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At least 181 records · Page 10

Demonstrating Computational Equivalence Between Continuous and Discrete Adjoint Methods by Calculating Time-Dependent Adjoint Solutions with Neutron Diffusion Models

The continuous adjoint method and the discrete adjoint method are two alternative approaches used to calculate adjoint solutions for adjoint systems. The continuous adjoint method derives adjoint equations analytically from continuous forward equations and then solves the adjoint equations either analytically or numerically in a discretized form whereas the discrete adjoint method calculates the adjoint solutions directly from the discretized forward equations. With regard to the methodology development and calculation procedure, distinct differences are well recognized between the two methods. For certain reasons, both methods are exclusively preferred and commonly used by different computational communities, but limited studies clarify the connections between the two adjoint methods from either of the communities. Herein, this paper demonstrates the computational equivalence between the continuous and discrete adjoint methods by investigating time-dependent adjoint solutions to the two-group neutron diffusion model in nuclear reactor analysis problems using both methods. Adjoint solutions can be used to estimate system parameters for reactor safety analysis. Appropriate final state conditions for the adjoint systems are specified in both of the methods, and the conditions are clarified with proper physical explanations. With the help of an event-based case study on neutron diffusion models, the accuracy of the time-dependent adjoint fluxes obtained from both methods is verified, and the pros and cons of both adjoint methods are examined. More importantly, the computational equivalence of both methods is demonstrated when they are applied to multigroup neutron diffusion systems. The advantage of calculating time-dependent adjoint fluxes by directly solving time-dependent adjoint systems rather than taking steady-state approximations as in common practice is also demonstrated.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Sensitivities of time-dependent temperature profile predictions for NSTX with the multi-mode model

The Multi-Mode Model (MMM) for turbulent transport was applied to a large set of well-analyzed discharges from the National Spherical Torus Experiment (NSTX) in order to evaluate its sensitivities to a wide range of plasma conditions. MMM calculations were performed for hundreds of milliseconds in each discharge by performing time-dependent predictive simulations with the 1.5D tokamak integrated modeling code TRANSP. A closely related study (Lestz et al 2025 Plasma Phys. Control. Fusion 67 105029) concluded that MMM predicted electron and ion temperature profiles that were in reasonable agreement with NSTX observations, generally outperforming a different reduced transport model, TGLF. This finding motivates the more thorough investigation of the characteristics of the MMM predictions conducted in this work. The simulations with MMM have electron energy transport dominated by electron temperature gradient modes in the examined discharges with relatively low plasma β (ratio of kinetic plasma pressure to magnetic field pressure) and high collisionality, transitioning to a mixture of different modes for higher β and lower collisionality. The thermal ion diffusivity predicted by MMM is much smaller than the neoclassical contribution, in line with previous experimental analysis of NSTX. Nonetheless, the electron and ion temperature profiles are coupled via collisional energy exchange and thus sensitive to which transport channels are predicted. The time-dependent simulations with MMM are robust to the simulation start time, converging to remarkably similar temperature profiles later during the discharge. MMM typically overpredicts confinement relative to NSTX observations, leading to the prediction of overly steep temperature profiles. Plasmas with spatially broader temperature profiles, higher plasma β, and longer energy confinement times tend to be predicted by MMM with better agreement with the experiment. As a result, these findings provide useful context for understanding the regime-dependent tendencies of MMM in anticipation of self-consistent, time-dependent predictive simulations of NSTX-U discharges with these same modeling tools.

MMM↗

Transverse-momentum-dependent pion structures from lattice QCD: Collins-Soper kernel, soft factor, TMDWF, and TMDPDF

We present the first lattice quantum chromodynamics (QCD) calculation of the pion valence-quark transverse-momentum-dependent parton distribution function (TMDPDF) within the framework of large-momentum effective theory (LaMET). Using correlators fixed in the Coulomb gauge (CG), we computed the quasi-TMD beam function for a pion with a mass of 300 MeV, a fine lattice spacing of 𝑎 =0.06 fm, and multiple large momenta up to 3 GeV. The intrinsic soft functions in the CG approach are extracted from form factors with large momentum transfer, and as a byproduct, we also obtain the corresponding Collins-Soper (CS) kernel. Our determinations of both the soft function and the CS kernel agree with perturbation theory at small transverse separations (𝑏 ⊥ ) between the quarks. At larger 𝑏 ⊥ , the CS kernel remains consistent with recent results obtained using both CG and gauge-invariant TMD correlators in the literature. By combining next-to-leading logarithmic factorization of the quasi-TMD beam function and the soft function, we obtain an 𝑥-dependent pion valence-quark TMDPDF for transverse separations 𝑏 ⊥ ≳1 fm. Interestingly, we find that the 𝑏 ⊥ dependence of the phenomenological parametrizations of TMDPDF for moderate values of 𝑥 are in reasonable agreement with our QCD determinations. In addition, we present results for the transverse-momentum-dependent wave function for a heavier pion with 670 MeV mass.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Ionization of HCCI Neutral and Cations by Strong Laser Fields Simulated With Time Dependent Configuration Interaction

Strong field ionization of neutral iodoacetylene (HCCI) can produce a coherent superposition of the X and A cations. This superposition results in charge migration between the CC π orbital and the iodine π-type lone pair which can be monitored by strong field ionization with short, intense probe pulses. Strong field ionization of the X and A states of HCCI cation was simulated with time-dependent configuration interaction using singly ionized configurations and singly excited, singly ionized configurations (TD-CISD-IP) and an absorbing boundary. Studies with static fields were used to obtain the 3-dimensional angular dependence of instantaneous ionization rates by strong fields and the orbitals involved in producing the cations and dications. The frequency of charge oscillation is determined by the energy separation of the X and A states; this separation can change depending on the direction and strength of the field. Furthermore, fields along the molecular axis can cause extensive mixing between the field-free X and A configurations. For coherent superpositions of the X and A states, the charge oscillations are characterized by two frequencies–the driving frequency of the laser field of the probe pulse and the intrinsic frequency due to the energy separation between the X and A states. For linear and circularly polarized pulses, the ionization rates show marked differences that depend on the polarization direction of the pulse, the carrier envelope phase and initial phase of the superposition. Varying the initial phase of the superposition at the beginning of the probe pulse is analogous to changing the delay between the pump and probe pulses. The charge oscillation in the coherent superposition of the X and A states results in maxima and minima in the ionization yield as a function of the superposition phase

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Dependable classical-quantum computing systems engineering

Increasing evidence suggests quantum computing (QC) complements traditional High-Performance Computing (HPC) by leveraging its unique capabilities, leading to the emergence of a new, hybrid paradigm, QHPC. However, this integration introduces new challenges, with dependability–defined by reproducibility, resiliency, and security and privacy–emerging as a central concern for building trustworthy systems that provide an advantage to the users. This paper proposes a framework for dependable QHPC system design, organized around these three pillars. We identify integration challenges, anticipate roadblocks, and highlight productive synergies across QC, HPC, cloud platforms, and network security. Drawing from both classical computing principles and quantum-specific insights, we present a roadmap for co-design that supports robust hybrid architectures. Our approach offers concrete metrics for assessing dependability, provides design guidance for engineers working at the QC-HPC interface, and surfaces new engineering questions around complexity, scale, and fault tolerance. Ultimately, designing for dependability is key to realizing practical, scalable QHPC systems and accelerating the broader quantum ecosystem capable of translating quantum promises into actual application delivery.

HPC↗

One-loop matching for spin-dependent quasi-TMDs

Transverse momentum dependent parton distribution functions (TMDPDFs) provide a unique probe of the three-dimensional spin structure of hadrons. We construct spin-dependent quasi-TMDPDFs that are amenable to lattice QCD calculations and that can be used to determine spin-dependent TMDPDFs. We calculate the short-distance coefficients connecting spin-dependent TMDPDFs and quasi-TMDPDFs at one-loop order. We find that the helicity and transversity distributions have the same coefficient as the unpolarized TMDPDF. We also argue that the same is true for pretzelosity and that this spin universality of the matching will hold to all orders in αs. Thus, it is possible to calculate ratios of these distributions as a function of longitudinal momentum and transverse position utilizing simpler Wilson line paths than have previously been considered.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Constraining the Chiral Magnetic Effect with charge-dependent azimuthal correlations in Pb-Pb collisions at $ \sqrt{s_{\mathrm{NN}}} $ = 2.76 and 5.02 TeV

Systematic studies of charge-dependent two- and three-particle correlations in Pb-Pb collisions at $ \sqrt{s_{\mathrm{NN}}} $ = 2.76 and 5.02 TeV used to probe the Chiral Magnetic Effect (CME) are presented. These measurements are performed for charged particles in the pseudorapidity ( η ) and transverse momentum ( p T ) ranges | η | < 0 . 8 and 0 . 2 < p T < 5 GeV/ c . A significant charge-dependent signal that becomes more pronounced for peripheral collisions is reported for the CME-sensitive correlators γ 1, 1 =$\langle4cos( φ α + φ β - 2Ψ 2 )$\rangle$ and γ 1, - 3 = $\langle$cos( φ α - 3 φ β + 2Ψ 2 )$\rangle$. The results are used to estimate the contribution of background effects, associated with local charge conservation coupled to anisotropic flow modulations, to measurements of the CME. A blast-wave parametrisation that incorporates local charge conservation tuned to reproduce the centrality dependent background effects is not able to fully describe the measured γ 1 , 1 . Finally, the charge and centrality dependence of mixed-harmonics three-particle correlations, of the form γ 1, 2 = $\langle$cos( φ α + 2 φ β - 3Ψ 3 )$\rangle$, which are insensitive to the CME signal, verify again that background contributions dominate the measurement of γ 1 , 1 .

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Submicron immunoglobulin particles exhibit FcγRII-dependent toxicity linked to autophagy in TNFα-stimulated endothelial cells

In intravenous immunoglobulins (IVIG), and some other immunoglobulin products, protein particles have been implicated in adverse events. Role and mechanisms of immunoglobulin particles in vascular adverse effects of blood components and manufactured biologics have not been elucidated. We have developed a model of spherical silica microparticles (SiMPs) of distinct sizes 200–2000 nm coated with different IVIG- or albumin (HSA)-coronas and investigated their effects on cultured human umbilical vein endothelial cells (HUVEC). IVIG products (1–20 mg/mL), bare SiMPs or SiMPs with IVIG-corona, did not display significant toxicity to unstimulated HUVEC. In contrast, in TNFα-stimulated HUVEC, IVIG-SiMPs induced decrease of HUVEC viability compared to HSA-SiMPs, while no toxicity of soluble IVIG was observed. 200 nm IVIG-SiMPs after 24 h treatment further increased ICAM1 (intercellular adhesion molecule 1) and tissue factor surface expression, apoptosis, mammalian target of rapamacin (mTOR)-dependent activation of autophagy, and release of extracellular vesicles, positive for mitophagy markers. Toxic effects of IVIG-SiMPs were most prominent for 200 nm SiMPs and decreased with larger SiMP size. Using blocking antibodies, toxicity of IVIG-SiMPs was found dependent on FcγRII receptor expression on HUVEC, which increased after TNFα-stimulation. Similar results were observed with different IVIG products and research grade IgG preparations. In conclusion, submicron particles with immunoglobulin corona induced size-dependent toxicity in TNFα-stimulated HUVEC via FcγRII receptors, associated with apoptosis and mTOR-dependent activation of autophagy. Testing of IVIG toxicity in endothelial cells prestimulated with proinflammatory cytokines is relevant to clinical conditions. Our results warrant further studies on endothelial toxicity of sub-visible immunoglobulin particles.

59 BASIC BIOLOGICAL SCIENCES↗

Grain size dependencies of intergranular solute segregation in nanocrystalline materials

Grain boundary segregation is of increasing importance for stabilizing nanocrystalline alloys, and while segregation is typically modeled as a scale-independent phenomenon, at the finest nanocrystalline grain sizes there are several sources of grain size dependence. Here we provide quantitative detail on two grain size dependencies not previously elaborated, both of which arise from the spectrality of intergranular segregation sites. The first of these arises because a change in grain size affects which portions of the segregation spectrum are occupied by the solutes, with no change in the shape or nature of the spectrum itself. The second of these arises from the presence of higher-order grain junctions, which have unique segregation behaviors and an increasing relative presence at finer grain sizes. This paper uses molecular statics to quantify these size dependencies in detail for the case of an Al(Mg) binary alloy. Together, these two effects combined have a significant effect on the effective McLean segregation energy of more than 6 kJ/mol (from approximately -18.5 kJ/mol at 5 nm to -12.5 kJ/mol at more than 40 nm), with the majority of grain size dependence arising from the spectrality of segregation sites.

36 MATERIALS SCIENCE↗

Zng1 is a GTP-dependent zinc transferase needed for activation of methionine aminopeptidase

The evolution of zinc (Zn) as a protein cofactor altered the functional landscape of biology, but dependency on Zn also created an Achilles' heel, necessitating adaptive mechanisms to ensure Zn availability to proteins. A debated strategy is whether metallochaperones exist to prioritize essential Zn-dependent proteins. Here, we present evidence for a conserved family of putative metal transferases in human and fungi, which interact with Zn-dependent methionine aminopeptidase type I (MetAP1/Map1p/Fma1). Deletion of the putative metal transferase in Saccharomyces cerevisiae (ZNG1; formerly YNR029c) leads to defective Map1p function and a Zn-deficiency growth defect. In vitro, Zng1p can transfer Zn 2+ or Co 2+ to apo-Map1p, but unlike characterized copper chaperones, transfer is dependent on GTP hydrolysis. Proteomics reveal mis-regulation of the Zap1p transcription factor regulon due to loss of ZNG1 and Map1p activity, suggesting that Zng1p is required to avoid a compounding effect of Map1p dysfunction on survival during Zn limitation.

59 BASIC BIOLOGICAL SCIENCES↗

Temperature-dependent changes in gas chromatographic separation metrics for trihexyl(tetradecyl)phosphonium-based ionic liquid stationary phases and comparison to conventional polysiloxane stationary phases

Here, to assess whether the trihexyl(tetradecyl)phosphonium chloride ([P 66614 + ][Cl - ]) ionic liquid (IL), employed as a gas chromatographic stationary phase, exhibits temperature-dependent phase transitions or structural heterogeneity, retention thermodynamics for probe molecules of varied chemical structure were investigated by gas chromatography (GC) over the temperature range of 25 to 64 °C using van’t Hoff analysis. All van’t Hoff plots for n-alkanes (C8–C12) and other probe analytes were linear, indicating the absence of detectable phase-transition behavior. The [P 66614 + ][Cl - ] IL was further compared with the [P 66614 + ] bis[(trifluoromethyl)sulfonyl]imide ([P 66614 + ][NTf 2 - ]) IL and commercial polysiloxane stationary phases in terms of temperature-dependent resolution behavior and chromatographic selectivity over the temperature range of 28–52 °C. The resolution factors of analytes in mixtures obtained using gas chromatography–mass spectrometry (GC–MS) and the summation of resolution values decreased smoothly with temperature on both IL stationary phases and on the dimethylphenylcyano-substituted polymeric stationary phase (OV-1701), whereas the poly(50% diphenyl/50% dimethyl siloxane) stationary phase (SPB-50) exhibited irregularities in its temperature-dependent summation of resolution profile, showing a distinct maximum in the temperature range of 34–40 °C. Selectivity values for the IL stationary phases were largely determined by the anion, with the [P 66614 + ][Cl - ] IL providing enhanced separation between polar and aromatic analytes, while the [P 66614 + ][NTf 2 - ] IL favored dispersive and π-π interactions that resulted in a reversal of elution order for some aliphatic–aromatic and alkyne-containing analyte pairs. Capillary columns prepared using different surface activation methods and coated with identical [P 66614 + ][Cl - ] IL stationary phase showed indistinguishable temperature-dependent trends in summation of resolution value and selectivity. An evaluation of analyte-specific selectivity provides insight into the characteristic separation behavior of the stationary phases and enables identification of analyte classes that are more efficiently separated on the [P 66614 + ]-based IL stationary phases compared to conventional stationary phase materials.

Chromatographic selectivity↗

Spin-dependent Seebeck and Nernst effects in an ideal skyrmion gas

In this work, we theoretically and numerically study spin-dependent Seebeck and Nernst effects in 2D ferromagnetic materials with the topological spin texture (skyrmion and vortex) ideal gas. From the numerical solution of the matrix Boltzmann equation for a nonequilibrium distribution function and the Lippmann–Schwinger equation for a T-matrix we find the strong nonlinear behaviors in the thermoelectric coefficients depending on skyrmion/vortex diameters and electron concentrations. In particular, the dramatic dependences in the Seebeck and Nernst coefficients take place at larger magnetic texture sizes where the abrupt sign flip in the vortex Seebeck and Nernst coefficients occurs in the narrow region of electron concentrations. In this case the normalized Nernst coefficient changes from +5 to -7. The spin-dependent thermoelectric coefficients are proportional to T at low temperatures for all skyrmion/vortex sizes.

36 MATERIALS SCIENCE↗

In-situ determination of strain during transient burst testing and the temperature dependence of Zircaloy-4 claddings

Understanding fuel system behavior during postulated loss-of-coolant accidents is pertinent for continued safe and efficient operation of light water reactors, particularly as higher burnups are being pursued and safety margins re-evaluated. Conventional mechanical models for the incumbent Zr alloys typically rely on the assumption that steady-state creep is the dominant fuel cladding response during transient accident conditions. To investigate this assumption, simulated accident burst testing was performed on Zircaloy-4 claddings with balloon behavior measured in-situ. Here, two distinct loading conditions were utilized during burst testing: (1) constant-gas-inventory where pressure was allowed to increase with temperature and (2) constant pressure. In-situ strains and strain rates were measured via 2-dimensional digital image correlation techniques and synchronized with temperature to determine deformation dependencies. The temperature dependence of strain rate was characterized by a two segment Arrhenius relationship, with a distinct transition between the high and low temperature/strain regimes. The average activation energy of the lower temperature/strain regime was 328 ± 25 kJ/mol, in agreement with the ~320 kJ/mol used for conventional LOCA models. However, the higher temperature/strain segment, which encompassed most of ballooning, showed increased activation energies as well as a dependence on whether the burst region was in view. For tests that burst away from the camera view, the average high temperature/strain segment activation energy was 635 ± 150 kJ/mol. For samples where the rupture opening formed in view, the average activation energy was 1015 ± 179 kJ/mol. This observed shift in temperature dependence indicates a transition in deformation mechanism at the end of life, possibly to time independent failure mechanisms, which has not yet been visualized in the literature for Zr alloys. Parameters at the transition points were analyzed to determine thresholds for this change in behavior, which occurred at an average hoop strain of 6.9 ± 2.1 %.

36 MATERIALS SCIENCE↗

Line tension induced character angle dependence of dislocation mobility in FCC alloys

Here, we explore the character angle dependence of dislocation-solute interactions in a face-centered cubic random Fe0.70Ni0.11Cr0.19 alloy through molecular dynamics (MD) simulations of dislocation mobility. Using the MD mobility data, we determine the phonon and thermally activated solute drag parameters which govern mobility for each dislocation character angle. The resulting parameter set indicates that, surprisingly, the solute energy barrier does not depend on character angle. Instead, only the zero-temperature flow stress—which is dictated by the activation area for thermal activation—is dependent on character angle. By analyzing the line roughness from MD simulations and the geometry of a bowing dislocation line undergoing thermal activation, we conclude that the character angle dependence of the activation area in this alloy is governed by the dislocation line tension, rather than the dislocation-solute interaction itself. Our findings motivate further investigation into the line geometry of dislocations in solid solutions.

36 MATERIALS SCIENCE↗

Shape- and Orientation-Dependent Scattering of Isolated Gold Nanostructures Using Polarized Dark-Field Microscopy

In this work, we demonstrate a simple and robust method for measuring the shape- and orientation-dependent optical scattering of various plasmonic nanostructures adsorbed onto a solid surface using polarized dark-field microscopy. By analyzing the dark-field scattering images of gold nanostructures using grazing incidence polarized light with a bench-top microscope, we are able to correlate optical scattering from the individual nanostructures with their shape and orientation. Depending on the size, shape, and orientation of the plasmonic nanostructures, they exhibit characteristic angle- and polarization-dependent scattering signals. Extracting the red, green, and blue channels of the scattering signals from a color-imaging detector as a function of azimuthal angle provides a polar plot of color intensity values that is characteristic of the underlying nanostructure. Examples are presented for various nanostructures, including spherical nanoparticles, nanotriangles, and nanorods. Experimental results are complemented by numerical calculations of the scattering spectra of representative model nanostructures. We demonstrate that the polarization- and orientation-dependent scattering behavior is a consequence of various localized surface plasmon modes existing in the nanostructures and can be used to verify the shape of individual objects as well as quickly identify the orientation of numerous objects on a densely populated substrate. We anticipate that this method will provide a rapid and efficient complement to the typical structural analysis of nanoparticles that is achieved by electron microscopy as well as providing a simple method for generating detailed information of the optical scattering of various types of individual plasmonic nanostructures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Resolving the Coverage Dependence of Surface Reaction Kinetics with Machine Learning and Automated Quantum Chemistry Workflows

Microkinetic models for catalytic systems require estimation of many thermodynamic and kinetic parameters that can be calculated for isolated species and transition states using ab initio methods. However, the presence of nearby coadsorbates on the surface can dramatically alter these thermodynamic and kinetic parameters causing them to be dependent on species coverage fractions. As there are combinatorially many coadsorbed configurations on the surface, computing the coverage dependence of these parameters is far less straightforward. We present a framework for generating and applying machine learning models to predict coverage-dependent parameters for microkinetic models. Our toolkit enables automatic calculation and evaluation of coadsorbed configurations allowing us to sample 2,000 coadsorbed adsorbates and transition states (TSs) for a diverse set of 9 reactions on Cu(111), a challenging surface, with four possible coadsorbates. This dataset was then used to train subgraph isomorphic decision trees (SIDTs) to predict the stability and association energy of configurations. We were able to achieve mean absolute errors (MAEs) of 0.106 eV on adsorbates, 0.172 eV on TSs, and due to natural error cancellation in SIDTs for relative properties, 0.130 eV on reaction energies and 0.180 eV on activation barriers. In conclusion, we describe how to use these models to predict coverage-dependent corrections for adsorbates and TSs and demonstrate on H*, HO*, and O* comparing the generated SIDT model with an iteratively refined version.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Real-Time Time-Dependent Nuclear–Electronic Orbital Approach: Dynamics beyond the Born–Oppenheimer Approximation

The quantum mechanical treatment of both electrons and nuclei is crucial in nona- diabatic dynamical processes such as proton-coupled electron transfer. The nuclear electronic orbital (NEO) method provides an elegant framework for including nuclear quantum effects beyond the Born-Oppenheimer approximation. To enable the study of nonequilibrium properties, we derive and implement a real-time NEO (RT-NEO) approach based on time-dependent Hatree-Fock or density functional theory, in which both the electronic and nuclear degrees of freedom are propagated in a time-dependent variational framework. Nuclear and electronic spectral features can be resolved from the time-dependent dipole moment computed using the RT-NEO method. The test cases demonstrate the dynamical interplay between the quantum nuclei and the electrons through vibronic coupling. Moreover, vibrational excitation in the RT-NEO approach is demonstrated by applying a resonant driving eld, and electronic excitation is demonstrated by simulating excited state intramolecular proton transfer. This work shows that the RT-NEO approach is a promising tool to study nonadiabatic quantum dynamical processes within a time-dependent variational description for the coupled electronic and nuclear degrees of freedom.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Universal Size-Dependent Stokes Shifts in Lead Halide Perovskite Nanocrystals

Size-dependent photoluminescence Stokes shifts (Δ E s ) universally exist in CsPbX 3 (X = Cl – , Br – , or I – ) perovskite nanocrystals (NCs). Δ E s values, which range from ~15 to 100 meV for NCs with average edge lengths ( l ) from approximately 13 to 3 nm, are halide-dependent such that Δ E s (CsPbI 3 ) > Δ E s (CsPbBr 3 ) ≳ Δ E s (CsPbCl 3 ). Observed size-dependent Stokes shifts are not artifacts of ensemble size distributions as demonstrated through measurements of single CsPbBr 3 NC Stokes shifts ((Δ E s ) = 42 ± 5 meV), which are in near quantitative agreement with associated ensemble ( l = 6.8 ± 0.8 nm) Δ E s values (Δ E s ≈ 50 meV). Transient differential absorption measurements additionally illustrate no significant spectral dynamics on the picosecond time scale that would contribute to Δ E s . This excludes polaron formation as being responsible for Δ E s . Overall, the results point to an origin for Δ E s , intrinsic to the size-dependent electronic properties of individual perovskite NCs.

36 MATERIALS SCIENCE↗