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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 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Nonresonant Raman Control of Ferroelectric Polarization

Important advances is recently made in the search for materials with complex multi-phase landscapes that host photoinduced metastable collective states with exotic functionalities. In almost all cases so far, the desired phases are accessed by exploiting light–matter interactions via the imaginary part of the dielectric function through above-bandgap or resonant mode excitation. Nonresonant Raman excitation of coherent modes is experimentally observed and proposed for dynamic material control, but the resulting atomic excursion is limited to perturbative levels. Here, in this study, this challenge is overcome by employing nonresonant ultrashort pulses with low photon energies well below the bandgap. Using mid-infrared pulses, ferroelectric reversal is induced in lithium niobate, and the large-amplitude mode displacements are characterized through femtosecond stimulated Raman scattering and second harmonic generation. This approach, validated by first-principle calculations, defines a novel method for synthesizing hidden phases with unique functional properties and manipulating complex energy landscapes at reduced energy consumption and ultrafast speeds.

Shi, Jiaojian [Stanford Univ., CA (United States);↗
DOE OSTI2025

Revealing Parallel Inter‐ and Intra‐Ligand Charge Transfer Dynamics in [Ru(L) 2 (dppz)] 2+ Molecular Lightswitch with N K‐Edge X‐Ray Absorption Spectroscopy

In photoactive metal complexes the localization of photoexcited charges dictates the site of chemical reactivity, but few studies measure the charge redistribution in these systems with spatial precision. Herein, we track the inter- and intra-ligand charge transfer processes that underpin light-driven charge separation in the well-studied “molecular lightswitch” [Ru(bpy) 2 dppz] 2+ (aqueous [Ruthenium II (2,2′-bipyridine)2(dipyrido[3,2-a:2′,3′-c]phenazine)] 2+ [Cl − ] 2 ) by probing the electronic structure of ligand nitrogen atoms in real-time using ultrafast X-ray absorption spectroscopy and first principles calculations. We confirm the localization of excited electron density on the phenazine N atoms of dppz and we newly identify two parallel electron transfer pathways to populate this state. Sub-70 fs electron transfer to the phenazine portion of dppz is observed and attributed to intra-ligand electron transfer following Ru-to-dppz metal-to-ligand charge transfer (MLCT) excitation. This fast charge transfer was not reported in prior ultrafast studies. The slower (ca. 2 ps) charge transfer reported extensively in time-resolved optical absorption and emission studies is reassigned here to inter-ligand electron “hopping” between nearly isoenergetic ligand moieties following Ru-to-bpy MLCT excitation. In conclusion, the results demonstrate much faster charge separation than previously identified in this well-studied system, highlighting how extended azaacene ligand motifs promote the competitive charge transfer processes needed to drive light-driven electron transfer chemistry.

Donor-acceptor systems↗
DOE OSTI2026

Strong long-wavelength electron-phonon coupling in Ta 2 ⁢Ni⁡(Se,S) 5

The search for intrinsic excitonic insulators (EI) has long been confounded by coexisting electron–phonon coupling in bulk materials. Although the ground state of an EI may be difficult to differentiate from density-wave orders or other structural instabilities, excited states offer distinctive signatures. One way to provide clarity is to directly inspect the phonon spectral function for long wavelength broadening caused by phonon interaction with the high velocity EI phason. Here, in this study, we report that the quasi-one-dimensional (quasi-1D) EI candidate Ta 2 NiSe 5 shows extremely anisotropic phonon broadening and softening in the semimetallic normal state. In contrast, such behavior is completely absent in the broken symmetry state of Ta 2 NiSe 5 and in the isostructural Ta 2 NiS 5 , where the latter has a fully gapped normal state. By contrasting the expected phonon lifetimes in the BCS and BEC limits of a putative EI, our results suggest that the phase transition in Ta 2 Ni(Se,S) 5 family is closely related to strong interband electron–phonon coupling. We experimentally determine the dimensionless coupling $\frac{g}{ω_0}$ ∼ 10, revealing Ta 2 Ni(Se,S) 5 as a rare “ultrastrong coupling” material.

Kang, Zhibo [Yale University, New Haven, CT (Unite↗
DOE OSTI2026

A tutorial on high-order harmonic generation in atoms, molecules, and condensed matter

This tutorial introduces strong-field-driven high-order harmonics, their experimental generation and characterization techniques, and their main applications including attosecond pulse generation and ultrafast spectroscopy of the target material. We begin from the use of atomic targets, where the first high-order harmonic generation (HHG) experiments were realized in the late 1980s. Then, we briefly discuss the basics of the microscopic generation mechanism and how various steps of the mechanism were exploited in applications such as generating isolated attosecond pulses and probing molecular orbitals. We introduce and describe the standard experimental approaches for condensed phase HHG, where we discuss unique technical challenges of the use of solid-state materials, such as the mitigation of plasma formation and laser damage. We cover the fundamentals of high-harmonic spectroscopy in condensed matter systems, such as wide bandgap dielectrics, semiconductors, liquid media, and 2D-crystals. We provide some examples of rapidly emerging spectroscopic capabilities, such as for probing crystal symmetries, Berry phases, and associated non-trivial topological properties of the source material. Finally, we provide an overview of the research field, including some of the challenges, opportunities, and open questions.

Attosecond pulses↗
DOE OSTI2025

Wavelength-dependent photodissociation of iodomethylbutane

Ultrashort XUV pulses of the Free-Electron-LASer in Hamburg (FLASH) were used to investigate laser-induced fragmentation patterns of the prototypical chiral molecule 1-iodo-2-methyl-butane (C 5 H 11 I) in a pump-probe scheme. Ion velocity-map images and mass spectra of optical-laser-induced fragmentation were obtained for subsequent FEL exposure with photon energies of 63 eV and 75 eV. These energies specifically address the iodine 4d edge of neutral and singly charged iodine, respectively. The presented ion spectra for two optical pump-laser wavelengths, i.e., 800 nm and 267 nm, reveal substantially different cationic fragment yields in dependence on the wavelength and intensity. For the case of 800-nm-initiated fragmentation, the molecule dissociates notably slower than for the 267 nm pump. The results underscore the importance of considering optical-laser wavelength and intensity in the dissociation dynamics of this prototypical chiral molecule that is a promising candidate for future studies of its asymmetric nature.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2026

Ultrafast population and structural dynamics of a Ni-bipyridine photoredox catalyst reveal a significant deactivation pathway

The ultrafast excited state pathways and dynamics of NiII-bipyridine complexes influence the yield of photochemical processes involved in their catalytic cross-coupling reactions. Here we present ultrafast Ni K x-ray emission spectroscopy (XES) and x-ray solution scattering (XSS) of a NiII-bipyridine aryl halide complex, [Ni(t-Bubpy)(o-tol)Br], to quantify the excited state population dynamics and structural changes of the pre-catalyst. Due to the local spin-sensitivity of XES, the population dynamics of metal-to-ligand charge transfer (MLCT) and metal-centered (MC) excited states is established. A rapid ground state recovery pathway is newly identified, representing a significant deactivation pathway during photocatalysis. Furthermore, the pseudotetrahedral structure of the long-lived MC excited state is unambiguously identified and refined by XSS. The results advance our understanding of the ultrafast relaxation mechanisms that impact the photocatalytic mechanism and yield for NiII-bipyridine aryl halide cross-coupling catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Control of intense light with avalanche-ionization plasma gratings

High-peak-power lasers are fundamental to high-field science: increased laser intensity has enabled laboratory astrophysics, relativistic plasma physics, and compact laser-based particle accelerators. However, the meter-scale optics required for multi-petawatt lasers to avoid light-induced damage make further increases in power challenging. Plasma tolerates orders-of-magnitude higher light flux than glass, but previous efforts to miniaturize lasers by constructing plasma analogs for conventional optics were limited by low efficiency and poor optical quality. We describe a new approach to plasma optics based on avalanche ionization of atomic clusters that produces plasma volume transmission gratings with dramatically increased diffraction efficiency. We measure an average efficiency of up to 36% and a single-shot efficiency of up to 60%, which is comparable to key components of high-power laser beamlines, while maintaining high spatial quality and focusability. These results suggest that plasma diffraction gratings may be a viable component of future lasers with peak power beyond 10 PW.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2025

Polaritonic quantum matter

Polaritons are quantum mechanical superpositions of photon states with elementary excitations in molecules and solids. The light–matter admixture causes a characteristic frequency-momentum dispersion shared by all polaritons irrespective of the microscopic nature of material excitations that could entail charge, spin, lattice or orbital effects. Polaritons retain the strong nonlinearities of their matter component and simultaneously inherit ray-like propagation of light. Polaritons prompt new properties, enable new opportunities for spectroscopy/imaging, empower quantum simulations and give rise to new forms of synthetic quantum matter. Here, we review the emergent effects rooted in polaritonic quasiparticles in a wide variety of their physical implementations. We present a broad portfolio of the physical platforms and phenomena of what we term polaritonic quantum matter. We discuss the unifying aspects of polaritons across different platforms and physical implementations and focus on recent developments in: polaritonic imaging, cavity electrodynamics and cavity materials engineering, topology and nonlinearities, as well as quantum polaritonics.

light–matter interaction↗
DOE OSTI2025

Direct Observation of the ππ* to nπ* Transition in 2-Thiouracil via Time-Resolved NEXAFS Spectroscopy

The photophysics of nucleobases has been the subject of both theoretical and experimental studies over the past decades due to the challenges posed by resolving the steps of their radiationless relaxation dynamics, which cannot be described in the framework of the Born–Oppenheimer approximation (BOA). In this context, the ultrafast dynamics of 2-thiouracil has been investigated with a time-resolved NEXAFS study at the Free Electron Laser FLASH. Near Edge X-ray Absorption Fine Structure spectroscopy (NEXAFS) can be used to observe electronic transitions in ultrafast molecular relaxation. We performed time-resolved UV-pump/X-ray probe absorption measurements at the sulfur 2s (L1) and 2p (L2/3) edges. We are able to identify absorption features corresponding to the S2 (ππ*) and S1 (nπ*) electronic states. We observe a delay of 102 ± 11 fs in the population of the nπ* state with respect to the initial optical excitation and interpret the delay as the time scale for the S2 → S1 internal conversion. We furthermore identify oscillations in the absorption signal that match a similar observation in our previous X-ray photoelectron spectroscopy study on the same molecule.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Observation of early events in the photoactivation of Myxobacterial phytochrome using time-resolved serial femtosecond crystallography

Myxobacteria are non-photosynthetic, soil-dwelling bacteria distinguished by a multicellular stage in their life cycle known as fruiting bodies that are stimulated by light. Myxobacterial phytochromes are candidates for the perception of red-light. The mechanism how light is perceived and converted to a physiological response is unknown. Here, time-resolved serial femtosecond crystallographic (TR-SFX) experiments were conducted on microcrystals of the photosensory core module of the Stigmatella aurantiaca bacteriophytochrome 2 (SaBphP2). Initial events of the Z to E isomerization reaction of the covalently bound, open-chain tetrapyrrole biliverdin (BV) chromophore were determined. At 3 ps after light activation, the BV ring-D assumes a configuration needed for the isomerization. At 100 ps, a mixture of BV in the Z or E configuration is observed in subunit A, while in the other subunit the chromophore remains in the Z configuration. In conjunction with prior results, these structures reveal the molecular mechanism of phytochrome activation in the photomorphogenesis of the myxobacteria and provide the molecular foundation for physiological responses to red light in other bacteria.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

In-situ probing of the Fischer-Tropsch reaction on Co single crystal surfaces up to 1 bar

The surface chemistry of the Fischer-Tropsch catalytic reaction over Co has still several unknows. Here, we report an in-situ X-ray photoelectron spectroscopy study of Co$(0001)$ and Co$(10\bar{1}4)$, and in-situ high energy surface X-ray diffraction of Co$(0001)$ during the Fischer-Tropsch reaction at 0.15 bar - 1 bar and 406 K - 548 K in a H 2 /CO gas mixture. We find that these Co surfaces remain metallic under all conditions and that the coverage of chemisorbed species ranges from 0.4–1.7 monolayers depending on pressure and temperature. The adsorbates include CO on-top, C/-C x H y and various longer hydrocarbon molecules, indicating a rate-limiting direct CO dissociation pathway and that only hydrocarbon species participate in the chain growth. The accumulation of hydrocarbon species points to the termination step being rate-limiting also. Furthermore, we demonstrate that the intermediate surface species are highly dynamic, appearing and disappearing with time delays after rapid changes in the reactants’ composition.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Discovery Science and Inertial Fusion Energy Research at the Jupiter Laser Facility (Research Performance Progress Report)

The goal of this project is to provide operational support to run the Jupiter Laser Facility within the LaserNetUS network to achieve the following four objectives: • Develop new science, techniques, and platforms for discovery science and IFE research, in partnership with academia, other LaserNetUS nodes, and the greater community. • Advance the development of secondary sources of photons and particles for applications relevant to discovery science and IFE; • Serve as a testbed for new laser, optical, target, and diagnostic capabilities that will advance IFE; • Attract, train, and retain talent in high-energy-density and laser science that will be essential in furthering development of IFE, and help build new collaborations between national laboratory and academic researchers. We have accomplished our four objectives by: • Providing access to the three JLF platforms (Titan, Janus, and COMET) to LaserNetUS users after their proposals have been independently reviewed and ranked by the LaserNetUS PRP; • Providing expertise and technical capabilities to support focused science research thrusts at the facility; • Promoting and maintaining technical relationships and collaborations with other members of the LaserNetUS community to nurture and grow the discovery science and IFE workforce— especially students and early career scientists—on LaserNetUS facilities. • Augmenting JLF with specific improvements while coordinating efforts with LLNL organizations and collaborators to provide users with optimal laser, target, and diagnostic resources to help them maximize technical impact.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2025

Anomalously slow hot carrier cooling and insulator-to-metal transition in a photo-doped Mott insulator

Photo-doped Mott insulators can exhibit novel photocarrier transport and relaxation dynamics and non-equilibrium phases. However, time-resolved real-space imaging of these processes are still lacking. Here, we use scanning ultrafast electron microscopy (SUEM) to directly visualize the spatial-temporal evolution of photoexcited species in a spin-orbit assisted Mott insulator α-RuCl 3 . At low optical fluences, we observe extremely long hot photocarrier transport time over one nanosecond, almost an order of magnitude longer than any known values in conventional semiconductors. At higher optical fluences, we observe nonlinear features suggesting a photo-induced insulator-to-metal transition, which is unusual in a large-gap Mott insulator. Our results demonstrate the rich physics in a photo-doped Mott insulator that can be extracted from spatial-temporal imaging and showcase the capability of SUEM to sensitively probe photoexcitations in strongly correlated electron systems.

42 ENGINEERING↗
DOE OSTI2026

Selective CO 2 Reduction by Bis(bipyridine)cobalt(II) Catalysts: The Role of Pendant Pyridine as a Proton Acceptor

Electrochemical CO 2 reduction reaction (CO 2 RR) catalyzed by molecular earth-abundant metal catalysts is a promising strategy to convert CO 2 into value-added products. One recent trend in this field has been focusing on the rational design of catalysts by incorporating redox-active ligands and modifying the secondary coordination sphere (SCS) to achieve efficient and selective CO 2 RR. Herein, we report a series of Co bis­(bipyridine) catalysts featuring various dangling groups, such as pyridine, tertiary amine, or butyl, in the secondary coordination sphere (Co-PyMe, Co-Py, Co-PrN, and Co-Bu). Efficient, selective electrocatalytic CO 2 RR was achieved by the complexes after the generation of triply reduced intermediate consisting of a Co I center and a dianionic ligand, producing CO as the major product and trace amount of H 2 . Strong correlations with the identity of dangling groups and turnover frequency (TOF) have been observed, in which Co-PyMe displayed the highest TOF (1086 s –1 in MeCN/H 2 O). Mechanistic studies indicated that the acceleration of CO 2 RR with pyridine-functionalized catalysts were derived from the protonation of pyridine dangling groups which participated as weak acids in the H-bonding network with exogenous proton sources, stabilizing CO 2 -bound intermediates and facilitating proton transfer. In addition, precatalytic CO 2 binding and activation at the third reduction (−2.1 V) was revealed by CV and SEC-IR studies. The resultant doubly reduced CO-bound species acted as a trapping state which inhibited CO 2 RR electrocatalysis. Regeneration of active species was accessed via reductive dissociation of CO at a more negative potential. In conclusion, this study highlights the combined effects of redox-active ligands and pyridine/pyridinium as SCS groups on CO 2 RR catalysis and provides design principles for future development of CO 2 RR catalysts utilizing pyridine/pyridiniums as SCS functional groups to fine-tune the catalytic activity.

CO2 reduction↗
DOE OSTI2025

Photolytic activation of Ni (II) X 2 L explains how Ni-mediated cross coupling begins

Nickel photocatalysis has recently become vital to organic synthesis, but how the Ni (II) X 2 L pre-catalyst (X = Cl, Br; L = bidentate ligand) becomes activated to Ni (I) XL has remained puzzling and is typically addressed on a case-by-case basis. Here, we reveal a general mechanism where light induces photolysis of the Ni (II) -X bond, either via direct excitation or triplet energy transfer. Photolysis produces Ni (I) XL and a halogen radical, X*. Subsequent hydrogen atom abstraction, often from the solvent, produces a C(sp 3 ) radical, R*, that recombines with Ni (I) to form organonickel(II) complexes, Ni (II) XRL. Rather than acting as a loss pathway, Ni (II) XRL behaves as a light-activated reservoir of Ni (I) via photolysis of the Ni (II) -C bond. These results explain the role of the solvent in protecting the catalyst from off-cycle dimerization, demonstrate that two photons are often required to drive the reaction, and show how tuning the ligand can control the concentration of active Ni (I) species.

08 HYDROGEN↗
DOE OSTI2026

Over 8 hours of continuous operation of a free-electron laser driven by a laser-plasma accelerator

Since the emergence of laser-plasma accelerators (LPAs), substantial work has been dedicated to using LPAs to drive free-electron lasers (FELs) for a broad range of applications. Despite recent breakthroughs, which have proven the fundamental feasibility of operating FELs with an LPA source, stable FEL operation over multiple hours without operator input had yet to be achieved. In this work, we report significant improvements to the stability of a hundred terawatt laser system, resulting in successful demonstration of reliable, long-term operation of an LPA-driven FEL in the self-amplified spontaneous emission (SASE) regime at 420 nm. The LPA source delivered 100 MeV electron beams at 1 Hz with high stability over more than 10 h, enabling over 8 h of continuous FEL operation without operator input. The acquired data were subsequently used to investigate correlations between the measured undulator radiation and parameters of the drive laser, plasma source, and electron beam. The revealed connections between LPA and FEL performance gave important additional insights into ways to further improve and stabilize the system, thus demonstrating the capability of our setup to serve as a powerful platform for future studies of LPA-driven FEL operation. The one-of-a-kind integration of multiple stabilization concepts onto the LPA facility discussed in this manuscript yielded significant accelerator and light source improvements (with residual correlations suggesting even more is possible), which will positively impact LPA applications at large.

Kohrell, Finn [Lawrence Berkeley National Laborato↗
DOE OSTI2023

Broadband Photoconductive Sampling in Gallium Phosphide

Abstract Direct measurements of the electric field of light enable new observations of light–matter interactions. In the near‐infrared and visible spectral ranges, this typically relies on techniques that exploit nonlinearities in gases or solids, which limits their sensitivity. Here, a method for the detection of broadband near‐infrared fields spanning more than one octave from 110 to 220 THz based on linear absorption in a semiconductor is demonstrated. This technique, which avoids complex vacuum setups and works under ambient conditions, employs linear photoconductive sampling (LPS) in gallium phosphide. Simulations reveal that the response function of LPS is concerned with the intensity envelope of the gate field, in contrast to electro‐optic sampling, relaxing the stringent temporal requirements on the gate pulse.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Laser Powder Bed Fusion Additive Manufacturing In-Process Monitoring and Optimization Using Thermionic Emission Detection

In this project, the emission of electrons during laser powder bed fusion additive manufacturing was identified and investigated to resolve the underlying dynamics driven by laser-material interactions. Laser powder bed fusion involves the selective laser melting of metal powder particles layer by layer which fuse together forming a larger 3D structure. Laser-based additive manufacturing approaches such as laser powder bed fusion hold the potential to revolutionize manufacturing of complex metal components in the aerospace, medical, and automotive industries. However, the difficulty in producing defect-free components by metal 3D printing is a major hurdle for widespread commercial adoption. This project resolved important dynamics in laser powder bed fusion including the identification of plasma formation mechanisms, transitions between laser-induced melting modes and stochastic precursors to defect formation. These findings were realized through implementation of electronic sensing diagnostics into an existing testbed system and harnessing capabilities developed for the time dependent analysis of laser powder bed fusion datasets. Importantly, the results advance our understanding of laser-material interactions and reveal that detection of thermionic emission can also resolve information critical to optimization of the laser powder bed fusion fabrication process. The findings are critical for advancing our fundamental understanding of the laser powder bed fusion process and can help assure the requisite fidelity of fabricated components.

36 MATERIALS SCIENCE↗