Search NASA⌕ Search

SEARCH · Search NASA

Results for “RAMAN SCATTERING”

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.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 91 records · Page 5

When do molecular polaritons behave like optical filters?

This review outlines several linear optical effects featured by molecular polaritons arising in the collective strong light–matter coupling regime. Under weak laser irradiation and when the single-molecule light–matter coupling can be neglected (often in the limit when the number of molecules per photon mode is large), we show that the excited-state molecular dynamics under collective strong coupling can be exactly replicated without the cavity using a shaped (or “filtered”) laser, whose field amplitude is enhanced by the cavity quality factor, shining on the bare molecules. As a consequence, the absorption within a cavity can be understood as the overlap between the polariton transmission and the bare molecular absorption, suggesting that polaritons act in part as optical filters. This framework demystifies and provides a straightforward explanation for a large class of experiments and theoretical models in molecular polaritonics, highlighting that the same effects can be achieved without the cavity with shaped laser pulses. With a few modifications, this simple conceptual picture can also be adapted to understand the incoherent nonlinear response of polaritonic systems. This review establishes a clear distinction between polaritonic phenomena that can be fully explained through classical linear optics and those that require a quantum electrodynamics approach. It also highlights the need to differentiate between effects that necessitate polaritons (i.e., hybrid light–matter states) and those that can occur in the weak coupling regime. Here, we further discuss that certain quantum optical effects like fluorescence can be partially described as optical filtering, whereas some others like cavity-induced Raman scattering go beyond this. Further exploration in these areas is needed to uncover novel polaritonic phenomena beyond optical filtering.

Schwennicke, Kai [University of California, San Di↗

Time-resolved magneto-optical effects in the altermagnet candidate MnTe

α -MnTe is an antiferromagnetic semiconductor with above room temperature T N = 310 K, which is promising for spintronic applications. Recently, it was reported to be an altermagnet, containing bands with momentum-dependent spin splitting; time-resolved experimental probes of MnTe are, therefore, important both for understanding novel magnetic properties and potential device applications. Here, we investigate ultrafast spin dynamics in epitaxial MnTe(001)/InP(111) thin films using pump-probe magneto-optical measurements in the Kerr configuration. At room temperature, we observe an oscillation mode at 55 GHz that does not appear at zero magnetic field. Combining field and polarization dependence, we identify this mode as a magnon, likely originating from inverse stimulated Raman scattering. Magnetic field-dependent oscillations persist up to at least 335 K, which could reflect coupling to known short-range magnetic order in MnTe above T N . Additionally, we observe two optical phonons at 3.6 and 4.2 THz, which broaden and redshift with increasing temperature.

Gray, Isaiah↗

Quantifying the thermal effect and methyl radical production in nanosecond repetitively pulsed glow discharges applied to a methane-air flame

In this work, we investigated non-equilibrium plasma produced by nanosecond repetitively pulsed glow discharges applied across a lean premixed methane-air flame. The flame is stationary, axisymmetric, and laminar. The discharges are applied on the symmetry axis crossing the reactant gases, flame front, and product gases, allowing phase-locked averaged measurements and comparisons with axisymmetric numerical simulations. The thermal effect and methyl radical production are quantified in the discharge in the reactant gas region. One-dimensional, two-beam, hybrid, femtosecond-picosecond, coherent anti-Stokes Raman scattering is used to acquire spatial and temporal profiles of temperature and oxygen-to-nitrogen concentration ratio. Photo-fragmentation laser-induced fluorescence is used to acquire quantitative two-dimensional profiles of methyl radicals in the discharge providing the first quantitative imaging of methyl produced ahead of a flame by plasma-induced methane dissociation. The spatial profiles of temperature and oxygen-to-nitrogen concentration ratio are in steady state, indicating that individual discharges have an insignificant heating effect. Upper and lower bounds of the produced mole fraction of methyl radicals in the plasma are obtained due to uncertainties in the collisional quenching rates of excited state methylidyne radicals in the plasma. The discharges produce a maximum of 600–1100 ppm of methyl radicals upstream of the flame front within 25 ns. This amount is similar to the predicted methyl mole fraction for the flame without plasma and thus represents a significant chemical perturbation to the reactants upstream of the flame front. The produced methyl follows an exponential decay in the first microsecond after the discharge with a decay constant of 8 µs close to the flame, and 0.8 µs further from the flame. The decay then deviates from the exponential curve and the methyl persists for tens of microseconds. The results suggest that for the tested configuration, the thermal effect of individual discharges through fast gas heating is negligible, while active chemical species are produced in large quantities in the reactant gases, upstream of the flame front.

hybrid fs-ps CARS↗

Atomic Coherence of 2 Minutes and Instability of 1.5 × 10 −18 at 1 s in a Wannier-Stark Lattice Clock

We explore the limits of atomic coherence and measurement precision in a 87 Sr optical lattice clock. We perform a detailed characterization of key effects, including lattice Raman scattering and atomic collisions in a shallow lattice configuration, determining a 174(28) s 3 𝑃 0 clock state lifetime. Investigation of atomic coherence across a range of lattice depths and atomic densities reveals decoherence mechanisms related to photon scattering and atomic interaction. At a reduced density, we observe a coherence time of 118(9) s, approaching the fundamental limit set by spontaneous emission. Guided by this coherence understanding, we demonstrate a clock instability for an atomic ensemble of 1.5 × 10 −18 at 1 s in fractional frequency units. Our results are important for further advancing the state of the art of an optical lattice clock for fundamental physics applications.

atomic, optical, & lattice clocks↗

Frustration-driven magnetic correlations in the spin-$\frac{5}{2}$ triangular lattice antiferromagnet RbFe⁢(HPO 3 ) 2

Here, a detailed study of the structural and magnetic properties of a spin-5/2 triangular lattice antiferromagnet RbFe⁢(HPO 3 ) 2 is presented using x-ray diffraction, magnetization, heat capacity, and 31 P nuclear magnetic resonance (NMR) experiments on a polycrystalline sample. The crystal structure features an equilateral triangular lattice of Fe 3+ ions. The thermodynamic measurements reveal the onset of a magnetic long-range order at 𝑇 N⁢1 ≃7.8K in zero field, followed by another low-temperature field-induced ordering at 𝑇 N⁢2 in higher fields. The transition at 𝑇 N⁢1 is further confirmed from the NMR spin lattice relaxation measurements. The value of the frustration ratio (𝑓≃7) implies moderate spin frustration in the compound. The 31 P NMR spectra exhibit two distinct spectral lines corresponding to two inequivalent phosphorus sites (P1 and P2), consistent with the crystal structure. The P1 site is strongly coupled with an isotropic hyperfine coupling of 𝐴$^{iso}_{hf}$ = 0.55⁢(2)⁢ T/𝜇 B while the P2 site is weakly coupled with 𝐴$^{iso}_{hf}$ = 0.25⁢(3)⁢ T/𝜇 B with the Fe 3+ ions. The magnetic susceptibility and NMR shift data are described well assuming a spin-5/2 isotropic triangular lattice antiferromagnetic model with an average exchange coupling of 𝐽/𝑘 B = 2.8⁢(2)⁢K. Below 𝑇 N⁢1 , the spectra evolve into a nearly rectangular powder pattern, indicating a commensurate antiferromagnetic type order. The 31 P spin-lattice relaxation rate well below 𝑇N⁢1 follows a 𝑇 3 temperature dependence, implying a two-magnon Raman scattering mechanism in the ordered state. Three well-defined phase regimes are clearly ascertained in the 𝐻−𝑇 phase diagram, reflecting a weak magnetic anisotropy in the compound.

Nagpal, V. [Indian Institute of Science Education ↗

Evidence of distinct nonpolar/polar ordering at long/short ranges in relaxor ferroelectrics

Distinct atomic nonpolar/polar ordering is determined at long, intermediate, and short ranges using synchrotron x-ray diffraction, Raman scattering, and pair distribution function data in K 0.5 Na 0.5 NbO 3 -doped BaTiO 3 -based relaxor ferroelectrics, viz., (1 - x) Ba 0.9 Sr 0.1 TiO 3 -x KNN 50. Two different polar phases with distinct symmetries are identified at short/intermediate ranges for x = 0.10, where a monoclinic phase at short ranges gradually transforms into a rhombohedral phase at intermediate ranges. Here, in contrast, a nonpolar phase with average cubic symmetry is found to be stable at long ranges for a wide temperature range (100 ≤ T ≤ 500 K). The polar behavior of short/intermediate-range ordering is quantified in terms of the amplitude of ferroelectric phonon mode $Γ^-_4$ (q = 0, 0, 0) (which corresponds to the zone center of the cubic Brillouin zone). The amplitude of the $Γ^-_4$ phonon mode increases with decreasing temperature, suggesting the enhancement of ferroelectric polarization at short/intermediate ranges on lowering temperatures. Enhanced ferroelectric polarization at low temperature is also visible and evident by ferroelectrostriction and is quantified by the increase in magnitude of spontaneous volume ferroelectrostriction. Consequently, Zero thermal expansion is observed at low temperatures.

36 MATERIALS SCIENCE↗

Thermal disorder and phonon softening in the ferroelectric phase transition of lead titanate

We report a molecular dynamics study of ab initio quality of the ferroelectric phase transition in crystalline PbTi⁢O3. We model anharmonicity accurately in terms of potential energy and polarization surfaces trained on density functional theory data with modern machine learning techniques. Our simulations demonstrate that the transition has a strong order-disorder character, in agreement with diffraction experiments, and provide fresh insight into the approach to equilibrium across the phase transition. We find that the emergence and disappearance of the macroscopic polarization is driven by dipolar switching at the nanometer scale. We also computed the infrared optical absorption spectra in both the ferroelectric and the paraelectric phases, finding good agreement with the experimental Raman frequencies. Often, the almost ideal displacive character of the soft mode detected by Raman scattering in the paraelectric phase has been contrasted with the order-disorder character of the transition suggested by diffraction experiments. We settle this issue by showing that the soft mode coexists with a strong Debye relaxation associated with thermal disordering of the dipoles. The Debye relaxation feature is centered at zero frequency and appears near the transition temperature in both the ferroelectric and the paraelectric phases.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Floquet engineering of polaritonic amplification in dispersive photonic time crystals

In this study, we investigate the dynamics of dispersive photonic time crystals (PTCs) and their potential applications for controlling light-matter interaction. Using the Lorentz-Drude as dispersive material model, we analyze the effects of periodic modulation of dispersion parameters through both theoretical and numerical analysis, revealing the emergence of hybrid bandgaps from the interaction of polaritonic branches with distinctive characteristics. Our study demonstrates that dispersive PTCs offer novel excitation channels and amplification possibilities, that require lower modulation frequencies compared to nondispersive systems thus alleviating experimental challenges for the realization of PTCs in the optical regime. These findings pave the way for advancements in polaritonic lasing and resonant Raman scattering.

Classical optics↗

Optimal filtering and generation of entangled photons for quantum applications in the presence of noise

Filtering is commonly used in quantum optics to reject noise photons, and also to enable interference between independent photons. However, filtering the joint spectrum of photon pairs can reduce the inherent coincidence probability or loss-independent heralding efficiency. Here we investigate filtering for multiphoton applications based on entanglement and interference (e.g., quantum teleportation). We multiplex C-band entangled photons and C-band classical communications into the same long-distance fibers, which enables scalable low-loss quantum networking but requires filtering of spontaneous Raman scattering noise from classical light. Using tunable-bandwidth filters, low-jitter detectors, and polarization filters, we distribute wavelength-degenerate time-bin entangled photons in the C band (1536.5 nm) over 25 km/25 km standard fibers (50 km) each carrying 10 Gbit/s C-band classical data signals. Narrow filtering enables milliwatt-level C-band power, which exceeds the power achieved by comparable studies by roughly an order of magnitude and could feasibly support terabit per second classical rates. We evaluate how performance depends on pump and filter bandwidths, multipair emission, filter shapes, loss, phase matching, and how quantum information is measured. We find a trade-off between reducing noise impact and increasing single-mode purity, and discuss mitigation methods toward optimal multiphoton applications. Importantly, these results apply to noise in free space and in quantum devices (sources, frequency converters, switches, detectors, etc.) and provide insight into filter-induced degradation of single-photon purity and rates even in noise-free environments.

Thomas, Jordan M. [Fermilab; Northwestern U.]↗

Spectroscopy in Nanoscopic Cavities: Models and Recent Experiments

The ability of nanophotonic cavities to confine and store light to nanoscale dimensions has important implications for enhancing molecular, excitonic, phononic, and plasmonic optical responses. Spectroscopic signatures of processes that are ordinarily exceedingly weak such as pure absorption and Raman scattering have been brought to the single-particle limit of detection, while new emergent polaritonic states of optical matter have been realized through coupling material and photonic cavity degrees of freedom across a wide range of experimentally accessible interaction strengths. In this review, we discuss both optical and electron beam spectroscopies of cavity-coupled material systems in weak, strong, and ultrastrong coupling regimes, providing a theoretical basis for understanding the physics inherent to each while highlighting recent experimental advances and exciting future directions.

Chemistry↗

Defect passivation in nanostructured silica for stable birefringence in polarization optics

Nanostructured materials with anisotropic microstructure exhibit direction-dependent refractive index, known as form birefringence. One of the main advantages of these nanostructured materials is that the ease of fabrication significantly reduces the cost of production. However, their birefringence is affected by humidity as well as time. The hypothesis is that defects, particularly silanols, are responsible. Here, in this work, we present the use of hexamethyldisilazane (HMDS) vapor as a passivation strategy. Using spectroscopic ellipsometry and Raman scattering, the data show that HMDS successfully passivates silanol groups and promotes O-Si-O bond formation, resulting in improved stability. The results demonstrate a simple method to enhance the reliability of all-silica polarization optics offering potential advancements for high-power laser components.

Mireles, Marcela [Univ. of Rochester, NY (United S↗

Temporal reflection from short pump pulses inside a dispersive nonlinear medium: the impact of pump parameters

We have studied, through a series of experiments and numerical simulations, how temporal reflection from an intense pump pulse inside a photonic crystal fiber is affected by parameters of the pump pulse used to form a moving high-index boundary. We used femtosecond pump pulses, which slow down inside the fiber as their spectrum red-shifts because of intrapulse Raman scattering. Temporal reflection of probe pulses occurs from such decelerating pump pulses. We changed the width and chirp of our pump pulses with a 4f pulse shaper capable of providing both spectral filtering and frequency chirping. We found that temporal refection exhibited novel features, to our knowledge, when pump pulses were made wider or chirped. In both cases, two or more reflected pulses were produced at different wavelengths in a specific range of the initial pump-probe delays. Furthermore, numerical simulations reveal that the origin of such novel features is related to the complex nonlinear evolution of pump pulses inside optical fibers.

47 OTHER INSTRUMENTATION↗

Comparative study of spectral broadening and few-cycle compression of Yb:KGW laser pulses in gas-filled hollow-core fibers

While industrial-grade Yb-based amplifiers have become very prevalent, their limited gain bandwidth has created a large demand for robust spectral broadening techniques that allow for few-cycle pulse compression. In this work, we perform a comparative study between several atomic and molecular gases as media for spectral broadening in a hollow-core fiber geometry. Exploiting nonlinearities such as self-phase modulation, self-steepening, and stimulated Raman scattering, we explore the extent of spectral broadening and its dependence on gas pressure, the critical power for self-focusing, and the optimal regime for few-cycle pulse compression. Using a 3-mJ, 200-fs input laser pulses, we achieve 17 fs, few-cycle pulses with 80% fiber energy transmission efficiency. The optimal parameters can be scaled for higher or lower input pulse energies with appropriate gas parameters and fiber geometry.

Shalaby, Islam (ORCID:0000000332846636)↗

Quantum teleportation coexisting with classical communications in optical fiber

The ability for quantum and conventional networks to operate in the same optical fibers would aid the deployment of quantum network technology on a large scale. Quantum teleportation is a fundamental operation in quantum networking, but has yet to be demonstrated in fibers populated with high-power conventional optical signals. Here we report, to the best of our knowledge, the first demonstration of quantum teleportation over fibers carrying conventional telecommunications traffic. Quantum state transfer is achieved over a 30.2-km fiber carrying 400-Gbps C-band classical traffic with a Bell state measurement performed at the fiber’s midpoint. To protect quantum fidelity from spontaneous Raman scattering noise, we use optimal O-band quantum channels, narrow spectro-temporal filtering, and multi-photon coincidence detection. Fidelity is shown to be well maintained with an elevated C-band launch power of 18.7 dBm for the single-channel 400-Gbps signal, which we project could support multiple classical channels totaling many terabits/s aggregate data rates. These results show the feasibility of advanced quantum and classical network applications operating within a unified fiber infrastructure.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Quantum entanglement distribution coexisting with high-rate, broadband classical optical communications over a real-world fiber connecting remote, synchronized nodes

Compatibility with existing classical network infrastructure offers a scalable path towards deploying large-scale quantum networks. Here, we demonstrate O-band polarization-encoded quantum entanglement distribution over an installed 24.4-km fiber while coexisting with a state-of-the-art fully loaded C-band classical communications line system and a picosecond-level precision L-band synchronization signal. The classical system carries two 800-Gbps channels while the remainder of the C-band is filled with amplified spontaneous emission, as is standard for such state-of-the-art communications systems. We examine the spontaneous Raman scattering spectrum generated from this broadband C-band light and offer insights into wavelength allocation for O-band quantum channels. Optimal wavelength selection and narrow filtering enable well-preserved Bell state fidelity when coexisting with 21.4-dBm aggregate launch power across the C-band suitable for 36-Tbps transmission. To the best of our knowledge, this is the first implementation of entanglement-based quantum communications between two remote nodes coexisting with independent classical communications traffic. We demonstrate coexistence of quantum entanglement with ultra-high power levels and record classical bandwidth, offering promise for real-world entanglement-based networking integrated within high-capacity communications infrastructure.

Talcott, Gina M. [Northwestern U.] (ORCID:00000002↗

Advanced Model Development for Large Eddy Simulation of Oxy-Combustion and Supercritical Carbon Dioxide Power Cycles

A joint experimental and numerical study is performed to observe the characteristics of a supercritical carbon dioxide turbulent mixing layer in the presence of strong nonlinearities in the thermodynamic and transport properties. A bespoke experimental setup is designed and employed for this purpose and provides insight into macroscopic mixing behavior. The mixing is experimentally observed using two techniques: shadowgraphy and spontaneous Raman scattering. Qualitative and quantitative intensity fields obtained via these techniques yield instantaneous and mean density data. Spanwise temperature data is also collected using analogue resistance temperature detectors. These measurements are used to quantify the level of mixed material within the field. The experimental data are supplemented by a companion high-fidelity numerical study. The numerical results are obtained through fully resolved, three-dimensional direct numerical simulation. The numerical dataset permits observation of the near-field mixing characteristics, which are difficult to measure experimentally due to the rapid dynamics and sharp thermophysical gradients in this area. Qualitative field visualizations are presented, followed by quantitative mixed material results and observations regarding thermodynamic property trends at select locations within the field. One-dimensional spectra of the turbulent kinetic energy and solenoidal dissipation are provided to observe the spectral characteristics of the flow. Reynolds stress anisotropy is analyzed graphically through anisotropy invariance maps (Lumley triangles). The mixing quantification, spectral data and anisotropy analysis of a flow at these thermodynamic conditions represent the main outcomes of the work.

20 FOSSIL-FUELED POWER PLANTS↗

Time-dependent phenomena in correlated materials

Understanding time-dependent processes and light-matter interaction in strongly correlated materials, and the interplay between electronic, orbital, vibrational, and spin degrees of freedom, is a cornerstone of condensed matter. These mechanisms can be proven by measuring the response of the systems to time-dependent perturbations. The corresponding time scales are dictated by the way light couples to the different excitations, and how these excitations exchange energy and momentum. Our research advances our understanding of these processes, and the interpretation of different equilibrium and time-resolved spectroscopies. Our project encompasses two main themes: (i) developing and refining computational techniques to study non-equilibrium spectroscopies including non-perturbative effects and (ii) applications to non-equilibrium phenomena. We have developed a new computational approach that works directly in the time domain: by including all the degrees of freedom involved in the scattering process (e.g. electrons, photons, neutrons), we solve the time dependent problem: a faithful numerical simulation of the experiment. By measuring the energy and momentum of the outgoing particles, we can extract information about the energy and momentum absorbed by the system. Prior to our work, people attempting to model and calculate non-equilibrium spectral functions relied on a description of the scattering cross section based on a formulation in the frequency domain, a treatment that is extremely cumbersome and complex. Our technique works in and out of equilibrium and can reproduce spectra by several spectroscopic techniques, such as time-resolved photoemission, neutron scattering, Raman, X-ray spectroscopies (RIXS, Auger, XAS, XMCD), and, by not relying on analytical approximations, yields results that reveal novel overlooked transient mechanisms. These tools provide sorely needed intuition for understanding the phenomenology of strongly correlated materials and will help experimentalists in identifying signatures of relevant excitations in pump-probe experiments, such as those conducted in DOE supported facilities.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Pump depletion and the Raman gap in ignition-scale plasmas

Laser-plasma instabilities under ignition conditions for direct-drive inertial confinement fusion are studied using two-dimensional Particle-in-Cell simulations with a combination of in-plane (PP) and out-of-the-plane (SP) lasers. The results show that stimulated Raman side scattering can induce significant pump depletion and form a gap in the Raman scattered light spectra that have been observed in experiments.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗