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DOE OSTI2026

Directional dependence of equilibrated TLD-400 chips in multiple radiation fields

Fielding of thermoluminescent dosimeters (TLDs) for measurement of photon radiation dose in experiments is the standard practice for γ-irradiation facilities, pulsed power x-ray facilities, and reactor facilities at Sandia National Laboratories (SNL). Due to the high-dose experimental conditions and the mixed ( 1 n, γ) fields in these facilities, SNL radiation metrologists have historically used CaF 2 :Mn TLDs (also known as TLD-400). Recent inquiries to the radiation metrology staff have raised concerns that the aluminum-equilibrated TLD-400 chips may exhibit a directionally dependent response. The metrologists were asked whether the dose measured by the chip may be impacted by the angle of incidence on the equilibrated TLD. To provide a thorough answer to this query, a set of adjoint Monte Carlo radiation transport calculations was performed for three different equilibrated TLDs as well as bare TLD chips using the Integrated Tiger Series (ITS) code. The key feature of the adjoint calculations performed in this study is that each photon escaping the modeled geometry was tallied into angular bins to provide information on both the energy and angular dependence of the equilibrated chip. After the adjoint Monte Carlo calculations were completed, the resulting energy-dependent response function for each angular bin was convolved with multiple photon energy spectra representing various radiation facilities at SNL. The radiation facilities selected for analysis span a range of photon energies from approximately 1 keV up to approximately 20 MeV. Thus, the presented results are applicable to a wide variety of radiation facilities around the world. Although the bare TLD-400 chip was expected to display the largest variation due to the photon angle of impact on the dosimeter, the dosimeter with the thinnest aluminum equilibrator (SNL thin equilibrated TLD-400) was determined to have the biggest differential between the impact angle with the maximum dose ( D max ) and the impact angle with the minimum dose ( D min ). However, the SNL normal equilibrated TLD-400 chip demonstrated a dramatic reduction in that differential between maximum and minimum dose angles. The reduction in this differential is one of the dominant factors in experimenters’ choice to field these dosimeters at SNL radiation facilities. The results from the PNNL (Hanford) energy-flattening field capsule are consistent with the previous publications. The differential dose responses due to the photon impact angle indicate that experimenters should strive to field their TLD-400 dosimeters in a consistent manner to avoid additional uncertainty in the measurements based on dosimeter orientation.

Adjoint radiation transport↗

DOE OSTI2022

Excitation Intensity- and Size-Dependent Halide Photosegregation in CsPb(I 0.5 Br 0.5 ) 3 Perovskite Nanocrystals

Although broad consensus exists that photoirradiation of mixed-halide lead perovskites leads to anion segregation, no model today fully rationalizes all aspects of this near ubiquitous phenomenon. In this work, we quantitatively compare experimental, CsPb(I 0.5 Br 0.5 ) 3 nanocrystal (NC) terminal anion photosegregation stoichiometries and excitation intensity thresholds to a band gap-based, thermodynamic model of mixed-halide perovskite photosegregation. Mixed-halide NCs offer strict tests of theory given physical sizes, which dictate local photogenerated carrier densities. We observe that mixed-anion perovskite NCs exhibit significant robustness to photosegregation, with photosegregation propensity decreasing with decreasing NC size. Observed size- and excitation intensity-dependent photosegregation data agree with model predicted size- and excitation intensity-dependent terminal halide stoichiometries. Established correspondence between experiment and theory, in turn, suggests that mixed-halide perovskite photostabilities can be predicted a priori using local gradients of (empirical) Vegard’s law expressions of composition-dependent band gaps.

36 MATERIALS SCIENCE↗

DOE OSTI2014

Density functional and theoretical study of the temperature and pressure dependency of the plasmon energy of solids

The temperature and pressure dependency of the volume plasmon energy of solids was investigated by density functional theory calculations. The volume change of crystal is the major factor responsible for the variation of valence electron density and plasmon energy in the free electron model. Hence, to introduce the effect of temperature and pressure for the density functional theory calculations of plasmon energy, the temperature and pressure dependency of lattice parameter was used. Also, by combination of the free electron model and the equation of state based on the pseudo-spinodal approach, the temperature and pressure dependency of the plasmon energy was modeled. The suggested model is in good agreement with the results of density functional theory calculations and available experimental data for elements with the free electron behavior.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2015

Angular radiation temperature simulation for time-dependent capsule drive prediction in inertial confinement fusion

The x-ray drive on a capsule in an inertial confinement fusion setup is crucial for ignition. Unfortunately, a direct measurement has not been possible so far. We propose an angular radiation temperature simulation to predict the time-dependent drive on the capsule. A simple model, based on the view-factor method for the simulation of the radiation temperature, is presented and compared with the experimental data obtained using the OMEGA laser facility and the simulation results acquired with VISRAD code. We found a good agreement between the time-dependent measurements and the simulation results obtained using this model. The validated model was then used to analyze the experimental results from the Shenguang-III prototype laser facility. More specifically, the variations of the peak radiation temperatures at different view angles with the albedo of the hohlraum, the motion of the laser spots, the closure of the laser entrance holes, and the deviation of the laser power were investigated. Furthermore, the time-dependent radiation temperature at different orientations and the drive history on the capsule were calculated. The results indicate that the radiation temperature from “U20W112” (named according to the diagnostic hole ID on the target chamber) can be used to approximately predict the drive temperature on the capsule. In addition, the influence of the capsule on the peak radiation temperature is also presented.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2015

Composition dependence of dielectric properties in Se{sub 100-x}Cu{sub x} glassy alloys

In this paper we report the composition dependent of dielectric properties in Se{sub 100-x}Cu{sub x} (x = 0, 2, 4 and 6) glassy alloys. The temperature and frequency dependence of the dielectric constants and the dielectric losses in the above glassy systems in the frequency range (1k Hz-5 M Hz) and temperature range (300 K–350 K) have been measured. It has been found that dielectric constant and the dielectric loss both are highly dependent on frequency and temperature and also found to increase with increasing concentration of Cu in pure amorphous Se. The role of Cu, as an impurity in the pure a-Se glassy alloy, is also discussed in terms of electronegativity difference between the elements used in making the aforesaid glassy system. Apart from this, the results have been also correlated in terms of a dipolar model which considers the hopping of charge carriers over a potential barrier between charged defect states.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2015

Kinetic isotope effect of the {sup 16}O + {sup 36}O{sub 2} and {sup 18}O + {sup 32}O{sub 2} isotope exchange reactions: Dominant role of reactive resonances revealed by an accurate time-dependent quantum wavepacket study

The O + O{sub 2} isotope exchange reactions play an important role in determining the oxygen isotopic composition of a number of trace gases in the atmosphere, and their temperature dependence and kinetic isotope effects (KIEs) provide important constraints on our understanding of the origin and mechanism of these and other unusual oxygen KIEs important in the atmosphere. This work reports a quantum dynamics study of the title reactions on the newly constructed Dawes-Lolur-Li-Jiang-Guo (DLLJG) potential energy surface (PES). The thermal reaction rate coefficients of both the {sup 18}O + {sup 32}O{sub 2} and {sup 16}O + {sup 36}O{sub 2} reactions obtained using the DLLJG PES exhibit a clear negative temperature dependence, in sharp contrast with the positive temperature dependence obtained using the earlier modified Siebert-Schinke-Bittererova (mSSB) PES. In addition, the calculated KIE shows an improved agreement with the experiment. These results strongly support the absence of the “reef” structure in the entrance/exit channels of the DLLJG PES, which is present in the mSSB PES. The quantum dynamics results on both PESs attribute the marked KIE to strong near-threshold reactive resonances, presumably stemming from the mass differences and/or zero point energy difference between the diatomic reactant and product. The accurate characterization of the reactivity for these near-thermoneutral reactions immediately above the reaction threshold is important for correct characterization of the thermal reaction rate coefficients.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2015

Improving Planck calibration by including frequency-dependent relativistic corrections

The Planck satellite detectors are calibrated in the 2015 release using the 'orbital dipole', which is the time-dependent dipole generated by the Doppler effect due to the motion of the satellite around the Sun. Such an effect has also relativistic time-dependent corrections of relative magnitude 10{sup −3}, due to coupling with the 'solar dipole' (the motion of the Sun compared to the CMB rest frame), which are included in the data calibration by the Planck collaboration. We point out that such corrections are subject to a frequency-dependent multiplicative factor. This factor differs from unity especially at the highest frequencies, relevant for the HFI instrument. Since currently Planck calibration errors are dominated by systematics, to the point that polarization data is currently unreliable at large scales, such a correction can in principle be highly relevant for future data releases.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2026

California Trees Seasonally Use Augmented Water Sources: Water Isotope Tracking in a Groundwater‐Dependent Ecosystem

Sustainable groundwater management must account for the needs of groundwater dependent ecosystems. To understand the relationship of ecosystems and seasonal water use, we studied the stable isotope composition (δ 18 O and δ 2 H) of water in streamside trees in a semi-arid streamside environment (Livermore, California, USA). We sampled seven trees at two sites every other month from April 2024 through April 2025 for tree xylem stable water isotope signatures. These data were compared to potential source waters: precipitation, imported surface water, soil water and regional groundwaters. Large daily precipitation events were found to be isotopically similar to regional groundwater and were thus treated as one water source. A Bayesian mixing model using stable water isotopes was used to determine the ratios of these three potential source waters (small daily precipitation events, groundwater/large daily precipitation events and imported water) present in tree xylem water. On average, tree water sources include 32% imported water (SD = 9%), 35% small daily precipitation events (SD = 10%) and 33% groundwater (SD = 3%), with significant seasonal variation (t summer-winter = 30.8, p < 0.01), particularly drawing more imported water (more than 55%) in the summer. While small daily precipitation events contribute only 10% of the total precipitation in our dataset, it represents a third of water used by trees. In addition, while these ecosystems are designated as groundwater dependent ecosystems, the trees use approximately one third imported water and even more during dry summer months. This approach provides water managers with a practical tool for quantifying ecosystem water needs, supporting data-driven decisions and regulatory compliance. While California's Sustainable Groundwater Management Act emphasizes supporting groundwater dependent ecosystems, it allows flexibility in demonstrating benefits. In conclusion, our methodology provides a way to document that management actions (such as managed aquifer recharge with imported water) deliver measurable co-benefits to GDEs.

Geosciences↗

DOE OSTI2018

Study of Critical Current and n-Values of 2G HTS Tapes: Their Magnetic Field-Angular Dependence

Since many applications of YBCO tapes operate in external magnetic fields, it is necessary to investigate the magneto-angular dependence of critical current and n-values in coated conductors. In this paper, five commercial YBCO tapes with different microstructures produced by three different manufacturers are chosen. The selected samples have a width of 2.0, 4.0, 4.8, 6.0 or 12 mm, with copper, brass or stainless steel laminations. The critical current density dependence J{sub c}(B, θ) and n-values characteristics n(B, θ) of the tapes are comprehensively measured under various magnetic fields and orientations. Afterwards, the obtained experimental data sets are successfully fitted using a novel multi-objective model which considers the material anisotropy. By using this approach, a fitting function I{sub c}(B, θ) can always be obtained to accurately describe the experimental data, regardless of the fabrication and width differences of the superconducting tapes. Moreover, our experiment shows that when subject to different external magnetic fields, the angular dependence of n-values characteristics is directly correlated with the corresponding critical current profiles. Our results are helpful to predict the critical current of electromagnetically interacting 2G HTS wires, thereby improving the design and performance of the devices made from YBCO tapes.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2019

Spatially dependent embedded self-shielding method for nonuniform temperature distribution

The embedded self-shielding method (ESSM) is simple and robust, and applicable to any geometrical configuration to account for resonance self-shielding by performing fixed source transport calculations. ESSM is very similar to the subgroup method, which has been successful in the MPACT neutronics code developed by CASL. The subgroup method introduces errors in a least-squares fitting process that is used to generate subgroup quadrature sets and cannot be applied to thermal energy groups, as ESSM introduces error for spatially dependent self-shielded cross sections inside the fuel. This study focused on integrating the conventional ESSM with an improved Stoker-Weiss method to obtain spatially dependent resonance self-shielded cross sections for a nonuniform fuel temperature distribution. Here, the proposed method would serve as a substitute for the subgroup method in high fidelity simulations using CASL’s VERA. Benchmark results show that this new, spatially dependent ESSM (SDESSM) is an appropriate candidate to replace the subgroup method.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2014

Age-dependent changes in diastolic Ca{sup 2+} and Na{sup +} concentrations in dystrophic cardiomyopathy: Role of Ca{sup 2+} entry and IP{sub 3}

Highlights: • Age-dependent increase in [Ca{sup 2+}]{sub d} and [Na{sup +}]{sub d} in mdx cardiomyocytes. • Gadolinium significantly reduced both [Ca{sup 2+}]{sub d} and [Na{sup +}]{sub d} at all ages. • IP{sub 3}-pathway inhibition reduced cations concentrations in dystrophic cardiomyocytes. - Abstract: Duchenne muscular dystrophy (DMD) is a lethal X-inherited disease caused by dystrophin deficiency. Besides the relatively well characterized skeletal muscle degenerative processes, DMD is also associated with a dilated cardiomyopathy that leads to progressive heart failure at the end of the second decade. The aim of the present study was to characterize the diastolic Ca{sup 2+} concentration ([Ca{sup 2+}]{sub d}) and diastolic Na{sup +} concentration ([Na{sup +}]{sub d}) abnormalities in cardiomyocytes isolated from 3-, 6-, 9-, and 12-month old mdx mice using ion-selective microelectrodes. In addition, the contributions of gadolinium (Gd{sup 3+})-sensitive Ca{sup 2+} entry and inositol triphosphate (IP{sub 3}) signaling pathways in abnormal [Ca{sup 2+}]{sub d} and [Na{sup +}]{sub d} were investigated. Our results showed an age-dependent increase in both [Ca{sup 2+}]{sub d} and [Na{sup +}]{sub d} in dystrophic cardiomyocytes compared to those isolated from age-matched wt mice. Gd{sup 3+} treatment significantly reduced both [Ca{sup 2+}]{sub d} and [Na{sup +}]{sub d} at all ages. In addition, blockade of the IP{sub 3}-pathway with either U-73122 or xestospongin C significantly reduced ion concentrations in dystrophic cardiomyocytes. Co-treatment with U-73122 and Gd{sup 3+} normalized both [Ca{sup 2+}]{sub d} and [Na{sup +}]{sub d} at all ages in dystrophic cardiomyocytes. These data showed that loss of dystrophin in mdx cardiomyocytes produced an age-dependent intracellular Ca{sup 2+} and Na{sup +} overload mediated at least in part by enhanced Ca{sup 2+} entry through Gd{sup 3+} sensitive transient receptor potential channels (TRPC), and by IP{sub 3} receptors.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2019

A micromorphically regularized Cam-clay model for capturing size-dependent anisotropy of geomaterials

Here we introduce a regularized anisotropic modified Cam-clay (MCC) model which captures the size-dependent anisotropic elastoplastic responses for clay, mudstone, shales, and sedimentary rock. By homogenizing the multiscale anisotropic effects induced by clay particle aggregate, clusters, peds, micro-fabric, and mineral contact across length scales, we introduce two distinctive anisotropic mechanisms for the MCC model at the material point and mesoscale levels. We first employ a mapping that links the anisotropic stress state to a fictitious isotropic principal stress-space to introduce anisotropy at the material point scale. Then, the mesoscale anisotropy is introduced via an anisotropic regularization mechanism. This anisotropic regularization mechanism is triggered by introducing gradient-dependence of the internal variables through a penalty method such that the resultant gradient-enhanced plastic flow may exhibit anisotropic responses non-coaxial to the stress gradient of the yield function. The influence of the size-dependent anisotropy on the formation of the shear band and the macroscopic responses of the effective media are analyzed in 2D and 3D numerical examples.

42 ENGINEERING↗

DOE OSTI2021

Skeletal model reduction with forced optimally time dependent modes

Skeletal model reduction based on local sensitivity analysis of time dependent systems is presented in which sensitivities are modeled by forced optimally time dependent (f-OTD) modes. The f-OTD factorizes the sensitivity coefficient matrix into a compressed format as the product of two skinny matrices, i.e. f-OTD modes and f-OTD coefficients. The modes create a low-dimensional, time dependent, orthonormal basis which capture the directions of the phase space associated with most dominant sensitivities. These directions highlight the instantaneous active species, and reaction paths. Evolution equations for the f-OTD modes and coefficients are derived, and the implementation of f-OTD for skeletal reduction is described. For demonstration, skeletal reduction is conducted of the constant pressure ethylene-air burning in a zero-dimensional reactor, and new reduced models are generated. The laminar flame speed, the ignition delay, and the extinction curve as predicted by the models are compared against some existing skeletal models in literature for the same detailed model. Finally, the results demonstrate the capability of f-OTD to eliminate unimportant reactions and species in a systematic, efficient and accurate manner.

42 ENGINEERING↗

DOE OSTI2020

Distributionally robust facility location problem under decision-dependent stochastic demand

While the traditional facility location problem considers exogenous demand, in some applications, locations of facilities could affect the willingness of customers to use certain types of services, e.g., carsharing, and therefore they also affect realizations of random demand. Moreover, a decision maker may not know the exact distribution of such endogenous demand and how it is affected by location choices. In this paper, we consider a distributionally robust facility location problem, in which we interpret the moments of stochastic demand as functions of facility-location decisions. We reformulate a two-stage decision-dependent distributionally robust optimization model as a monolithic formulation, and then derive exact mixed-integer linear programming reformulation as well as valid inequalities when the means and variances of demand are piecewise linear functions of location solutions. We conduct extensive computational studies, in which we compare our model with a decision-dependent deterministic model, as well as stochastic programming and distributionally robust models without the decision-dependent assumption. Here, the results show superior performance of our approach with remarkable improvement in profit and quality of service under various settings, in addition to computational speed-ups given by formulation enhancements. These results draw attention to the need of considering the impact of location decisions on customer demand within this strategic-level planning problem.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2013

Molecular dynamics studies of the size and temperature dependence of the kinetics of freezing of Fe nanoparticles

Molecular dynamics (MD) computer simulations have been carried out and a novel modified technique of Voronoi polyhedra has been performed to identify solid-like particles in a molten nanoparticle. This technique works quite well in analyzing the effects of particle size on nucleation rates of iron nanoparticles in the temperature range of 750–1160 K. Nanoparticles with 1436 and 2133 Fe atoms have been examined and the results are compared with those obtained earlier with Fe{sub 331} nanoparticles. Nucleation rates for freezing obtained from MD simulations for Fe{sub 2133} vary from 8.8×10{sup 34} m{sup 3}/s to 4.1×10{sup 35} m{sup 3}/s at over a temperature range from 1160 K to 900 K, Rates for. Fe{sub 1436} and Fe{sub 331} are somewhat higher. Nucleation rates increase as supercooling deepens until the viscosity of the liquid increases sharply enough to slow down the rate. Bt applying classical nucleation theory, the interfacial free energy between solid and liquid cab be estimated From this and other thermodynamic information can be derived a theoretical expression for the size-dependence of the heat of fusion of nanoparticles. Results agreed quite well with those observed in our MD observations. An earlier expression in the literature for this size-dependence was shown to be incorrect. The size dependence of melting point is discussed. - Graphical abstract: Critical nuclei of crystallization. Display Omitted - Highlights: • Solid state material synthesis. • Material structure. • Experimental study of nucleation in condensed materials. • Computation study of nucleation in condensed materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2018

Length-scale-dependent nanoindentation creep behaviour of Ti/Al multilayers by magnetron sputtering

This study presented length-scale-dependent room temperature creep behaviour of Ti/Al multilayers by nanoindentation. Ti/Al multilayers with individual layer thickness ranging from 10 nm to 250 nm were prepared by a direct current magnetron sputtering method. Microstructural analysis showed that the prepared Ti/Al multilayers were polycrystalline, with strong Ti (0002) and Al (111) texture. Nanoindentation creep tests were performed to examine the time-dependent creep deformation, stress exponent, creep strain rate sensitivity and contact creep compliance of the multilayers at room temperature. It was found that both the maximum creep deformation and the creep strain rate sensitivity increase with an increase in the individual layer thickness, indicating a length-scale-dependent creep behaviour of the Ti/Al multilayers. The values of stress exponent were found to lay in the range of 15.74–61.46, implying that the creep behaviour of the multilayers was controlled by the dislocation creep mechanism. Finally, the contact creep compliances of the Ti/Al multilayers were well modelled by a two-element Kelvin-Voigt model. From this, it was determined that the creep numbers and retardation times increased with increased individual layer thickness.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2013

Temperature-dependent adsorption of surfactant molecules and associated crystallization kinetics of noncentrosymmetric Fe(IO{sub 3}){sub 3} nanorods in microemulsions

Graphical abstract: - Highlights: • Crystallization of Fe(IO{sub 3}){sub 3} in microemulsions probed by hyper-Rayleigh scattering. • A faster growth and a better shape control of nanorods are obtained at 80 °C. • Different persistent cell deformations are related to the crystallization kinetics. • A temperature-dependent adsorption of surfactants on nanorods is suggested. - Abstract: Aggregation-induced crystallization of iron iodate nanorods within organic–inorganic aggregates of primary amorphous precursors is probed by time-dependent hyper-Rayleigh scattering measurements in Triton X-100 based-microemulsions. In the context of a growing interest of noncentrosymmetric oxide nanomaterials in multi-photon bioimaging, we demonstrate by a combination of X-ray diffraction and electron microscopy that an increase in the synthesis of temperature results in faster crystallization kinetics and in a better shape-control of the final Fe(IO{sub 3}){sub 3} nanorods. For initial microemulsions of fixed composition, room-temperature synthesis leads to bundles of 1–3 μm long nanorods, whereas shorter individual nanorods are obtained when the temperature is increased. Results are interpreted in terms of kinetically unfavorable mesoscale transformations due to the strong binding interactions with Triton molecules. The interplay between the nanorod crystallization kinetics and their corresponding unit cell deformation, evidenced by lattice parameter refinements, is attributed to a temperature-dependent adsorption of surfactants molecules at the organic–inorganic interface.

36 MATERIALS SCIENCE↗

DOE OSTI2017

Facile synthesis and temperature-dependent luminescence of single-phase dual-emitting CdTe@NaNO{sub 3} composite

Graphical abstract: Single-phase dual-emitting CdTe@NaNO{sub 3} composite was prepared by a facile and efficient aqueous ethanol phase assisted coprecipitation method. Its use in self-referencing luminescent thermometry was tested, by exploiting the temperature-dependence of fluorescence intensity ratio (green/red) in range of 273–473 K. - Highlights: • Single-phase green and red dual-emitting CdTe@NaNO{sub 3} composite was prepared. • CdTe QDs embedded in NaNO{sub 3} matrices exhibit photoluminescence quantum yields of 35%. • Temperature-dependent luminescent properties of CdTe@NaNO{sub 3} composite were studied. • It could be a good candidate for ratiometric temperature sensing with a high relative sensitivity. - Abstract: Single-phase dual-emitting CdTe@NaNO{sub 3} composite was prepared by a facile and efficient aqueous ethanol phase assisted coprecipitation method, providing a new type of solid-state luminescent material with processability, robustness and high luminescence. Cubic-shape Green + Red (G + R) CdTe@NaNO{sub 3} composite particles display single-excitation, dual-emission with two well-resolved, intensity-comparable fluorescence peaks. Its application potential in ratiometric luminescent thermometry was tested, by exploiting the temperature-dependence of fluorescence intensity ratio (green/red) in range of 273–473 K, and the maximum sensitivity is found to be 0.6183% K{sup −1} at 473 K. The results indicate that dual-emitting G + R CdTe@NaNO{sub 3} composite could be considered as potential candidates for ratiometric temperature sensing.

36 MATERIALS SCIENCE↗