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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 235 records · Page 13
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Realizing Wide-Gamut Human-Centric Display Lighting with K 3 AlP 3 O 9 N:Eu 2+

Abstract Computers, televisions, and smartphones are revolutionized by the invention of InGaN blue light-emitting diode (LED) backlighting. Yet, continual exposure to the intense blue LED emission from these modern displays can cause insomnia and mood disorders. Developing “human-centric” backlighting that uses a violet-emitting LED chip and a trichromatic phosphor mixture to generate color images is one approach that addresses this problem. The challenge is finding a blue-emitting phosphor that possesses a sufficiently small Stokes’ shift to efficiently down-convert violet LED light and produce a narrow blue emission. This work reports a new oxynitride phosphor that meets this demand. K 3 AlP 3 O 9 N:Eu 2+ exhibits an unexpectedly narrow (45 nm, 2206 cm -1 ), thermally robust, and efficient blue photoluminescence upon violet excitation. Computational modeling and temperature-dependent optical property measurements reveal that the narrow emission arises from a rare combination of preferential excitation and site-selective quenching. The resulting chromaticity coordinates of K 3 AlP 3 O 9 N:Eu 2+ lie closer to the vertex of the Rec. 2020 than a blue LED chip and provides access to ≈10% more colors than a commercial tablet when combined with commercial red- and green-emitting phosphors. Alongside the wide gamut, tuning the emission from the violet LED and phosphor blend can reduce blue light emissions to produce next-generation, human-centric displays.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Luminescent MOFs (LMOFs): recent advancement towards a greener WLED technology

The replacement of traditional incandescent, halogen and fluorescent lamps by white light emitting diodes (WLEDs) is expected to reduce the global electricity consumption by one-third by 2030, according to the US Department of Energy. The current WLED technology uses rare-earth element (REE) based phosphor materials, which, not only is cost-intensive but also constitutes an environmental concern. Hence, researchers are in a quest for a new-generation of opto-electronic materials that can replace the conventional phosphors in WLEDs and thus aim towards a cleaner and more energy efficient lighting technology for the future. Luminescent metal–organic frameworks (LMOFs) have recently emerged as a new sub-class of MOFs which have demonstrated enormous potential for applications in sensing, imaging, optoelectronics and in solid-state lighting (SSL) technology. LMOFs could be game changers as lighting phosphors due to advantages such as high luminescence quantum yield, tunable excitation and emission which can be achieved by rational design and optimization of metal centers, linkers, and the guest molecules, facile fabrication into devices, and structural robustness. These clear advantageous features of LMOFs make them score over other contemporary materials, and enable them to be futuristic phosphor materials for WLED technology. Here, in this feature article, we will provide an overview of the most recent developments of LMOF-based phosphor materials for SSL with a special focus on WLED technology. The emphasis will be centered around REE-free LMOFs, as the aim is to direct the attention of the readers towards a more viable and greener lighting technology.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Laboratory Validation of Integrated Lighting Systems Retrofit Performance and Energy Savings

Light-emitting diodes (LED) fixtures and lamps have emerged as leading technologies for general illumination and are a well-established energy efficiency retrofit measure in commercial buildings (from around 2% of installed fixtures and lamps in 2013 to 28% by 2020). Retrofit approaches that integrate elements, such as networked controls, daylight dimming, and advanced shade technologies lag in comparison. Integrated retrofits have been shown to increase savings over single end-use retrofits, but are perceived as higher complexity and risk. More validation of integrated lighting system performance is needed. This study presents results from laboratory testing of three packages combining fixtures, networked controls, task tuning, and daylight dimming, advanced shades, and lighting layout changes. We characterize performance in perimeter open-office zones, finding energy savings from 20% for daylight dimming and automated shades (no LED retrofit) to over 70% for LED retrofits with advanced controls and shades or lighting layout changes. We present some implementation details, including lessons learned from installation and commissioning in the laboratory setting. We also discuss cost-benefit analysis approaches for the types of packages presented, including the need to quantify and incorporate energy and non-energy benefits for advanced shades packages, which enhance occupant comfort but add significant cost.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2020

Luminescence Quenching via Deep Defect States: A Recombination Pathway via Oxygen Vacancies in Ce-Doped YAG

Luminescence quenching via nonradiative recombination channels limits the efficiency of optical materials such as phosphors and scintillators and therefore has implications for conversion efficiency and device lifetimes. In materials such as Ce-doped yttrium aluminum garnet (YAG:Ce), quenching shows strong dependence on both temperature and activator concentration, limiting the fabrication of high-intensity white-light emitting diodes with high operating temperatures. Here, we reveal by means of first-principles calculations an efficient recombination mechanism in YAG:Ce that involves oxygen vacancies and gives rise to thermally activated concentration quenching. We demonstrate that the key requirements for this mechanism to be active are localized states with strong electron-phonon coupling. These conditions are commonly found for intrinsic defects such as anion vacancies in wide band gap materials. The present findings are therefore relevant to a broad class of optical materials and shine light on thermal quenching mechanisms in general.

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

The Influence of Structural Dynamics in Two-Dimensional Hybrid Organic–Inorganic Perovskites on Their Photoluminescence Efficiency — Neutron Scattering Analysis

Two-dimensional hybrid organic–inorganic perovskites (HOIPs) have emerged as promising materials for light-emitting diode applications. In this study, by using time-of-flight neutron spectroscopy we identified and quantitatively separated the lattice vibrational and molecular rotational dynamics of two perovskites, butylammonium lead iodide (BA)2PbI4 and phenethyl-ammonium lead iodide (PEA) 2 PbI 4 . By examining the corresponding temperature dependence, we found that the lattice vibrations, as evidenced by neutron spectra, are consistent with the lattice dynamics obtained from Raman scattering. We revealed that the rotational dynamics of organic molecules in these materials tend to suppress their photoluminescence quantum yield (PLQY) while the vibrational dynamics did not show predominant correlations with the same. Additionally, we observed photoluminescence emission peak splitting for both systems, which becomes prominent above certain critical temperatures where the suppression of PLQY begins. This study suggests that the rotational motions of polarized molecules may lead to a reduction in exciton binding energy or the breaking of degeneracy in exciton binding energy levels, enhancing non-radiative recombination rates, and consequently reducing photoluminescence yield. These findings offer a deeper understanding of fundamental interactions in 2D HOIPs and could guide the design of more efficient light-emitting materials for advanced technological applications.

Rajeev, Haritha Sindhu [Univ. of Virginia, Charlot↗
DOE OSTI2020

Ultrafast Exciton Transport with a Long Diffusion Length in Layered Perovskites with Organic Cation Functionalization

Abstract Layered perovskites have been employed for various optoelectronic devices including solar cells and light‐emitting diodes for improved stability, which need exciton transport along both the in‐plane and the out‐of‐plane directions. However, it is not clear yet what determines the exciton transport along the in‐plane direction, which is important to understand its impact toward electronic devices. Here, by employing both steady‐state and transient photoluminescence mapping, it is found that in‐plane exciton diffusivities in layered perovskites are sensitive to both the number of layers and organic cations. Apart from exciton–phonon coupling, the octahedral distortion is revealed to significantly affect the exciton diffusion process, determined by temperature‐dependent photoluminescence, light‐intensity‐dependent time‐resolved photoluminescence, and density function theory calculations. A simple fluorine substitution to phenethylammonium for the organic cations to tune the structural rigidity and octahedral distortion yields a record exciton diffusivity of 1.91 cm 2 s −1 and a diffusion length of 405 nm along the in‐plane direction. This study provides guidance to manipulate exciton diffusion by modifying organic cations in layered perovskites.

Xiao, Xun↗
DOE OSTI2020

Metalorganic chemical vapor deposition of ZnGeN 2 films on GaN: effects of cation stoichiometry on surface morphology and crystallinity

Novel optoelectronic device designs based on the heterostructures of III-N and II-IV-N 2 are promising to advance device performance significantly. For example, by utilizing InGaN-ZnGeN 2 quantum well (QW) structures instead of pure InGaN, the band structure engineering in the QW active region can lead to improved electron-hole wavefunction overlap, and thus enhance the radiative efficiency for photon generation. These novel heterostructures have great potential to address the current challenge of low quantum efficiency in InGaN QW based light emitting diodes emitting in green and beyond. The materials development of ZnGeN 2 is still at an early stage as compared to the much matured GaN material system. In an ideal octet rule preserving ordered structure of ZnGeN 2 , every N atom is coordinated by exactly two Zn and two Ge atoms. However, local violation of octet rule can be caused by non-ideal coordination of N by the cations. The disordered structure is thermodynamically less favorable but can still be achieved, for example, in kinetics-limited growth regime. The ordered ZnGeN 2 has a bandgap very close to that of GaN (~3.4 eV) and a lattice mismatch of <0.1% with GaN. Interestingly, the valence band of ZnGeN 2 has been predicted to be ~1 eV above that of GaN, which has inspired novel designs for high efficiency light emitters. In this work, we investigated the metalorganic chemical vapor deposition (MOCVD) of ZnGeN 2 films on GaN/c-sapphire templates. Diethylzinc (DEZn), germane (GeH4) and ammonia were used as the precursors for Zn, Ge and N, respectively. A systematic study was conducted to investigate the cation stoichiometry as a function of growth temperature (TG), total reactor pressure (P) and DEZn/GeH 4 molar flow rate ratio (RII/IV). Under the investigated growth window, the Zn/(Zn+Ge) composition in the films, determined from energy dispersive X-ray spectroscopy, decreased monotonically with increase in TG but increased with increase in P and RII/IV. Atom probe tomography data did not indicate the presence of any secondary phases such as Zn 3 N 2 or Ge 3 N 4 . The surface morphology and crystallinity of the grown films had strong correlation with the Zn/(Zn+Ge) composition. The scanning electron microscopy images showed that the near-stoichiometric films have planar surfaces whereas Zn-rich films had crystallites on their surface and the Zn-poor films had faceted surface. Scanning transmission electron microscopy (STEM) imaging revealed that the Zn-rich and Zn-poor films have columnar and filament-like morphology, respectively, whereas the near-stoichiometric films have continuous film-like cross-sectional morphology. TEM nano-diffraction patterns as well as X-ray diffraction 2θ-ω scan profiles indicate that the near stoichiometric films are single crystalline. Nano-diffraction pattern of the stoichiometric films resembled that of a disordered ZnGeN 2 structure. Room temperature Raman spectra of near-stoichiometric films showed only the phonon density of states like features of a cation disordered ZnGeN 2 . Cathodoluminescence and photoluminescence spectra measured at different temperatures had similar features with peak emission wavelength at ~ 2 eV. In conclusion, the stoichiometry of ZnGeN 2 films can be widely tuned by tuning the MOCVD growth parameters. The surface morphology and the crystallinity of the films were found to have strong correlation with the Zn/(Zn+Ge) composition. The stoichiometric ZnGeN 2 films grown on GaN were demonstrated with uniform surface morphology and high crystalline quality. The results from this work will provide pathway to implement ZnGeN 2 in device structures.

Karim, Md Rezaul↗
DOE OSTI2023

Recycling the Energy of Indoor Light: Highly Efficient Organic Photovoltaics via a Ternary Strategy

A ternary approach in organic photovoltaics (OPV) is simple and reliable to effectively tune the optical, electrical and morphological properties of the photoactive layer for high efficiency as well as long-term stability under 1 sun. However, there have been few papers reporting spectra and weak illumination compared to outdoor light. In this study, by using two compatible 16 structures, we demonstrate a simultaneous modulation of light absorption and molecular donor polymers (PM7 and PM7 D1) with slightly-different band gaps and similar chemical packing under ambient conditions, which resulted in efficient indoor OPVs exhibiting power conversion efficiency (PCE) over 20% under 1000 lux of warm white light-emitting diode (2900 K). From morphological analysis, we infer that PM7 serves to seed nucleation of PM7 D1 in the ternary blend, templating its crystallization and alignment along the PM7 backbone. Such templating effect leads to increased domain spacing and relative degree of crystallinity (rDoC) compared to those of each binary system. We further show that higher rDoC helps suppress both bimolecular and trap-assisted recombination of photogenerated charges in the ternary devices. As a result, the complementary absorption and synergistic molecular assembly of the two donor polymers enhance the short-circuit current density as to increase the average PCEs from 9.6 to 10.3% under 1 sun and from 18.7 to 20.0% under 1000 lux. We envision that our strategy of incorporating both a planar and a flexible donor polymer with similar chemical structures can be generally applicable to attain a high performance ternary OPV under both 1 sun and indoor light.

14 SOLAR ENERGY↗
DOE OSTI2020

Electrical injection and transport in Teflon-diluted hole transport materials

Diluting small molecule organic semiconductor hole transport materials with Teflon AF (TAF) dramatically increases their thermal/morphological stability while counterintuitively also increasing the current density in hole-only diodes. Here, we explore the origin of this current enhancement in co-evaporated blends of TAF and N,N'-Di(1-naphthyl)-N,N'-diphenyl-(1,1'-biphenyl)-4,4'-diamine (NPD) and find that it results from improved hole injection and not from a mobility enhancement due to semiconductor dilution effects. Whereas electroabsorption measurements indicate that an interface dipole shift of up to 0.5 eV (depending on TAF concentration) aides hole injection at the indium-tin-oxide anode, time-of-flight and temperature-dependent current-voltage measurements show that the mobility of 25 vol% TAF:NPD blends decreases by roughly an order of magnitude relative to neat NPD despite having slightly lower energetic disorder. For comparison, diluting with 25 vol% high density polyethylene achieves a similar reduction in energetic disorder but only decreases the mobility by a factor of two. Furthermore, these results highlight the tradeoff between reducing energetic disorder and frustrating percolation in diluted organic semiconductors, and represent a step toward thermally-evaporated polymer-small molecule composites that maintain high mobility while offering improved morphological stability and lower refractive index for organic light emitting diodes.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Pure edge-dislocation half-loops in low-temperature Ga⁢N for V-defect formation

Lateral injection of carriers through semipolar crystallographic planes into c-plane QWs is one of the new frontiers in III-N light-emitting diodes (LEDs), especially for long wavelengths. Strategic use of V-defects has proven to be the most promising method for lateral injection, and creating optimal V-defect structure and density is an important research area for reducing forward voltage and increasing wall plug efficiency. Here, in this article, we present a novel method for forming V-defects in nominally unstressed low-temperature Ga⁢N through the generation of pure edge-dislocation half-loops. We present a detailed material science analysis of the loops via scattering-contrast electron microscopy. The loops have pure-edge character with Burgers vector 1/3 ⁢⟨$11\bar{2}0$⟩, and form in a sessile orientation on {$11\bar{2}0$} a-planes. The two arms of the loops are inclined such that the extra half-planes face down toward the growth substrate. The dislocation loops can be used to intentionally form V-defects through conditions of kinetically limited growth: these conditions also favor nucleation of V-defects at ∼100% of other threading dislocations in the Ga⁢N templates. Patterned sapphire substrates (PSS) are one of the most important substrates for III-N LED growth because of their superior light extraction. However, due to its low threading dislocation density, PSS have not been used extensively for V-defect LEDs. This work provides a pathway for improved control of V-defect formation and density on LEDs grown on sapphire with the goal of enabling uniform lateral injection in these V-defect engineered LEDs with low forward voltage, including PSS for high light extraction.

LEDs↗
DOE OSTI2022

High Temperature Optocoupler for 3D High Density Power Modules

The goal of this proposed research is to develop a reliable high-temperature optocouplers, which can operate at 250°C with at least ten-year lifetime, and replace isolation transforms as the galvanic isolation solution for the 3D integration of high density power modules. The electrification of future transportations (i.e., electric vehicles) will continuously drive the demand for high density power modules. Optocouplers (i.e., packaged light emitter and detector) as a promising candidate to replace bulky isolation transformers are highly desirable to facilitate the continuous scale-down of gate driver circuitry that will lead to 3D high density power modules and achieve disruptive performance in terms of thermal management, power density, power efficiency, reliability and operating environments. However, regular semiconductor optoelectronic materials and devices have significant difficulty functioning in the harsh environments designated for high density power module usage (such as operation at high temperatures). Ultimately, it is not the intrinsic properties of power devices that prevent their use at higher temperatures, but rather the low voltage electronics needed to drive them and the packaging that surrounds them. The typical operating temperature for optocouplers is only up to 100°C, due to the limitations of light emitting diode (LED) devices inside and packaging materials. A systematic characterization methodology will be developed to analyze the performance, lifetime and reliability of LED devices and distinguish multiple failure mechanisms at high temperatures. An original methodology of “design for reliability” will be developed to design the optoelectronic devices with high reliability and long lifetime at high temperatures. A new architecture of high temperature high reliable optocouplers will be developed, fabricated and demonstrated with continuous operating at 250°C. The development of efficient, reliable high density 3D power modules is the foundation for energy efficiency and energy reliability. Enabled with advanced 3D integration and packaging technologies, high density power module solutions can achieve much more superior performance over the conventional discrete solutions in terms of efficiency, thermal management and power density. The proposed concept of high temperature optocouplers as the galvanic isolation solution for high density power modules will bring together interdisciplinary research involving the wide bandgap materials, optoelectronics, high reliable device design, electronics packaging and power modules. A streamline of skilled personnel would be trained including graduate and undergraduate students, local engineers and scientists which are in great demand to both academia and optoelectronics industry. The proposed research topics, such as, solid state lighting and high temperature device reliability, are currently of major interest at the Department of Energy, in particular, Sandia National Laboratories. This project can enhance collaborations between the University of Arkansas (UA) and Sandia National Laboratories. The findings of the proposed research are expected to be integrated into high density 3-D power modules at the Engineering Research Center for Power Optimization for Electro-Thermal Systems (POETS).

42 ENGINEERING↗
DOE OSTI2020

Thermally Activated Delayed Photoluminescence: Deterministic Control of Excited-State Decay

Thermally activated photophysical processes are ubiquitous in numerous organic and metal-organic molecules, leading to chromophores with excited state properties that can be considered an equilibrium mixture of the available low-lying states. Relative populations of the equilibrated states are governed by temperature. Such molecules have been devised as high quantum yield emitters in modern organic light-emitting diode technology and for deterministic excited state lifetime control to enhance chemical reactivity in solar energy conversion and photocatalytic schemes. This recent discovery of thermally activated photophysics at CdSe nanocrystal-molecule interfaces enables a new paradigm wherein molecule-quantum dot constructs are used to systematically generate material with predetermined photophysical response and excited state properties. Semiconductor nanomaterials feature size-tunable energy level engineering, which considerably expands the purview of thermally activated photophysics beyond what is possible using only molecules. This Perspective is intended to provide a non-exhaustive overview of the advances that led to the integration of semiconductor quantum dots in thermally activated delayed photoluminescence (TADPL) schemes and to identify important challenges moving into the future. The initial establishment of excited state lifetime extension utilizing triplet-triplet excited-state equilibria is detailed. Next, advances involving the rational design of molecules composed of both metal-containing and organic-based chromophores that produce the desired TADPL are described. Lastly, the recent introduction of semiconductor nanomaterials into hybrid TADPL constructs is discussed, paving the way towards the realization of fine-tuned deterministic control of excited state decay. It is envisioned that libraries of synthetically facile composites will be broadly deployed as photosensitizers and light emitters for numerous synthetic and optoelectronic applications in the near future.

14 SOLAR ENERGY↗
DOE OSTI2024

Unraveling the Luminescence Quenching Mechanism in Strong and Weak Quantum-Confined CsPbBr 3 Triggered by Triarylamine-Based Hole Transport Layers

Luminescence quenching by hole transport layers (HTLs) is one of the major issues in developing efficient perovskite light-emitting diodes (PeLEDs), particularly prominent in blue-emitting devices. While a variety of material systems have been used as interfacial layers, the origin of such quenching and the type of interactions between perovskites and HTLs are still ambiguous. Here, we present a systematic investigation of the luminescence quenching of CsPbBr 3 by a commonly employed hole transport polymer, Poly(9,9-dioctylfluorene-alt-N-(4-sec-butylphenyl)-diphenylamine) (TFB) in LEDs. Strong and weakly quantum-confined CsPbBr 3 (nanoplatelets (NPLs)/nanocrystals (NCs)) are rationally selected to study the quenching mechanism by considering the differences in their morphology, energy level alignments, and quantum confinement. The steady-state and time-resolved Stern-Volmer plots unravel the dominance of dynamic and static quenching at lower and higher concentrations of TFB, respectively, with maximum quenching efficiency of 98%. The quenching rate in NCs is faster than in NPLs owing to their longer PL lifetimes and weak quantum confinement. The ultrafast transient absorption results support these dynamics and rule out the involvement of Forster or Dexter energy transfer. Finally, the 1D 1 H and 2D NOESY NMR study confirms the exchange of native ligands at the NCs surface with TFB, leading to dark CsPbBr 3 -TFB ensemble formation accountable for luminescence quenching. This highlights the critical role of the triarylamine functional group on TFB (also the backbone of many HTLs) in the quenching process. These results shed light on the underlying reasons for the luminescence quenching in PeLEDs and will help to choose the interfacial layers rationally for developing efficient LEDs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Effect of Anisotropic Confinement on Electronic Structure and Dynamics of Band Edge Excitons in Inorganic Perovskite Nanowires

Inorganic lead halide perovskite nanostructures show promise as the active layers in photovoltaics, light emitting diodes, and other optoelectronic devices. They are robust in the presence of oxygen and water, and the electronic structure and dynamics of these nanostructures can be tuned through quantum confinement. Here we create aligned bundles of CsPbBr3 nanowires with widths resulting in quantum confinement of the electronic wave functions and subject them to ultrafast microscopy. We directly image rapid one-dimensional exciton diffusion along the nanowires, and we measure an exciton trap density of roughly one per nanowire. Using transient absorption microscopy, we observe a polarization-dependent splitting of the band edge exciton line, and from the polarized fluorescence of nanowires in solution, we determine that the exciton transition dipole moments are anisotropic in strength. Furthermore, our observations are consistent with a model in which splitting is driven by shape anisotropy in conjunction with long-range exchange.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Surface-binding molecular multipods strengthen the halide perovskite lattice and boost luminescence

Reducing the size of perovskite crystals to confine excitons and passivating surface defects has fueled a significant advance in the luminescence efficiency of perovskite light-emitting diodes (LEDs). However, the persistent gap between the optical limit of electroluminescence efficiency and the photoluminescence efficiency of colloidal perovskite nanocrystals (PeNCs) suggests that defect passivation alone is not sufficient to achieve highly efficient colloidal PeNC-LEDs. Here, we present a materials approach to controlling the dynamic nature of the perovskite surface. Our experimental and theoretical studies reveal that conjugated molecular multipods (CMMs) adsorb onto the perovskite surface by multipodal hydrogen bonding and van der Waals interactions, strengthening the near-surface perovskite lattice and reducing ionic fluctuations which are related to nonradiative recombination. The CMM treatment strengthens the perovskite lattice and suppresses its dynamic disorder, resulting in a near-unity photoluminescence quantum yield of PeNC films and a high external quantum efficiency (26.1%) of PeNC-LED with pure green emission that matches the Rec.2020 color standard for next-generation vivid displays.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Performance of Spherical Quantum Well Down Converters in Solid State Lighting

We report the color conversion performance of amber and red emitting quantum dots (QDs) on InGaN solid-state lighting (SSL) light emitting diode (LED) packages. Spherical quantum well (SQW) architectures (CdS/CdSe 1- x S x /CdS) were prepared using a library of thio- and selenourea synthesis reagents and high throughput synthesis robotics. CdS/CdSe 1- x S x QDs with narrow luminescence bands were coated with thick CdS shells (thickness = 1.6-7.5 nm) to achieve photoluminescence quantum yields (PLQY) up to 88% at amber and red emission wavelengths (λ max = 600-642 nm, FWHM < 45 nm). The photoluminescence from SQWs encapsulated in silicone and deposited on LED packages was monitored under accelerated aging conditions (oven temperature = 85 °C, relative humidity = 5-85%, blue optical power density = 3-45 W/cm 2 ) by monitoring the red photon output over several hundred hours of continuous operation. The growth of a ZnS shell on the SQW surface increases the stability under long-term operation but also reduces the PLQY, especially of SQWs with thick CdS shells. The results illustrate that the outer ZnS shell layer is key to optimizing the PLQY and the long-term stability of QDs during operation on SSL packages.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Quantum Shell in a Shell: Engineering Colloidal Nanocrystals for a High-Intensity Excitation Regime

Many optoelectronic processes in colloidal semiconductor nanocrystals (NCs) suffer an efficiency decline under high-intensity excitation. This issue is caused by Auger recombination of multiple excitons, which converts the NC energy into excess heat, reducing the efficiency and life span of NC-based devices, including photodetectors, X-ray scintillators, lasers, and high-brightness light-emitting diodes (LEDs). Recently, semiconductor quantum shells (QSs) have emerged as a promising NC geometry for the suppression of Auger decay; however, their optoelectronic performance has been hindered by surface-related carrier losses. Here, we address this issue by introducing quantum shells with a CdS–CdSe–CdS–ZnS core–shell–shell–shell multilayer structure. Further, the ZnS barrier inhibits the surface carrier decay, which increases the photoluminescence (PL) quantum yield (QY) to 90% while retaining a high biexciton emission QY of 79%. The improved QS morphology allows demonstrating one of the longest Auger lifetimes reported for colloidal NCs to date. The reduction of nonradiative losses in QSs also leads to suppressed blinking in single nanoparticles and low-threshold amplified spontaneous emission. We expect that ZnS-encapsulated quantum shells will benefit many applications exploiting high-power optical or electrical excitation regimes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Two-dimensional-lattice-confined single-molecule-like aggregates

Intermolecular distance largely determines the optoelectronic properties of organic matter. Conventional organic luminescent molecules are commonly used either as aggregates or as single molecules that are diluted in a foreigner matrix. They have garnered great research interest in recent decades for a variety of applications, including light-emitting diodes, lasers and quantum technologies, among others. However, there is still a knowledge gap on how these molecules behave between the aggregation and dilution states. Here we report an unprecedented phase of molecular aggregate that forms in a two-dimensional hybrid perovskite superlattice with a near-equilibrium distance, which we refer to as a single-molecule-like aggregate (SMA). By implementing two-dimensional superlattices, the organic emitters are held in proximity, but, surprisingly, remain electronically isolated, thereby resulting in a near-unity photoluminescence quantum yield, akin to that of single molecules. Moreover, the emitters within the perovskite superlattices demonstrate strong alignment and dense packing resembling aggregates, allowing for the observation of robust directional emission, substantially enhanced radiative recombination and efficient lasing. Molecular dynamics simulations together with single-crystal structure analysis emphasize the critical role of the internal rotational and vibrational degrees of freedom of the molecules in the two-dimensional lattice for creating the exclusive SMA phase. Furthermore, this two-dimensional superlattice unifies the paradoxical properties of single molecules and aggregates, thus offering exciting possibilities for advanced spectroscopic and photonic applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗