Resonant Perfect Absorption Yielded by Zero-Area Pulses
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74 ATOMIC AND MOLECULAR PHYSICS↗
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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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Non-resonant picosecond three-wave mixing in the gas phase
We report on the experimental observation of non-resonant, second-order optical sum-frequency generation (SFG) in five different atomic and molecular gases. The measured signal is attributed to a SFG process by characterizing its intensity scaling and its polarization behavior. We show that the electric quadrupole mechanism cannot explain the observed trends and suggest a mechanism based on symmetry breaking along the incident beam path arising from laser-induced species ground state number density gradients. Our results demonstrate that the SFG is about four orders of magnitude stronger than the third-harmonic generation (THG) and independent from any externally applied electric fields. In conclusion, these features make this method suitable for gas number density measurements at the picosecond time scale in reactive flows and plasmas.
LaCombe, Grayson↗
Replication Data for: Deconstructing Chirality: Probing Local and Non-local Effects in Azobenzene Derivatives with X-ray Circular Dichroism
Resolving molecular chirality at the atomic scale remains a critical challenge in chemistry. Conventional Optical Circular Dichroism spectroscopy often overlooks subtle and localized structural features. Here, we computationally investigate site-specific X-ray Circular Dichroism (XCD) across a series of trans-azobenzene derivatives to deconstruct and interpret chiroptical signals at the atomic level. Our modeling reveals that XCD is capable of distinguishing dichroic contributions arising from both a local chiral center and global molecular twist, revealing their intricate interplay and potential for constructive or destructive interference. We show that sterically-induced global distortions can dominate the XCD signal in some cases, even suppressing the response from the chiral center itself. This insight suggests a new molecular design principle for tuning chiroptical activity, which we extend by proposing strategies to achieve unidirectional photoisomerization through steric gearing. Altogether, this work establishes a quantitative framework for engineering chiroptical responses, laying the foundation for the design of functional chiral systems utilizing principles of unidirectional molecular motor-like conformational dynamics.
Chemistry↗
Molecular beam epitaxy growth of IrO 2 using plasma-only oxidation
Growth of IrO 2 films via molecular beam epitaxy (MBE) using an oxygen plasma as the sole oxidant is demonstrated for the first time. We investigate the oxidizing conditions required for IrO 2 by characterizing the species present in the plasma using optical emission spectroscopy and comparing the thermodynamic equilibrium between Ir/IrO 2 under atomic and molecular oxygen. Across the pressure range accessible, monatomic oxygen was the primary reactive species present in the plasma. IrO 2 films were grown under varying Ir flux, oxygen pressure, and substrate temperature to understand growth thermodynamics and kinetics. Structural characterization assessed film phase and composition, crystallinity, strain, and surface morphology. The optimized films from this study validate plasma-only reactive growth by MBE as a successful method for growing IrO 2 .
36 MATERIALS SCIENCE↗
Diffusion quantum Monte Carlo approach to the polaritonic ground state
Making and using polaritonic states (i.e., hybrid electron-photon states) for chemical applications has recently become one of the most prominent and active fields that connects the communities of chemistry and quantum optics. Modeling of such polaritonic phenomena using ab initio approaches calls for new methodologies, leading to the reinvention of many commonly used electronic structure methods, such as Hartree-Fock, density functional, and coupled cluster theories. Here in this work, we explore the formally exact diffusion quantum Monte Carlo approach to obtain numerical solutions to the polaritonic ground state during the dissociation of the H 2 molecular system. Here, we examine various electron-nuclear-photon properties throughout the dissociation, such as changes to the minimum of the cavity Born-Oppenheimer surface, the localization of the electronic wave function, and the average mode occupation. Finally, we directly compare our results to that obtained with state-of-the-art, yet approximate, polaritonic coupled cluster approaches.
74 ATOMIC AND MOLECULAR PHYSICS↗
Gas in merging galaxies
We present observations of the neutral hydrogen, ionized hydrogen, and starlight of galaxies chosen from the 'Toomre Sequence' of merging galaxies. This sequence is meant to represent the progressive stages of the merger of two disk galaxies into a single elliptical-like remnant. The galaxies in this study span the full range of this sequence. The stars and atomic gas are very differently distributed, with the stars more widely distributed at early stages, and the gas much more widely distributed at later stages. Large quantities of neutral gas are sent to large radii (greater than or approximately equal to 100 h(exp -1) kpc), and still persist even after the central remnant has relaxed to an r(sup 1/4) light profile. There are a few times 10(exp 9) solar masses h(exp -2) of both molecular and atomic gas in each of these systems. Throughout the different stages, about half of the total gas mass lies within the galaxies' optical bodies. The fraction of this mass that is in neutral hydrogen drops rapidly in the later stage mergers, suggesting that atomic gas is processed into molecular gas, stars, and hot gas during the merger and resulting starburst. Star formation occurs at all stages of the interaction, both within the tails and in the central bodies. In the early stages, the H(alpha) shows many arcs and plumes. In the late stages, there are large H 2 regions in the tails which are associated with large quantities of neutral hydrogen. There is always a very good correlation between optical, H(alpha), and H1 peaks, with N(sub H1) greater than or approximately equal 3 x 10(exp 20) cm(exp -2) at the location of the H2 regions in the tails.
Hibbard, John E.↗
Photolithography of atomic layer resist
In a method of atomic precision advanced manufacturing (APAM), an atomic or molecular resist layer on a substrate surface is selectively depassivated by locally exciting the substrate surface with an optical beam effective to eject adsorbed atoms or molecules from the substrate surface. The substrate surface is further processed by exposing it to a precursor gas, decomposing the precursor gas to release a dopant, and incorporating the dopant into the substrate surface.
Katzenmeyer, Aaron Michael↗
Space Shuttle main engine OPAD: The search for a hardware enhanced plume
The process of applying spectroscopy to the Space Shuttle Main Engine (SSME) for plume diagnostics, as it exists today, originated at Marshall Space Flight Center in Huntsville, Alabama, and its implementation was assured largely through the efforts of Sverdrup AEDC, in Tullahoma, Tennessee. This team continues to lead and guide efforts in the plume diagnostics arena. The process, Optical Plume Anomaly Detection (OPAD), formed the basis for various activities in the development of ground-based systems as well as the development of in-flight plume spectroscopy. OPAD currently provides and will continue to provide valuable information relative to future systems definitions, instrumentation development, code validation, and data diagnostic processing. OPAD is based on the detection of anomalous atomic and molecular species in the SSME plume using two complete, stand-alone optical spectrometers. To-date OPAD has acquired data on 44 test firings of the SSME at the Technology Test Bed (TTB) at MSFC. The purpose of this paper will be to provide an introduction to the OPAD system by discussing the process of obtaining data as well as the methods of examining and interpreting the data. It will encompass such issues as selection of instrumentation correlation of data to nominal engine operation, investigation of SSME component erosion via OPAD spectral data, necessity and benefits of plume seeding, application of artificial intelligence (AI) techniques to data analysis, and the present status of efforts to quantify specie erosion utilizing standard plume and chemistry codes as well as radiative models currently under development.
Powers, W. T.↗
The ratio of molecular to atomic gas in infrared luminous galaxies
In infrared luminous galaxies the ratio of the CO(1 - 0) to H I integrated fluxes increases with the far-infrared excess, f(fir)/f(b). All infrared active galaxies with f(fir)/f(b) greater than 2 have molecular to atomic gas mass fractions greater than 0.5. Among the galaxies with the higher infrared excesses there are systems with strikingly small atomic mass fractions, where less than 15 percent of the total mass of interstellar gas is in atomic form. The optical morphology of luminous infrared galaxies indicates that the majority, if not all, of these objects are interacting systems. These observations suggest that the overall mass fraction of molecular to atomic gas, and the infrared luminosities per nucleon of interstellar gas are enhanced during galaxy-galaxy interactions.
Mirabel, I. F.↗
Demonstration of a MOT in a sub-millimeter membrane hole
Abstract We demonstrate the generation of a cold-atom ensemble within a sub-millimeter diameter hole in a transparent membrane, a so-called “membrane MOT”. With a sub-Doppler cooling process, the atoms trapped by the membrane MOT are cooled down to 10 $$\upmu$$ μ K. The atom number inside the unbridged/bridged membrane hole is about $$10^4$$ 10 4 to $$10^5$$ 10 5 , and the $$1/e^2$$ 1 / e 2 -diameter of the MOT cloud is about 180 $$\upmu$$ μ m for a 400 $$\upmu$$ μ m-diameter membrane hole. Such a membrane device can, in principle, efficiently load cold atoms into the evanescent-field optical trap generated by the suspended membrane waveguide for strong atom-light interaction and provide the capability of sufficient heat dissipation at the waveguide. This represents a key step toward the photonic atom trap integrated platform (ATIP).
74 ATOMIC AND MOLECULAR PHYSICS↗
Development and Application of Novel Diagnostics for Arc-Jet Characterization
This NASA-Ames University Consortium Project has focused on the design and demonstration of optical absorption sensors using tunable diode laser to target atomic copper impurities from electrode erosion in thc arc-heater metastable electronic excited states of molecular nitrogen, atomic argon, aid atomic oxygen in the arcjet plume. Accomplishments during this project include: 1. Design, construction, and assembly of optical access to the arc-heater gas flow. 2. Design of diode laser sensor for copper impurities in the arc-heater flow. 3 . Diode laser sensor design and test in laboratory plasmas for metastable Ar(3P), O(5S), N(4P), and N2(A). 4. Diode laser sensor demonstration measurements in the test cell to monitor species in the arc-jet plume.
Hanson, R. K.↗
LDRD FY25 Program Overview
As Lawrence Livermore National Laboratory’s (LLNL’s) Laboratory Directed Research and Development (LDRD) program enters its fifth decade of leading-edge research and development, its impact and importance have never been stronger. The program continues to advance strategic investments in pioneering science, technology, and engineering, ensuring LLNL will be ready to deliver on our mission as it evolves over the coming decades. Investing in LDRD research, and the people who perform this critical work, gives LLNL the ability to sustain our role as a leader in the Department of Energy and National Nuclear Security Administration enterprise. The LDRD program enables high-risk, high-payoff research that anticipates emerging threats and future mission needs. By nurturing the ingenuity of the Lab’s greatest asset, its people, LDRD funding advances not only our research but also grows and nurtures our workforce: engaging future innovators with student mentoring, challenging postdoctoral researchers to apply their skills to support national security, and strengthening the leadership skills of early career staff. This annual report documents how LDRD investments advance LLNL’s science, technology, and engineering across our mission space. To assess LDRD’s impact we track both short and long-term metrics such as peer-reviewed publications, number of students, or professional fellows. In addition to reviewing these metrics, I encourage you to delve deeper into the breadth of science and technology that illustrate the strategic value of this research portfolio. For instance, a recent exploratory research project used advanced manufacturing to construct miniaturized three-dimensional ion traps for a quantum computer with reduced quantum error rates to enable applications that address national security missions and support basic science. Another project has delved into studying detonation by examining deflagration to enhance the safety and security of the nuclear weapons stockpile. LDRD researchers are also deploying AI agents on two of the world’s most powerful supercomputers to automate and accelerate inertial confinement fusion experiments. Other teams are delivering more accurate optical constants to enable improved validation for aluminum to advance atomic and molecular physics models. LDRD-driven discoveries of how metals deform under extreme conditions strengthen our ability to model and design materials for demanding national security environments. National security challenges are increasingly complex and continuously evolving. LDRD focuses our most innovative science and technology on these challenges, ensuring the Laboratory is developing creative, forward-leaning solutions for our nation and the world. The following pages feature highlights of published scientific advances, patents, and honors that stem from LDRD investments. As you read this report, I hope you will understand how these investments position the Laboratory, and our partners, to meet the demands of the decades ahead.
36 MATERIALS SCIENCE↗
Ultrafast electron dynamics in platinum and gold thin films driven by optical and terahertz fields
Here, we investigate the ultrafast electron dynamics triggered by terahertz and optical pulses in thin platinum and gold films by probing their transient optical reflectivity. The response of the platinum film to an intense terahertz pulse is similar to the optically induced one and can be described by a two-temperature model with a 20% larger electron–phonon coupling for the terahertz-driven dynamics compared to the optically induced one, ascribed to an additional nonthermal electron–phonon coupling contribution. Surprisingly, gold films exhibit a much smaller terahertz pulse-induced reflectivity change and with a sign opposite to the optical case. Additionally we explain this remarkable observation with field emission of electrons due to Fowler–Nordheim tunneling, enabled in samples with thicknesses below the structural percolation threshold, where nanostructuring promotes near-field enhancement. Our results provide a fundamental insight into the ultrafast processes relevant to modern electro- and magneto-optical applications.
74 ATOMIC AND MOLECULAR PHYSICS↗
Improved optical standing-wave beam splitters for dilute Bose–Einstein condensates
Bose–Einstein condensate (BEC)-based atom interferometry exploits low temperatures and long coherence lengths to facilitate high-precision measurements. Progress in atom interferometry promises improvements in navigational devices like gyroscopes and accelerometers, as well as applications in fundamental physics such as accurate determination of physical constants. Previous work demonstrates that beam splitters and mirrors for coherent manipulation of dilute BEC momentum in atom interferometers can be implemented with sequences of non-resonant standing-wave light pulses. While previous work focuses on the optimization of the optical pulses’ amplitude and duration to produce high-order momentum states with high fidelity, we explore how varying the shape of the optical pulses affects optimal beam-splitter performance, as well as the effect of pulse shape on the sensitivity of optimized parameters in achieving high fidelity in high-momentum states. Here, in simulations of two-pulse beam splitters utilizing optimized square, triangle, and sinc-squared pulse shapes applied to dilute BECs, we, in some cases, reduce parameter sensitivity by an order of magnitude while maintaining fidelity.
74 ATOMIC AND MOLECULAR PHYSICS↗
Time-Evolving Chirality Loss in Molecular Photodissociation Monitored by X-ray Circular Dichroism Spectroscopy
In this work, the ultrafast photoinduced chirality loss of 2-iodobutane is studied theoretically by time- and frequency-resolved X-ray circular dichroism (TRXCD) spectroscopy. Following an optical excitation, the iodine atom dissociates from the chiral center, which we capture by quantum non-adiabatic molecular dynamics simulations. At variable time delays after the pump, the resonant X-ray pulse selectively probes the iodine and carbon atom involved in the chiral dissociation through a selected core-to-valence transition. The TRXCD signal at the iodine L 1 edge accurately captures the timing of C–I photodissociation and thereby chirality loss, c.a 70 fs. The strong electric dipole–electric quadrupole (ED–EQ) response makes this signal particularly sensitive to vibronic coherence at the high X-ray regime. At the carbon K-edges, the signals monitor the molecular chirality of the 2-butyl radical photoproduct and the spin state of the iodine atom. The ED–EQ response is masked under the strong electric dipole-magnetic dipole response, making this signal intuitive for the electronic population. The evolution of the core electronic states and its chiral sensitivity is discussed. Overall, the element-specific TRXCD signal provides a detailed picture of molecular dynamics and offers a unique sensitive window into the time-dependent chirality of molecules.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Control Design for Inhomogeneous-Broadening Compensation in Single-Photon Transducers
We report a transducer of single photons between microwave and optical frequencies can be used to realize quantum communication over optical fiber links between distant superconducting quantum computers. A promising scalable approach to constructing such a transducer is to use ensembles of quantum emitters interacting simultaneously with electromagnetic fields at optical and microwave frequencies. However, inhomogeneous broadening in the transition frequencies of the emitters can be detrimental to this collective action. In this paper, we utilize a gradient-based optimization strategy to design the temporal shape of the laser field driving the transduction system to mitigate the effects of inhomogeneous broadening. We study the improvement of transduction efficiencies as a function of inhomogeneous broadening in different single-emitter cooperativity regimes and correlate it with a restoration of super-radiance effects in the emitter ensembles. Furthermore, to assess the optimality of our pulse designs, we provide certifiable bounds on the design problem and compare them to the achieved performance.
74 ATOMIC AND MOLECULAR PHYSICS↗
Multipolariton control in attosecond transient absorption of autoionizing states
Tunable attosecond transient absorption spectroscopy is an ideal tool for studying and manipulating autoionization dynamics in the continuum. We investigate near-resonant two-photon couplings between the bright 3s –1 4p and dark 3s –1 4f autoionizing states of argon that lead to Autler-Townes-like interactions, forming entangled light-matter states or polaritons. We observe that one-photon couplings with intermediate dark states play an important role in this interaction, leading to the formation of multiple polaritonic branches whose energies exhibit avoided crossings as a function of the dressing-laser frequency. Our experimental measurements and theoretical essential-state simulations show good agreement and reveal how the delay, frequency, and intensity of the dressing pulse govern the properties of autoionizing polariton multiplets. Furthermore, these results demonstrate new pathways for quantum control of autoionizing states with optical fields.
74 ATOMIC AND MOLECULAR PHYSICS↗
Photochemistry sample sticks for inelastic neutron scattering
Every material experiences atomic and molecular motions that are generally termed vibrations in gases and liquids or phonons in solid state materials. Optical spectroscopy techniques, such as Raman, infrared absorption spectroscopy, or inelastic neutron scattering (INS), can be used to measure the vibrational/phonon spectrum of ground state materials properties. A variety of optical pump probe spectroscopies enable the measurement of excited states or elucidate photochemical reaction pathways and kinetics. So far, it has not been possible to study photoactive materials or processes in situ using INS due to the mismatch between neutron and photon penetration depths, differences between the flux density of photons and neutrons, cryogenic temperatures for INS measurements, vacuum conditions, and a lack of optical access to the sample space. These experimental hurdles have resulted in very limited photochemistry studies using INS. Here we report on the design of two different photochemistry sample sticks that overcome these experimental hurdles to enable in situ photochemical studies using INS, specifically at the VISION instrument at Oak Ridge National Laboratory. We demonstrate the use of these new measurement capabilities through (1) the in situ photodimerization of anthracene and (2) the in situ photopolymerization of a 405 nm photoresin using 405 nm excitation as simple test cases. Furthermore, these new measurement apparatus broaden the science enabled by INS to include photoactive materials, optically excited states, and photoinitiated reactions.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗