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All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Achieving Multimodal and Multicolor Luminescence in LaAlO 3 :Pr 3+ , Gd 3+ via Trap Engineering and Energy Transfer

Achieving multimodal luminescence within a single phosphor is vital for multifunctional applications but remains challenging due to complex color tuning and trap engineering. In this study, we report Pr 3+ and Gd 3+ co‐doped LaAlO 3 (LAO:PG) phosphors, designed through careful modulation of multilevel traps and Pr 3+ → Gd 3+ energy transfer dynamics. These materials exhibit diverse luminescence modes, including down‐conversion luminescence (DCL), up‐conversion luminescence (UCL), persistent luminescence (PersL), optically stimulated luminescence (OSL), and thermally stimulated luminescence (TSL) across a wide spectral range. Unlike previously studied Pr 3+ ‐doped LAO, the co‐doped LAO:PG shows DCL in both UV‐visible and NIR regions and displays ultraviolet‐C UCL under visible excitation. Notably, we observe, for the first time, PersL lasting several minutes in these phosphors—an improvement over the non‐PersL behavior of Pr 3+ ‐only doped LAO. Additionally, the LAO:PG phosphors exhibit strong OSL response. TSL analysis reveals five distinct trap levels linked to these properties. Density functional theory calculations further correlate intrinsic defects to these traps, supporting a proposed mechanism for the observed multimodal luminescence. These findings highlight LAO:PG as a promising platform for developing advanced phosphors with integrated luminescence modes, paving the way for future applications in data storage, phototherapy, and anti‐counterfeiting technologies.

Chemistry↗
DOE OSTI2026

Entropy-defect synergy for dual luminescence mechanism in spinel: Time-resolved anti-counterfeiting and fingerprint visualization

Multimodal luminescent materials, while promising for anti-counterfeiting, often lack dynamic time-dependent responses and controllable spatial distribution, limiting their encryption capabilities in the spatiotemporal dimension. Here, this work presents a coordinated control strategy based on entropy and defect engineering, and uses a backpropagation (BP) neural network for material screening to successfully prepare spinel Mg 0.8 (Fe 0.04 Co 0.04 Ni 0.04 Cu 0.04 Zn 0.04 )Cr 2 O 4 (MgA 5 CO) phosphors with time-dependent dynamic luminescence behavior. This phosphor simultaneously activated the d-d transition luminescence (∼618 nm) derived from Co 2+ /Cr 3+ and the defect luminescence (∼398 nm) related to zinc vacancies (V Zn ) in a single-phase solid solution. The phosphor exhibits a time-dependent color evolution from pink to purple under fixed-wavelength excitation, due to the different excited-state dynamics and decay lifetimes associated with the d-d transition and defect luminescence. Structural characterization and spectral analysis confirmed the existence of V Zn and its significant role in defect luminescence process. The fluorescent and dynamic luminescent properties of entropy-based spinel oxide enable its use in advanced anti-counterfeiting applications like fingerprint recognition and color-changing dedicated anti-counterfeiting mark, showing promise in high-end and time-dynamic anti-counterfeiting fields. This research not only developed a new type of fluorescent dynamic anti-counterfeiting material, but also provided a new idea for constructing advanced optical functional materials with multiple luminescence mechanisms.

Defect project↗
DOE OSTI2024

Trap‐Engineering the Persistent Luminescence of Ca 3 Ga 4 O 9 :Tb 3+ via Al 3+ Substitution for Optical Data Storage

Abstract Optically stimulated luminescence (OSL) materials hold great potential for optical data storage (ODS) and anticounterfeiting applications. Nevertheless, the scarcity of suitable luminescent materials with deep‐level traps remains a significant obstacle. Herein, a host substation strategy have been employed to tune the persistent luminescence (PersL) and OSL properties of Ca 3 Ga 4 O 9 :Tb 3+ by Al 3+ substitution through trap engineering and demonstrated their potential. Specifically, the photoluminescence of the Ca 2.985 (Ga 1‐y% Al y% ) 4 O 9 :0.5%Tb 3+ of Tb 3+ is first investigated due to its different occupancies of Ca 2+ . The influence of host substitution on the crystal structure, trap depth, trap density, PersL, and OSL properties have further investigated. A series of strong PersL and OSL peaks from the Ca 2.985 (Ga 1‐y% Al y% ) 4 O 9 :0.5%Tb 3+ with bluish‐green emissions have been observed. The Ca 2.985 (Ga 1‐y% Al y% ) 4 O 9 :0.5%Tb 3+ have shown controllable photon release upon thermal and optical stimuli, enhancing their performance for ODS. Thermally stimulated luminescence suggests that vacancy and defect concentrations inside the Ca 3‐x% (Ga 1‐y% Al y% ) 4 O 9 :x%Tb 3+ can be manipulated by Tb 3+ doping and Al 3+ substitution, which ultimately leads to the formation of deep traps and a broad distribution of traps with increased deep trap concentration. The work demonstrates that trap engineering through Al 3 ⁺ substitution is an effective method for tuning PersL and OSL properties of Ca 2.985 (Ga 1‐y% Al y% ) 4 O 9 :0.5%Tb 3+ for ODS.

Abeywickrama, Thulitha M. [Department of Chemistry↗
DOE OSTI2025

High-pressure Cr 3+ luminescence and Raman spectroscopy of a natural MgAl 2 O 4 spinel to ∼60 GPa

Cr 3+ luminescence and Raman spectroscopy of a natural spinel were collected up to ∼60 GPa at ambient temperature using a Ne or a 4:1 methanol-ethanol mixture as the pressure transmitting media. Here, in the Ne experiments above ∼40 GPa, and in the 4:1 methanol–ethanol experiments above ∼20 GPa, all luminescence emission lines shift non-linearly, and by 59 GPa the spectra are broadened and are significantly changed. The Raman modes shift smoothly to higher frequencies with pressure, with a slight change in slope above 40 GPa, with no kinks or discontinuities. By ∼60 GPa, only the most intense Eg mode remains resolvable, appearing broadened and reduced in intensity. The change in slope in the Raman modes and luminescence bands may be due to a change in the compression mechanism of spinel. When spinel was decompressed from 40 GPa all changes were fully reversible; however, when the samples were decompressed from 54 to 60 GPa in Ne and 59 GPa in 4:1 methanol-ethanol the spectra were irreversibly changed. The change in the luminescence spectra and the Raman spectra are likely due to a pressure induced disorder of the anions or partial amorphization between 40 and 60 GPa.

Cr3+↗
DOE OSTI2025

Room temperature crystal field splitting of curium resolved by circularly polarized luminescence spectroscopy

Coordination of Cm(III) with a chiral decadentate ligand N,N,N',N'-tetrakis[(6-carboxypyridin-2-yl)methyl]-1,2-diaminocyclohexane (tpadac) generated complexes with strong luminescence allowing for the unprecedented measurement of well-resolved Cm(III) circularly polarized luminescence spectra. Quantitative resolution of the electronic structure of the [Cm(tpadac)][K] complexes was achieved at room temperature, highlighting the strength of the combination of luminescence and circularly polarized luminescence spectroscopies to unravel the fundamental electronic structure of Cm(III). These results are a clear demonstration that these spectroscopies are powerful yet simple tools for the fundamental understanding of electronic structure, which opens the door to future investigations of other Cm(III) complexes in geometries relevant to nuclear applications, and even other 5f-elements.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Self‐Trapped Hole Migration and Defect‐Mediated Thermal Quenching of Luminescence in α‐ and β‐Ga 2 O 3

Gallium oxide (Ga 2 O 3 ) is a promising ultrawide bandgap semiconductor for next-generation power electronics and optoelectronic devices. Here, temperature-dependent and polarization-resolved photoluminescence excitation spectroscopy data, complemented by hybrid-functional first-principles calculations, are presented, and a microscopic model is derived that explains the interplay of hole migration, defect trapping, and carrier recombination at defects underlying thermal quenching phenomena in α- and β-Ga 2 O 3 . In α-Ga 2 O 3 , the UV emission is attributed to self-trapped holes, while the blue luminescence arises from defect-related processes, including gallium split vacancies and their defect complexes. Calculations reveal an energy barrier of 88 meV for self-trapped hole migration in α-Ga 2 O 3 , consistent with activation energies from temperature-dependent photoluminescence. This enables efficient trapping by defects, enhancing blue luminescence and quenching UV emission. In β-Ga 2 O 3 , a higher migration barrier of 0.36 eV reduces the defect trapping, allowing the UV self-trapped hole emission to remain intense, with blue luminescence emerging only at elevated temperatures. These results establish a direct link between self-trapped hole migration, defect trapping, and thermal quenching of emission in both phases. The insights advance the understanding of carrier dynamics in ultrawide bandgap oxides and may guide defect engineering for high-performance functional devices.

Hajizadeh, Nima [Leibniz-Institut im Forschungsver↗
DOE OSTI2024

Fabrication of metal-organic framework thin films for luminescent sensing applications

Metal−organic frameworks (MOFs) have emerged as an exciting material class due to their nearly infinite design space: an inexhaustible combination of metal centers, organic linkers, and reaction conditions may be leveraged to obtained desired optical, physical, and chemical properties. This rich synthetic diversity enables properties such as pore dimensions and functionality to be rationally tailored for highly selective and sensitive detection of target analytes. Luminescent MOF-based sensors in particular offer advantages including low cost, portability, and ease-of-use. Often, performance is maximized by utilizing the luminescent MOF in thin film form, for example by integrating the film onto an optical fiber, yet the synthesis of high-quality MOF thin films often requires tedious, expensive, and/or slow approaches. Here, we demonstrate a rapid, simple strategy for growing copper MOFs using metal oxide templates; the concept is first demonstrated with a well-studied system, copper-1,3,5-benznetricarboxylate (Cu-BTC). Variables such as the choice of solvent, pH, and the choice of the copper salt anion all govern thin film quality. We then extend this method to synthesize a solvent and metal-responsive copper MOF that is particularly effective at detecting aluminum, an economically critical metal, at trace concentrations using a fully portable luminescence spectrometer. Taken together, this work demonstrates a convenient, versatile, and sustainable method for developing high quality MOF thin film-based optical sensors.

Crawford, Scott↗
DOE OSTI2025

Orchestrating Spontaneous Emission With Metasurfaces: Recent Advances in Engineering Thermal, Luminescent, and Quantum Emissions

Metasurfaces have emerged as powerful tools for controlling spontaneous emission, offering unprecedented control over light-matter interactions at sub-wavelength scales. While metasurfaces are traditionally utilized for shaping coherent electromagnetic waves, they have recently extended their capabilities to control incoherent or spontaneous emission. This examines review how metasurfaces can enhance and precisely control properties of thermal, luminescent, and quantum emission. In thermal emission, metasurfaces enable control over spatial, temporal, and spin coherence, offering new possibilities for applications such as energy harvesting, radiative cooling and heat assisted ranging and detection. For luminescent emission, metasurfaces significantly improve emission rates, quantum efficiency, and directionality, driving innovations in lighting and display technologies. For controlling quantized spontaneous emission, metasurfaces are instrumental in enhancing single-photon sources and enabling novel functionalities in quantum states through photon-pair generation, which is vital for quantum communication, meteorology, and computing. Here, despite these advancements several challenges to increase the operational bandwidths, accelerate and develop simulation strategies, and fabrication complexities persist. Emerging trends are also discussed, such as dynamic metasurfaces and their integration with nanophotonic platforms, which could further expand the capabilities of light-emitting metasurfaces.

Luminescence↗
DOE OSTI2024

Self‐Standing Chiral Covalent Organic Framework Thin Films with Full‐Color Tunable Guest‐Induced Circularly Polarized Luminescence

Abstract Exploring self‐standing chiral covalent organic framework (COF) thin films with controllable circularly polarized luminescence (CPL) is of paramount significance but remains a challenging task. Herein, we demonstrate the first example of self‐standing chiral COF films employing a polymerization‐dispersion‐filtration strategy. Pristine, low‐quality chiral COF films were produced by interfacial polymerization and then re‐dispersed into COF colloidal solutions. Via vacuum assisted assembly, these COF colloids were densely stacked and assembled into self‐standing, pure chiral COF films ( L‐ / D‐ CCOF‐F) that were transparent, smooth, crack‐free and highly crystalline. These films were tunable in thicknesses, areas, and roughness, along with strong diffuse reflectance circular dichroism (DRCD) and cyan CPL signals, showing an intrinsic luminescence asymmetric factor ( g lum ) of ~4.3×10 −3 . Furthermore, these COF films served as host adsorbents to load various achiral organic dye guests through adsorption. The effective chiral transfer and energy transfer between CCOF‐F and achiral fluorescent dyes endowed the dyes with strong chirality and tunable DRCD, resulting in intense, full‐color‐tunable solid‐state CPL. Notably, the ordered arrangement of dye guest molecules within the preferentially oriented chiral pores of CCOF‐F contributed to an amplified | g lum | factor of up to 7.2×10 −2 , which is state‐of‐the‐art for COF‐based CPL materials. This work provides new insights into the design and fabrication of self‐standing chiral COF films, demonstrating their great potential for chiroptical applications.

Tang, Xihao↗
DOE OSTI2025

Pressure–Modulated Luminescence Enhancement and Quenching in a Hydrogen–Bonded Organic Framework

Light emission in the solid state is central for illumination, sensing, and imaging applications. Unlike luminescence in dilute solutions, where the excited states are unimolecular in nature, intermolecular interaction plays a significant role in the quantum yield of solid-state luminophores, manifested as competing aggregation-caused quenching (ACQ) and aggregation-induced enhancement (AIE). Both effects are extensively studied in various systems; however, it remains unclear how their competition depends on molecular conformation and intermolecular stacking. Here the direct observation of pressure-modulated AIE-ACQ competition in a crystalline hydrogen-bonded organic framework (HOF) is reported. Using in situ spectroscopies and computational modeling, the intramolecular vibration and intermolecular π–π stacking directly responsible for the non-radiative decay of the excited state are identified. The extent of these two contributions is modulated by hydrostatic pressure and guest molecules in the HOF pores. Furthermore, this work demonstrates a physically neat model system to understand and control solid-state luminescence, and a potential material platform for piezoluminescent sensing.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Luminescent Zn 2 GeO 4 :Mn 2+ Nanoparticles with High Quantum Yield for Salivary Protein Detection

Zinc germanate doped with Mn 2+ (Zn 2 GeO 4 :Mn 2+ ) is known to be a green luminescence phosphor with many applications in biosensing and bioimaging. This study presents a simple method for creating small size Zn 2 GeO 4 :Mn 2+ nanoparticles using a combination of the coprecipitation–molten salt synthesis method. These nanoparticles exhibit bright green luminescence under UV excitation. After surface functionalization, these nanoparticles were then used to develop a fluorescence resonance energy transfer (FRET)-based immunoassay. This immunoassay shows a detection range of 5–20 ng/mL of C-reactive protein (CRP), which suggests its potential for simple solution CRP detection and broader applications in protein biosensing.

biosensing↗
DOE OSTI2024

Advances in the photon avalanche luminescence of inorganic lanthanide-doped nanomaterials

Photon avalanche (PA)—where the absorption of a single photon initiates a ‘chain reaction’ of additional absorption and energy transfer events within a material—is a highly nonlinear optical process that results in upconverted light emission with an exceptionally steep dependence on the illumination intensity. Over 40 years following the first demonstration of photon avalanche emission in lanthanide-doped bulk crystals, PA emission has been achieved in nanometer-scale colloidal particles. The scaling of PA to nanomaterials has resulted in significant and rapid advances, such as luminescence imaging beyond the diffraction limit of light, optical thermometry and force sensing with (sub)micron spatial resolution, and all-optical data storage and processing. In this review, we discuss the fundamental principles underpinning PA and survey the studies leading to the development of nanoscale PA. Finally, we offer a perspective on how this knowledge can be used for the development of next-generation PA nanomaterials optimized for a broad range of applications, including mid-IR imaging, luminescence thermometry, (bio)sensing, optical data processing and nanophotonics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Technical Routes to Achieve High Circular Polarized Luminescence in Chiral Perovskites: A Mini‐Review

Chiral hybrid organic-inorganic perovskites (HOIPs) have emerged as promising materials for optoelectronic and spintronic applications, leveraging unique properties such as circularly polarized luminescence (CPL), circularly polarized nonlinear optical (NLO) emission, and chiral-induced spin selectivity (CISS). However, challenges remain in stabilizing these materials under environmental stresses and precisely controlling chirality for scalable use. This review summarizes five main strategies to induce chirality in HOIPs, i.e., direct incorporation of chiral cations, surface modification with chiral ligands, ion doping, template-induced chirality, and chiral metasurfaces. Each approach offers distinct advantages for optimizing CPL efficiency and device stability, paving the way for next-generation applications in CPL detectors, information encryption, spintronic devices, etc.

14 SOLAR ENERGY↗
DOE OSTI2025

Optimizing energy yield of monolithic perovskite/silicon tandem solar cells in real-world Conditions: The impact of luminescent coupling

Efficient light management is key to maximizing power conversion efficiency (PCE) in monolithic perovskite/silicon tandem solar cells. Achieving peak efficiency requires closely matched current generation in all junctions, especially in integrated configurations. However, real-world conditions vary significantly due to factors such as sunlight spectrum, diffuse-to-direct sunlight ratio, angular distribution of light, subcell temperature coefficients, and ground reflection. This study introduces a comprehensive optical and device simulation to optimize perovskite/silicon tandem cells, considering experimental luminescent coupling (LC) efficiency and its dependence on working conditions, alongside variations in radiative recombination, effect of temperature on absorptivity spectra, and cloud cover. Our results show potential energy yield improvements of up to 1.4 % with LC, based on current perovskite radiative recombination records, and up to 4 % with direct bandgap materials. Although radiative recombination's dependence on excitation intensity reduces output power and requires thicker absorbers, LC compensates for these losses. LC also lowers the optimized bandgap for the perovskite top cell from 1.72 eV to 1.64–1.68 eV, or even lower in regions with redshifted irradiance. Additionally, optimization revealed that thinner silicon bottom cells require a higher perovskite top cell bandgap, impacting the balance between fabrication cost and cell stability.

14 SOLAR ENERGY↗
DOE OSTI2025

Near-IR Luminescence Tuning in a Series of Chalcogenophene Carboxylate-Decorated Neodymium Dimers

Here, the solvothermal synthesis of a series of Nd dimers decorated with various chalcogenophene carboxylates and 2,2':6',2"-terpyridine of the general formula, [Nd 2 (µ-XC 5 H 3 O 2 ) 2 (XC 5 H 3 O 2 ) 4 (N 3 C 15 H 11 ) 2 (H 2 O) 2 ] where X = O, S, Se, and Te, is reported. The solid-state structures were characterized using single-crystal X-ray diffraction (scXRD) and all the complexes are isomorphous, despite substitution of the heterocyclic chalcogen; phase purity was confirmed via powder X-ray diffraction (pXRD). Vibrational spectroscopy was collected and correlations between chalcogen identity and the binding strength of the carboxylate groups of the chalcogenophene ligands with each metal center were shown to be independent of chalcogen identity. All four complexes displayed Nd(III)-based near-IR luminescence and exhibited ligand-sensitized emission. Varying the chalcogenophene chromophore enabled tuning of the sensitizing triplet state energy level, as evidenced by an 8-fold increase in the sensitization of the TeCA-decorated dimer relative to the other chalcogenophene congeners. This behavior was rationalized by comparing the Nd(III) acceptor and ligand donor states across the series. The donor triplet state of each ligand was estimated via low-temperature (77 K) phosphorescence measurements from 1:1 mixtures with Gd(III); these were found to be 24,631 cm –1 for furan-2-carboxylic acid (FCA), 23,764 cm –1 for thiophene-2-carboxylic acid (TCA), 22,548 cm –1 for selenophene-2-carboxylic acid (SeCA), and 21,186 cm –1 for tellurophene-2-carboxylic acid (TeCA). The greater sensitization efficiency of TeCA is the result of well-matched ligand donor and metal acceptor levels and thus suppression of nonradiative back-energy transfer. More broadly, triplet energy level information for these ligands serves as a guide for future application to other target metals based on the electronic properties necessary to effect efficient sensitization.

Coordination Chemistry↗
DOE OSTI2025

Structural and Electronic Tuning of Luminescent Zn II Complexes Based on an o -Terphenyl Ligand Motif

Here, the structural and photophysical properties of five chiral Zn complexes incorporating a carbazolate (Cz) donor that is electronically decoupled from a pyridyl acceptor by an ortho -connection to a bridging phenylene group are presented. The bidentate ligand in the unsubstituted bis-ligated parent complex was methylated at key positions to constrain the torsional freedom of the donor/acceptor moieties, resulting in three structurally modified bis-ligated derivatives, all exhibiting energy gaps between the singlet and triplet excited states (ΔE ST ) between 22 and 27 meV. Methylation improves the photoluminescence quantum yield (up to 30% in solution), while the low ΔE ST of these complexes allows for dual-emission properties in all of the bis-ligated derivatives. Structural modification of the Cz/pyridyl ligand was also investigated by linking the unsubstituted bidentate ligand to generate a tetradentate, tetrapodal ligand. The solution-state structure of the tetradentate ligand is similar in its free and ligated forms, featuring a binding site reminiscent of enzymes and metal-sequestering ligands. The resulting tetradentate complex [Zn(N 2 R 2 )] shows enhanced through-bond conjugation, increasing the ΔE ST to 89 meV, thereby eliminating the dual-emission characteristics of the bis-ligated complexes. Furthermore, this complex shows a 50-fold improvement in hydrolytic stability in organic solution relative to the parent complex. These compounds and their analyses are intended to enrich the understanding of compounds exhibiting through-space charge transfer and guide the search for earth-abundant metal complexes for applications in photosensitization and luminescence.

aromatic compounds↗
DOE OSTI2026

Performance of Quantum Dot Coatings for Luminescent Solar Concentrating Windows: Cooperative Research and Development Final Report, CRADA Number CRD-16-00640

The two major outcomes from this DOE supported collaboration between UbiQD and NREL were: 1) an expert analysis/modeling of the expected performance and cost of luminescent solar concentrating windows with quantum dot coatings, and 2) critical R&D characterization of materials and device performance analysis using equipment and processes that are too expensive for UbiQD to perform in-house. The latter also included third-party validation of the device performance with an NREL-certified conversion efficiency that was ultimately published. (see ACS Energy Lett. 2018 and recently ACS Appl. Energy Mater. 2020).

14 SOLAR ENERGY↗
DOE OSTI2025

Lifting Triplet Degeneracy Through Organic‐Cation Driven Structural Perturbation to Modulate Luminescence of Sb 3+ ‐Doped Double Perovskite

The spin-orbit coupling (SOC) and the Jahn-Teller effect (JTE) alter the orbital degeneracy in materials, leading to unique optical, electronic, and magnetic properties essential in spintronics, quantum computing, and light-emitting diodes (LEDs). Here, the study employs luminescent p-xylylenediammonium (PXA) instead of Cs+ in Cs2NaInCl6 to yield 2D Sb3+-doped (PXA)2NaInCl8 double perovskite and demonstrates a non-degenerate triplet state resulting from enhanced JTE in the strong SOC regime, featuring distinct emission centers. Consequently, a broadband emission from both PXA and [SbCl6]3− spans the entire spectrum (350–750 nm), representing a rare single-source multi-emissive 2D perovskite. With in-depth comparative structural, temperature-dependent photo-physical, and theoretical studies, it is elucidated that the synergistic effect of SOC and JTE on the Eg and T2g lattice modes modulate the electronic structure of [SbCl6]3− by splitting the doubly degenerate E levels of 3 T$^{*}_{1u}$ into non-degenerate states. The physical model, supported by theoretical studies, explains the energy level splitting required to realize two kinds of radiative minima in the relaxed excited state.

36 MATERIALS SCIENCE↗