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At least 127 records · Page 7

Non-Equilibrium Plasma Interactions with Biomaterials, Biological Solutions and Tissues

Cold atmospheric pressure plasma discharges offer an abundant source of reactive oxygen and nitrogen species (RONS) at room temperature enabling unique interactions with biomaterials, biological solutions and tissues. These interactions particularly with living matter are presently an important intellectual frontier in plasma science with promising potential applications ranging from human health care to advanced biomaterial processing. Exciting case studies have been reported that illustrate the huge potential of cold atmospheric plasma technology in wound healing and cancer treatment. The interaction of plasma with conducting and dielectric biomaterials such as tissue strongly influences the plasma properties. In turn this changes the impact of the plasma on the biomaterial. Particularly in the case of living matter, liquid based solutions are ubiquitous which complicates interfacial processes. The lack of insight into the underlying mechanisms of the interaction of plasma with wounds and tumors is currently a bottleneck for the further development of the technology and gives rise to many interesting scientific questions. This project was focused on plasma properties and kinetics during plasma-biomaterial interactions. Both DC pulsed and RF driven atmospheric pressure plasma jets, extensively used by the plasma community were studied. The bio-interfaces included hydrogel as a tissue model, (saline) solutions, bacteria and virus. Plasma diagnostics used include Thomson scattering, Rayleigh scattering, Raman scattering, (two-photon absorption) laser induced fluorescence, optical emission spectroscopy, absorption spectroscopy, molecular beam mass spectrometry and fast imaging allowing to determine electron densities and temperatures, ionic species, reactive species including radicals, gas temperatures, gas composition, electric fields and solution components transferred to the gas phase.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Development of Polycrystalline Photoelectrodes with Optimum Compositions and Morphologies for Solar Fuel Production via Electrochemical Synthesis (Final Technical Report)

Photoelectrochemical cells (PECs) can utilize solar energy for water splitting to produce H 2 as a clean fuel. The most critical components of a water-splitting PEC are semiconductor electrodes (photoelectrodes) that absorb solar energy to generate photoexcited charge carriers and transport them to the electrode/electrolyte interface for water reduction and oxidation reactions. While efficient PEC hydrogen production has been successfully demonstrated on the laboratory scale, the commercial viability of PECs depends critically on the cost of H 2 produced by the PECs, which is affected by the cost of PEC construction. Therefore, identifying promising inexpensive semiconductor electrodes is important. The goal of this project was to bring an advancement in the synthesis and understanding of inexpensive polycrystalline photoelectrodes based on oxides. Oxide-based semiconductors are inexpensive, easy to fabricate, and relatively more stable in aqueous media compared to other types of semiconductors. This project developed new electrodeposition methods to produce a variety of oxide-based semiconductor electrodes with precisely controlled compositions and morphologies to enhance photon absorption, electron-hole separation, and the use of electrons and holes for desired chemical reactions. The resulting high-quality photoelectrodes were investigated to establish the structure-composition-morphology-photoelectrochemical property relationships to identify the advantages and limitations of each oxide semiconductor system.

14 SOLAR ENERGY↗

Interactions of a Microdischarge with a Premixed Flame (Final Technical Report)

In this project we introduced an experimental platform that facilitates the study of the two-way interaction of plasma and flame, and the exploration of the impact of the spatial location of the discharge on its kinetics, in a controlled environment. The experimental platform is a mesoscale CH4/air premixed flame burner that also acts as a dielectric barrier discharge (DBD) operated by nanosecond pulsed voltage. A unique feature of this setup is that the DBD utilizes transparent electrodes, made of Indium Tin Oxide (ITO), to unlock optical access along the line-of-sight parallel to the dominant electric field. This platform is suitable to study both the forward problem (impact of plasma-on-flame), which manifests itself as a modified flame speed as well as flame wrinkling; and the backward problem (impact of flame-on-plasma), which includes plasma regime transitions, between microdischarges and uniform modes, driven by the flame passage. Prior work at MIT has focused on electrical measurements and direct imaging studies of the plasma-flame interaction through the ITO electrode. This project, which was awarded experimental runtime at the Low-temperature Plasma Research Facility (PRF) at Sandia National Laboratories, quantifies the flame-plasma interaction through temporally resolved measurement of key radicals (oxygen atom, O) produced by the nanosecond repetitively pused discharge (NRPD) in an individual microdischarge, using two-photon absorption laser-induced fluorescence (TALIF).

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Intermediate Bandgap (IB) Cu 3 VS x Se 4−x Nanocrystals as a New Class of Light Absorbing Semiconductors

A new family of highly uniform, cubic-shaped Cu 3 VS x Se 4−x (CVSSe; 0 ≤ x ≤ 4) nanocrystals based on earth-abundant materials with intermediate bandgaps (IB) in the visible range is reported, synthesized via a hot-injection method. The IB transitions and optical band gap of the novel CVSSe nanocrystals are investigated using ultraviolet-visible spectroscopy, revealing tunable band gaps that span the visible and near-infrared regimes. The composition-dependent relationships among the crystal phase, optical band gap, and photoluminescence properties of the novel IB semiconductors with progressive substitution of Se by S are examined in detail. High-resolution transmission electron microscopy and scanning electron microscopy characterization confirm the high crystallinity and uniform size (~19.7 nm × 17.2 nm for Cu 3 VS 4 ) of the cubic-shaped nanocrystals. Density functional theory (DFT) calculations based on virtual crystal approximation support the experimental findings, showing good agreement in lattice parameters and band gaps across the CVSSe series and lending confidence that the targeted phases and compositions have been successfully realized. A current conversion efficiency, i.e., incident photon-to-current efficiency, of 14.7% was achieved with the p-type IB semiconductor Cu 3 VS 4 . These novel p-type IB semiconductor nanocrystals hold promise for enabling thin film solar cells with efficiencies beyond the Shockley–Queisser limit by allowing sub-band-gap photon absorption through intermediate-band transitions, in addition to the conventional direct-band-gap transition.

Cu3VSxSe4−x↗

32.9% Efficient Tandem Solar Cell with Strain-Balanced GaInAs/GaAsP Quantum Wells: Preprint

We demonstrate single and dual junction solar cells with up to 80 strain-balanced GaInAs/GaAsP quantum wells (QWs), in order to extend the range of photon absorption. The net average stress in the quantum well layers is =12 MPa, despite coherent stresses in the individual layers that are 35-70 times greater. The GaAs-QW cell has a certified efficiency of (27.2 ± 0.2)% at one-sun; the GaInP/GaAs-QW tandem has a certified record one-sun efficiency of (32.9 ± 0.5)%. We will discuss the architecture of the devices, the physics behind the high performance, and pathways to further improvement.

GaAsP↗

Optical device having a light-emitting structure and a waveguide integrated capacitor to monitor light

Examples described herein relate to an optical device with an integrated light-emitting structure to generate light and a waveguide integrated capacitor to monitor light. The light-emitting structure may emit light upon the application of electricity to the optical device. The waveguide integrated capacitor may be formed under the light-emitting structure to monitor the light emitted by the light-emitting structure. The waveguide integrated capacitor includes a waveguide region carrying at least a portion of the light. The waveguide region includes one or more photon absorption sites causing the generation of free charge carriers relative to an intensity of the light confined in the waveguide region resulting in a change in the conductance of the waveguide region.

Srinivasan, Sudharsanan↗

Quasiparticle Poisoning of Superconducting Qubits from Resonant Absorption of Pair-Breaking Photons

The ideal superconductor provides a pristine environment for the delicate states of a quantum computer: because there is an energy gap to excitations, there are no spurious modes with which the qubits can interact, causing irreversible decay of the quantum state. As a practical matter, however, there exists a high density of excitations out of the superconducting ground state even at ultralow temperature; these are known as quasiparticles. Observed quasiparticle densities are of order 1 μ m - 3 , tens of orders of magnitude greater than the equilibrium density expected from theory. Nonequilibrium quasiparticles extract energy from the qubit mode and can induce dephasing. Here we show that a dominant mechanism for quasiparticle poisoning is direct absorption of high-energy photons at the qubit junction. We use a Josephson junction-based photon source to controllably dose qubit circuits with millimeter-wave radiation, and we use an interferometric quantum gate sequence to reconstruct the charge parity of the qubit. We find that the structure of the qubit itself acts as a resonant antenna for millimeter-wave radiation, providing an efficient path for photons to generate quasiparticles. A deep understanding of this physics will pave the way to realization of next-generation superconducting qubits that are robust against quasiparticle poisoning.

Liu, Chuan-Hong↗

Extending water vapor measurement capability of photon-limited differential absorption lidars through simultaneous denoising and inversion

Abstract. The micropulse differential absorption lidar (MPD) was developed at Montana State University (MSU) and the National Center for Atmospheric Research (NCAR) to perform range-resolved water vapor (WV) measurements using low-power lasers and photon-counting detectors. The MPD has proven to produce accurate WV measurements up to 6 km altitude. However, the MPD's ability to produce accurate higher-altitude WV measurements is impeded by the current standard differential absorption lidar (DIAL) retrieval methods. These methods are built upon a fundamental methodology that algebraically solves for the WV using the MPD forward models and noisy observations, which exacerbates any random noise in the lidar observations. The work in this paper introduces the adapted Poisson total variation (PTV) specifically for the MPD instrument. PTV was originally developed for a ground-based high spectral resolution lidar, and this paper reports on the adaptations that were required in order to apply PTV on MPD WV observations. The adapted PTV method, coined PTV-MPD, extends the maximum altitude of the MPD from 6 to 8 km and substantially increases the accuracy of the WV retrievals starting above 2 km. PTV-MPD achieves the improvement by simultaneously denoising the MPD noisy observations and inferring the WV by separating the random noise from the non-random WV. An analysis with 130 radiosonde (RS) comparisons shows that the relative root-mean-square difference (RRMSE) of WV measurements between RS and PTV-MPD exceeds 100 % between 6 and 8 km, whereas the RRMSE between RS and the standard method exceeds 100 % near 3 km. In addition, we show that by employing PTV-MPD, the MPD is able to extend its useful range of WV estimates beyond that of the ARM Southern Great Plains Raman lidar (RRMSE exceeding 100 % between 3 and 4 km); the Raman lidar has a power-aperture product 500 times greater than that of the MPD.

54 ENVIRONMENTAL SCIENCES↗

Nonresonant two-photon x-ray absorption in Cu

We present a real-space Green's function theory and calculations of two-photon x-ray absorption (TPA). Our focus is on nonresonant 𝐾-shell TPA in metallic Cu, which has been observed experimentally at intense x-ray free electron laser (XFEL) sources. The theory is based on an independent particle Green's function treatment of the Kramers-Heisenberg equation and an approximation for the sum over nonresonant intermediate states in terms of a static quadrupole transition operator. XFEL effects are modeled by a partially depleted 𝑑 band. This approach is shown to give results for 𝐾-shell TPA in quantitative agreement with XFEL experiment and with a Bethe-Salpeter equation approach. Furthermore, we also briefly discuss many-body corrections and TPA sum rules.

Approximation methods for many-body systems↗

Entangled Photon Spectroscopy

Conspectus The enhanced interest in quantum-related phenomena has provided new opportunities for chemists to push the limits of detection and analysis of chemical processes. As some have called this the second quantum revolution, a time has come to apply the rules learned from previous research in quantum phenomena toward new methods and technologies important to chemists. While there has been great interest recently in quantum information science (QIS), the quest to understand how nonclassical states of light interact with matter has been ongoing for more than two decades. Our entry into this field started around this time with the use of materials to produce nonclassical states of light. Here, the process of multiphoton absorption led to photon-number squeezed states of light, where the photon statistics are sub-Poissonian. In addition to the great interest in generating squeezed states of light, there was also interest in the formation of entangled states of light. While much of the effort is still in foundational physics, there are numerous new avenues as to how quantum entanglement can be applied to spectroscopy, imaging, and sensing. These opportunities could have a large impact on the chemical community for a broad spectrum of applications. Here, we discuss the use of entangled (or quantum) light for spectroscopy as well as applications in microscopy and interferometry. The potential benefits of the use of quantum light are discussed in detail. From the first experiments in porphyrin dendrimer systems by Dr. Dong-Ik Lee in our group to the measurements of the entangled two photon absorption cross sections of biological systems such as flavoproteins, the usefulness of entangled light for spectroscopy has been illustrated. These early measurements led the way to more advanced measurements of the unique characteristics of both entangled light and the entangled photon absorption cross-section, which provides new control knobs for manipulating excited states in molecules. The first reports of fluorescence-induced entangled processes were in organic chromophores where the entangled photon cross-section was measured. These results would later have widespread impact in applications such as entangled two-photon microscopy. From our design, construction and implementation of a quantum entangled photon excited microscope, important imaging capabilities were achieved at an unprecedented low excitation intensity of 10 7 photons/s, which is 6 orders of magnitude lower than the excitation level for the classical two-photon image. New reports have also illustrated an advantage of nonclassical light in Raman imaging as well. From a standpoint of more precise measurements, the use of entangled photons in quantum interferometry may offer new opportunities for chemistry research. Experiments that combine molecular spectroscopy and quantum interferometry, by utilizing the correlations of entangled photons in a Hong–Ou–Mandel (HOM) interferometer, have been carried out. The initial experiment showed that the HOM signal is sensitive to the presence of a resonant organic sample placed in one arm of the interferometer. In addition, parameters such as the dephasing time have been obtained with the opportunity for even more advanced phenomenology in the future.

36 MATERIALS SCIENCE↗

Manipulating Core Excitations in Molecules by X-Ray Cavities

Core excitations on different atoms are highly localized and therefore decoupled. By placing molecules in an x-ray cavity the core transitions become coupled via the exchange of cavity photons and form delocalized hybrid light-matter excitations known as core polaritons. Here, we demonstrate these effects for the two inequivalent carbon atoms in 1,1-difluoroethylene. Polariton signatures in the x-ray absorption, two-photon absorption, and multidimensional four-wave mixing signals are predicted.

74 ATOMIC AND MOLECULAR PHYSICS↗

Non-destructive identification of absorptive damage sites by photoluminescence brightening

We present a non-destructive photoluminescence (PL) imaging strategy for probing damage growth behavior in fused silica under laser irradiation. Transient wide-field PL image measurements were conducted at varying excitation intensities to investigate the dynamics of radiative defect generation and annihilation in laser-induced damage sites. Our results reveal that, while low excitation intensities predominantly induce PL quenching due to defect annihilation, high-intensity excitation (>0.3 GW/cm 2 at 532 nm) triggers pronounced PL brightening (PLB), indicative of radiative defect generation. Image analysis demonstrates that PLB events are strongly correlated with subsequent damage growth (10 J/cm 2 at 351 nm), whereas overall PL intensity is not. No optically detectable morphological changes were observed during PLB, confirming the non-destructive nature of the technique. We propose that PLB arises from defect-assisted absorption of multiple photons at pre-existing absorptive centers, which enhances local absorptivity and initiates further defect formation. These findings establish PLB monitoring as a sensitive diagnostic tool for identifying damage sites with elevated absorptivity, enabling targeted maintenance and improved laser damage management in optical materials.

Materials science↗

Momentum-exchange interactions in a Bragg atom interferometer suppress Doppler dephasing

Large ensembles of laser-cooled atoms interacting through infinite-range photon-mediated interactions are powerful platforms for quantum simulation and sensing. Here we realize momentum-exchange interactions in which pairs of atoms exchange their momentum states by collective emission and absorption of photons from a common cavity mode, a process equivalent to a spin-exchange or XX collective Heisenberg interaction. The momentum-exchange interaction leads to an observed all-to-all Ising-like interaction in a matter-wave interferometer. A many-body energy gap also emerges, effectively binding interferometer matter-wave packets together to suppress Doppler dephasing in analogy to Mössbauer spectroscopy. The tunable momentum-exchange interaction expands the capabilities of quantum interaction–enhanced matter-wave interferometry and may enable the realization of exotic behaviors, including simulations of superconductors and dynamical gauge fields.

Science & Technology - Other Topics↗

Self-absorption and Phonon Pulse Shape Discrimination in Scintillating Bolometers

In this work, we show that self-absorption of photons in scintillating bolometers can differentiate phonon pulse shapes between α (or nuclear recoil) and β/γ signals. This enables phonon pulse shape discrimination for particle identification. We establish a detector signal model that includes self-absorption and compare the simulated phonon pulse shapes with previously reported experimental results. The model predicts increase in pulse shape difference at higher self-absorption. Based on this result, we propose a new design of scintillating bolometers using 4π light reflectors for maximized self-absorption and only a single phonon readout, instead of light detectors that are typically employed for particle discrimination in scintillating bolometers.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Energy deposition model in STREAM with photon transport

Recent efforts have been taken to implement a photon transport module for the neutron transport analysis code STREAM, considering the explicit photon energy distribution in the problem instead of using the locally deposition assumption as employed in previous STREAM versions. The current energy release model in STREAM based on the On-the-fly energy released per fission model is modified accordingly to account for the photon energy deposition computed explicitly by this module. The impacts of the modified energy release model with photon transport in STREAM on the power distribution, fuel temperature and other core parameters during depletion with feedback calculations are studied on several problems from the VERA benchmark suit. Overall, the photon transport provides a better power map for depletion and feedback calculations, especially when strong gamma emitters are present. The fuel temperature, in general, is decreased when the photon transport is employed because fission gammas have been transported out of their birthplace. The new energy deposition model in STREAM with photon transport indicates that gamma energy accounts for about 9.7% of the total energy released in a fresh VERA5 2D core and rises to 10.5% at the End of Cycle. Around 2.5% of the total energy released will be deposited in the coolant in this 2D core. (authors)

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Photon-shot-noise-limited transient absorption soft X-ray spectroscopy at the European XFEL

Femtosecond transient soft X-ray absorption spectroscopy (XAS) is a very promising technique that can be employed at X-ray free-electron lasers (FELs) to investigate out-of-equilibrium dynamics for material and energy research. Here, a dedicated setup for soft X-rays available at the Spectroscopy and Coherent Scattering (SCS) instrument at the European X-ray Free-Electron Laser (European XFEL) is presented. It consists of a beam-splitting off-axis zone plate (BOZ) used in transmission to create three copies of the incoming beam, which are used to measure the transmitted intensity through the excited and unexcited sample, as well as to monitor the incoming intensity. Since these three intensity signals are detected shot by shot and simultaneously, this setup allows normalized shot-by-shot analysis of the transmission. For photon detection, an imaging detector capable of recording up to 800 images at 4.5 MHz frame rate during the FEL burst is employed, and allows a photon-shot-noise-limited sensitivity to be approached. The setup and its capabilities are reviewed as well as the online and offline analysis tools provided to users.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Multilayer Lateral Heterostructures of Van Der Waals Crystals with Sharp, Carrier–Transparent Interfaces

Abstract Research on engineered materials that integrate different 2D crystals has largely focused on two prototypical heterostructures: Vertical van der Waals stacks and lateral heterostructures of covalently stitched monolayers. Extending lateral integration to few layer or even multilayer van der Waals crystals could enable architectures that combine the superior light absorption and photonic properties of thicker crystals with close proximity to interfaces and efficient carrier separation within the layers, potentially benefiting applications such as photovoltaics. Here, the realization of multilayer heterstructures of the van der Waals semiconductors SnS and GeS with lateral interfaces spanning up to several hundred individual layers is demonstrated. Structural and chemical imaging identifies {110} interfaces that are perpendicular to the (001) layer plane and are laterally localized and sharp on a 10 nm scale across the entire thickness. Cathodoluminescence spectroscopy provides evidence for a facile transfer of electron‐hole pairs across the lateral interfaces, indicating covalent stitching with high electronic quality and a low density of recombination centers.

36 MATERIALS SCIENCE↗