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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

Characterization of n-Type Iodine-Doped and Indium-Doped CdTe/Cd-Se-Te Thin Films Fabricated by Close-Spaced Sublimation Epitaxy

In this study, n-type CdTe thin films, specifically iodine-doped CdTe (CdTe:I), indium-doped CdTe (CdTe:In), and indium-doped Cd-Se-Te (CST:In), were synthesized using close-spaced sublimation epitaxy (CSSE). Characterization techniques secondary ion mass spectrometry (SIMS), electron backscatter diffraction (EBSD), Hall-effect measurements, and time-resolved photoluminescence (TRPL) were employed to analyze the chemical, structural, and electronic properties of these materials. The results indicated epitaxial single crystal CSSE films grew on the single crystal substrates, with carrier density ranging from 10^14 - 10^16 cm -3 , and after post-annealing, the minority-carrier lifetimes reach near the radiative limit. Additionally, a preliminary exploration of homojunction structures with an n- type (CdTe:In /CST:In /CdTe:I) /CdTe:P /Cu /Mo configuration was performed. The best device performance was achieved with CdTe:I including CdS aiding in band alignment, resulting in a power conversion efficiency (..eta..) of 2.61% with open circuit voltage (Voc) of 850 mV, fill factor (FF) of 47.8%, and short-circuit current (Jsc) of 6.44 mA/cm 2 . The observed low Jsc and efficiency may be attributed to a buried junction and a poor interface, due to dopant interdiffusion. Consequently, further investigations focusing on interface optimization, diffusion blocking, and reduced recombination through passivation, are crucial to enhancing the efficiency of CSSE CdTe homojunction devices in the future.

cadmium compounds↗

3D velocity map imaging of electrons with TPX3CAM

In this report we demonstrate three-dimensional velocity map imaging of low energy electrons using a TPX3CAM, where the three-dimensional momentum information [$p_x, p_y, p_z$] is encoded in position and timing [x, y, t] of hits on the camera sensor. We make use of the camera sensor for the [x, y] information and a constant fraction discriminator and fast time to digital converter in the camera for the time information. We illustrate the capabilities of our apparatus by presenting above threshold ionization measurements of xenon, which produces well defined structures in the momentum resolved photoelectron yield.

79 ASTRONOMY AND ASTROPHYSICS↗

Molecular chemisorption of N 2 on IrO 2 (110)

We investigated the adsorption of N 2 on stoichiometric and O-rich IrO 2 (110) surfaces using temperature programmed desorption (TPD) experiments and density functional theory (DFT) calculations. TPD shows that N 2 desorbs predominantly from the stoichiometric-IrO 2 (110) surface in a well-defined peak at 270 K for N 2 coverages below about 0.5 ML, and that a shoulder centered near 235 K develops in the N 2 TPD traces as the coverage approaches saturation, indicating that adsorbed N 2 molecules become destabilized at high N 2 coverage. Experiments of N 2 adsorption onto O-rich IrO 2 (110) surfaces provide evidence that N 2 adsorbs exclusively on the coordinatively-unsaturated Ir atoms (Ircus) of the surface, and that pre-adsorbed O-atoms (“on-top” oxygen) stabilize adsorbed N 2 molecules, causing the main N 2 TPD peak to shift toward higher temperature with increasing oxygen coverage. Consistent with prior results, our DFT calculations predict that an N 2 molecule preferentially adsorbs into an upright configuration on an Ircus atom of the IrO 2 (110) surface and achieves a binding energy of about 100 kJ/mol. The computed binding energy agrees well with our experimental estimate of ~90 kJ/mol for low N 2 coverages on stoichiometric IrO 2 (110). Lastly, the DFT calculations also quantitatively reproduce the observed stabilization of N 2 by co-adsorbed on-top O-atoms and predict the destabilization of N 2 on IrO 2 (110) as the N 2 adlayer becomes crowded at high coverage.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

TiO2 Nanocrystal-Framed Li 2 TiSiO 5 Platelets for Low-Voltage Lithium Battery Anode

Titanium-based anode materials are attracting considerable attention for use in high-performance lithium-ion batteries, but the compromised energy density caused by high voltage plateaus and unsatisfactory capacities severely retards their practical applications. Herein, a molten-salt synthesis of Li 2 TiSiO 5 crystalline platelets and a subsequent selective facet modification by in situ growth of TiO 2 nanocrystal frames are facilely achieved. The discharge voltage plateau at around 0.5 V renders the Li 2 TiSiO 5 anode safe compared with graphite and confers a high energy density compared with zero-strain Li 4 Ti 5 O 12 anode. With the optimized size, structure, and content of modified TiO2 nanocrystals associated with the exposed (001) plane of Li 2 TiSiO 5 , the Li 2 TiSiO 5 -based anodes can deliver a capacity of above 300 mAh g -1 , enhanced rate performance, and a capacity retention of 66% after 10 000 cycles. In situ X-ray diffraction and ex situ transmission electron microscopy have demonstrated the structural stability of the anodes upon charge/discharge. Further theoretical calculation reveals 3D migration paths of Li + ions in Li 2 TiSiO 5 . The selective modification of in situ grown TiO2 nanocrystals on certain facets of crystallites opens a new door for the development of electrode materials possessing superior electrochemical properties.

anodes↗

Corrosion of novel reactive silver ink and commercial silver-based metallizations in diluted acetic acid

Silver-based metallizations in photovoltaic modules are susceptible to corrosion by acetic acid generated in ethylene vinyl acetate encapsulated modules, resulting in power losses over time. Here, three silver-based metallizations are exposed to diluted acetic acid, in concentrations representative of that found in field-exposed modules. Compositional, morphological, and structural changes of the metallizations are studied over 3000 h of exposure to diluted acetic acid using Raman spectroscopy mapping, X-ray diffraction, and scanning electron microscopy. The three metallizations studied are: 1) a commercial high-temperature fire-through Ag paste, commonly used for Si diffused junction solar cells; 2) a commercial low-temperature paste normally used for silicon heterojunction cells; and 3) a novel low-temperature reactive silver ink shown to be suitable for photovoltaic applications. We find distinct corrosion rates for the high-temperature silver paste and reactive silver ink in the presence of diluted acetic acid. However, the low-temperature silver paste appears to be more corrosion resistant, likely due to a polymer layer that protects the silver particles.

36 MATERIALS SCIENCE↗

Diethylenetriamine-functionalized graphene oxide: Insights into ion adsorption and applications in rare earth element separation

The growing demand for critical minerals and materials requires atom- and energy-efficient, selective separations to overcome the challenges posed by the similar chemical and physical properties of the rare earth elements (REEs) and their low concentrations in unconventional domestic feedstocks. Here, in this study, we developed diethylenetriamine-functionalized graphene oxide (DETA-GO) as a membrane material for REE adsorption and separation. Synthesis conditions were optimized to maximize nitrogen incorporation while also preserving GO dispersibility for facile membrane fabrication. We investigated the mechanism of amine functionalization, the nitrogen-bonding configurations, the organization of the interlayer transport channels, and the resulting effects on ion and water transport for REE separations. Neat-GO and DETA-GO multilayer laminate membranes were fabricated by vacuum filtration onto polymer supports. To investigate the effects of amine functionalization, the membranes were characterized using scanning electron microscopy, Raman, Fourier transform infrared, and X-ray photoelectron spectroscopy, as well as grazing-incidence X-ray diffraction measurements. Ion permeation experiments with representative lanthanum (La 3+ ) and ytterbium (Yb 3+ ) solutions revealed enhanced ion adsorption and water transport through DETA-GO membranes compared to neat-GO. The strong affinity of the membranes for multivalent REEs was also validated with conductivity and inductively coupled plasma mass spectrometry measurements. Atomistic insight into the role of amine functionalization in modulating nanochannel architecture and long-term stability, optimizing adsorption sites, and regulating REE and water transport was obtained using classical molecular dynamics simulations. Collectively, our joint experimental and theoretical study demonstrates the potential of DETA-GO membranes for selective REE separations, offering insights into ion-binding mechanisms, water-transport properties, and nanochannel optimization for the recovery of critical materials from aqueous feedstocks.

Adsorbent↗

Passivation‐Induced Species Dynamics and Microstructural Evolution in Solid‐State Lithium–Sulfur Cathodes

Solid-state lithium–sulfur (SSLS) batteries offer high theoretical energy density, yet their practical viability is hindered by poor sulfur utilization and limited rechargeability. At the core of this challenge lies the passivating nature of Li 2 S, which restricts ionic and electronic transport, suppresses interfacial activity, and severely impedes the reversibility of electrochemical reactions. In this study, we elucidate the mechanistic origins of these limitations by resolving how charge and discharge species form, grow, and spatially evolve within the cathode microstructure under varied current densities and electrode compositions. By resolving the species distribution at the particle scale and coupling it with Raman spectroscopy and X-ray diffraction, we demonstrate how Li 2 S formation induces localized surface passivation that progressively limits electrochemical accessibility within the cathode microstructure. Sulfur utilization is found to be strongly governed by the interplay between sulfur loading, residual porosity, and interfacial architecture. High sulfur contents result in buried, electrochemically isolated domains due to poor solid electrolyte (SE) percolation, while low sulfur contents trigger SE degradation via parasitic reactions. The resulting sulfur-porosity maps delineate the mechanistic boundaries between reversible and transport-limited regimes, offering actionable design guidance for SSLS cathodes with enhanced sulfur utilization.

electrode microstructure↗

Design and Development of Stable Nanocrystalline High‐Entropy Alloy: Coupling Self‐Stabilization and Solute Grain Boundary Segregation Effects

Abstract Grain growth is prevalent in nanocrystalline (NC) materials at low homologous temperatures. Solute element addition is used to offset excess energy that drives coarsening at grain boundaries (GBs), albeit mostly for simple binary alloys. This thermodynamic approach is considered complicated in multi‐component alloy systems due to complex pairwise interactions among alloying elements. Guided by empirical and GB‐segregation enthalpy considerations for binary‐alloy systems, a novel alloy design strategy, the “ pseudo‐binary thermodynamic ” approach, for stabilizing NC‐high entropy alloys (HEAs) and other multi‐component‐alloy variants is proposed. Using Al 25 Co 25 Cr 25 Fe 25 as a model‐HEA to validate this approach, Zr, Sc, and Hf, are identified as the preferred solutes that would segregate to HEA‐GBs to stabilize it against growth. Using Zr, NC‐Al 25 Co 25 Cr 25 Fe 25 HEAs with minor additions of Zr are synthesized, followed by annealing up to 1123 K. Using advanced characterization techniques— in situ X‐ray diffraction (XRD), scanning/transmission electron microscopy (S/TEM), and atom probe tomography, nanograin stability due to coupling self‐stabilization and solute‐GB segregation effects is reported in HEAs up to substantially high temperatures. The self‐stabilization effect originates from the preferential GB‐segregation of constituent HEA‐elements that stabilizes NC‐Al 25 Co 25 Cr 25 Fe 25 up to 0.5 T m ( T m –melting temperature). Meanwhile, solute‐GB segregation originates from Zr segregation to NC‐Al 25 Co 25 Cr 25 Fe 25 GBs; this results in further stabilization of the phase and grain‐size (≈14 nm) up to ≈0.58 and ≈0.64 T m , respectively.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Optimization of La 2 NiO 4+δ Electrolysis Cell Oxygen Electrode through Surfactant-Enabled LaCoO 3±δ Nanocatalyst Deposition

Lanthanum nickelate (LNO) has shown promise as a Cr-resistant air electrode material for SOECs but has suboptimal surface oxygen exchange properties. Nanocoating of the LNO surface with lanthanum cobaltite (LCO) was chosen to improve cell performance as a surface oxygen conductor. The work focused on the implementation of a two-step nano-LCO film deposition utilizing catechol molecules in a porous LNO electrode. The subgoals of the work were to maintain nanosized LCO particles/ grains to increase active surface area and to control the regularity/ homogeneity of the coating across the microstructure. To achieve these goals, a novel surfactant-enhanced liquid infiltration method was utilized, where nucleation sites were spread across the electrode structure to control the location and size of LCO particles. Various catechol surfactant compositions were evaluated for their ability to control the kinetics of nanoparticle deposition and the homogeneity of the coating. Chelated LCO was characterized by X-ray diffraction (XRD), which found a substantial improvement in LCO formation with surfactant addition and determined polymerized norepinephrine to be the best-performing surfactant, with 88.4% pure LCO formed at low temperature. X-ray photoelectron spectroscopy (XPS) confirmed LCO nanostructures formed by the two-step infiltration process, showing no impurities and a stable perovskite structure. Deposition kinetics were analyzed using atomic force microscopy (AFM), correlating infiltration times and solution molarity to nanoparticle size and distribution, the results of which were confirmed in symmetrical cell samples by scanning electron microscopy (SEM). Electrochemical impedance spectroscopy (EIS) testing demonstrated substantial improvements in polarization resistance, where the nanocoating reduced the resistance by ∼55% to 0.152 Ω·cm 2 at 700 °C and 0.039 Ω·cm 2 at 800 °C. Electrical conductivity relaxation (ECR) at this temperature confirmed an improved surface oxygen exchange coefficient of the LCO + LNO heterostructure predicted by the Bode data from EIS, alongside a reduction in activation energy by about 30%.

Deposition↗

Synthesis and ion-irradiation tolerance of the Dy2TiO5 polymorphs

In developing improvements in nuclear fuels, work has been conducted in replacing boron with lanthanides to act as neutron absorbent materials. To further this development for the first time the three major polymorphs of Dy2TiO5 have been fabricated as bulk, single-phase materials in a systematic study. Crystal structure refinement has been carried out from powder x-ray diffraction data, with further structural detail attained via electron diffraction. A cubic phase, defect-pyrochlore, Fd-3m space group, was found with cell parameter a = 10.2996 (1) angstrom and oxygen x48f positional parameter = 0.331 (1). Dy2TiO5 was also fabricated as a bulk, single-phase compound with hexagonal symmetry, P6(3)/mmc space group, with cell parameters a = b = 3.6307(2), c = 11.8963(8) angstrom. The radiation response for each of the polymorphs has been investigated in-situ via 1 MeV Kr - ion-irradiation and transmission electron microscopy characterisation at the IVEM-TANDEM facility, Argonne National Laboratory. Critical temperatures, T-c, for maintaining crystallinity during irradiation were determined and showed Dy2TiO5 with either orthorhombic or cubic symmetry to perform the best, with the lowest T-c values of 711 and 761 K respectively when compared with the hexagonal form. These relatively low T-c values may be attributed to different characteristics for each phase; high anti-site defect formation energy for the orthorhombic symmetry, and the ability to accommodate disorder for the cubic symmetry.

Burnable poison↗

Microwave-assisted ammonia decomposition over metal nitride catalysts at low temperatures

The negative environmental impact of fossil fuel-based energy systems has unveiled the need to develop a CO x -free sustainable hydrogen (H 2 ) economy. Employing a microwave-assisted route, a ternary metal nitride catalyst (i.e., Co 2 Mo 3 N), and a low-temperature-pressure NH 3 decomposition process, this study investigated the possibility of developing a distributed H 2 production process. Here, this study not only explored lower cost-based catalyst systems but also the use of a microwave reactor to increase the energy efficiency of the process. Results from catalytic NH 3 decomposition experiments, performed in microwave reactors on Co 2 Mo 3 N catalyst, demonstrated the peak energy efficiency (of ~0.006 kgH 2 /kWh) at 400 °C in ambient pressure (with an NH 3 conversion >90%) which was around ninety times (~90 x) more efficient than a conventional system. Activation energy calculation also displayed a 20% less energy requirement for the microwave-based process (~31 kJ mol -1 ) than the conventional system (~37 kJ mol -1 ), indicating the advantage of the microwave-based process. Further microwave-assisted catalytic measurements and characterization of the Co 2 Mo 3 N catalyst, using x-ray diffraction (XRD) technique and scanning electron microscopic (SEM) images, revealed the excellent stability of this material at its peak performance (at 400 °C) and illustrated the potential of using this catalyst for a sustainable, economic, and energy-efficient approach for producing CO x -free H 2 .

08 HYDROGEN↗

Understanding formation mechanisms of intermetallic compounds in dissimilar Al/steel joint processed by resistance spot welding

Here, this paper confirmed the formation mechanism of intermetallic compounds (IMCs) in Al/steel resistance spot welds with transmission electron microscopy, electron backscatter diffraction, nanoindentation and thermodynamic calculations. In particular, the formation of AlFe with BCC_B2 structure, which is not commonly seen in welds, was identified. The formation mechanism of IMCs at the high welding energy region is described as follows. Al 13 Fe 4 first nucleates from the Al side, followed by Al 5 Fe 2 growth with Fe atoms accumulating at the Al 13 Fe 4 grain boundaries. Then, Al 5 Fe 2 grains grow continuously to coarse columnar grains, and AlFe forms at the interface of Al 5 Fe 2 grains and the ferrite phase. Lastly, the needle-like Al 13 Fe 4 forms in the cooling process. At the middle welding energy region, only equiaxed Al 5 Fe 2 and small Al 13 Fe 4 grains are formed at the interface because of the lower diffusion rates of Al and Fe, hence postponing the growth of Al 5 Fe 2 and Al 13 Fe 4 . At the low welding energy region, only sporadic Al 5 Fe 2 and Al 13 Fe 4 grains are formed surrounded by the Al phase.

42 ENGINEERING↗

Correlating Rate-Dependent Transition Metal Dissolution between Structure Degradation in Li-Rich Layered Oxides

Understanding the mechanism of the rate-dependent electrochemical performance degradation in cathodes is crucial to developing fast charging/discharging cathodes for Li-ion batteries. Here, in this work, taking Li-rich layered oxide Li 1.2 Ni 0.13 Co 0.13 Mn 0.54 O 2 as the model cathode, the mechanisms of performance degradation at low and high rates are comparatively investigated from two aspects, the transition metal (TM) dissolution and the structure change. Quantitative analyses combining spatial-resolved synchrotron X-ray fluorescence (XRF) imaging, synchrotron X–ray diffraction (XRD) and transmission electron microscopy (TEM) techniques reveal that low-rate cycling leads to gradient TM dissolution and severe bulk structure degradation within the individual secondary particles, and especially the latter causes lots of microcracks within secondary particles, and becomes the main reason for the fast capacity and voltage decay. In contrast, high-rate cycling leads to more TM dissolution than low-rate cycling, which concentrates at the particle surface and directly induces the more severe surface structure degradation to the electrochemically inactive rock-salt phase, eventually causing a faster capacity and voltage decay than low-rate cycling. These findings highlight the protection of the surface structure for developing fast charging/discharging cathodes for Li-ion batteries.

25 ENERGY STORAGE↗

Photoexcitation of Fe 3 O Nodes in MOF Drives Water Oxidation at pH=1 When Ru Catalyst Is Present

Abstract Artificial photosynthesis strives to convert the energy of sunlight into sustainable, eco‐friendly solar fuels. However, systems with light‐driven water oxidation reaction (WOR) at pH=1 are rare. Broadly used [Ru(bpy) 3 ] 2+ (bpy=2,2’‐bipyridine) photosensitizer has a fixed +1.23 V potential which is insufficient to drive most water oxidation catalysts (WOCs) in acid, while Fe 2 O 3 , featuring the highly oxidizing holes, is not stable at low pH. Here, the key examples of Fe‐based metal–organic framework (MOF) water oxidation photoelectrocatalysts active at pH=1 are presented. Fe‐MIL‐126 and Fe MOF‐dcbpy structures were formed with 4,4’‐biphenyl dicarboxylate (bpdc), 2,2’‐bipyridine‐5,5’‐dicarboxylate (dcbpy) linkers and their mixtures. Presence of dcbpy linkers allows integration of metal‐based catalysts via coordination to 2,2’‐bipyridine fragments. Fe‐based MOFs were doped with Ru‐based precursors to achieve highly active MOFs bearing [Ru(bpy)(dcbpy)(H 2 O) 2 ] 2+ WOC. Materials were analyzed with X‐ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infra‐red (FTIR) spectroscopy, resonance Raman, X‐ray absorption spectroscopy, fs optical pump‐probe, electron paramagnetic resonance (EPR), diffuse reflectance and electric conductivity measurements and were modeled by band structure calculations. It is shown that under reaction conditions, Fe III and Ru III oxidation states are present, indicating rate‐limiting electron transfer in MOF. Fe 3 O nodes emerge as photosensitizers able to drive prolonged O 2 evolution in acid. Further developments are possible via MOF's linker modification for enhanced light absorption, electrical conductivity, reduced MOF solubility in acid, Ru‐WOC modification for faster WOC catalysis, or Ru‐WOC substitution to 3d metal‐based systems. The findings give further insight for development of light‐driven water splitting systems based on Earth‐abundant metals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

In Situ Recrystallization of Co-Evaporated Cu(In,Ga)Se2 Thin Films by Copper Chloride Vapor Treatment towards Solar Cell Applications

Cu(In,Ga)Se2 (or CIGS) thin films and devices were fabricated using a modified three-stage process. Using high deposition rates and a low temperature during the process, a copper chloride vapor treatment was introduced in between the second and third stages to enhance the films properties. X-ray diffraction and scanning electron microscopy demonstrate that drastic changes occur after this recrystallization process, yielding films with much larger grains. Secondary ion mass spectrometry shows that the depth profile of many elements is not modified (such as Cu, In and Se) while others change dramatically (such as Ga and Na). Because of the competing effects of these changes, not all parameters of the solar cells are enhanced, yielding an increase of 15% in the device efficiency at the most.

14 SOLAR ENERGY↗

Voltage and temperature effects on low cobalt lithium-ion battery cathode degradation

Degradation of low cobalt lithium-ion cathodes was tested using a full factorial combination of upper cut-off voltage (4.0 V and 4.3 V vs. Li/Li + ) and operating temperature (25 °C and 60 °C). Half-cell batteries were analyzed with electrochemical and microstructural characterization methods. Electrochemical performance was assessed with galvanostatic cycling, cyclic voltammetry (CV), and electrochemical impedance spectroscopy (EIS) supported by distribution of relaxation times (DRT) analysis. Electrode microstructure was characterized with scanning electron microscopy (SEM), X-ray diffraction (XRD), and X-ray absorption near edge structure (XANES) imaging. Higher cut-off voltage cycling shows presence of NiO x formation, a low diffusivity rock-salt phase, in both CV and XRD data. XRD patterns confirmed that the rock-salt phase was beginning to form at the low cut-off voltage at high temperature, but in much lower intensity than at the high cut-off voltage. Higher temperature accelerates degradation processes at both voltages. Degradation factors at high temperature include NiO x formation, cathode material dissolution, and electrolyte decomposition. SEM analysis suggests that supporting phases may isolate and disconnect active material particles reducing capacity retention and battery life cycle. DRT analysis and XANES imaging show that both high temperature samples revealed a NiO x phase based on an increased diffusive impedance and a visible shift in the XANES spectra. The low cut-off voltage, high temperature sample showed a split peak and shift to lower energies indicating early formation of the NiO x phase. The diffusive impedance, which hinders intercalation and deintercalation, is driven by the formation of the NiO x phase. While primarily driven by cut-off voltage, elevated temperature also contributes to this degradation mechanism.

electrochemical impedance spectroscopy↗

Speckle contrast of interfering fluorescence X-rays

With the development of X-ray free-electron lasers (XFELs), producing pulses of femtosecond durations comparable with the coherence times of X-ray fluorescence, it has become possible to observe intensity–intensity correlations due to the interference of emission from independent atoms. This has been used to compare durations of X-ray pulses and to measure the size of a focused X-ray beam, for example. Here it is shown that it is also possible to observe the interference of fluorescence photons through the measurement of the speckle contrast of angle-resolved fluorescence patterns. Speckle contrast is often used as a measure of the degree of coherence of the incident beam or the fluctuations of the illuminated sample as determined from X-ray diffraction patterns formed by elastic scattering, rather than from fluorescence patterns as addressed here. Commonly used approaches to estimate speckle contrast were found to suffer when applied to XFEL-generated fluorescence patterns due to low photon counts and a significant variation of the excitation pulse energy from shot to shot. A new method to reliably estimate speckle contrast under such conditions, using a weighting scheme, is introduced. The method is demonstrated by comparing the speckle contrast of fluorescence observed with pulses of 3 fs to 15 fs duration.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗