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WIREs Energy Environ.
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Advances in plasmon‐enhanced upconversion luminescence phenomena and their possible effect on light harvesting for energy applications

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The focus of the review is on the recent advances of inorganic materials used for upconversion luminescence as well as the effect of plasmonic metals on the efficiency of the overall system. Central to the review is the effect of these upconverting luminescence materials coupled with plasmonic metals on photovoltaic cells and photocatalysts performance. The diffuse nature of sun light on earth (low flux) and its weak energy (low frequency) are the main hurdles for practical applications related to energy‐intensive processes. Upconversion luminescence materials increase light energy (high frequency) with weak efficiency, and when combined with plasmonics (potentially providing high local light flux), the overall efficiency of the system can be improved. Examples in this review are exclusively based on lanthanide compounds as light‐converting devices and on Au and Ag as plasmonic metals. Due to the so called ‘lanthanides contraction,’ the f‐orbitals of lanthanide cations are shielded from the outside environment (chemical bonds) when compared to early transition metals. This and the many energy levels associated with these f‐orbitals make them (particularly the Ln3+ 4f10, 4f11, 4f12, and 4f13) the most suitable materials for multiple energy transfer systems so far. While upconversion luminescence was first observed over half a century ago, since the pioneering work of Auzel, coupling it with plasmonics has only attracted attention in the last few years, and a limited amount of work is currently available. This review has compiled representative work in the field with the aim to motivate researchers to exploit this concept, which is central to light–matter interaction, and its effect on chemical reactions relevant to energy and the environment. WIREs Energy Environ 2017, 6:e254. doi: 10.1002/wene.254

(a) Energy diagram showing absorption of light and the processes involved in the emission of light as fluorescence and phosphorescence. (b) The Stokes shift of the excitation and emission spectra of a fluorophore.
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Photocatalytic degradation of methylene orange (MO) aqueous solution in the presence of various samples under (a) UV, (b) visible, and (c) near‐infrared (NIR). Schematic illustration of the photocatalysis mechanisms under (d) UV, (e) visible, and (f) NIR irradiation, respectively. (Adapted from Ref .)
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(a) Schematic illustration of the formation process of the NYF@TiO2–Au core–shell microspheres. (b, c) TEM. (d) HRTEM. (e) The UV–vis–NIR absorption spectra. (f) PL spectra at excitation wavelength of 975 nm of NYF, NYF@TiO2, and NYF@TiO2–2 wt% Au. (Adapted from Ref .)
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(a) Sketch of the Au‐UC–CdTe–ZnO photoelectrode and the mechanism of energy conversion from near‐infrared (NIR) to chemical fuel. (b) UC emission spectra of the Au‐x‐UC (x = 0, 0.2, 0.4, 1.0 and 2.0 wt%) suspended in water at a controlled concentration of 10 mg mL−1 of UC. (c) Gas evolution of the Au‐x‐UC–CdTe–ZnO (x = 0, 0.2, 0.4, 1.0 and 2.0 wt%) and ZnO as a photoanode in 0.5 M Na2SO4 solution. (Adapted from Ref . Copyright 2013 Royal Society of Chemistry)
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(a) PL spectra of SYE, SYE/A, and SYE/A@T (see text for abbreviations). (b) J–V curves of DSSCs with different photoelectrodes under AM1.5G light. (Source from 44. Copyright 2016 Elsevier)
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Photovoltaic performance of ultrathin (≈8 µm), nanostructured silicon microcells embedded in plasmonically enhanced UC medium. (a) Representative J–V curves of individual ultrathin, nanostructured silicon solar microcells at various substrate configurations, including plain SU‐8 (black), plain Ag (red), plain Ag with UC luminophores (blue), nanostructured Ag (green), and nanostructured Ag with UC luminophores (orange), measured under AM1.5G standard solar illumination (1000 W m−2). (b) The ratio of Jsc increase (ΔJsc = Jsc − Jsc, plain Ag) of nanostructured silicon microcells on a plain Ag substrate with UCNC (blue), a nanostructured Ag substrate without (green), and with (orange) UCNC, with respect to the Jsc on a plain Ag substrate without UCNC (Jsc, plain Ag) extracted from J–V measurements under narrow band illumination. (Source from Ref .)
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(a) Schematic illustration of optical processes of incident photons in the integrated composite PV system, where silicon microcells are embedded in a polymeric wave‐guiding medium on a nanostructured plasmonic substrate without (top) and with (bottom) UC luminophores. (b) Emission spectra of UC polymeric medium containing NaYF4: Yb3+, Er3+ nanocrystals at various substrate configurations including a plain SU‐8, SU‐8 nanoholes, plain Ag, and Ag hybrid nanostructures. A 968‐nm CW laser (12 W cm−2) was illuminated at an incidence angle of  ≈ 5°, and the emitted light was collected by a fiber optic‐connected spectrometer. (Source from Ref .)
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Contour plots of electric field intensity profiles for a plain Ag (first column), nanoholes (second column), nanoposts (third column), and hole/post hybrid nanostructures (fourth column) of Ag under normally incident illumination at wavelengths of 980 (top), 660 (middle), and 540 nm (bottom), respectively, at the optimal geometry of each configuration at phole (or post) = 700 nm (i.e., Dhole = 300 nm, hhole = 340 nm for nanoholes; Dpost = 450 nm, hpost = 80 nm for nanoposts; Dhole = 540 nm, hhole = 440 nm, Dpost = 330 nm, hpost = 120 nm for hybrids). (Source from Ref .)
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(a) The schematic configuration of the DSS cell consisting of an external front layer of Yb2O3/Au nanocomposites as the UC film. (b) The photo I–V characteristics of Yb2O3/Au‐DSSC or NaYF4: Yb3+,Er3+ ‐DSSC under 980‐nm light illumination (1.18 W mm−2). (c) The photo I–V characteristics of the DSSC with and without the Yb2O3/Au layer under 790–830 nm illumination (3.57 W mm−2); the inset shows PCE (%) of Yb2O3/Au‐DSSC versus the near‐infrared (NIR) excitation wavelength. (Adapted from Ref 42. Copyright 2014 American Chemical Society)
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(a) Power‐dependent white light emission spectra of Yb2O3 (0.36 − 1.18 W mm−2) under 980‐nm laser excitation. (b) Power‐dependent white light emission spectra of Yb2O3/Au (0.25 − 1.18 W mm−2) under 980‐nm laser excitation. (Adapted from Ref 42. Copyright 2014 American Chemical Society)
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(a) UV–vis absorption spectra of Au NPs, NaYF4:Yb, Er NPs, and NaYF4: Yb, Er@ SiO2 @ Au nanocomposites. (b) J–V curves of DSSCs with different photoanodes. (Adapted from Ref 41. Copyright 2014 Royal Society of Chemistry)
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(a) Schematic diagram of DSSCs with UC and plasmonic rear reflector film. (b) J–V curves of DSSCs with different films. (Source from Ref 40. Copyright 2013 Royal Society of Chemistry)
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UC PL emission spectra of rear reflector films. (Source from Ref . Copyright 2013 Royal Society of Chemistry)
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(a) Scanning electron micrograph of a gold pyramid array, made by optical lithography and anisotropic KOH etching, with 2 µm periodicity. The inset shows a higher‐resolution image of the gold pyramid at a steep angle. (b) Schematic of the energy transfer, upconversion, and quenching processes at the top and bottom of the gold pyramid substrate. The ultrasmooth gold pyramid provides a good platform to study these photo‐physical processes in the doped‐lanthanide nanoparticles. (c) UC luminescence spectra for the green and red light observed from 29 nm NaYF4:Yb3+/Er3+ particles on glass, gold, and gold pyramid substrates, respectively. The table shows a summary of the upconversion emission intensity ratio of the green to red (G/R), UC emission from 4H11/2 to 4S3/2 level (IH/IS), the temperature estimates for the substrates using the ratio of 4H11/2 to 4S3/2 level (for phonon‐assisted cooling in Er3+). (Adapted from . Copyright 2014 American Chemical Society)
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Calculated quantum yield qa, excitation rate γexc, and fluorescence rate γem as a function of the separation distance, z (nm), between the gold nanoparticle and the fluorescent molecule. γexc and γem are normalized with their corresponding free space values (z → ∞). The solid curves are the result of multiple multipole calculations, whereas the dashed curves correspond to the dipole approximation in which all higher‐order multipoles of gold nanoparticles were ignored. In (a), the particle diameter is d = 80 nm, and in (b), it is indicated in the figure. The excitation wavelength is λ = 650 nm and ɛ = −2.99 + i1.09 (gold). (Source from Ref 37. Copyright 2006 American Physical Society)
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Energy migration‐mediated upconversion (EMU) scheme involving four types of lanthanide ions in a core–shell design. (a) A sensitizer ion (type I) transfers its excitation energy to an accumulator ion (type II), followed by energy transfer from the high‐lying excited state of the accumulator to a migrator ion (type III), then followed by the migration of excitation energy via the migrator ion sublattice through the core–shell interface. The migrating energy is trapped by the activator ion (type IV) and gives the upconverted emission. ‘nx’ = random hopping through many type‐III ions; (b) a proposed energy transfer mechanism corresponding to (a). (c) Schematic design of a lanthanide‐doped NaGdF4@NaGdF4 core–shell nanoparticle for EMU (X: activator ion). (d) Emission spectra of the nanoparticles in the ultraviolet spectral region showing the sensitized emission of Gd3+ by Tm3+, supporting the existence of energy transfer from Tm3+ to Gd3+. (Adapted from Ref . Copyright 2011 Nature Publishing Group)
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UC mechanism of the lanthanide UC materials (a) Yb3+ and Er3+, (b) Yb3+ and Tm3+ or (c) Yb3+ and Ho3+. (Adapted from Ref . Copyright 2015 American Chemical Society)
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(a) General energy schematic illumination related to the excited state absorption process; (b)–(f) general energy schemes related to energy transfer upconversion processes; (b) energy transfer followed by excited state absorption; (c) successive energy transfers; (d) cross‐relaxation upconversion; (e) cooperative sensitization; and (f) cooperative luminescence. (Adapted from Ref . Copyright 2015 American Chemical Society)
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Energy scheme showing (a) two photon absorption process and (b) UC luminescence.
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