Search NASA⌕ Search

SEARCH · Search NASA

Results for “RP”

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.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Charge carrier dynamics in two-dimensional hybrid perovskites: Dion–Jacobson vs. Ruddlesden–Popper phases

Two-dimensional (2D) halide perovskites are promising materials for environmentally stable next-generation optoelectronic device applications. Besides the widely investigated Ruddlesden–Popper (RP) phases, Dion–Jacobson (DJ) phases are attracting considerable attention due to their rapid emergence as efficient solar cell materials. However, there is very little atomistic understanding of the charge carrier dynamics under ambient conditions for these DJ-phases, limiting the possibilities to tune their optoelectronic performances through compositional engineering routes. In this study, by combining nonadiabatic molecular dynamics with time-domain density functional theory methods at room temperature, we compare the dominant non-radiative carrier recombination and dephasing processes in RP and DJ monolayered lead halide perovskites. Our systematic study demonstrates that performance-limiting nonradiative carrier recombination processes greatly depends on the electron–phonon interactions induced by structural fluctuations and instantaneous charge localization in these materials. The stiffer interlayer packing due to the presence of single spacer dications, which separates the lead iodide slabs, reduces the thermal fluctuations in the DJ-phase to a greater extent than that in the RP-phase 2D-perovskites. Specific electronic coupling between the closely spaced lead iodide layers enhances the delocalization of band-edge charge densities in DJ-phase systems. Compared to the RP-phase, reduced inelastic electron–phonon scattering in DJ-phase perovskites significantly limits intrinsic non-radiative recombination processes. The consequent enhancement in the photogenerated charge carrier lifetime makes DJ-phase perovskites potentially suitable for various optoelectronic devices. The computational insights gained from this study allow us to outline a set of robust design principles for DJ-phase perovskites to strategically tune their optoelectronic properties.

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

High-performance Ruddlesden–Popper perovskite oxide with in situ exsolved nanoparticles for direct CO 2 electrolysis

Carbon dioxide (CO 2 ) is one of the principal greenhouse gases accountable for global warming and extreme climate changes. Electrochemically converting CO 2 into carbon monoxide (CO) is a promising approach for CO 2 utilization in achieving industrial decarbonization. High-temperature CO 2 electrolysis via solid oxide electrolysis cells (SOECs) has great potential, including high-energy efficiency, fast electrode kinetics, and competitive cost; however, this technology still has challenges associated with developing highly active, robust CO 2 electrodes for SOECs. We report novel Ruddlesden–Popper structured Pr 1.2 Sr 0.8 Mn 0.4 Fe 0.6 O 4–δ (RP-PSMF) with in situ exsolved Fe nanoparticles as the CO 2 electrode in SOECs for direct CO 2 conversion to CO. The mechanism of CO 2 electrolysis is studied by using the distribution of relaxation times method from electrochemical impedance spectroscopy. La 0.8 Sr 0.2 Ga 0.8 Mg 0.2 O 3–δ (LSGM)-electrolyte supported SOECs with the RP-PSMF cathode have achieved exceptionally high current densities of 2.90, 1.61, 0.91, and 0.48 A·cm –2 at an applied voltage of 1.5 V at 800, 750, 700, and 650 °C, respectively. Moreover, SOECs with the RP-PSMF cathode have exhibited a stable electrolysis performance for 100 h under a current cycling operation. Here, these results suggest that RP-PSMF with exsolved Fe nanoparticles is a highly promising cathode for high-temperature direct CO 2 electrolysis cells.

03 NATURAL GAS↗
DOE OSTI2023

Local cation ordering in compositionally complex Ruddlesden–Popper n = 1 oxides

The Ruddlesden–Popper (RP) layered perovskite structure is of great interest due to its inherent tunability, and the emergence and growth of the compositionally complex oxide (CCO) concept endows the RP family with further possibilities. Here, a comprehensive assessment of thermodynamic stabilization, local order/disorder, and lattice distortion was performed in the first two reported examples of lanthanum-deficient La n+1 B n O 3n+1 (n = 1, B = Mg, Co, Ni, Cu, Zn) obtained via various processing conditions. Chemical short-range order (CSRO) at the B-site and the controllable excess interstitial oxygen (δ) in RP-CCOs are uncovered by neutron pair distribution function analysis. Reverse Monte Carlo analysis of the data, Metropolis Monte Carlo simulations, and extended x-ray absorption fine structure analysis implies a modest degree of magnetic element segregation on the local scale. Further, ab initio molecular dynamics simulations results obtained from special quasirandom structure disagree with experimentally observed CSRO but confirm Jahn–Teller distortion of CuO 6 octahedra. These findings highlight potential opportunities to control local order/disorder and excess interstitial oxygen in layered RP-CCOs and demonstrate a high degree of freedom for tailoring application-specific properties. They also suggest a need for expansion of theoretical and data modeling approaches in order to meet the innate challenges of CCO and related high-entropy phases.

36 MATERIALS SCIENCE↗
DOE OSTI2020

The effect of ram-pressure stripping on dwarf galaxies

ABSTRACT Ram-pressure stripping (RPS) is a well observed phenomenon of massive spiral galaxies passing through the hot intracluster medium (ICM) of galaxy clusters. For dwarf galaxies (DGs) within a cluster, the transformation from gaseous to gas-poor systems by RPS is not easily observed and must happen in the outskirts of clusters. In a few objects in close by galaxy clusters and the field, RPS has been observed. Since cluster early-type DGs also show a large variety of internal structures (unexpected central gas reservoirs, blue stellar cores, composite radial stellar profiles), we aim in this study to investigate how ram pressure (RP) affects the interstellar gas content and therefore the star formation (SF) activity. Using a series of numerical simulations, we quantify the dependence of the stripped-off gas on the velocity of the infalling DGs and on the ambient ICM density. We demonstrated that SF can be either suppressed or triggered by RP depending on the ICM density and the DGs mass. Under some conditions, RP can compress the gas, so that it is unexpectedly retained in the central DG region and forms stars. When gas clouds are still bound against stripping but lifted from a thin disc and fall back, their new stars form an ellipsoidal (young) stellar population already with a larger velocity dispersion without the necessity of harassment. Most spectacularly, star clusters can form downstream in stripped-off massive gas clouds in the case of strong RP. We compare our results to observations.

Steyrleithner, P.↗
DOE OSTI2020

Proteomic Tissue-Based Classifier for Early Prediction of Prostate Cancer Progression

Although ~40% of screen-detected prostate cancers (PCa) are indolent, advanced-stage PCa is a lethal disease with 5-year survival rates around 29%. Identification of biomarkers for early detection of aggressive disease is a key challenge. Starting with 52 candidate biomarkers, selected from existing PCa genomics datasets and known PCa driver genes, we used targeted mass spectrometry to quantify proteins that significantly differed in primary tumors from PCa patients treated with radical prostatectomy (RP) across three study outcomes: (i) metastasis ≥1-year post-RP, (ii) biochemical recurrence ≥1-year post-RP, and (iii) no progression after ≥10 years post-RP. Sixteen proteins that differed significantly in an initial set of 105 samples were evaluated in the entire cohort (n = 338). A five-protein classifier which combined FOLH1, KLK3, TGFB1, SPARC, and CAMKK2 with existing clinical and pathological standard of care variables demonstrated significant improvement in predicting distant metastasis, achieving an area under the receiver-operating characteristic curve of 0.92 (0.86, 0.99, p = 0.001) and a negative predictive value of 92% in the training/testing analysis. This classifier has the potential to stratify patients based on risk of aggressive, metastatic PCa that will require early intervention compared to low risk patients who could be managed through active surveillance.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2020

Fine Structures in the Main Sequence Revealed by Gaia Data Release 2

The Hertzsprung–Russell diagram (HRD) is fully examined using the Fourier analysis. This work shows more stars are above the gap in the lower main sequence than below it, and this implies that stars spend more time above the gap while they undergo variability associated with the {sup 3}He instability. The enhanced HRD also shows the width of the gap is not linear and depends on the G{sub BP}−G{sub RP} color up until G{sub BP}−G{sub RP}=2.7. Beyond this color limit, the gap is hardly seen. Besides, a new low density region is revealed for the first time centered at M {sub G} ≈ 10.7 and G {sub BP} − G {sub RP} ≈ 2.8, which is below the lower right corner of the gap. This work also shows that the main sequence appears to have fine stripes where stellar densities are relatively low or high compared to their adjacent regions on the main sequence. These stripes can be seen throughout the main sequence of stars redder than G {sub BP} − G {sub RP} = 0.8 and are not limited to any specific color or spectral type. Slopes of these features are different from the main sequence, but are pretty consistent throughout the main sequence, with a few exceptions. We are perplexed by these new features, but the complexities of stellar atmospheric features and opacities of dwarfs may have caused these patterns.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2023

Mass measurement of 27 P to constrain type-I x-ray burst models and validate the isobaric multiplet mass equation for the $A = 27, T = \frac{3}{2}$ isospin quartet

Background: Light curves are the primary observable of type-I x-ray bursts. Computational x-ray burst models must match simulations to observed light curves. Most of the error in simulated curves comes from uncertainties in rp process reaction rates, which can be reduced via precision mass measurements of neutron-deficient isotopes in the rp process path. Purpose: Perform a precise atomic mass measurement of 27 P. Use this new measurement to calculate rp process reaction rates and input these rates into an x-ray burst model to reduce simulated light curve uncertainty. Use the mass measurement of 27 P to validate the isobaric multiplet mass equation (IMME) for the A = 27 T = 3/2 isospin quartet which 27 P belongs to. Method: High-precision Penning trap mass spectrometry utilizing the time-of-flight ion cyclotron resonance technique was used to determine the atomic mass of 27 P. The MESA code (Modules for Experiments in Stellar Astrophysics) was then used to simulate x-ray bursts using a one-dimensional multizone model to produce updated light curves. Results: The mass excess of 27 P was measured to be –670.7(6) keV, a 14-fold precision increase over the mass reported in the 2020 Atomic Mass Evaluation (AME2020). The 26 Si(p, $γ$) 27 P– 27 P($γ$, p) 26 Si rate equilibrium has been determined to a higher precision based on the precision mass measurement of 27 P. x-ray burst light curves were produced with the MESA code using the new reaction rates. Changes in the mass of 27 P seem to have minimal effect on light curves, even in burster systems tailored to maximize impact. Conclusion: The mass of 27 P does not play a significant role in x-ray burst light curves. It is important to understand that more advanced models do not just provide more precise results, but often qualitatively different ones. This result brings us a step closer to being able to extract stellar parameters from individual x-ray burst observations. In addition, the IMME has been validated for the A = 27, T = 3/2 quartet. The normal quadratic form of the IMME using the latest data yields a reduced $χ$ 2 of 2.9. Finally, the cubic term required to generate an exact fit to the latest data matches theoretical attempts to predict this term.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2026

Stabilizing Iodine in 2D Mixed Halide Perovskites: Dion–Jacobson Versus Ruddlesden–Popper Phases

Iodine electrochemistry plays an important role in driving iodide‐oxidation induced halide migration in 3D halide perovskites. When subjected to light illumination or electrochemical bias, mixed halide perovskites undergo halide segregation followed by iodine expulsion from the crystal lattices. To mitigate such intrinsic halide ion mobility in 3D perovskites, lower‐dimensional (2D) perovskites are employed as barriers to stabilize the perovskite layers. Interestingly, 2D halide perovskites also exhibit halide ion mobility that is dependent on the binding configuration, viz., Ruddlesden–Popper (RP) and Dion–Jacobson (DJ) phases. Hybrid RP‐DJ perovskites with a mixed Br:I ratio of 50:50 show increased stability following continuous photoirradiation. Spectroscopic studies that probe iodine migration and expulsion in photoirradiated 2D films of different configurations are presented here. The effective strategy of blending two different 2D phases (RP‐DJ) offers new opportunities to develop stable 2D/3D perovskite interfaces in solar cells.

2D halide perovskites↗
DOE OSTI2021

Barriers to carriers: faults and recombination in non-stoichiometric perovskite scintillators

Abstract Tuning the efficiency and speed of charge carrier recombination in inorganic scintillators can potentially improve their performance in diverse applications. Recent work suggests that this maybe be achieved via a two-phase scintillator AB that naturally phase separates into A -rich and B -rich domains. In addition, a favorable electronic structure and band-edge alignment such that the charge carriers are confined or are thermodynamically driven to preferentially accumulate in one of the two domains, might lead to an improved radiative recombination rate. Here, we use density functional theory computations and ab initio molecular dynamics (AIMD), including non-adiabatic molecular dynamics (NAMD) simulations, to examine an alternative phase structure and its potential impact on recombination. Using a model perovskite SrTiO $$_3$$ 3 system with one-, two- and three-dimensional Ruddlesden–Popper (RP) phases, we demonstrate that RP faults induce band structure changes in the material that can act as barriers to carrier transport. Our AIMD/NAMD simulations indicate competing effects of a lower mean free path (potentially enhancing the desired radiative recombination and overall scintillating efficiency) and faster non-radiative recombination (undesired) due to enhanced electron–phonon coupling in the faulted system. Full exploitation of such a rational design approach would require tuning of the effective scintillation efficiency by varying the perovskite chemistry using appropriate arrangements of RP faults in the bulk material. Finally, other effects, such as the tendency of point defects to segregate at the interface, that might affect the overall performance, are briefly discussed. We expect the basic results found here to apply to other nanostructured scintillators. Graphical Abstract

36 MATERIALS SCIENCE↗
DOE OSTI2022

Spectroscopic characterization of Mn 2+ and Cd 2+ coordination to phosphorothioates in the conserved A9 metal site of the hammerhead ribozyme

Phosphorothioate modifications have widespread use in the field of nucleic acids. As substitution of sulfur for oxygen can alter metal coordination preferences, the phosphorothioate metal-rescue experiment is a powerful method for identifying metal coordination sites that influence specific properties in a large RNAs. The A9/G10.1 metal binding site of the hammerhead ribozyme (HHRz) has previously been shown to be functionally important through phosphorothioate rescue experiments. While an A9-S Rp substitution is inhibitory in Mg 2+ , thiophilic Cd 2+ rescues HHRz activity. Mn 2+ is also often used in phosphorothioate metal-rescue studies but does not support activity for the A9-S Rp HHRz. Here, we use EPR, electron spin-echo envelope modulation (ESEEM), and X-ray absorption spectroscopic methods to directly probe the structural consequences of Mn 2+ and Cd 2+ coordination to R p and S p phosphorothioate modifications at the A9/G10.1 site in the truncated hammerhead ribozyme (tHHRz). The results demonstrate that while Cd 2+ does indeed bind to S in the thio-substituted ligand, Mn 2+ coordinates to the non–sulfur oxo group of this phosphorothioate, regardless of isomer. Computational models demonstrate the energetic preference of Mn—O over Mn—S coordination in metal-dimethylthiophosphate models. In the case of the tHHRz, the resulting Mn 2+ coordination preference of oxygen in either R p or S p A9 phosphorothioates differentially tunes catalytic activity, with Mn—O coordination in the A9-S Rp phosphorothioate enzyme being inhibitory.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Active control of resistive wall mode via modification of external tearing index

Modification of the external tearing index, Δ ext ′ , by magnetic feedback is analytically investigated for the purpose of controlling the resistive plasma resistive wall mode (RP-RWM). The matching method is pursued by deriving expressions for the close-loop Δ ext ′ and by linking it to the counterpart from the inner layer. Various feedback coil configurations are found to generally reduce Δ ext ′ and stabilize the RWM, with either proportional or derivative control. Feedback modification of Δ ext ′ is found to be generally independent of the inner layer resistive interchange index D R , confirming that feedback action primarily modifies the solution in the outer ideal region for the RP-RWM. Exception occurs when either the inner layer favorable curvature effect becomes sufficiently large or the feedback action is sufficiently strong to introduce a rotating RP-RWM in the static plasma, leading to complex-valued close-loop Δ ext ′ . The perturbed magnetic energy dissipation in the outer region, associated with the eddy current in the resistive wall, is identified as the key physics reason for feedback induced complex Δ ext ′ . Similar results are also obtained for active control of the external kink instability, whose open-loop growth rate is significantly reduced by inclusion of the plasma resistivity. Within the single poloidal harmonic approximation, which is most suitable for the matching approach, external active coils combined with poloidal sensors are often found to be more efficient for feedback stabilization of the mode at large proportional gain values. This counter-intuitive result is explained as the lack of (non-resonant) poloidal harmonics for proper description of the feedback coil geometry.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

The DESI One-Percent survey: exploring the Halo Occupation Distribution of Emission Line Galaxies with AbacusSummit simulations

The One-Percent survey of the Dark Energy Spectroscopic Instrument collected ~ 270k emission line galaxies (ELGs) at 0.8 < z < 1.6. The high completeness of the sample allowed the clustering to be measured down to scales never probed before, 0.04 Mpc/h in rp for the projected 2-point correlation function (2PCF) and 0.17 Mpc/h in galaxy pair separation s for the 2PCF monopole and quadrupole. The most striking feature of the measurements is a strong signal at the smallest scales, below 0.2 Mpc/h in rp and 1 Mpc/h in s. We analyse these data in the halo occupation distribution framework. We consider different distributions for central galaxies, a standard power law for satellites with no condition on the presence of a central galaxy and explore several extensions of these models. For all considered models, the mean halo mass of the sample is found to be log10 $\langle$Mh$\rangle$ ~ 11.9. We obtain a satellite mean occupation function which agrees with physically motivated ELG models only if we introduce central-satellite conformity, meaning that the satellite occupation is conditioned by the presence of central galaxies of the same type. To achieve in addition a good modelling of the clustering between 0.1 and 1 Mpc/h in rp, we allow for ELG positioning outside of the halo virial radius and find 0.5% of ELGs residing in the outskirts of halos. Furthermore, the satellite velocity dispersion inside halos is found to be ~ 30% larger than that of the halo dark matter particles. These are the main findings of our work. Here we investigate assembly bias as a function of halo concentration, local density or local density anisotropies and observe no significant change in our results. We split the data sample in two redshift bins and report no significant evolution with redshift. Lastly, changing the cosmology in the modelling impacts only slightly our results.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

Design and Performance Characterization of RADICAL-Pilot on Leadership-Class Platforms

Many extreme scale scientific applications have workloads comprised of a large number of individual highperformance tasks. The Pilot abstraction decouples workload specification, resource management, and task execution via job placeholders and late-binding. As such, suitable implementations of the Pilot abstraction can support the collective execution of large number of tasks on supercomputers. We introduce RADICAL-Pilot (RP) as a portable, modular and extensible Pilot enabled runtime system. We describe RP's design, architecture and implementation. We characterize its performance and show its ability to scalably execute workloads comprised of tens of thousands heterogeneous tasks on DOE and NSF leadership-class HPC platforms. Specifically, we investigate RP's weak/strong scaling with CPU/GPU, single/multi core, (non)MPI tasks and python functions when using most of ORNL Summit and TACC Frontera. RADICAL-Pilot can be used stand-alone, as well as the runtime for third-party workflow systems.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2023

Spectral statistics of a minimal quantum glass model

Glasses have the interesting feature of being neither integrable nor fully chaotic. They thermalize quickly within a subspace but thermalize much more slowly across the full space due to high free energy barriers which partition the configuration space into sectors. Past works have examined the Rosenzweig-Porter (RP) model as a minimal quantum model which transitions from localized to chaotic behavior. In this work we generalize the RP model in such a way that it becomes a minimal model which transitions from glassy to chaotic behavior, which we term the “Block Rosenzweig-Porter” (BRP) model. We calculate the spectral form factors of both models at all timescales larger than the inverse spectral width. Whereas the RP model exhibits a crossover from localized to ergodic behavior at the Thouless timescale, the new BRP model instead crosses over from glassy to fully chaotic behavior, as seen by a change in the steepness of the ramp of the spectral form factor.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

The Influence of 10 Unique Chemical Elements in Shaping the Distribution of Kepler Planets

The chemical abundances of planet-hosting stars offer a glimpse into the composition of planet-forming environments. To further understand this connection, we make the first ever measurement of the correlation between planet occurrence and chemical abundances for ten different elements (C, Mg, Al, Si, S, K, Ca, Mn, Fe, and Ni). Leveraging data from the Apache Point Observatory Galactic Evolution Experiment (APOGEE) and Gaia to derive precise stellar parameters (${\sigma }_{{R}_{\star }}\approx 2.3 \% $, ${\sigma }_{{M}_{\star }}\approx 4.5 \% $) for a sample of 1018 Kepler Objects of Interest, we construct a sample of well-vetted Kepler planets with precisely measured radii (${\sigma }_{{R}_{p}}\approx 3.4 \% $). After controlling for biases in the Kepler detection pipeline and the selection function of the APOGEE survey, we characterize the relationship between planet occurrence and chemical abundance as the number density of nuclei of each element in a star's photosphere raised to a power, β. varies by planet type, but is consistent within our uncertainties across all ten elements. For hot planets (P = 1–10 days), an enhancement in any element of 0.1 dex corresponds to an increased occurrence of ≈20% for super-Earths (Rp = 1–1.9 R⊕) and ≈60% for sub-Neptunes (Rp = 1.9–4 R⊕). Trends are weaker for warm (P = 10–100 days) planets of all sizes and for all elements, with the potential exception of sub-Saturns (Rp = 4–8 R⊕). Finally, we conclude this work with a caution to interpreting trends between planet occurrence and stellar age due to degeneracies caused by Galactic chemical evolution and make predictions for planet occurrence rates in nearby open clusters to facilitate demographics studies of young planetary systems.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2023

ANS MiNES 2023 Poster

The dynamic mechanical properties of four varieties of high purity graphite as well as the depth of penetration (DoP) of a small-scale shaped charge into these grades was experimentally determined. The grades chosen were PCEA, NBG-18, and NBG-25. These grades provide a wide range of physical properties: in density from 1.80 – 1.85 g/cc, in maximum particle size from 10s to 1000s of µm, and in porosity from 18% to 20%. The quasistatic and dynamic compressive strengths of each grade were determined and correlated to their physical properties. The split Hopkinson pressure bar experiments showed both the dynamic strength and dominant shear failure mechanisms. A small scale shaped charge was used to compare the resistance of graphite to hypervelocity jet impacts: the Teledyne RP-4. The RP-4 has a 1.01” outer diameter and 3.44 g of RDX with an RP-80 booster (86 mg PETN + 123 mg RDX). A select number of samples were analyzed using X-Ray Computed Tomography (XCT), allowing for the full characterization of the undisturbed wound channel. A selection of other samples were physically sectioned and wound channels mapped from the sections. In addition to DoP, the wound geometry was characterized in terms of total volume and diameter at different depths. The wound channel characteristics for each grade were correlated to the compressive strengths and physical properties. In several of the test samples, the wound channel diameter was smaller than the diameter of the shaped charge slug just behind where the slug had penetrated the sample. These results indicated that the wound geometry was dependent on the compressive hysteresis behavior of graphite.

36 MATERIALS SCIENCE↗
DOE OSTI2021

A novel optical sensor for Pb 2+ detection based on in-situ formation of Ruddlesden-Popper phase (C 4 H 9 NH 3 ) 2 PbBr 4 perovskite

On account of the concentration sensitive photoluminescence (PL) property of the lead-based Ruddlesden-Popper (RP) phase perovskite material, a novel sensing mechanism for highly selective Pb 2+ detection based on the in-situ formation of highly emissive luminescence structure matrix (C 4 H 9 NH 3 ) 2 PbBr 4 has been demonstrated. The sensor exhibits high sensitivity and selectivity for detecting Pb 2+ in complex metal cations mixture solution. This research reports a novel type of sensor mechanism based on the in-situ formation of luminescent lead-based RP phase perovskite. Here, it paves the way for developing highly selective optical sensors for detecting heavy metal cations via their corresponding luminescence structure matrix.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Point Defects in Two-Dimensional Ruddlesden–Popper Perovskites Explored with Ab Initio Calculations

Two-dimensional Ruddlesden–Popper (RP) halide perovskites stand out as excellent layered materials with favorable optoelectronic properties for efficient light-emitting, spintronic, and other spin-related applications. However, properties often determined by defects are not well understood in these perovskite systems. This work investigates the ground state electronic structure of commonly formed defects in a typical RP perovskite structure by density functional theory. Our study reveals that these 2D perovskites generally retain their defect tolerance with limited perturbation of the electronic structure in the case of neutral-type point defects. In contrast, donor/acceptor defects induce deep midgap states, potentially causing harm to the material’s electronic performance. To retain positive intrinsic properties, the halide vacancies and interstitial defects should be avoided. The observed strong electron localization results in trap states and consequently leads to reduced device performance. Finally, this understanding can guide experimental efforts that aim for improved 2D halide perovskite-based device performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗