Photoluminescence Enhancement Research Articles

Quantum size luminescence effect in local field enhancement of Ag NP added Er3+ glass system

This research investigates the effect of silver (Ag) addition on the photoluminescence enhancement properties of 20Li2O–5Bi2O3-(74-x)TeO2–1Er2O3-xAg glass samples, aiming to optimize luminescence for applications in optical amplifiers and laser technologies. The enhancement of luminescence properties for both upconversion 4S3/2 → 4I15/2 green band and 4F9/2 → 4I15/2 red peak luminescence observed are analyzed by quantum yield ξ and relative intensity enhancement (I/Io) parameters. The enhancement on green luminescence properties are observed with high ξgreen and I/Iogreen at x < 1 mol% which can be explained within the cavity quantum electrodynamics (CQED) framework due to very low dipolar localized surface plasmon mode volume Veff (∼10–20 × 10−22 m3) allowing stronger quantum size luminescence effect. Meanwhile, the quenching of ξgreen (0.61) at x≥ 1 mol% may indicate the weaker quantum size luminescence effect. An anomalous enhancement on red luminescence properties with high ξred (2.07) and I/Iored (1.79) at x = 1.25 mol% cannot be explained by CQED framework but from phonon-assisted energy transfer (PET) mechanism occurred due to structural changes. The near-field and far-field parameters of AgNP are simulated. Results demonstrated stronger near field electric field distribution enhancement at x = 0.5 mol% and x = 0.75 mol%. This suggests that an optimal AgNP radius exists for promoting the quantum size luminescence effect in our glass samples, falling within the range of 50.00–60.00 nm. Further supporting this conclusion, theoretical calculations using light intensity scattering efficiency (Qsca) revealed the highest values between 50.00 and 70.00 nm of AgNP radius in our glass samples.

Influence of Quadrupolar Molecular Transitions within Plasmonic Cavities.

Optical nanocavities have revolutionized the manipulation of radiative properties of molecular and semiconductor emitters. Here, we investigate the amplified photoluminescence arising from exciting a dark transition of β-carotene molecules embedded within plasmonic nanocavities. Integrating a molecular monolayer into nanoparticle-on-mirror nanostructures unveils enhancements surpassing 4 orders of magnitude in the initially light-forbidden excitation. Such pronounced enhancements transcend conventional dipolar mechanisms, underscoring the presence of alternative enhancement pathways. Notably, Fourier-plane scattering spectroscopy shows that the photoluminescence excitation resonance aligns with a higher-order plasmonic cavity mode, which supports strong field gradients. Combining quantum chemistry calculations with electromagnetic simulations reveals an important interplay between the Franck-Condon quadrupole and Herzberg-Teller dipole contributions in governing the absorption characteristics of this dark transition. In contrast to free space, the quadrupole moment plays a significant role in photoluminescence enhancement within nanoparticle-on-mirror cavities. These findings provide an approach to access optically inactive transitions, promising advancements in spectroscopy and sensing applications.

Active Learning of Ligands That Enhance Perovskite Nanocrystal Luminescence.

Ligands play a critical role in the optical properties and chemical stability of colloidal nanocrystals (NCs), but identifying ligands that can enhance NC properties is daunting, given the high dimensionality of chemical space. Here, we use machine learning (ML) and robotic screening to accelerate the discovery of ligands that enhance the photoluminescence quantum yield (PLQY) of CsPbBr3 perovskite NCs. We developed a ML model designed to predict the relative PL enhancement of perovskite NCs when coordinated with a ligand selected from a pool of 29,904 candidate molecules. Ligand candidates were selected using an active learning (AL) approach that accounted for uncertainty quantified by twin regressors. After eight experimental iterations of batch AL (corresponding to 21 initial and 72 model-recommended ligands), the uncertainty of the model decreased, demonstrating an increased confidence in the model predictions. Feature importance and counterfactual analyses of model predictions illustrate the potential use of ligand field strength in designing PL-enhancing ligands. Our versatile AL framework can be readily adapted to screen the effect of ligands on a wide range of colloidal nanomaterials.

Brilliant quantum dots’ photoluminescence from a dual-resonance plasmonic grating

Semiconductor quantum dots (QDs) have recently caused a stir as a promising and powerful lighting material applied in real-time fluorescence detection, display, and imaging. Photonic nanostructures are well suited for enhancing photoluminescence (PL) due to their ability to tailor the electromagnetic field, which raises both radiative and nonradiative decay rate of QDs nearby. However, several proposed structures with a complicated manufacturing process or low PL enhancement hinder their application and commercialization. Here, we present two kinds of dual-resonance gratings to effectively improve PL enhancement and propose a facile fabrication method based on holographic lithography. A maximum of 220-fold PL enhancement from CdSe/CdS/ZnS QDs are realized on 1D Al-coated photoresist (PR) gratings, where dual resonance bands are excited to simultaneously overlap the absorption and emission bands of QDs, much larger than those of some reported structures. Giant PL enhancement realized by cost-effective method further suggests the potential of better developing the nanostructure to QD-based optical and optoelectronic devices.

Deterministic Areal Enhancement of Interlayer Exciton Emission by a Plasmonic Lattice on Mirror.

The emergence of interlayer excitons (IX) in atomically thin heterostructures of transition metal dichalcogenides (TMDCs) has drawn great attention due to their unique and exotic optical and optoelectronic properties. Because of the spatially indirect nature of IX, its oscillator strength is 2 orders of magnitude smaller than that of the intralayer excitons, resulting in a relatively low photoluminescence (PL) efficiency. Here, we achieve the PL enhancement of IX by more than 2 orders of magnitude across the entire heterostructure area with a plasmonic lattice on mirror (PLoM) structure. The significant PL enhancement mainly arises from resonant coupling between the amplified electric field strength within the PLoM gap and the out-of-plane dipole moment of IX excitons, increasing the emission efficiency by a factor of around 47.5 through the Purcell effect. This mechanism is further verified by detuning the PLoM resonance frequency with respect to the IX emission energy, which is consistent with our theoretical model. Moreover, our simulation results reveal that the PLoM structure greatly alters the far-field radiation of the IX excitons preferentially to the surface normal direction, which increases the collection efficiency by a factor of around 10. Our work provides a reliable and universal method to enhance and manipulate the emission properties of the out-of-plane excitons in a deterministic way and holds great promise for boosting the development of photoelectronic devices based on the IX excitons.

Positive and Negative Effects under Light Illumination in Halide Perovskites

Metal halide perovskites (MHPs) have excellent characteristics and present great potential in a broad range of applications such as solar cells, light‐emitting diodes, and photodetectors. However, the light stability of devices remains an unresolved issue and has received great research attention. Under light illumination, MHPs exhibit various anomalous phenomena, such as photoluminescence (PL) enhancement, defect curing, PL blinking, and phase segregation. These phenomena are commonly considered intimately correlated with the performance and stability of MHP devices. In recent years, significant efforts have been made experimentally and theoretically toward understanding the physical origins of these anomalous effects. However, most research focuses on negative effects while the positive effects are mostly ignored. Herein, the positive effects and the negative effects of light soaking in MHPs are systematically discussed with a classification of the correlated physical mechanisms by specifically focusing on variation occurring in timescale from second to hour, corresponding to the unique ionic–electronic interaction. This intends to provide a new insight into ion effects on excellent properties of perovskites, and deep physical understanding of charge‐carrier and ion dynamics in perovskite, and theoretical guidelines for the fabrication of high‐quality and stability perovskite‐based photovoltaic and photoelectric devices.

Printable Light-Emitting Metasurfaces with Enhanced Directional Photoluminescence.

Nanoimprint lithography is gaining popularity as a cost-efficient way to reproduce nanostructures in large quantities. Recent advances in nanoimprinting lithography using high-index nanoparticles have demonstrated replication of photonic devices, but it is difficult to confer special properties on nanostructures beyond general metasurfaces. Here, we introduce a novel method for fabricating light-emitting metasurfaces using nanoimprinting lithography. By utilizing quantum dots embedded in resin, we successfully imprint dielectric metasurfaces that function simultaneously as both emitters and resonators. This approach to incorporating quantum dots into metasurfaces demonstrates an improvement in photoluminescence characteristics compared to the situation where quantum dots and metasurfaces are independently incorporated. Design of the metasurface is specifically tailored to support photonic modes within the emission band of quantum dots with a large enhancement of photoluminescence. This study indicates that nanoimprinting lithography has the capability to construct nanostructures using functionalized nanoparticles and could be used in various fields of nanophotonic applications.

Fröhlich resonance splitting in hybrid GaN nanowire-Ag nanoparticle structures

Plasmonic nanoparticles (NPs) have attracted significant attention due to their unique optical properties and broad optoelectronic and photonic applications. We investigate modifications of emission in hybrid structures formed by 60 nm silver NPs and GaN planar nanowires (NWs). Bare GaN NWs exhibit photoluminescence (PL) spectra dominated by broad bands peaking at ∼3.44 eV and ∼3.33 eV, attributed to basal plane stacking faults. In hybrids, two new narrow PL lines appear at 3.36 and 3.31 eV, resulting in PL enhancement at these energies. While the 3.36 eV line in hybrid structures can be explained using the Fröhlich resonance approximation based on the electric dipole concept, the appearance of two features at 3.36 and 3.31 eV indicates the splitting of resonance lines. This phenomenon is explained in framework of theoretical model based on the interaction of the dipole with its charge image, taking into account the quadrupole moment of the silver sphere and the quadrupole field of the charge image. A good agreement is obtained between the calculated Fröhlich resonance frequencies and the experimental PL lines in hybrid structures.

Light-induced photoluminescence enhancement in chiral CdSe quantum dot films.

Chiral quantum dots (QDs) are promising materials applied in many areas, such as chiral molecular recognition and spin selective filter for charge transport, and can be prepared by facile ligand exchange approaches. However, ligand exchange leads to an increase in surface defects and reduces the efficiencies of radiative recombination and charge transport, which restricts further applications. Here, we investigate the light-induced photoluminescence (PL) enhancement in chiral L- and D-cysteine CdSe QD thin films, providing a strategy to increase the PL. The PL intensity of chiral CdSe QD films can be significantly enhanced over 100 times by continuous UV laser irradiation, indicating a strong passivation of surface defects upon laser irradiation. From the comparative measurements of the PL intensity evolutions in vacuum, dry oxygen, air, and humid nitrogen atmospheres, we conclude that the mechanism of PL enhancement is photo-induced surface passivation with the assistance of water molecules.

Giant Photoluminescence Enhancement of Monolayer WSe2 Using a Plasmonic Nanocavity with On-Demand Resonance.

Monolayer transition metal dichalcogenides (TMDs) are considered promising building blocks for next-generation photonic and optoelectronic devices, owing to their fascinating optical properties. However, their inherent weak light absorption and low quantum yield severely hinder their practical applications. Here, we report up to 18000-fold photoluminescence (PL) enhancement in a monolayer WSe2-coupled plasmonic nanocavity. A spectroscopy-assisted nanomanipulation technique enables the assembly of a nanocavity with customizable resonances to simultaneously enhance the excitation and emission processes. In particular, precise control over the magnetic cavity mode facilitates spectral and spatial overlap with the exciton, resulting in plasmon-exciton intermediate coupling that approaches the maximum emission rate in the hybrid system. Meanwhile, the cavity mode exhibits high radiation directivity, which overwhelmingly directs surface-normal PL emission and leads to a 17-fold increase in the collection efficiency. Our approach opens up a new avenue to enhance the PL intensity of monolayer TMDs, facilitating their implementation in highly efficient optoelectronic devices.

Exploring the electro-optical properties of nematic liquid crystal through incorporation of ZnCuGaS2 core/shell quantum dots

ABSTRACT The current study focuses on elucidating the interaction mechanisms between ZnCuGaS2 quantum dots (QDs) and nematic liquid crystals (NLCs) (5CB), intending to comprehend how this interaction leads to the alteration of electro-optical properties of the host material. Various concentrations of QDs were incorporated into NLCs and investigated to examine their emission and transmittance characteristics. Remarkably, an enhancement (~68%) in photoluminescence was observed for the concentration of 0.04 wt. %, adding an intriguing aspect to the findings. A notable decrease in the threshold voltage, from 1.5 V (in pure NLC) to 0.5 V, was observed for the optimised concentration (0.04 wt. %) calculated using transmittance-voltage measurement. This sample exhibited a noteworthy improvement in optical transmission, showing an increase by 2.7 times compared to pure NLC. Fundamentally, the introduction of QDs leads to a reduction in light leakage centres and ionic impurities, consequently enhancing radiative recombination. Moreover, the memory effect of the sample was evident in the capacitance-voltage data, revealing that the NLC with QDs significantly increased the capacitance value from 290 pF to 466 pF when compared to the pure NLC. The objective of the present research is to examine the impact of QDs on NLC concerning key parameters such as mentioned above.

Photoluminescence Enhancement and Carrier Dynamics of Charged Biexciton in Monolayer WS2 Coupled with Plasmonic Nanocavity

Monolayer two-dimensional transition metal dichalcogenide (TMD)-based materials have become one of the ideal platforms for the study of multibody interactions due to their rich excitonic complexes. The coupling between optical nanocavity and material has become an important means for manipulating the optical properties of materials, but there are few studies on the coupling of nanocavities and the multi-body effect in materials. In this study, we investigate the optical properties of silver nanodisk (Ag ND) arrays covering a monolayer WS2. In the experimental sample, we observed a ~114.3-fold photoluminescence enhancement of charged biexciton in the heterostructure region, as compared to the monolayer WS2 region, a value which is much higher than those for exciton (~2.2-fold) and trion (~16.4-fold), a finding which is attributed to the Fano resonant coupling between monolayer WS2 and the Ag ND. By means of time-resolved spectroscopy, we studied the carrier dynamics in the hybrid system. Our findings reveal that resonant coupling promotes the formation and radiation recombination processes of the charged biexciton, significantly reducing the radiative recombination lifetime by ~15-fold, which is much higher than the measurement in exciton (~2-fold). Our results provide an opportunity to understand the multibody physics of coupling with nanocavities, which could facilitate the application of multi-body excitons in the fields of light-emitting devices and lasers, etc.

Reduced phonon coupling via controlled defect levels in blue emitting CsPbBr3 nanoplatelets

Metal-halide perovskites (MHPs) are promising materials for light-emitting diodes (LEDs) because of their high color purity, wide gamut, and low-cost processing. However, blue-emitting MHP LEDs exhibit low external quantum efficiencies because they are more susceptible to defect states with a larger energy bandgap compared to their green and red counterparts. Current strategies for achieving blue-emitting MHP LEDs involve compositional engineering; however, the ion migration of mixed halides imposes significant challenges related to abundant trap states. Therefore, in this study, we systematically investigated the effects of short organic and inorganic ligands with characteristic molecular structures and adjacent moieties on the optoelectronic characteristics of low-dimensional CsPbBr3 nanoplatelets (NPLs) used as blue emitters in PeLEDs. Inorganic ligand (i.e., hydrazine monohydrobromide; HZBr) treatment achieved the most significant photoluminescence enhancement (∼10 fold) while preserving crystalline morphology and colloidal stability. Temperature-dependent photophysical properties reveal that HZBr treatment eliminates band tail states arising from lower defect levels in highly confined CsPbBr3 NPLs. Therefore, it suppresses defect trapping and electron–phonon coupling, thereby reducing thermal quenching properties. The HZBr-treated NPLs were integrated into blue perovskite LEDs and demonstrated a narrow emission peak at 471 nm.

Large‐Scale Ultrastable 2D Inorganic Molecular Crystal BiBr3 and Heterostructures with Superior Photoluminescence Enhancement

AbstractIn contrast to conventional atomic crystals, two‐dimensional inorganic molecular crystals (2DIMCs) possess a unique crystal structure composed of small molecules held together by van der Waals force. Such distinctive structure grants them specific chemical and physical properties highly suitable for electronic and optoelectronic applications. However, the synthesis of 2DIMCs has posed significant challenges due to the inherent issues such as uncontrollable growth orientation stemming from their natural crystalline isotropy and poor stability resulting from the weak intermolecular connections. Addressing these obstacles, the preparation of large‐scale and highly‐stable 2DIMC BiBr3, and its heterostructure are reported here by developing crystallization orientation engineering strategies. This approach has successfully yielded centimeter‐scale 2DIMC BiBr3 with a clean and dense surface, showcasing exceptional long‐term air‐stability exceeding 80 days. Furthermore, the universal growth of large‐scale 2DIMC BiBr3 is demonstrated on diverse substrates, including SiO2, Al2O3, and MoS2 monolayers. Notably, the resultant 2D BiBr3/MoS2 heterostructure exhibits remarkable photoluminescence enhancement. This contribution paves a universal avenue for the mature synthesis of large‐scale 2DIMCs with superior stability, holding great promise for prompting their integration in practical electronic and optoelectronic devices.

Photoluminescence Enhancement in Silica-Confined Ligand-Free Perovskite Nanocrystals by Suppression of Silanol-Induced Traps and Phase Impurities.

The detriments of intrinsic silanol groups in mesoporous silica to the photoluminescence (PL) of lead halide perovskite nanocrystals (LHP NCs) confined in the template have never been determined and clearly elucidated. Here, we disclose that silanol-induced Cs+ and Br- deficiencies prompt the generation of traps and CsPb2Br5 impurities. The temperature-dependent PL spectra verify the higher energetic barrier of trap states in CsPbBr3 NCs confined in silanol-rich mesoporous silica. Femtosecond transient absorption spectra reveal the trapped state mediates a broadband photoinduced absorption and long-lived decay pathway of CsPbBr3 NCs in silanol-rich templates. A remarkable improvement (up to 160-fold) in PL quantum yields is realized by simple silanol elimination. This work demonstrates the detrimental effects of silanol sites on the PL properties of LHP NCs impregnated in mesoporous silica and provides a new perspective for the ligand-free synthesis of high-quality LHP NCs in mesoporous templates by facile impregnation for practical applications.

Shielding Effects Provide a Dominant Mechanism in J-Aggregation-Induced Photoluminescence Enhancement of Carbon Nanotubes.

The unique photophysical properties of single-walled carbon nanotubes (SWCNTs) exhibit great potential for bioimaging applications. This led to extensive exploration of photosensitization methods to improve their faint shortwave infrared (SWIR) photoluminescence. Here, we report the mechanisms of SWCNT-assisted J-aggregation of cyanine dyes and the associated photoluminescence enhancement of SWCNTs in the SWIR spectral region. Surprisingly, we found that excitation energy transfer between the cyanine dyes and SWCNTs makes a negligible contribution to the overall photoluminescence enhancement. Instead, the shielding of SWCNTs from the surrounding water molecules through hydrogen bond-assisted macromolecular reorganization of ionic surfactants triggered by counterions and the physisorption of the dye molecules on the side walls of SWCNTs play a primary role in the photoluminescence enhancement of SWCNTs. We observed 2 orders of magnitude photoluminescence enhancement of SWCNTs by optimizing these factors. Our findings suggest that the proper shielding of SWCNTs is the critical factor for their photoluminescence enhancement, which has important implications for their application as imaging agents in biological settings.

Photoluminescence Enhancement in Silica‐Confined Ligand‐Free Perovskite Nanocrystals by Suppression of Silanol‐Induced Traps and Phase Impurities

AbstractThe detriments of intrinsic silanol groups in mesoporous silica to the photoluminescence (PL) of lead halide perovskite nanocrystals (LHP NCs) confined in the template have never been determined and clearly elucidated. Here, we disclose that silanol‐induced Cs+ and Br− deficiencies prompt the generation of traps and CsPb2Br5 impurities. The temperature‐dependent PL spectra verify the higher energetic barrier of trap states in CsPbBr3 NCs confined in silanol‐rich mesoporous silica. Femtosecond transient absorption spectra reveal the trapped state mediates a broadband photoinduced absorption and long‐lived decay pathway of CsPbBr3 NCs in silanol‐rich templates. A remarkable improvement (up to 160‐fold) in PL quantum yields is realized by simple silanol elimination. This work demonstrates the detrimental effects of silanol sites on the PL properties of LHP NCs impregnated in mesoporous silica and provides a new perspective for the ligand‐free synthesis of high‐quality LHP NCs in mesoporous templates by facile impregnation for practical applications.

Plasmonic Diamond Membranes for Ultrafast Silicon Vacancy Emission.

Silicon vacancy centers (SiVs) in diamond have emerged as a promising platform for quantum sciences due to their excellent photostability, minimal spectral diffusion, and substantial zero-phonon line emission. However, enhancing their slow nanosecond excited-state lifetime by coupling to optical cavities remains an outstanding challenge, as current demonstrations are limited to ∼10-fold. Here, we couple negatively charged SiVs to sub-diffraction-limited plasmonic cavities and achieve an instrument-limited ≤8 ps lifetime, corresponding to a 135-fold spontaneous emission rate enhancement and a 19-fold photoluminescence enhancement. Nanoparticles are printed on ultrathin diamond membranes on gold films which create arrays of plasmonic nanogap cavities with ultrasmall volumes. SiVs implanted at 5 and 10 nm depths are examined to elucidate surface effects on their lifetime and brightness. The interplay between cavity, implantation depth, and ultrathin diamond membranes provides insights into generating ultrafast, bright SiV emission for next-generation diamond devices.

Extremely Enhanced Photoluminescence in MoS2-Derived Quantum Sheets.

Molybdenum disulfide (MoS2) quantum sheets (QSs) are attractive for applications due to their tunable energy band structures and optical and electronic properties. The photoluminescence quantum yield (PLQY) of MoS2 QSs achieved by mechanical and liquid exfoliation and chemical vapor deposition is low. Some studies have reported that chemical treatment and elemental doping can improve the PLQY of transition metal dichalcogenides (TMDs), but this is limited by complex instruments and reactions. In this study, a heat treatment method based on a polar solvent is reported to improve the PLQY and photoluminescence (PL) intensity of MoS2 QSs at room temperature. The absolute PLQY of treated MoS2 QSs is increased to 18.5%, and the PL intensity is increased by a factor of 64. This method is also effective for tungsten disulfide (WS2) QSs. The PL enhancement of QSs is attributed to oxidation of the edges. Such passivation/deformation of MoS2 QSs facilitates the radiative route rather than the nonradiative route, resulting in extreme enhancement of the PL. Our work could provide novel insights/routes toward the PL enhancement of TMD QSs.

Aqueous synthesis of photoluminescence enhanced CuInS2/ZnS quantum dots via the facile hot injection growth of AgInS2 interlayer

In this study, the hot injection of Ag ions to enhance the PL performance of aqueous-phase CuInS2/ZnS quantum dots (QDs) via the formation of AgInS2 interlayer is first developed. Different amount of Ag doping by hot injection realizes the precise tuning of the peak wavelength from 649 nm to 684 nm, while the photoluminescence quantum yield is also improved from 14.79% to 26.8% due to the formation of the AgInS2 interlayer on the surface of CuInS2 QDs. The results of various characterizations demonstrate the formation of AgInS2 interlayer and explain the enhanced PL performance of CuInS2 QDs. This will expand the understanding of the PL enhancement of the aqueous-phase CuInS2/ZnS QDs and solidify the foundation for subsequent practical research to further realize the potential of aqueous CuInS2 QDs.