Bin Dong, Key Laboratory of New Energy and Rare Earth Resource Utilization of State Ethnic Affairs Commission, Key Laboratory of Photosensitive Materials & Devices of Liaoning Province, School of Physics and Materials Engineering, Dalian Minzu University, 18 Liaohe West Road, Dalian 116600, Liaoning, China. E-mail: dong@dlnu.edu.cn
Abstract
Rare-earth-doped upconversion nanocrystals (UCNCs), with unique anti-Stokes emission, have been extensively explored, while their performances are hindered by the restriction of parity-forbidden 4f-4f transitions, making their emission difficult to control and resulting in low quantum yields. Current research primarily relies on modifying dopant types and concentrations, matrix composition, particle size,
Keywords
1. Introduction
Rare-earth (RE)-doped upconversion nanocrystals (UCNCs) constitute a unique class of luminescent materials capable of converting multiple low-energy near-infrared (NIR) photons into higher-energy ultraviolet (UV) or visible (Vis) emissions, underpinned by the unique electronic structure of lanthanide ions[1,2]. A defining bottleneck of RE upconversion lies in the parity-forbidden nature of 4f-4f electronic transitions, a constraint dictated by quantum mechanical selection rules. The 4f orbitals of lanthanide ions are spatially shielded by outer 5S25P6 orbitals, resulting in minimal overlap with the electromagnetic field of incident light and extremely weak electric dipole transition probabilities[3,4]. This intrinsic limitation directly manifests in two critical performance drawbacks: inherently low photoluminescence quantum yields (PLQYs, initially < 0.1% under moderate irradiance) due to dominant non-radiative decay pathways (e.g., phonon-assisted relaxation, surface defect quenching), and poor controllability over emission properties (spectral linewidth, polarization, directionality), which collectively hinder UCNC applications in low-power, high-precision
The root cause of these challenges stems from the need for a fundamental understanding of 4f electron transition behavior to regulate absorption and emission processes. Lanthanide 4f electrons exhibit unique radial distribution and spin-orbit coupling effects, with transitions primarily mediated by weak electric dipole and magnetic dipole interactions[7,8]. The shielding effect of outer orbitals not only reduces transition probabilities but also leads to narrow absorption linewidths (~1-10 nm) and sensitivity to local crystal fields. Thus, effectively regulating 4f electron transitions requires precise control over the interaction between electrons and the surrounding electromagnetic environment[9,10].
Manipulating the local optical field emerges as a rational strategy to regulate 4f electron transition processes, as it bypasses the intrinsic parity-forbidden limitation by enhancing the effective electromagnetic field-matter coupling. Specific mechanisms to address the aforementioned challenges include: (1) Concentrating incident light via plasmonic hotspots or dielectric resonant modes to compensate for small 4f-4f absorption cross-sections (~10-20 cm2); (2) Modulating the radiative decay rate of 4f electrons via high-Q resonators to suppress non-radiative decay and improve PLQYs; (3) Tailoring the local density of optical states (LDOS) via photonic structures to enhance transition probabilities of 4f electrons; (4) Using wavefront shaping or resonant filtering to align broad excitation sources with narrow 4f absorption lines, boosting photon harvesting efficiency. These mechanisms collectively enable active regulation of 4f electron transitions, complementing conventional materials engineering[11,12]. Early studies focused on compositional and morphological engineering of the NCs themselves, like optimizing dopant ratios, core-shell architectures, and phonon environments to suppress non-radiative decay[13-15]. These efforts raised the absolute quantum yields from < 0.1 % to > 10 % under modest irradiance, yet the absorption cross-sections of parity-forbidden 4f-4f transitions remain intrinsically small (~10-20 cm2), and the broad spectral bandwidths of conventional excitation sources still overlap poorly with the narrow linewidths of lanthanide ions. Consequently, most incident photons remain unabsorbed[16-18].
The past decade has witnessed a paradigm shift: instead of treating UCNCs as an isolated emitter, researchers now engineer the surrounding electromagnetic environment to concentrate, spectrally filter, and dynamically re-route the excitation light. This has been enabled by parallel revolutions in nanophotonics, spanning plasmonic antennas, dielectric metasurfaces, high-Q
In this review, we examine how light-field engineering strategies complement, rather than compete with, conventional materials optimizations (Scheme 1). Section 2 dissects the design principles for manipulating optical fields at three complementary length scales: local-field enhancement (plasmonic hotspots and photonic crystal band-edge modes), resonant-mode management (dielectric metasurfaces and optical microcavities), and macroscopic wavefront shaping (microlens arrays and liquid-crystal modulators). Each subsection links theoretical metrics (e.g., Purcell factor, LDOS, and external quantum yield) to experimentally observed gains in UC efficiency and spectral tunability, elucidating the underlying physical links between optical field manipulation and 4f electron transition regulation. Building upon this enhanced control over light-mater interactions, Section 3 reviews the transformative applications enabled by engineered upconversion luminescence (UCL), where rational light-field design has broken performance bottlenecks in key areas including high-sensitivity photodetectors (PDs) and solar cells. By uniting the traditionally separate communities of materials chemistry and nanophotonics, engineered light fields are poised to redefine the efficiency ceiling and application space of rare-earth upconversion.

Scheme 1. Schematic illustration of the main strategies for light-field modulating UCL. The source of the pictures are explained in the following text. UCL: upconversion luminescence.
2. Light-Field Engineering Strategies
2.1 Local-field enhancement
2.1.1 Plasmonic nanostructures
In 1985, Malta et al. reported the fluorescence properties of borosilicate glass co-doped with metal nanoparticles and Eu3+ ions, laying early groundwork for plasmon-lanthanide interactions[24]. Subsequent research established that the localized surface plasmon resonance (LSPR) properties, and thus their efficacy in enhancing UCL, are governed by the nanostructures’ size, shape, and composition. Anisotropic morphologies, in particular, enable broad spectral tuning to match narrow 4f absorption lines of specific lanthanide ions[25]. For instance, sharp features in silver nanoprisms induce spectral shifts over 4 nm per CH2 unit in adsorbed molecules, far exceeding the sensitivity of periodic gold film arrays[26-28]. A critical advancement in plasmon-enhanced UCL has been the quantitative mapping of the distance-dependent interplay between enhancement and quenching. A representative study employed layer-by-layer polyelectrolyte spacers to precisely tune the separation between upconversion nanoparticles (UCNPs) and gold nanorods (Au NRs) antennas. A maximum 22.6-fold UCL enhancement was achieved at an optimal spacer thickness of ~8 nm, demonstrating the narrow window for near-field enhancement before non-radiative energy transfer to the metal dominates[29]. Parallel progress in synthesis has enabled precise geometric control of hybrid nanostructures. Methods such as interfacial energy modulation in mixed solvents allow reproducible fabrication of anisotropic architectures (core-shell, eccentric, and Janus) in a single reaction, paving the way for structures optimized for specific lanthanide emitters[30].
Systematic investigations have further detailed the size-dependent modulation of UCL. For example, Mendez-Gonzalez et al. showed that for Au NPs (4-66 nm), strong quenching via energy transfer peaks at a small optimal size; beyond this size, plasmonic enhancement becomes dominant, counterbalancing and eventually surpassing quenching[31]. Ananda Das et al. designed the lithographically fabricated metal-insulator-metal (MIM) nanostructures, achieving over 1,000-fold UCL enhancement. The

Figure 1. SPR engineering for UCL. (a-b) The cross-section SEM image of resist hole array template after UCNP dropcast step (a) and angled SEM image of MIM after resist removal (b); (c) Schematic illustration for the preparation of 2D UCNP-Au BNSLs through evaporation-driven growth; (d-e) The TEM image of UCNP-Au BNSL isostructural with NaZn13 phase (d), and its [100] projection (e); (f) AFM topographic images of nanoantennae-load UCNP with different configurations and related polar plots of normalized UCL intensity; (g) The cross-section focused ion beam-SEM image of its 3D conceptual illustration. The pictures on the right show the experimental UCL from the pMBs compared to that of the reference structure. Republished with permission from[32,33,35,36]. SPR: surface plasmon resonance; UCL: upconversion luminescence; SEM: scanning electron microscopy; UCNP: upconversion nanoparticle; MIM: metal-insulator-metal; BNSLs: binary nanoparticle superlattices; AFM: atomic force microscopy.
The LSPR in heavily doped semiconductors arises from collective oscillations of intrinsic holes or excess free charge carriers introduced by high-level doping. In contrast to noble metal-based plasmonic materials, these semiconductor materials exhibit notably higher photochemical stability and lower carrier densities, resulting in LSPR absorption peaks that are predominantly located in the NIR region[38-40]. Recent research has been dedicated to harnessing this semiconductor LSPR for UCL modulation, with a focus on elucidating the underlying physical mechanisms to guide the rational design of enhancement strategies. A representative study involves unique Cu2-xS plasmonic quantum dots and their interaction with UCNPs[41]. This work demonstrates that the LSPR in Cu2-xS stems from surface ligand-confined carriers, exhibiting broadening, redshift, and diminution upon heating. An 8 nm MoO3-spaced

Figure 2. LSPR modulating UCL. (a-b) Schematic illustration of the Cu2-xS/MoO3/UCNPs composite structure (a) and its power-dependent UCL enhancement mechanisms (b), showcasing distinct responses at high and low excitation power; (c) Enhancement factors of Cu2-xS/MoO3/UCNPs and Au/MoO3/UCNPs film as a function of excitation power density; (d) Schematic illustration of the CsxWO3/NaYF4/monolayer-NaYF4:Yb3+, Er3+@NaYF4:Yb3+, Tm3+ (CS1) and CsxWO3/NaYF4/monolayer-NaYF4:Yb3+, Tm3+@NaYF4:Yb3+, Er3+ (CS2) hybrid structures; (e-f) Enhancement factors of Tm3+ and Er3+ ions emissions in CsxWO3/NaYF4/CS1 (e) and CsxWO3/NaYF4/CS2 (f), respectively; (g) Schematic of directional-Au@Ag NRs monolayer films; (h) Top-view SEM picture of directional-Au@Ag NRs/UCNPs hybrids, and the inset is the cross-sectional view of SEM; (i) Polarization dependence of UC enhancement factors of random-Au@Ag NRs/UCNPs and directional-Au@Ag NRs/UCNPs hybrids. Republished with permission from[41-43]. LSPR: localized surface plasmon resonance; UCL: upconversion luminescence; NRs: nanorods; UCNPs: upconversion nanoparticles.
2.1.2 Photonic crystals (PCs)
The development of UC-based devices featuring micro/nano-engineered photofields represents a transformative approach for capturing low-energy photons and converting them into higher-energy emissions. Such structures have been shown to enhance UCL by several orders of magnitude. Nevertheless, energy dissipation and insufficient photon absorption typically result in excitation thresholds exceeding 1 mW/cm2, which surpasses retinal safety limits and restricts applications in wearable UC optics. Wang et al. demonstrated the integration of core-shell UC microspheres (~500 nm) that induce IR field convergence, NaYF4:Yb, Er

Figure 3. PCs modulating UCL. (a-b) Schematic illustration of the UCCL composed of microspheres (a) and its treatment of RD in rabbit eyes (b); (c) Images exhibiting pupil constriction from the control, RD, and RD with UCCL rabbits under the dark, 532 nm, and 980 nm light stimulation, respectively; (d) Utilization of sub-bandgap photons with a rear photonic upconverter for charge generation in solar cells; (e) The SEM image of a 1D TiO2/PMMA PCs with embedded UCNPs; (f) Schematic of the MnO2 modified UCNPs composites integrated with a PCs-PDMS array for dual-mode glucose detection; (g) Schematic of the evaporation-induced co-assembly process using pre-synthesized NCs; (h-i) Fabrication of highly ordered IOFs based on ITO (h) and zinc ferrite NCs (i) building blocks, respectively; (j-k) Schematic of the UC PDs based on an InSe/Si-PCC heterostructures (j) and its calculated distributions of electric-field |E| of the resonance mode in the x-y and x-z planes (k); (l) UCNPs/2D Si3N4 PCs structure schematics and its high-magnification SEM image. Republished with permission from[12,46-50]. PCs: photonic crystals; UCL: upconversion luminescence; UCCL: upconversion contact lens;
Local modulation of optical fields using plasmonic materials or PCs offers a promising approach to enhance UCL in UCNCs. However, current strategies are limited to static enhancement, and dynamic modulation of UCL remains unexplored, hindering its application in information processing devices. A dynamic UC modulation system was constructed using electro-responsive tungsten suboxide plasmonic photonic crystals (WO3-x PPCs), as illustrated in Figure 4a,b. By integrating UCNPs with WO3-x PPCs, we achieved reversible electric-field control (±1.6 V) over both the PBG and LSPR, leading to tunable enhancement of UCL by a factor of ~5-26 (Figure 4c,d,e,f). This modulation is attributed to voltage-dependent changes in the W5+/W65+ ratio, which alter the refractive index and oxygen vacancy concentration, thereby shifting the photonic and plasmonic resonances[51]. The development of a bilayer PC film with dual stopbands enabled resonant enhancement of both excitation and emission in core-shell UCNPs, yielding over 150-fold fluorescence enhancement under low-power IR excitation (1.7 W/cm2)[52]. This facilitated ultrasensitive detection of prostate-specific antigen (detection limit: 0.01 ng/mL). Separately, in single-particle studies, a cascade amplifier integrating a PMMA PC with CsxWO3 NPs produced a ~1,600-fold UCL boost from a single UCNP (Figure 4g,h,i), demonstrating utility in sensing with a detection limit of 0.25 nM for dithiothreitol[53]. Based on spectral management strategies, core-shell structured UCNPs excitable at both 808 nm and 980 nm were synthesized and subsequently assembled with PCs to amplify UCL. Leveraging this architecture, flexible dual-narrowband NIR PDs were constructed using a PCs/UCNPs/MAPbI3 hybrid design. These devices demonstrate remarkable detection performance, a low operational power threshold, and excellent mechanical flexibility, as summarized in Figure 4h,i,j[54]. However, the primary limitation of PC-based UCL modulation is its narrow enhancement spectral bandwidth, which requires precise matching of the PBG to the excitation source and emitter’s absorption lines, hindering broadband operation and practical integration[55].

Figure 4. PCs modulating UCL. (a) Fabrication process of WO3-x PPCs; (b) Electric-field modulation of the WO3-x PPCs structures; (c) Optical appearance of WO3-x PPCs before and after application of ± bias voltages; (d) Bragg wavelength of different WO3-x PPCs as a function of applied voltage; (e) UV-vis-NIR absorption spectra of WO3-x PPCs under the different potentials; (f) The corresponding variation of the ratio of W5+/W6+ to the refractive index in WO3-x PPCs under different bias voltages; (g-h) Schematic illustration of the OPCs/CsxWO3/UCNP composite structure (g) and its SEM image (h); (i) UCL spectra in OPCs/CsxWO3/UCNP hybrids structure and other comparison samples; (j) SEM image of PCs/UCNPs hybrids structure; (k-l) Schematic illustration of double narrowband NIR PDs based on PCs/UCNPs/MAPbI3 composites (k) and its photocurrents change with bending times (l). Republished with permission from[51,53,54]. PCs: photonic crystals; UCL: upconversion luminescence; WO3-x PPCs: electro-responsive tungsten suboxide plasmonic photonic crystals; UV: ultraviolet; NIR: near-infrared; OPCs: ordered photonic crystals; UCNP: upconversion nanoparticle; SEM: scanning electron microscopy;
2.2 Resonant-mode management
2.2.1 Dielectric metasurfaces
In 1946, Purcell proposed a concise expression to evaluate the enhancement of the spontaneous emission rate by a resonant cavity under the weak-coupling regime, known as the Purcell factor. It is given by[56]:
where Q denotes the quality factor of the cavity, representing its ability to confine light in time, and Veff is the effective mode volume, characterizing the spatial confinement of the electromagnetic field. The Purcell factor directly correlates the enhancement of spontaneous emission with the spatiotemporal confinement properties of the cavity, serving as a fundamental tool for understanding and studying light-matter interactions in optical resonators[57,58]. In recent years, with the rapid development of micro-nano fabrication technologies, optical metasurfaces, as a class of artificially structured materials, have emerged as a key platform for controlling light fields at the subwavelength scale. As a breakthrough in subwavelength photonics, the foundational design principles of metasurfaces for arbitrary wavefront modulation were first established via geometric phase engineering, with early experimental realizations demonstrating unprecedented control over light reflection, refraction, and polarization at visible-NIR wavelengths[59,60]. These pioneering works laid the groundwork for the subsequent development of metasurfaces in light-matter interaction engineering beyond the UCNP field. In plasmonic nanostructures, the Veff is not constrained by the diffraction limit and can typically reach values on the order of 10-3(λ/2n)3, which can be further reduced to 10-7(λ/2n)3 through optimized design. Plasmonic nanocavities support highly localized optical fields and significantly enhanced light-matter interactions[61-63]. Nevertheless, their performance is hampered by high ohmic losses in metals, which limit the Q to typically less than a hundred. This results in short photon lifetimes and substantial dissipation into heat or radiation. Furthermore, the extreme subwavelength Veff constrains the flexible engineering of emission directivity and polarization. In contrast, dielectric PCs and metasurfaces exhibit fundamentally different behavior, as they leverage low-loss resonances to achieve high Q factors, albeit generally with larger mode volumes. The choice of material, dielectric or metallic, also critically influences the optical response. In all-dielectric realizations, a clear distinction emerges: PCs inhibit light propagation via PBGs, whereas metasurfaces locally tailor wavefronts through controlled phase, amplitude, or polarization modulation.
Bound states in the continuum (BICs) were originally proposed as eigenstates that remain localized despite existing within the continuous spectrum of propagating waves and were first experimentally realized in PCs and dielectric metasurfaces via symmetry protection[64-66]. Quasi-BICs, the leaky counterparts of BICs with finite Q-factors, were later developed to enable practical resonant light-matter interactions, with pioneering non-UCNP works demonstrating their extraordinary ability to engineer light confinement and nonlinear optical responses in all-dielectric nanostructures[67,68]. Exploiting the concept of quasi-BICs, Li’s research team and collaborators engineered a resonant TiO2 metasurface that provides simultaneous electric field intensity enhancements up to

Figure 5. Metasurfaces modulating UCL. (a) Schematic of the UCNP-integrated dielectric metasurface, which supports a high-Q quasi-BIC mode and a Mie resonance; (b) Unit cell design of the metasurface, featuring a pair of TiO2 nanobricks with a tilt angle of δ = ±10° on a SiO2 substrate; (c) Resonance characterization of dielectric metasurfaces; (d) Highly polarized UCL from the metasurface-UCNP systems; (e) Unit cell architecture of the silicon metasurface. A periodic array of four-cylinder silicon clusters
Nonlinear metasurfaces based on multiple quantum wells (MQWs) exhibit exceptional second-order nonlinearities for frequency UC, yet their efficiency is fundamentally limited by intensity saturation under CW pumping. Nefedkin et al. overcame this limitation by introducing a counterintuitive pumping scheme that resonantly couples a strong pump field to unpopulated upper electronic subbands[75]. Combined with an optimized MQW metasurface design, this approach suppresses saturation at practical intensity levels and significantly enhances MIR UC efficiency, and free from phase-matching constraints. They demonstrated a paradigm-shifting strategy by inverting the conventional pumping sequence to target unpopulated upper subbands (Figure 6a). This approach, integrated into a subwavelength trident-shaped metasurface resonator (Figure 6b), coherently channels x-polarized MIR waves into an enhanced intersubband nonlinear polarization, enabling high-efficiency Sum-Frequency generation without phase-matching requirements and sustaining saturation-free operation under CW excitation. Liu et al. reported strong upconverted circularly polarized luminescence (UC-CPL) from achiral core-shell UCNPs by leveraging a suspended bilayer gold metasurface with intrinsic chiral geometry, as illustrated in Figure 6c[76]. The structure enabled both plasmonic enhancement and chirality transfer, yielding a record luminescence dissymmetry factor (glum) of 0.95 at 894 nm (Figure 6d). This high polarization contrast stems from resonant coupling between the metasurface’s circular dichroism and the Nd3+ emission band, as confirmed by the distinct left- and

Figure 6. Metasurfaces modulating UCL. (a) 3-level system schemes modeling the subbands in a realistic MQW structure, the left and right diagram is conventional and the proposed scheme, respectively; (b) Unit-cell design and metasurface layout; (c) Structure diagram of UCNP-coated chiral metasurface; (d) LCP and RCP UCL spectra from UCNP-coated chiral metasurface; (e) Differentiated CPL spectra of UCNPs on chiral metasurface and blank membrane; (f) Photonic Rashba effect in upconversion photoluminescence. A phase-gradient dielectric metasurface coupled with UCNCs demonstrates spin-momentum locking of the emitted light; (g) Experimental demonstration of optical Rashba effect in UC photoluminescence; (h) Resonance characterization of the metasurface (110 nm) with a 200 nm UCNP/PMMA coating, showing the resonant modes and excitation wavelength. Republished with permission from[75-78]. UCL: upconversion luminescence; MQW: multiple quantum wells;
2.2.2 Optical microcavities (whispering-gallery and Fabry-Pérot (F-P))
Optical microcavities constitute a foundational class of micro- and nano-scale structures that enable spatiotemporal confinement of light, drastically enhancing light-matter interactions and affording precise control over optical modes. These structures operate by trapping photons via reflection mechanisms, such as distributed Bragg reflection or total internal reflection, thereby enabling prolonged photon circulation and substantial resonant field enhancement. Based on their mode confinement mechanisms, optical microcavities are broadly categorized into F-P cavities, whispering-gallery mode (WGM), and PC cavities. This section focuses on the first two types. The performance of an optical microcavity is commonly quantified by its photon decay rate. In classical terms, stronger photon confinement leads to longer photon lifetimes and slower field decay. The performance of a microcavity is quantified by its quality factor Q, a dimensionless figure of merit. The attainable Q value is intrinsically dependent on the cavity architecture, leading to substantial variation across different designs. For instance, with comparable fabrication precision, F-P cavities typically exhibit Q factors on the order of 103, whereas WGM can achieve values exceeding 106, a difference spanning three orders of magnitude. There are various mathematical definitions of Q, depending on the physical context. It is most prevalent from the link between Q, the photon lifetime (τc), and the resonant mode frequency (v), which can be calculated through following equation[82].
A higher Q corresponds to a stronger the limiting effect of the microcavity on photons, leading directly on a longer τc. Recent progress in semiconductor epitaxial growth techniques, particularly molecular beam epitaxy, has enabled remarkable improvements in the Q factors of optical microcavities. A representative achievement came in 2014 from the research group of Snoke et al., who demonstrated an F-P microcavity based on a Distributed Bragg reflector structure with a Q factor reaching the order of 106[83].
WGM resonators support stable electromagnetic resonances characterized by light waves circulating along a curved dielectric boundary via continuous total internal reflection. As illustrated in Figure 7a, resonance occurs when the optical path length of one complete round trip equals an integer multiple of the wavelength λ, leading to constructive interference of the recirculating light. For a microresonator of radius r, this condition is expressed by the following equation[84]:

Figure 7. (a) Schematic diagrams of WGM; (b) Image of the F-P microcavity based on UCNPs gain medium; (c) Reflection spectra of DBR and the aluminum mirror. Republished with permission from[86]. WGM: whispering-gallery mode; UCNPs: upconversion nanoparticles; DBR: distributed Bragg reflector; F-P: Fabry-Pérot.
where neff is the effective refractive index of the mode, nN is a positive integer representing the angular mode order, and λ is the resonant wavelength in vacuum.
A F-P microcavity is typically composed of two parallel planar mirrors. When these mirrors exhibit high reflectivity, light incident perpendicular to the mirror surfaces undergoes repeated reflections between them, resulting in photon oscillation along the cavity axis and a significant enhancement of the intracavity optical field. Denoting the cavity length as Lc and the refractive index of the intracavity medium as nc, m is a positive integer, and the resonant wavelength λ satisfies the standing-wave condition[85].
To achieve a high Q factor, distributed Bragg reflectors (DBRs) are often employed as an alternative to conventional planar mirrors. A DBR consists of a periodic stack of two or more semiconductor materials, arranged in an alternating ABAB sequence. Within each period, every layer has an optical thickness corresponding to a quarter of the resonant wavelength in the medium. Structurally, a DBR functions as a one-dimensional photonic crystal, efficiently reflecting light within its PBG due to the suppression of propagation. A key advantage of DBR-based semiconductor microcavities is the tunability of their PBG through geometric control of the period, while the reflectivity can be enhanced by increasing the number of repeating units. In such photonic crystal-derived cavities, the resonant frequency of confined photons is not solely governed by the cavity length and refractive index, but is strongly influenced by the bandgap properties of the DBR structure. Building on this principle, Zhu et al. constructed an F-P cavity featuring a quartz tube sandwiched between a DBR and an aluminum mirror, as illustrated in Figure 7b. A highly efficient core-shell UCNP solution served as the gain medium. By precisely tuning the reflectivity of the DBR and the aluminum mirror, the emission wavelength could be continuously shifted across the blue to red spectral regions, while the lasing linewidth was narrowed to a quarter of its original value (Figure 7c)[86].
Dong and Ren et al. engineered a novel class of microsphere-based optical resonators by incorporating rare-earth ions (Yb3+/Er3+ or Yb3+/Tm3+) doped KY3F10 and KMnF3 UCNCs via high-temperature melting and crystallization[87]. This judiciously tailored

Figure 8. WGM modulating UCL. (a) Design and fabrication of nano-GC microsphere for infrared-to-upconverted Vis lasres. The schematic illustrates the GC microstructure and the powder melting/heating process used for their batch production. Also simulated electric field distribution at 980 nm in a microsphere (radius R) evanescently coupled to a tapered fiber (diameter D, gap d); (b) Schematic diagram for simultaneous multiphoton absorption UC lasing of ZnO microwires; (c) Cavity-enhanced nonlinear process in ZnO microwires resonator. With increasing excitation power, the emission spectrum evolves from a broad spontaneous profile to pronounced WGM lasing; (d) The near-field emission picture of single microwire under different excitation power. (e) The illumination of the light transmission in a WGM microcavity filled with the toluene solution of BTZ-DMAC-4Br/BTZ-DMAC and DPA (9,10-diphenylanthracene); (f) Upconversion quantum yield versus excitation intensity for BTZ-DMAC-4Br; (g) Schematic illustration of synthesis of microlaser array; (h) Theoretical modeling of WGMs and propagation loss; (i) Schematic of single ZnO microrod based two photon-pumped WGM lasing; (j) Power-dependent lasing characteristics; (k) UC lasing performance comparison. Spectra from the glass precursor (blue) and Ho3+/Yb3+ co-doped oxyfluoride (red) microcavities under 167 μW, 980 nm pumping; (l) Power-dependent lasing spectral evolution of Ho3+/Yb3+ co-doped oxyfluoride microcavities; (m) Schematic of UC lasing in liquid-quenched UC microshperes. Illustration of a 980 nm pump laser exciting WGM in the microsphere, leading to circulative amplification and visible emission via Yb3+ to Er3+ ET; (n) Emission spectra of spectrally tuned lasers. Republished with permission from[87,89-94]. UCL: upconversion luminescence; GC: glass composite;
Baldo et al. demonstrated an F-P microcavity strategy to dramatically enhance solid-state TTA UC under subsolar flux[96]. As illustrated in Figure 9a, the cavity is constructed with a DBR and a silver mirror, confining an optical spacer and an upconverting layer containing PbS nanocrystal sensitizers. Through precise tuning of the cavity length, a resonant mode at 980 nm is established, yielding a 74-fold absorption enhancement and a 227-fold amplification of upconverted emission. Figure 9b reveals the optimized electric field distribution within the structure, confirming maximum field intensity localized in the active layer. This photonic engineering reduces the excitation threshold to 13 mW/cm2 and boosts the external quantum efficiency (EQE), highlighting the vital role of optical confinement in advancing low-intensity UC technologies. Yu and Yao et al. innovatively established 2D

Figure 9. F-P microcavity. (a) Schematic illustrations of the bilayer, single-mirror, and F-P microcavity configurations; (b) Cavity-enhanced electric field. Cross-sectional electric field profile at 980 nm versus bathocuproine spacer thickness, showing maximum field intensity in the PbS layer at 60 nm cavity length; (c) Lasing characteristics of RPP
2.3 Wavefront shaping
2.3.1 Microlens arrays
Composed of micro/nano scale optical elements, microstructure arrays derive their multifunctional capabilities from precisely engineered architectures that dictate light-matter interactions. Generally, optical microstructures include microgrooves, microprisms, and microlenses, which provide various optical functions due to their special geometrical features. Figure 10a categorizes fundamental types of microstructure arrays by their constituent element geometry. For arrays with unit dimensions spanning 0.5-5 μm, optical behavior is governed primarily by refractive and reflective phenomena. These architectures enhance light-harvesting efficiency through multi-channel imaging, thereby enabling system miniaturization. Furthermore, the integration of heterogeneous array architectures facilitates advanced functions including precision beam steering and smart scanning capabilities, as illustrated in Figure 10b[98].

Figure 10. Structural characterization of microstructure arrays. (a) Element shape of microstructure arrays, where ①, ②, ③, and ④ separately represents adjacent MLAs, distributed MLAs, triangular pyramid arrays, and rectangular pyramid arrays; (b) Function and applications of microstructure arrays with large element size. Republished with permission from[98]. MLAs: microlens arrays.
By taking advantage of the nonlinear excitation characteristics of MLAs, they can be utilized as an efficient photonic concentrator for boosting UCL at low pump levels. Liu et al. proposed to use polycarbonate MLAs to spatially modulate the excitation light, with a precisely defined period of 51.02 μm and lens curvature of 16.47 μm in height (Figure 11a,b), which functions as a non-invasive spatial light modulator that focuses incident NIR light into high-intensity micro-spots within the UCNP layer. As illustrated in Figure 11c, the mechanism hinges on the power-dependent quantum yield of UCL, by amplifying the local excitation irradiance via lens induced light confinement, the MLAs drastically elevate the rate of multi-photon absorption processes. This leads to distinct enhancement factors for green and red UCL bands from Er3+ and blue UCL band from Tm3+, consistent with their respective nonlinearity orders. Ray tracing simulations corroborate over two orders of magnitude local intensity gain, directly linking the geometric design of the MLAs to the enhanced photophysical dynamics[99].

Figure 11. Polycarbonate MLAs for light focusing. (a-b) SEM images of the cross-section view (a) and top view (b) morphology of microstructure; (c) Schematic illustration of MLAs-enhanced quantum yield of UCL because of its nonlinear response to excitation intensity. Republished with permission from[99]. MLAs: microlens arrays; SEM: scanning electron microscopy; UCL: upconversion luminescence.
Our group proposed a cascade optical field modulation strategy that synergistically integrates the superlensing effect of polymeric MLAs with the plasmonic resonance of Au NRs to achieve unprecedented UCL enhancement exceeding 104-fold[100]. As schematically illustrated in Figure 12a, the architecture sequentially couples far-field light strength through MLAs with near-field amplification via Au NRs. Systematic evaluation reveals that MLA-1, with optimized geometric parameters (35 μm diameter, 5.5 μm height), provides

Figure 12. MLAs modulating UCL. (a-b) Schematic illustration of the cascading amplification strategy for UCNCs; (b-c) Enhancement factors of MLA1-3 in MLA/CSS composites (a) and Au NR/CSS, MLA-1/CSS, and MLA-1/Au NR/CSS composites (b) at 808, 980, and 1,540 nm excitation, respectively; (d) Simulated electric field intensity distribution of Au/MLA-1 hybrid structures under the 808, 980, and 1,540 nm excitation; (e) The transmitted UCL spectra of HPU and MLAs/HPU under the 1,550 nm excitation at
Liu et al. established a paradigm for nonlinear photonic amplification through dielectric MLAs, demonstrating up to 105-fold UC enhancement via dual-wavefront engineering. The dielectric microbeads function as bi-functional optical elements that simultaneously concentrate excitation energy into subwavelength hotspots and collimate highly divergent emission[103]. As critically evidenced in Figure 12g, the microbeads transform the isotropic UC emission into a collimated beam, enhancing collection efficiency approximately eightfold through effective wavefront shaping. This synergistic interplay between excitation intensification and emission extraction operates independently of Purcell effects, distinguishing it fundamentally from plasmonic or cavity-based enhancement strategies.
2.3.2 Liquid-crystal modulators
Liquid-crystal spatial light modulators (LC-SLMs) represent programmable micro-/nanophotonic devices for optical-field engineering. By leveraging the electrically tunable birefringence of liquid crystals, LC-SLMs enable precise, dynamic control over the phase, amplitude, and polarization of an excitation beam at the microscale. This capability provides a direct pathway to enhance UCL by structuring the excitation field to maximize absorption and by tailoring the photonic environment to influence emission properties[104-107]. A compelling demonstration of this approach is the generation of UC-CPL from intrinsically achiral UCNPs, which is a significant challenge since their negligible native dissymmetry factor (|glum|) limits their utility in chiroptical applications. While embedding UCNPs in static chiral matrices (e.g., cholesteric liquid crystals, CLCs) can impart chirality, this method often lacks dynamic reconfigurability and can suffer from nanoparticle aggregation. LC-SLMs offer a transformative all-optical strategy. By imprinting a designed helical phase front onto the excitation beam, LC-SLMs directly induce chiroptical interactions at the absorption stage. This bypasses material compatibility constraints and grants real-time control over the handedness and intensity of UC-CPL, enabling enhanced |glum| and dynamic chiroptical devices[108,109].
This synergy is exemplified in hybrid architectures. For instance, an aligned film of upconversion nanorods can function as both a polarized emitter and an alignment layer for a CLC, forming a superhelical structure that converts linearly polarized UCL into pure CPL within the CLC’s PBG, with output tunable via external stimuli (Figure 13a)[110]. Beyond polarization control, the

Figure 13. Liquid-crystal modulators UCL. (a) CLC-UCNR hybrid structure and its polarization output. Diagram showing aligned UCNRs within a right-handed CLC matrix, where the helical superstructure converts intrinsic linearly polarized emission from nanorods into circularly polarized light via the PBG effect, yielding both CP and LP emission channels; (b) The chiral dual-annihilator system for controllable photon upconversion. Triplet-energy competition between two annihilators, mediated by thermally activated triplet energy transfer, enables multi-dimensional tuning of UC-CPL colour, distinguishable from downshifting CPL by excitation wavelength; (c) The
3. Optoelectronic Application Based on Light-Field Regulation
3.1 Photodetectors
UCNCs, featuring large Stokes/anti-Stokes shifts and excellent photostability can efficiently convert NIR photons into UV/Vis photons for absorption by narrow-bandgap semiconductors. Owing to their narrowband NIR wavelength-selective absorption, UCNCs serve as exceptional photosensitizers, offering a promising solution for developing next-generation wavelength-selective PDs

Figure 14. Optical filed modulated UCNCs-based PDs. (a) Absorption of perovskite (MAPbI3) films, Nd3+, Yb3+, and Er3+ and emission spectra from 1D2→3F4, 1G4→3H6, 2H11/2,
3.2 Solar cells
Notably, by transforming sub-bandgap NIR photons into usable above-bandgap light, UCNCs present an exciting opportunity to minimize non-absorption losses and surpass the Shockley-Queisser limit in photovoltaics[115,116]. In 2018, our group innovatively integrated UCNPs for broadband spectral harvesting in perovskite solar cells (PSCs) to extend the spectral response into NIR

Figure 15. Optical filed modulated UCNCs-based solar cells. (a) NIR and UV to Vis photon conversion for full spectrum response PSCs; (b) Reverse J-V characteristics of PSCs based on the control film and films integrated with UCNPs, UCNPs/IR-783 dye, and UCNPs/IR-783 dye/Au NPs composites under AM 1.5 G illumination; (c) IPCE spectra of PSCs with and without the UCNPs/IR-783 dye/Au NPs composite film. The inset is the structure of the UCNPs/IR-783 dye/Au NPs PSCs; (d) Schematic of the spectral range broadening of SSCs by CSSS, with an inset illustrating the CSSS-coated SSC under AM 1.5 G illumination; (e) UC PLQY of CSSS measured under 1,520 nm excitation at varying power densities, with extrapolated low-power PLQY; (f) IPCE spectra of CSSS-coated SSCs; inset shows the magnified response in the 1,100-2,200 nm region; (g) The structure and working mechanism diagram of dye-sensitized solar cells; (h) The structure and J-V characteristics of NaCsWO3@NaYF4@NaYF4:Yb, Er UCNPs based PSCs. Republished with permission from[118-121]. UCNCs: upconversion nanocrystals; NIR: near-infrared; UV: ultraviolet; PSCs: perovskite solar cells; UCNPs: upconversion nanoparticles;
4. Conclusions and Perspectives
In recent years, significant progress has been made in the engineering of nano-/micro-structures for UCL. This review systematically elaborates on strategies to control UCL through photonic structures, including plasmonic nanostructures, dielectric superstructures, optical microcavities, and wavefront shaping devices. Key advancements are: (1) plasmonic nanostructures, which enable localized field enhancement, boosting UCL intensity by several orders of magnitude; (2) optical microcavities, where resonance regulation improves luminescence efficiency and directionality; (3) dielectric superstructures, which leverage wavefront manipulation for UCL polarization control and spatial distribution modulation; (4) dynamic platforms (e.g., LC-SLMs), which realize real-time reconfiguration of UCL properties. These strategies effectively overcome intrinsic limitations of rare-earth ion 4f-4f transitions, opening new avenues for UCL in biological sensing and imaging, lasers, and optoelectronic devices[122].
Despite these advances, UCL micro-/Nanostructure regulation faces considerable challenges alongside development opportunities. Several fundamental issues must be addressed to advance the field: short effective light-matter interaction distances between excitation light and artificial micro-/nanostructures, narrow excitation wavelength ranges of conventional UC processes, and the need to optimize optical field distributions to shorten radiative lifetimes and enhance UCL[123]. A core unmet challenge lies in the perpetual trade-off between metallic field confinement/loss and dielectric Q-factor/mode volume[124]. Future advances hinge on emerging materials (2D materials, phase-change materials, and topological insulators) and hybrid designs, integrating low-loss confinement, dynamic tuning, and multifunctional synergy to transcend single-material limitations for efficient UCL under incoherent light[125].
Future progress will likely hinge on the synergistic, multi-scale integration of these complementary strategies, combining the nanoscale precision and high enhancement factors of resonant structures with the macroscopic adaptability of programmable optics to create hybrid systems that transcend the limitations of any single approach[126]. Building on this core principle, future research should focus on: designing broadband, multi-resonant composite structures (notably low-loss dielectric superstructures) integrating gradient geometric engineering and dispersion tailoring for efficient UCL under incoherent light excitation (e.g., sunlight); developing low-loss composite structures with high field enhancement and integrated photonic functionalities; exploring novel functionalities enabled by precise optical-field engineering beyond enhancement factors, including UCL for quantum information
Authors contribution
Ji Y: Conceptualization, writing-original draft, writing-review & editing.
Zhang T: Writing-review & editing.
Xu W, Dong B: Conceptualization, writing-review & editing.
Conflicts of interest
Bin Dong is an Editorial Board Member of Light Manipulation and Applications. The authors declare no conflicts of interest.
Ethical approval
Not applicable.
Consent to participate
Not applicable.
Consent for publication
Not applicable.
Availability of data and materials
Not applicable.
Funding
This work was supported by the National Key Research and Development Program of China (Grant No. 2024YFA1409904), National Natural Science Foundation of China (Grant No. 12474400, No. U24A202439, No. U2441222 and No. 62575048), the Science and Technique Foundation of Liaoning Province (Grant No. 2023JH2/101700309 and No. 2024JH3/50100028), and the Young Top Talents of Liaoning Province Xingliao Talent Plan (Grant No. XLYC2203170).
Copyright
© The Author(s) 2026.
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