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DOE OSTI2025

Precision measurement of lifetime and branching ratios of the 4⁢𝑓 13⁡ 5⁢𝑑⁢6⁢𝑠 1 ⁢[5/2] 5/2 state in Yb + ions

We report spectroscopic and time-resolved experimental observations to characterize the [Xe]⁢4⁢𝑓 13 ⁡( 2 𝐹$^𝑜_{5/2}$)⁢5⁢𝑑⁢6⁢𝑠⁡( 1 𝐷)⁢ 1 ⁢[5/2]$^𝑜_{5/2}$ state in 172 Yb + ions. We access this state from the metastable 4⁢𝑓 14 ⁡5⁢𝑑⁡( 2 𝐷 3/2,5/2 ) manifold and observe an unexpectedly long lifetime of 𝜏 = 37.9⁢(9) ⁢µ⁢s that allows visible Rabi oscillations and resolved-sideband spectroscopy. Using a combination of coherent population dynamics, high-fidelity detection and heralded state preparation, and optical pumping methods, we measure the branching ratios to the 2 𝐷 3/2 , 2 𝐷 5/2 , and 2 𝑆 1/2 states to be 0.359⁢(2), 0.639(2), and 0.0023⁢(16), respectively. The branching ratio to the 4⁢𝑓 13⁡ 6⁢𝑠 2 ⁡( 2 𝐹 7/2 ) is compatible with zero within our experimental resolution. We also report measurements of Landé 𝑔-factor of the 1 ⁢[5/2]$^𝑜_{5/2}$ state. Further, the branching ratio of the 2 𝐷 5/2 to 2 𝑆 1/2 decay in 172 Yb + was measured to be 0.188(3), improving its relative uncertainty by an order of magnitude. Our measurements provide experimental benchmarks for better understanding the atomic structure of Yb + ions, which still lacks accurate numerical descriptions, and the use of high-lying excited states for partial detection and qubit manipulation in the omg architecture.

74 ATOMIC AND MOLECULAR PHYSICS↗

NASA NTRS1994

Low Earth orbit durability evaluation of protected silicone for advanced refractive photovoltaic concentrator arrays

The need for efficient, cost effective sources of electrical power in space has led to the development of photovoltaic power systems which make use of novel refractive solar concentrators. These concentrators have been conceived in both point-focus and linear-focus designs. Current concentrator lenses are fabricated from flexible silicones with Fresnel facets along their inside surface. To insure the efficient operation of these power systems, the concentrator lenses must be durable and the silicone material must remain specularly transmitting over a reasonable lifetime in low Earth orbit (LEO) and other space environments. Because of the vulnerability of silicones to atomic oxygen and ultraviolet radiation in LEO these lenses have been coated with a multi-layer metal oxide protective coating. The objective of this research was to evaluate the LEO durability of the multilayer coated silicone for advanced refractive photovoltaic concentrator arrays with respect to optical properties and microstructure. Flat metal oxide coated silicone samples were exposed to ground-laboratory and in-space atomic oxyqen for durability evaluation.

Degroh, Kim K.↗

NASA NTRS1984

Atomic inner-shell transitions

Atomic inner-shell processes have quite different characteristics, in several important aspects, from processes in the optical regime. Energies are large, e.g., the 1s binding energy reaches 100 keV at Z = 87; relativistic and quantum-electrodynamic effects therefore are strong. Radiationless transitions vastly dominate over photon emission in most cases. Isolated inner-shell vacancies have pronounced single-particle character, with correlations generally contributing only approximately 1 eV to the 1s and 2p binding energies; the structure of such systems is thus well tractable by independent-particle self-consistent-field atomic models. For systems containing multiple deep inner-shell vacancies, or for highly stripped ions, the importance of relativistic intermediate coupling and configuration interaction becomes pronounced. Cancellation of the Coulomb interaction can lead to strong manifestations of the Breit interaction in such phenomena as multiplet splitting and hypersatellite X-ray shifts. Unique opportunities arise for the test of theory.

Crasemann, B.↗

DOE OSTI2021

Suppression of Helium Induced Cracking in Laser Repair Welding of Highly Irradiated Stainless Steels

Welding repair of irradiated nuclear reactor materials such as austenitic stainless steels used for the reactor internals has been challenging due to irradiation generated helium in the material matrix over an extended period of time. In this study, improved laser welding techniques, including the novel Auxiliary Beam Stress Improved (ABSI) technique that proactively manages the stresses during laser repair welding is investigated to substantially reduce or avoid the occurrence of intergranular helium-induced cracking (HeIC). Here, laser weld cladding, with and without ABSI technique, was applied to deposit weld metal on irradiated stainless steel (Type 304 L) blocks with various helium concentrations up to approximately 20 atomic parts per million (appm). Welded samples were cross-sectioned and analyzed using optical and electron microscopes. It was found that, with the improved laser welding techniques, no macroscopic (millimeter-sized) cracks were observed in any of the samples. Microscopic (less than 50 μm) cracks were present in the heat affected zone. Statistical analysis on the sample with the highest helium concentration (~20 appm) reveals that the ABSI technique could effectively reduce the size and amounts of microscopic cracks.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Tunable Perovskite-Derived Bismuth Halides: Cs 3 Bi 2 (Cl 1– x I x ) 9

Bismuth-based perovskites are of interest as safer alternatives to lead-based optoelectronic materials. Prior studies have reported on the compounds Cs 3 Bi 2 Cl 9 , Cs 3 Bi 2 I 9 , and Cs 3 Bi 2 Cl 3 I 6 . Here we examine a range of compounds of the formula Cs 3 Bi 2 (Cl 1–x I x ) 9 , where x takes values from 0.09 to 0.52. Powder and single-crystal X-ray diffraction were used to determine that all of these compounds adopt the layered vacancy-ordered perovskite structure observed for Cs 3 Bi 2 Cl 3 I 6 , which is also the high-temperature phase of Cs 3 Bi 2 Cl 9 . We find that, even with very small iodine incorporation, the structure is switched to that of Cs 3 Bi 2 Cl 3 I 6 , with I atoms displaying a distinct preference for the capping sites on the BiX 6 octahedra. Optical absorption spectroscopy was employed to study the evolution of optical properties of these materials, and this is complemented by density functional theory electronic structure calculations. Finally, three main absorption features were observed for these compounds, and with increasing x, the lowest-energy features are red-shifted.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Plasmonic Hot-Carrier Generation and Catalysis in Ti 3 C 2 O 2 from Real-Time TDDFT Simulations

Photoinduced hot electrons are central to plasmon-driven catalysis. Atomically thin Ti 3 C 2 O 2 , with high carrier density and broad optical absorption, offers a promising platform for plasmon-driven reactions. However, comprehensive investigations of its plasmon resonance, hot-carrier generation, and plasmonic catalytic performance remain limited. In this work, real-time time-dependent density functional theory (rt-TDDFT) was employed to study Ti 3 C 2 O 2 ’s plasmon excitation and hot-carrier generation from nonradiative plasmon damping. The temporal evolution of the dipole moment reveals plasmon resonance in Ti 3 C 2 O 2 , followed by strong plasmon damping that redistributes the stored energy to generate hot carriers. Ti 3 C 2 O 2 with low oxygen vacancy concentration (O v -Ti 3 C 2 O 2 ) exhibits plasmonic behavior resembling the pristine surface, and the plasmon-generated hot electrons can markedly reduce the dissociation barrier of CO 2 at the oxygen vacancy. These findings provide fundamental insights into the plasmonic properties of Ti 3 C 2 O 2 and how they drive its catalytic performance in surface reactions, which is valuable for advancing plasmon-driven catalysis.

CO2 reduction↗

DOE OSTI2022

Vapor-Phase Aggregation of Cerium Oxide Nanoparticles in a Rapidly Cooling Plasma

Local conditions, such as temperature and oxygen availability, have a pronounced effect on the formation and evolution of fallout following a nuclear explosion. While the behavior of nuclear-relevant materials such as uranium has begun to be explored under a wider range of environments, little is known about the behavior of plutonium. Here, using cerium as a surrogate, we track the vapor-phase aggregation of cerium oxide nanoparticles created in a plasma flow reactor under conditions of controlled temperature at two different oxygen fugacities. In situ optical emission spectroscopy is used to measure the variations in the spectral intensity of atomic and molecular species with temperature and oxygen content. We find that the relative rate of gas-phase oxidation of cerium is highly dependent on both temperature and local redox conditions within the flow reactor, to the extent that doubling the oxygen availability effectively doubles the amount of vapor-phase cerium monoxide at high temperatures (>2000 K). Condensed cerium oxide nanoparticles are also collected and analyzed ex situ via transmission electron microscopy and grazing-incidence small-angle X-ray scattering to determine their elemental composition, crystal structure, and size distribution. The size and morphology of the condensed nanoparticles are independent of local redox conditions, forming the same crystal type with the same size distribution regardless of oxygen availability. Postcondensation particle evolution, however, is found to be predominantly driven by temperature, with the average particle size increasing as particles cool and subsequently aggregate. These results expand our understanding of the chemical and physical behavior of refractory oxides that form during the early stages of fallout formation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

Molecular conducting magnetic heterostructures

Building molecular conducting magnets has been of considerable interest due to their metallic transport and magnetic properties. Conjugated aniline anions and transition-metal cations are recognized to synthesize such π–d interaction frameworks. Here, an interfacial assembly of quasi-two-dimensional aniline heterojunction frameworks is developed, which consists of a proton-aniline conducting layer (conductivity of 9.2 × 10 2 S cm -1 ) and a transition metal–aniline magnetic layer. The two-dimensional aniline coordination framework with pronounced π–d interactions is indispensable for obtaining ordered spin states and metallic transport conductivity. We apply optical and Raman spectroscopy to study the interactions between the metal cations and nitrogen atoms in the aniline chains. The bilayer heterostructure maintains a high conductivity of 3.5 × 10 2 S cm -1 and increased magnetization, while the coupling of metallic conducting and magnetic layers leads to an enhanced magnetoconductance of 0.4% under a magnetic field of 70 kOe.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Synthesis of a series of rare-earth-based multi-anion chalcogenide iodides RE 3 Si 2 Se x S 8− x I (RE = La, Ce, Pr, and Nd) using the flux-assisted boron–chalcogen mixture method

Single crystals and polycrystalline powders of rare earth mixed chalcogenide iodides La 3 Si 2 Se 1.21 S 6.79 I, Ce 3 Si 2 Se 1.39 S 6.61 I, Pr 3 Si 2 Se 1.22 S 6.78 I, and Nd 3 Si 2 Se 1.18 S 6.82 I were prepared using the reactive flux-assisted boron–chalcogen mixture (BCM) method at 850 °C. All compounds crystallized in the monoclinic crystal system, space group C2/c (space group number 15). The series adopts the La 3 Si 2 O 8 Cl structure type, containing isolated SiQ 4 tetrahedra connected by REQ 8 (RE = La, Ce, Pr and Nd) polyhedra; this arrangement creates tunnels that are filled by I atoms. The partial substitution of S by Se was carried out to modulate the optical properties. Phase pure samples and uniform solid solutions were obtained for all compositions as determined using powder X-ray diffraction patterns. Polycrystalline powders were used for physical property measurements, including magnetic susceptibility and UV-Vis diffuse reflectance. The solid-state UV-Vis data for the polycrystalline La 3 Si 2 Se 1.21 S 6.79 I, Ce 3 Si 2 Se 1.39 S 6.61 I, and Pr 3 Si 2 Se 1.22 S 6.78 I samples revealed band gaps of E g = 2.5(1), 2.2(1), and 2.3(1) eV, typical of semiconductors. Magnetic measurements indicated that Ce 3 Si 2 Se 1.39 S 6.61 I and Nd 3 Si 2 Se 1.18 S 6.82 I exhibit paramagnetic behavior with slightly negative Weiss constants θ = −25 and −38. The photoluminescence spectrum of Ce 3 Si 2 Se 1.39 S 6.61 I exhibits a broad emission band around ∼493 nm.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Interface creation on a mixed-terminated perovskite surface

In the field of complex oxide heterostructures, understanding of the initial substrate surface can be critical to fundamental studies regarding the development of emergent properties at the film–substrate interface. For this reason, a considerable amount of effort has gone into the development of techniques to achieve surfaces with single termination for a variety of perovskite single crystals. However, a decisive understanding of how an interface is created when epitaxial growth occurs on a mixed terminated surface remains lacking. Employing in situ synchrotron X-ray scattering during thin film growth by molecular beam epitaxy, we investigate the initial stages of growth on (LaAlO 3 )(Sr 2 AlTaO 6 ) (001) substrates with mixed termination. Using LaNiO 3 as a model system, we find that the surface layers of the substrate restructure during deposition such that while a NiO 2 monolayer is weakly bound, a LaO monolayer bonds strongly, effectively incorporating with (Al, Ta)O 2 from the surface and forming a La(Al, Ta)O 3 ultrathin film.  With regard to the synthesis of high-quality complex oxide heterostructures, it is important that the substrate meet an array of criteria related to the crystal structure, lattice parameter, thermodynamic properties, electrical and optical properties, and so on. In particular, the surface of the substrate should be atomically smooth and exhibit the step-terrace structure ideal for epitaxial thin film growth. Perovskite oxides with the formula ABO 3 have two possible (001) surfaces: AO (A-site termination) and BO 2 (B-site termination). The ability to consistently achieve one of these surface terminations on SrTiO 3 , i.e., TiO 2 , has helped SrTiO 3 become the predominant oxide in the field.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Substrate-enhanced photothermal nano-imaging of surface polaritons in monolayer graphene

Surface polaritons comprise a wealth of light–matter interactions with deep sub-wavelength scale confinement of electromagnetic modes. However, their nanoscale localized dissipation and thermalization processes are not readily accessible experimentally. Here, we introduce photothermal force microscopy to image surface plasmon polaritons (SPPs) in monolayer graphene through their non-radiative SiO2 substrate dissipation. We demonstrate the real-space SPP imaging via photo-induced atomic force detection, and from comparison with scattering-type scanning near-field optical microscopy imaging attribute the force response to substrate dissipation-enhanced thermal expansion. This work illustrates that nano-optical tip–sample induced dissipative forces facilitate a direct mechanical detection of surface polariton interactions with monolayer sensitivity.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2024

On the nature of two-photon transitions for a collection of molecules in a Fabry–Perot cavity

Here, we investigate the effect of a cavity on nonlinear two-photon transitions of a molecular system and we analyze how such an effect depends on the cavity quality factor, the field enhancement, and the possibility of dephasing. We find that the molecular response to strong light fields in a cavity with a variable quality factor can be understood as arising from a balance between (i) the ability of the cavity to enhance the field of an external probe and promote multiphoton transitions more easily and (ii) the fact that the strict selection rules on multiphoton transitions in a cavity support only one resonant frequency within the excitation range. Although our simulations use a classical level description of the radiation field (i.e., we solve Maxwell–Bloch or Maxwell–Liouville equations within the Ehrenfest approximation for the field–molecule interaction), based on experience with this level of approximation in the past studies of plasmonic and polaritonic systems, we believe that our results are valid over a wide range of external probing.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2020

Generation of gamma radiation by a subterawatt ultrashort laser pulse: optimisation of preplasma and pulse duration

We report an experimental and numerical study of the acceleration of electrons in a plasma interacting with a subterawatt laser pulse (intensity of ∼3 × 10{sup 18} W cm{sup −2} at a pulse duration of 50 fs). A preplasma layer on the surface of a molybdenum target is formed by an additional laser pulse with a duration of 8 ns and an intensity of ∼2 × 10{sup 12} W cm{sup −2}. It is shown that an increase in the laser pulse duration to 1700 fs at a constant energy (and a proportional decrease in intensity) leads to an increase in the yield of bremsstrahlung γ-radiation by more than an order of magnitude when the nanosecond pulse is ahead of the femtosecond one by 15 − 25 ns. Interferometry data and results of diagnostics of optical and γ-radiation of a plasma demonstrate that the collisional ionisation of atoms by electrons oscillating in the field of such a laser pulse plays an essential role in the formation of electron density profile. The sensitivity of the described effect to the level of amplified spontaneous emission is determined, despite the nanosecond pulse impact. Numerical simulations show that at a large pulse duration, the acceleration of electrons is stipulated by the beaking of plasma waves excited during stimulated Raman scattering of laser radiation. (paper)

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2026

Resonance Ionization Spectroscopy Experiment at Facility for Rare Isotope Beams

This manuscript reports on the commissioning of the Resonance Ionization Spectroscopy Experiment (RISE) at the BEam COoler and LAser spectroscopy (BECOLA) facility at Facility for Rare Isotope Beams (FRIB). The instrument implements the collinear resonance ionization spectroscopy technique for sensitive measurements of isotope shifts and hyperfine structure of short-lived isotopes produced at FRIB. The existing BECOLA beamline was extended to integrate an electrostatic ion-beam bender and an ion detector at ultrahigh vacuum. An injection-seeded titanium-sapphire laser and a multiharmonic pulsed neodymium-doped yttrium aluminum garnet laser were installed to perform resonant excitation and selective ionization. Commissioning tests were performed to demonstrate the capabilities of the instrument by measuring the hyperfine structure of stable 27 Al produced in an offline ion source. The RISE instrument is ready and operational for future studies of short-lived isotopes at FRIB.

Atomic spectra↗

DOE OSTI2022

Cold-atom quantum simulator for string and hadron dynamics in non-Abelian lattice gauge theory

We propose an analog quantum simulator for simulating real-time dynamics of (1+1)-dimensional non-Abelian gauge theory well within the existing capacity of ultracold-atom experiments. The scheme calls for the realization of a two-state ultracold fermionic system in a one-dimensional bipartite lattice, and the observation of subsequent tunneling dynamics. Being based on the loop string hadron formalism of SU(2) lattice gauge theory, this simulation technique is completely SU(2) invariant and simulates accurate dynamics of physical phenomena such as string breaking and/or pair production. The scheme is scalable and particularly effective in simulating the theory in the weak-coupling regime, and also a bulk limit of the theory in the strong-coupling regime up to certain approximations. This paper also presents a numerical benchmark comparison of the exact spectrum and real-time dynamics of lattice gauge theory to that of the atomic Hamiltonian with an experimentally realizable range of parameters.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2022

Direct evidence of the dominant role of multiphoton permanent-dipole transitions in strong-field dissociation of NO 2 +

We study laser-induced dissociation of a metastable NO 2+ ion-beam target into N + +O + , focusing on the prominent contribution by molecules breaking parallel to the polarization at high peak laser intensity (~10 15 W/cm 2 ). Our experimental results and time-dependent Schrödinger equation calculations show that, contrary to commonly held intuition that electronic transitions always prevail, the dominant process underlying this highly aligned dissociation is a multiphoton permanent-dipole transition involving only the electronic ground state and leading to its vibrational continuum. Strong-field permanent-dipole transitions should thus be considered generally, as they may play a significant role in other heteronuclear molecules. Moreover, their role should only grow in importance for longer wavelengths, a trending direction in ultrafast laser studies.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2023

Quantum Langevin theory for two coupled phase-conjugated electromagnetic waves

We provide a general macroscopic phenomenological formula of quantum Langevin equations for two coupled phase-conjugated electromagnetic fields with linear loss (gain) and complex nonlinear coupling coefficient. The macroscopic phenomenological formula is obtained from the coupling matrix to preserve the field commutation relations and correlations, which does not require knowing the microscopic details of light-matter interaction and internal atomic structures. To validate this phenomenological formula, we take spontaneous four-wave mixing in a double-Λ four-level atomic system as an example to numerically confirm that our macroscopic phenomenological result is consistent with that obtained from the microscopic Heisenberg-Langevin theory. We find that a complex-valued nonlinear coupling coefficient can lead to noises even without linear gain or loss. Lastly, we apply the quantum Langevin equations to study the effects of linear gain and loss, complex phase mismatching, as well as complex nonlinear coupling coefficient in entangled photon pair (biphoton) generation, particularly to their temporal quantum correlations.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2023

Enhancing strontium clock atom interferometry using quantum optimal control

Strontium clock atom interferometry is a promising new technology, with multiple experiments under development around the world to explore its potential for dark matter and gravitational wave detection. In these detectors, large momentum transfer using sequences of many laser pulses is necessary, and thus high-fidelity pulses are important since small errors become magnified. Quantum optimal control (QOC) is a framework for developing control pulse waveforms that achieve high fidelity and are robust against experimental imperfections. Resonant single-photon transitions using the narrow clock transition of strontium involve significantly different quantum dynamics than more established atom interferometry methods based on far-detuned two-photon Raman or Bragg transitions, which leads to new opportunities and challenges when applying QOC. Here, we study in simulation QOC pulses for strontium clock interferometry and demonstrate their advantage over basic square pulses (primitive pulses) and composite pulses in terms of robustness against multiple noise channels. In conclusion, this could improve the scale of large momentum transfer in Sr clock interferometers, paving the way to achieving these scientific goals.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗