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DOE OSTI2025

Predicting Cislunar Orbit Lifetimes from Initial Orbital Elements

The volume of space between Earth’s geosynchronous orbit out to the Moon’s sphere of influence, including the lunar Lagrange points, is crucial for the successful planning and execution of space missions, but not fully understood dynamically. This region is a part of cislunar space. Trajectories through cislunar space are influenced by the gravitational forces of the Sun, Earth, Moon, and other Solar System planets leading to typically unpredictable and chaotic trajectory behavior. It is therefore difficult to predict the stability of an trajectory through cislunar space from a set of initial conditions or orbital elements. We simulate one million cislunar orbits to train a self-organizing map (SOM) to cluster the trajectories and orbits into families based on how long they remain stable within the cislunar space. Using the trained SOM, we are able to predict the stable lifetime of a trajectory through cislunar space from a set of initial orbital elements to within an accuracy of 10% for 8% of simulated trajectories and within 50% for 43% of the simulated trajectories. Clustering in the SOM suggests that a variety of trajectory morphologies have similar lifetimes. Once trained, the SOM can predict the stable lifetime of a given cislunar trajectory within milliseconds. The methods developed in this work enable the rapid identification of stable cislunar orbits and trajectories that could be used for future space exploration. Moreover, the developed SOM method can generate orbital and trajectory lifetime estimates from minimal observational data, such as a single two line element, making it useful for early warning systems and large-scale sensor network operations.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2026

Simulations of Interacting Binary Systems—Pathways to Radio-bright Gamma-Ray Burst Progenitors

Although the association of gamma-ray bursts (GRBs) with massive stellar death is on firm footing, the nature of the progenitor system and the key ingredients required for a massive star to produce a GRB remain open questions. Here, we investigate the evolution of a 15–25M ⊙ massive star with a 10–15M ⊙ black hole (BH) using Modules for Experiments in Stellar Astrophysics. We quantify companion-influenced angular-momentum evolution over a stellar lifetime for orbital periods where tides are significant, varying stellar and BH masses, initial stellar spin, and accretion and dynamo prescriptions while tracking mass loss and angular momentum. The final spin is set by tidal torques versus stellar winds. For binaries that initially avoid Roche-lobe overflow, tides can spin up the star, but a late-stage expansion can drive tidal stripping; associated mass and angular-momentum loss can suppress spin-up. We find that massive-star BH binaries at comparable mass ratios may be potential GRB progenitors for short orbital periods (∼20–5 × 10 2 days) and long orbital periods (∼2 × 10 3 –4 × 10 3 days), where our suite of lifetime simulations reveals a favored parameter space with negligible mass loss and enough spin angular momentum to power a GRB jet. For initially nonrotating stars, this provides a lower limit on the final spin above a threshold estimate consistent with forming a postcollapse BH mass of 5–10M ⊙ with a spin parameter ≥ 0.5. For initially rapidly rotating stars, tidal interactions may sustain high spin when mass loss is negligible because the binary is not tidally synchronized.

Hernandez, Angel [Univ. of Colorado, Boulder, CO (↗

DOE OSTI2025

Spin switchable optical phenomena in Rashba band structures through intersystem crossing in momentum space in solution-processing 2D-superlattice perovskite film

Spin-switchable phenomena are a critical element for the development of spintronic and chiroptic devices. Herein we combine a 2D-superlattice perovskite (4,4-DFPD2PbI4) film with a ferromagnetic cobalt (Co) layer to form a multiferroic perovskite/Co interface, and demonstrate spin-switchable circularly polarized luminescence (CPL) between right-handed σ+ and left-handed σ− polarizations. When the ferromagnetic spins of Co at the Co/perovskite interface are altered between positive and negative magnetic field directions, the CPL from the 2D-superlattice perovskite switches from σ+ to σ− polarization. The magnetic field effects present a unique method to confirm that CPL is generated by the circular-orbital momentum of light-emitting excitons within Rashba band structures, eliminating artifacts involving structural birefringence. Our polarized neutron reflectometry measurements confirm a super long-range spin-orbit interaction occurring in the 2D-superlattice perovskite films. The temperature dependence of spin-switchable phenomenon indicates an extraordinarily long orbital polarization lifetime, reaching microseconds at room temperature and milliseconds at 5 K.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Resolve instrument onboard the X-Ray Imaging and Spectroscopy Mission

We present an overview of the design and in-flight performance of the Resolve soft X-ray spectrometer on the X-Ray Imaging and Spectroscopy Mission that was successfully launched on September 7, 2023, on a JAXA H-IIA rocket from the Tanegashima Space Center of Japan. The instrument has a 36-pixel array of microcalorimeters, 35 of which are at the focus of a high-throughput grazing-incidence X-ray mirror. The instrument has achieved its required operational base temperature of 0.05 K and a spectral resolution of 4.5 eV (FWHM) at 6 keV. The cooling chain was designed to provide a lifetime of at least 3 years in orbit and operate with and without liquid helium to provide redundancy and the longest operational lifetime for the instrument. Early indications are that the cryogen lifetime may reach 6 years with a cryogen-free mode thereafter. A series of onboard X-ray calibration sources produces energy scale calibration lines simultaneously while observing celestial sources. The overall design and in-flight performance of Resolve are described.

Astronomy and AstroPhysics↗

DOE OSTI2025

Systematic uncertainties in the measurement of the neutron lifetime using the Lunar Prospector neutron spectrometer

The lifetime of free neutrons measured in the laboratory has a longstanding disparity of ≈9 s. A space-based technique has recently been proposed to independently measure the neutron lifetime using interactions between the galactic cosmic rays and a low atmosphere planetary body. This technique has not produced competitive results yet due to constraints of nonoptimized data that contain large systematic errors. We use data from the neutron spectrometer on-board NASA's Lunar Prospector, and study two large systematics in the measurement of neutron lifetime: the lunar subsurface temperature and the lunar surface composition. We use the HeCd and HeSn neutron spectrometer data when the spacecraft was in a highly elliptical orbit during the orbit insertion period. We report the neutron lifetime using four different models that each have different choices of surface temperature and composition. The 5° [Prettyman et al ., J. Geophys. Res.: Planets 111, 2005JE002656 (2006)] and 2° [Wilson et al., Phys. Rev. C 104, 045501 (2021)] rebinned maps result in 777.6±11.7 s and 739.6±10.8 s, respectively. For the 20° map (Prettyman et al., 2006), constant equatorial and a latitude-dependent temperature model result in 738.6±10.8 s and 767.3±11.2 s, respectively. Increasing the complexities of the models accounting for the systematic effects increase the measured lifetime. However, the reported measurements are not competitive with the laboratory results due to large unaccounted systematics resulting from nonoptimized measurements and modeling assumptions. This work serves as a study of systematic uncertainties for future neutron lifetime measurements using the space-based technique. We estimate the effect on the lifetime from the choice of temperature model to be to be 28.7 ±15.5 s, and choice of compositional map (for 20° and 5° maps) to be 10.3 ±12.2 s.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2026

Hidden Spin-Valley Locking Stabilizes Nanosecond Spin Polarization in 2D Perovskites

Room-temperature spin control in semiconductors is fundamental to spin-optoelectronics. Although inversion symmetry breaking offers one path for spin control in semiconductors, strong spin dephasing at elevated temperatures remains a persistent limitation. Hidden spin polarization without global symmetry breaking provides another promising material design strategy, but robust spin stabilization from this effect has yet to be experimentally realized. Here we show spin stabilization at room temperature in two-dimensional hybrid organic-inorganic perovskites through hidden spin-valley locking. We use functional non-primary ammonium cations to induce symmetry-breaking distortions in the metal-halide layers, producing giant local spin splitting while preserving global inversion symmetry. Time-resolved circular dichroism measurements reveal optically generated spin-polarized carriers that persist for 686 ps in (AzOH)2PbI4 and 4.7 ns in the lead-free analogue (AzOH)2SnI4 at room temperature, without an external magnetic field. First-principles calculations suggest that these long lifetimes arise from hidden spin valleys, enhanced dielectric screening and reduced spin-orbit-induced scattering in the Sn-based compound. Our design paradigm unlocks inversion-symmetric semiconductors with ultralong spin lifetimes, broadening the materials options for light-driven spin control.

14 SOLAR ENERGY↗

DOE OSTI2024

Photoluminescence of a Uranium(IV) Alkoxide Complex

In this report, we describe the photoluminescence of a homoleptic uranium(IV) alkoxide complex. Excitation of [Li(THF)] 2 [U IV (O t Bu) 6 ] leads to the first example of photoluminescence from a well-defined actinide complex originating from an f–f excitation, supported by second order multiconfigurational electronic structure calculations including spin–orbit coupling. These calculations show strong spin–orbit coupling between the excited triplet and singlet states for the 5f-orbital manifold, which leads to a long-lived excited state lifetime of 0.85 s at low temperature. The photophysical properties of homoleptic uranium(V) and uranium(VI) tertbutoxide complexes are also presented; we find that oxidation of the uranium(IV) alkoxide results in quenching of luminescence in [Li(THF)][U V (O t Bu) 6 ] and [U VI (O t Bu) 6 ]. This is attributed to competing ligand to metal charge transfer absorption processes shifted to lower energy upon oxidation of the actinide center, which mask the relevant f–f transitions in the visible region of the electronic absorption spectrum.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

First-Principles Framework for the Prediction of Intersystem Crossing Rates in Spin Defects: The Role of Electron Correlation

Optically active spin defects in solids are promising platforms for quantum technologies. In this work, we present a first-principles framework to investigate intersystem crossing processes, which represent crucial steps in the optical spin-polarization cycle used to address spin defects. Considering the nitrogen-vacancy center in diamond as a case study, we demonstrate that our framework effectively captures electron correlation effects in the calculation of many-body electronic states and their spin-orbit coupling and electron-phonon interactions, while systematically addressing finite-size effects. We validate our predictions by carrying out measurements of fluorescence lifetimes, finding excellent agreement between theory and experiments. The framework presented here provides a versatile and robust tool for exploring the optical cycle of varied spin defects entirely from first principles.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2025

Hard–Soft Acid–Base Theory Explains Photoexcited Carrier Dynamics in Porphyrin/CNT Nanohybrids: Time-Domain Atomistic Analysis

We employ the fundamental chemical concepts of hard− soft acid−base to formulate general principles governing excited-state dynamics in zinc porphyrin (ZnP)/carbon nanotube (CNT) hybrids for energy photoconversion. Atomistic quantum dynamics simulations demonstrate that electron-withdrawing and donating substituents at the ZnP β-pyrrolic position strongly influence the dynamics. ZnP photoexcitation produces subpicosecond electron transfer (ET) from ZnP to CNT, in agreement with the experiment. Substitutions of CN by H and tBu accelerate the ET. The trend is directly related to the hard−soft acid−base concept because the soft−soft interaction between the t Bu- ZnP acid and the mild CNT base enhances the donor−acceptor coupling. Longer coherence and more active vibrational modes facilitate the ET in t Bu-ZnP/CNT. Electron−hole recombination in CN-ZnP/CNT occurs on a hundred picosecond time scale, nicely corroborated by the experiment. The exciton lifetime is extended beyond a nanosecond by the substitutions. The soft−soft interaction in t Bu-ZnP/ CNT increases the splitting between the highest occupied orbitals of the two subsystems, reduces their mixing, and decreases nonadiabatic coupling between the ground and excited states. Rapid decoherence and involvement of low-frequency vibrations favor longer lifetimes. Our investigation reveals that larger p K a of the β-pyrrolic acid gives rapid ET and slow recombination and provides detailed mechanistic information, essential for future optoelectronic applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Experimental Demonstration of a Two-Dimensional Nonlinear Integrable System in a Particle Accelerator

A two-dimensional nonlinear integrable system was experimentally demonstrated at the Fermilab Integrable Optics Test Accelerator. The system was implemented by inserting a special nonlinear magnet in a conventional accelerator lattice. We characterized the system by measuring lifetimes, transverse profiles and transverse oscillation frequencies of the 150-MeV electron beam as a function of the strength of the nonlinear insert. The measured shift of the working point and the amplitude-dependent detuning were consistent with theoretical predictions. We also observed the predicted bifurcation of the stable closed orbit. A striking consequence of the system's implementation was the possibility to operate the storage ring with integer tunes without lifetime degradation. This research opens up novel ways to design particle accelerators and to stabilize particle beams.

Wieland, John [Fermilab] (ORCID:0000000289718523)↗

DOE OSTI2025

Mechanistic Insight into Tunable Spin Relaxation in Two-Dimensional Type-II Ligand-Perovskite Heterostructures

Two-dimensional (2D) metal-halide perovskites with spin-dependent optical properties hold great promise for spintronic and quantum applications. However, their spin lifetimes, especially for n = 1 2D perovskites, are typically limited to subpicosecond time scales due to rapid spin relaxation driven by strong spin−orbit coupling (SOC), electron−hole exchange interactions, and phonon-mediated scattering. Here, we demonstrate that type-II ligand-perovskite heterostructures overcome these constraints by reducing electron−hole wave function overlap and exciton binding energy. Compared to the type-I 2D perovskite (PEA) 2 PbI 4 with a spin lifetime of 0.29 ps at room temperature, our engineered type-II systems achieve substantially extended spin lifetimes, ∼6.37 ps for (4Tm) 2 PbI 4 and ∼18.47 ps for (4TCNm) 2 PbI 4 . In both materials, spatial charge separation across the perovskite−ligand interface mitigates the Bir−Aronov− Pikus (BAP) mechanism. Temperature- and fluence-dependent measurements reveal Elliott−Yafet (EY)-dominated spin relaxation in (4Tm) 2 PbI 4 , consistent with the observation of coherent phonon oscillation, whereas (4TCNm) 2 PbI 4 exhibits D’yakonov−Perel (DP)-dominated spin relaxation, with weaker phonon coupling further suppressing the EY relaxation, enabling spin lifetimes up to ∼126.81 ps at 5 K. Our findings establish a structural design framework for tailoring spin dynamics in 2D perovskites, offering a promising strategy to engineering spin and optoelectronic properties via rational ligand engineering.

Excitons↗

DOE OSTI2026

Spin Polarization from Circularly Polarized Light Induced Charge Transfer

Here, we show how a spin polarization can be generated through the photoinduced electron transfer of an achiral donor–acceptor complex following chiral light excitation. In particular, we illustrate the basic energetic and symmetry requirements for chirality induced spin selectivity where the chirality emerges from the electronic degrees of freedom following excitation with circularly polarized light. We study this effect in a simple model of a metalloporphyrin complex with an axial acceptor ligand using quantum mechanical rate theories and numerical simulations. We find that the spin polarization emerges due to the selective excitation of a ring current within the porphryin, breaking the degeneracy of the two degenerate spin states. The resultant spin polarization increases with the spin orbit coupling between the metal in the porphyrin and the axial ligand, and is transient, with a lifetime dependent on the rate of dephasing from the Jahn–Teller distortion mode. This proposed effect should be observable in spin-resolved photoemission spectroscopy.

charge transfer↗

DOE OSTI2025

Coherent population trapping and spin relaxation of a silicon vacancy center in diamond at millikelvin temperatures

Here, we report experimental studies of coherent population trapping (CPT) and spin relaxation in a temperature range 4 K–100 mK in a silicon vacancy (SiV) center subject to a transverse magnetic field. The spin linewidth, which is determined by spin dephasing, is extracted from power dependent CPT linewidths. Near and below 1 K, phonon-induced spin dephasing becomes negligible compared with that induced by the spin bath of naturally abundant 13 C atoms. The temperature dependence of the spin dephasing rates agrees with the theoretical expectation that phonon-induced spin dephasing arises primarily from orbital relaxation induced by first order electron-phonon interactions. A nearly 100-fold increase in spin lifetime is observed when the temperature is lowered from 4 K to slightly below 1 K, indicating that two-phonon spin-flip transitions play an essential role in the spin relaxation of SiV ground states.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Pre- and post-launch operation of the Resolve soft X-ray spectrometer onboard the XRISM satellite

Resolve is a high-resolution X-ray spectrometer onboard the X-Ray Imaging and Spectroscopy Mission (XRISM), launched on September 6 (UT), 2023. The Resolve has performed better than its required spectral resolution (7 eV at full width at half maximum at 6 keV), both on the ground and in orbit, and has been confirmed to have comparable performance to the soft X-ray spectrometer onboard the ASTRO-H (Hitomi) satellite. The focal plane is composed of an array of microcalorimeter detectors operated at 50 mK to achieve the required energy resolution, and the cooling system is designed to satisfy the lifetime requirement of over 3 years. The focal plane and cooling system are contained in a vacuum-insulated dewar. The cooling system is equipped with a two-stage adiabatic demagnetization refrigerator (ADR) that uses superfluid liquid helium (LHe) as its heat sink. The system includes a third ADR stage that can be used to provide the heat sink when the helium is exhausted. A Joule–Thomson cooler and several two-stage Stirling coolers are used to reduce the heat load on the LHe. During pre-launch operations, we carried out a superfluid LHe top-off operation. The resultant amount of LHe onboard Resolve was over 35 L before launch, which is sufficient to meet the lifetime requirement. During post-launch operation, the LHe vent valve was opened 5 min after launch during rocket acceleration, and the cryocoolers were turned on after several orbits, as planned, which established stable cooling within the dewar. Pre- and post-launch operations for the Resolve instrument were planned around multiple constraints from launch vehicle operations; all were successfully completed, and the launch requirements were fully met.

X-Ray Imaging and Spectroscopy Mission↗

DOE OSTI2024

The Role of Spin–Orbit Coupling in the Linear Absorption Spectrum and Intersystem Crossing Rate Coefficients of Ruthenium Polypyridyl Dyes

The successful use of molecular dyes for solar energy conversion requires efficient charge injection, which in turn requires the formation of states with sufficiently long lifetimes (e.g., triplets). The molecular structure elements that confer this property can be found empirically, however computational predictions using ab initio electronic structure methods are invaluable to identify structure-property relations for dye sensitizers. The primary challenge for simulations to elucidate the electronic and nuclear origins of these properties is a spin-orbit interaction which drives transitions between electronic states. Here, in this work, we present a computational analysis of the spin-orbit corrected linear absorption cross sections and intersystem crossing rate coefficients for a derivative set of phosphonated tris(2,2'-bipyridine)ruthenium(2+) dye molecules. After sampling the ground state vibrational distributions, the predicted linear absorption cross sections indicate that the mixture between singlet and triplet states plays a crucial role in defining the line shape of the metal-to-ligand charge transfer bands in these derivatives. Additionally, an analysis of the intersystem crossing rate coefficients suggests that transitions from the singlet into the triplet manifolds are ultrafast with rate coefficients on the order of 10 13 s -1 for each dye molecule.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Gas and dust dynamics in γ Cephei-type disks

Context. Giant planets are observed orbiting the primary stars of close binary systems. Such planets may have formed in compact circumprimary disks, which once surrounded these stars, under conditions much different than those encountered around single stars. Aims. In order to quantify the effects of the strong gravitational perturbations exerted on circumprimary disk material, the three-dimensional (3D) dynamics of gas and dust in orbit around the primary star of a compact and eccentric binary system was modeled by applying the stellar and orbital parameters of γ Cephei, a well-known system that can be representative of a class of close binaries. Methods. Circumprimary gas was approximated as an Eulerian viscous and compressible fluid and modeled by means of 3D hydrodynamical simulations, assuming locally isothermal conditions in the medium around the primary star. Dust grains were modeled as Lagrangean particles, subjected to gravity and aerodynamic drag forces. Models that include a giant planet were also considered. Results. Models indicate that spiral density waves excited around pericenter passage propagate toward the inner boundary of the disk, through at least a few pressure scale-heights from the mid-plane, inducing radial and vertical mixing in the gas. However, perturbations imparted to gas, both in terms of eccentricity and precession, are far weaker than previously estimated by two-dimensional (2D) simulations. Models predict small eccentricities, ≲0.03, and slow retrograde precession. The addition of a giant planet does not change the low eccentricity state of the disk. The parameters applied to the disk would lead to the formation of a massive planet, many times the mass of Jupiter, in agreement with some observations. Micron to mm-size dust grains are well coupled to the gas, resulting in similar dynamics and statistically similar distributions of orbital elements. The planet only affects the dust distributions locally. In agreement with outcomes of recent 2D models, the lifetime of an isolated circumprimary disk would be brief, ~10 5 years, because of its compact nature, requiring a long-term external supply of mass to allow for the in situ formation of a giant planet.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2026

Role of the Character of the Excited State of Singly Reduced Rh 2 (II,II) Intermediates on Photocatalytic Activity

Singly reduced intermediates have recently been implicated as photoactive intermediates in a number of important reactions; however, their photophysical properties remain poorly understood. A series of dirhodium(II,II) complexes, cis-[Rh 2 (p-R-Form) 2 (bncn) 2 ] 2+ (bncn = benzo[c]cinnoline; p-R-Form = N,N′-di-p-R-phenylformamidinate), where R = −OCH 3 (1), −CH 3 (2), −H (3), −F (4), −Cl (5), and −CF 3 (6), and their respective radical anions were prepared and their excited state properties were investigated. Complex 3 acted as a singlemolecule photocatalyst for H 2 production with red light. Substitution on the formamidinate ligands in 1−6 affected the energy of the Rh 2 (δ*)/Form(π,nb) highest occupied molecular orbital (HOMO), consistent with the metal/ligand-to-ligand charge transfer ( 1 ML-LCT) absorption maxima and the 3 ML-LCT excited state lifetime, ranging from 1.6 ns in 1 to 54 ns in 6 in CH 3 CN. The highest turnover number for photocatalytic H 2 evolution was observed for 3, and the lowest values were for 1 and 6. The radical anion, [Rh 2 ] − , formed during photocatalysis, was shown to absorb a photon and undergo a second reduction. The lifetimes of the doublet excited states of [3] − and [6] − were 0.49 and 0.24 ns, respectively. Calculations showed that the lowest energy excited state in [3] − was 2 ML-LCT, whereas that in [6] − was a bncn − → Rh 2 (σ*) ligand-to-metal charge transfer ( 2 LMCT) state. The 2 LMCT state stabilized across the series from [1] − to [6] − , pointing at its role in modulating the photophysical properties. This work highlights the importance of the reductive quenching of [Rh 2 ] − and the generation of the doubly reduced species to effectively catalyze hydrogen evolution.

Absorption↗

DOE OSTI2025

Coulomb excitation of 80 Sr and the limits of the 𝑁 ≈ 𝑍 ≈ 40 island of deformation

The region of 𝑁 ≈ 𝑍 ≈ 40 has long been associated with strongly deformed nuclear configurations. The presence of this strong deformation was recently confirmed through lifetime measurements in 𝑁 ≈ 𝑍 Sr and Zr nuclei. Theoretically, however, these nuclei present a challenge due to the vast valence space required to incorporate all necessary orbitals. Recent state-of-the-art predictions indicate a near axial prolate deformation for 𝑁 = 𝑍 and 𝑁 = 𝑍+2 nuclei between 𝑁 = 𝑍 = 36 and 𝑁 = 𝑍 = 40. In this work we investigate the shores of this island of deformation through a sub-barrier Coulomb excitation study of the 𝑁 = 𝑍+4 nucleus, 80 Sr . Extracting a spectroscopic quadrupole moment of 𝑄 𝑠 ⁡($2^+_1$)= $0.5^{+0.8}_{−0.9}$𝑒⁢b, we find that 80 Sr is inconsistent with significant axial prolate deformation with a significance of 1.5⁢𝜎. This result, albeit with a large uncertainty, indicates that the predicted region of strong prolate deformation around 𝑁 = 𝑍 = 40 is tightly constrained to the quartet of nuclei: 76,78 Sr and 78,80 Zr .

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗