: mdl-28945237

RESUMO

Circularly polarized light (CPL) exerts a force of different magnitude on left- and right-handed enantiomers, an effect that could be exploited for chiral resolution of chemical compounds as well as controlled assembly of chiral nanostructures. However, enantioselective optical forces are challenging to control and quantify because their magnitude is extremely small (sub-piconewton) and varies in space with sub-micrometre resolution. Here, we report a technique to both strengthen and visualize these forces, using a chiral atomic force microscope probe coupled to a plasmonic optical tweezer. Illumination of the plasmonic tweezer with CPL exerts a force on the microscope tip that depends on the handedness of the light and the tip. In particular, for a left-handed chiral tip, transverse forces are attractive with left-CPL and repulsive with right-CPL. Additionally, total force differences between opposite-handed specimens exceed 10 pN. The microscope tip can map chiral forces with 2 nm lateral resolution, revealing a distinct spatial distribution of forces for each handedness.

19.
Nano Lett ; 17(7): 4172-4177, 2017 07 12.
Artigo em Inglês | MEDLINE | ID: mdl-28608687

RESUMO

Mechanical forces affect a myriad of processes, from bone growth to material fracture to touch-responsive robotics. While nano- to micro-Newton forces are prevalent at the microscopic scale, few methods have the nanoscopic size and signal stability to measure them in vivo or in situ. Here, we develop an optical force-sensing platform based on sub-25 nm NaYF4 nanoparticles (NPs) doped with Yb3+, Er3+, and Mn2+. The lanthanides Yb3+ and Er3+ enable both photoluminescence and upconversion, while the energetically coupled d-metal Mn2+ adds force tunability through its crystal field sensitivity. Using a diamond anvil cell to exert up to 3.5 GPa pressure or ∼10 µN force per particle, we track stress-induced spectral responses. The red (660 nm) to green (520, 540 nm) emission ratio varies linearly with pressure, yielding an observed color change from orange to red for α-NaYF4 and from yellow-green to green for d-metal optimized ß-NaYF4 when illuminated in the near infrared. Consistent readouts are recorded over multiple pressure cycles and hours of illumination. With the nanoscopic size, a dynamic range of 100 nN to 10 µN, and photostability, these nanoparticles lay the foundation for visualizing dynamic mechanical processes, such as stress propagation in materials and force signaling in organisms.

20.
Nano Lett ; 17(8): 4583-4587, 2017 08 09.
Artigo em Inglês | MEDLINE | ID: mdl-28661675

RESUMO

Manipulating the frequency of electromagnetic waves forms the core of many modern technologies, ranging from imaging and spectroscopy to radio and optical communication. The process of converting photons from higher to lower energy is easily accomplished and technologically widespread. However, upconversion, which is the process of converting lower-energy photons into higher-energy photons, is still a growing field of study with nascent applications and burgeoning interest. Here, we experimentally demonstrate a new photon upconversion technique mediated by hot carriers in plasmonic nanostructures. Hot holes and hot electrons generated via plasmon decay in illuminated metal nanoparticles are injected into an adjacent semiconductor quantum well where they radiatively recombine to emit higher-energy photons. Using GaN/InGaN quantum wells decorated with gold and silver nanoparticles, we show photon upconversion from 2.4 to 2.8 eV. The process scales linearly with illumination power and enables both geometry- and polarization-based tunability. The conversion of plasmonic losses into upconverted optical emission has the potential to impact bioimaging, on-chip wavelength conversion, and high-efficiency photovoltaics.

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