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Results for “Optical Response”

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 271 records · Page 15
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Time-Resolved Ultrafast Transient Polarization Spectroscopy to Investigate Nonlinear Processes and Dynamics in Electronically Excited Molecules on the Femtosecond Time Scale

Here, we report a novel experimental technique to investigate ultrafast dynamics in photoexcited molecules by probing the third-order nonlinear optical susceptibility. A non-colinear 3-pulse scheme is developed to probe the ultrafast dynamics of excited electronic states using the optical Kerr effect by time-resolved polarization spectroscopy. Optical heterodyne and optical homodyne detection are demonstrated to measure the third-order nonlinear optical response for the S 1 excited state of liquid nitrobenzene, which is populated by 2-photon absorption of a 780 nm 35 fs excitation pulse.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

Enhancing hyperspectral EELS analysis of complex plasmonic nanostructures with pan-sharpening

Nanoscale hyperspectral techniques—such as electron energy loss spectroscopy (EELS)—are critical to understand the optical response in plasmonic nanostructures, but as systems become increasingly complex, the required sampling density and acquisition times become prohibitive for instrumental and specimen stability. As a result, there has been a recent push for new experimental methodologies that can provide comprehensive information about a complex system, while significantly reducing the duration of the experiment. In this work, we present a pan-sharpening approach to hyperspectral EELS analysis, where we acquire two datasets from the same region (one with high spatial resolution and one with high spectral fidelity) and combine them to achieve a single dataset with the beneficial properties of both. This work outlines a straightforward, reproducible pathway to reduced experiment times and higher signal-to-noise ratios, while retaining the relevant physical parameters of the plasmonic response, and is generally applicable to a wide range of spectroscopy modalities.

36 MATERIALS SCIENCE↗
DOE OSTI2022

A quantitative model of charge injection by ruthenium chromophores connecting femtosecond to continuous irradiance conditions

A kinetic framework for the ultrafast photophysics of tris(2,2-bipyridine)ruthenium(II) phosphonated and methyl-phosphonated derivatives is used as a basis for modeling charge injection by ruthenium dyes into a semiconductor substrate. By including the effects of light scattering, dye diffusion, and adsorption kinetics during sample preparation and the optical response of oxidized dyes, quantitative agreement with multiple transient absorption datasets is achieved on timescales spanning femtoseconds to nanoseconds. In particular, quantitative agreement with important spectroscopic handles—the decay of an excited state absorption signal component associated with charge injection in the UV region of the spectrum and the dynamical redshift of a ~500 nm isosbestic point—validates our kinetic model. Pseudo-first-order rate coefficients for charge injection are estimated in this work, with an order of magnitude ranging from 10 11 to 10 12 s –1 . The model makes the minimalist assumption that all excited states of a particular dye have the same charge injection coefficient, an assumption that would benefit from additional theoretical and experimental exploration. Here, we have adapted this kinetic model to predict charge injection under continuous solar irradiation and find that as many as 68 electron transfer events per dye per second take place, significantly more than prior estimates in the literature.

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

Quantum dynamics simulations of the 2D spectroscopy for exciton polaritons

We develop an accurate and numerically efficient non-adiabatic path-integral approach to simulate the non-linear spectroscopy of exciton–polariton systems. This approach is based on the partial linearized density matrix approach to model the exciton dynamics with explicit propagation of the phonon bath environment, combined with a stochastic Lindblad dynamics approach to model the cavity loss dynamics. Through simulating both linear and polariton two-dimensional electronic spectra, we systematically investigate how light–matter coupling strength and cavity loss rate influence the optical response signal. Our results confirm the polaron decoupling effect, which is the reduced exciton–phonon coupling among polariton states due to the strong light–matter interactions. We further demonstrate that the polariton coherence time can be significantly prolonged compared to the electronic coherence outside the cavity.

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

Perspectives and progress on wurtzite ferroelectrics: Synthesis, characterization, theory, and device applications

Wurtzite ferroelectrics are an emerging material class that expands the functionality and application space of wide bandgap semiconductors. Promising physical properties of binary wurtzite semiconductors include a large, reorientable spontaneous polarization, direct band gaps that span from the infrared to ultraviolet, large thermal conductivities and acoustic wave velocities, high mobility electron and hole channels, and low optical losses. The ability to reverse the polarization in ternary wurtzite semiconductors at room temperature enables memory and analog type functionality and quasi-phase matching in optical devices and boosts the ecosystem of wurtzite semiconductors, provided the appropriate combination of properties can be achieved for any given application. In this article, advances in the design, synthesis, and characterization of wurtzite ferroelectric materials and devices are discussed. Highlights include: the direct and quantitative observation of polarization reversal of ~135 μC/cm 2 charge in Al 1-x B x N via electron microscopy, Al 1-x B x N ferroelectric domain patterns poled down to 400 nm in width via scanning probe microscopy, and full polarization retention after over 1000 h of 200 °C baking and a 2× enhancement relative to ZnO in the nonlinear optical response of Zn 1-x Mg x O. In conclusion, the main tradeoffs, challenges, and opportunities in thin film deposition, heterostructure design and characterization, and device fabrication are overviewed.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2022

Twisted bilayered graphenes at magic angles and Casimir interactions: correlation-driven effects

Twisted bilayered graphenes (TBGs) at magic angles are systems housing long ranged periodicity of moiré patterns together with short ranged periodicity associated with the individual graphenes. Such materials are a fertile ground for novel states largely driven by electronic correlations. Here we find that the ubiquitous Casimir force can serve as a platform for macroscopic manifestations of the quantum effects stemming from the magic angle bilayered graphenes properties and their phases determined by electronic correlations. In conclusion, by utilizing comprehensive calculations for the electronic and optical response, we find that Casimir torque can probe anisotropy from the Drude conductivities in nematic states, while repulsion in the Casimir force can help identify topologically nontrivial phases in magic angle TBGs.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Optical Interference for the Guidance of Cryogenic Focused Ion Beam Milling Beyond the Axial Diffraction Limit

Using a tri-coincident cryogenic FIB-SEM-LM system, we identify an interferometric optical response that can be used for targeting lamella production to fluorescently labelled structures with accuracy beyond the diffraction limit. We demonstrate the approach using synthetic samples of fluorescent beads embedded in micron-scale droplets of water. Here, we then apply the approach to capture virions inside host cells. Successful targeting is confirmed by cryogenic electron tomography revealing clusters of virions in intracellular vesicles.

Sica, Anthony V. [SLAC National Accelerator Labora↗
DOE OSTI2026

Casimir interactions between two parallel graphene sheets carrying steady-state drift currents

Here, we investigate the fluctuation-induced Casimir interactions between two parallel graphene sheets carrying steady-state drift currents. The graphene properties are modeled based on the shifted Fermi disk model to capture the nonequilibrium optical response of the system. We find that the drift current introduces a repulsive correction to the perpendicular to the layers Casimir interaction, thereby reducing the overall attractive force. Although the correction is repulsive, it does not overcome the underlying attraction between the layers. It also generates a lateral force that opposes the carrier flow direction. Both contributions are studied in terms of distance and drift velocity functionalities showing pathways for Casimir force control.

Ke, Modi [University of South Florida, Tampa, FL (↗
DOE OSTI2023

Interplay between disorder, local relaxation, and collective behavior for an ensemble of emitters outside versus inside a cavity

The interplay between collective optical response and molecular static and dynamic disorder is studied using simple effective Hamiltonians for an ensemble of two-level emitters inside and outside a single-mode cavity. We model environmental disorder by randomly modulating the molecular transition frequencies and the coupling between the emitters and the electromagnetic field. We also consider the effects of intermolecular interactions and orientational disorder. We investigate how these effects lead to new features in the steady-state absorption (outside the cavity), transmission spectra (inside the cavity), and the yield of local molecular processes such as a unimolecular reaction. Outside the cavity, the collective behavior is manifested in the linewidth of the steady-state absorption, the emission spectrum, and the local chemical yield. Inside the cavity, however, the collective behavior primarily determines the Rabi splitting. The effects of intermolecular interactions under orientational disorder are also studied. For the most part, for all types of disorder, if we increase disorder, we find a reduction in the collective nature of the molecular response (smaller effective N) and therefore the Rabi splitting contraction occurs with orientational disorder. Furthermore, we find that static disorder is more destructive to collective behavior than dynamic disorder.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Indications for Lifshitz transitions in the nodal-line semimetal ZrSiTe induced by interlayer interaction

The layered material ZrSiTe is currently extensively investigated as a nodal-line semimetal with Dirac-like band crossings protected by nonsymmorphic symmetry close to the Fermi energy. A recent infrared spectroscopy study on ZrSiTe under external pressure found anomalies in the optical response, providing hints for pressure-induced phase transitions at ≈4.1 and ≈ 6.5GPa. By pressure-dependent Raman spectroscopy and x-ray diffraction measurements combined with electronic band structure calculations we find indications for two pressure-induced Lifshitz transitions with major changes in the Fermi surface topology in the absence of lattice symmetry changes. These electronic phase transitions can be attributed to the enhanced interlayer interaction induced by external pressure. Overall, our findings demonstrate the crucial role of the interlayer distance for the electronic properties of layered van der Waals topological materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Quasiparticle self-consistent $GW$ energy band calculations for $\mathrm{Ge_3N_4}$ phases

Quasiparticle self-consistent GW (G Green's function, W screened Coulomb interaction) band structure calculations are presented for the α, β, and γ phases of Ge 3 N 4 . The GW corrections to the gap are substantial and the gaps are found to be 3.85, 3.86, and 3.56 eV for α, β, γ respectively, at the experimental lattice constants. Only the β phase has a direct gap. The α and β phases, which are closely related to each other in crystal structure, are consequently also found to have rather similar band structures. Nonetheless, some significant differences are found near the valence band maximum, which are related to the different interlayer interactions in the c direction. In the cubic spinel phase, the conduction band minima of s and p character are found close to each other. Effective masses are calculated for the relevant valence and conduction band edges and for the cubic case analyzed in terms of the Kohn-Luttinger effective Hamiltonian. Finally, the optical response functions from direct interband transitions are calculated.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

High harmonic generation governed by edge states in triangular graphene quantum dots

Here, we study theoretically interaction of short optical pulses with triangular graphene quantum dots. If such quantum dots have zigzag edges then there are in-gap degenerate edge states, the number of which depends on the size of the system. We show that the nonlinear optical response, such as high harmonic generation, of triangular quantum dots is sensitive to the initial electron population of their edge states. In general, the emission spectra of quantum dots have weak dependence on the number of occupied edge states, but if half of the edge states are initially occupied, which can be realized only in the quantum dots with even number of edge states, then the even high harmonics are strongly suppressed. The suppression is the strongest when the frequency of the pulse is well below the band gap and it is weak when the pulse frequency becomes comparable to the band gap of the system.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Absence of quantization in the circular photogalvanic effect in disordered chiral Weyl semimetals

The circularly polarized photogalvanic effect (CPGE) is studied in chiral Weyl semimetals with short-range quenched disorder. Without disorder, the topological properties of chiral Weyl semimetals lead to quantization of the CPGE, which is a second-order optical response. Furthermore, using a combination of diagrammatic perturbation theory in the continuum and exact numerical calculations via the kernel polynomial method on a lattice model, we show that disorder perturbatively destabilizes the quantization of the CPGE.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Radial Spin Texture of the Weyl Fermions in Chiral Tellurium

Trigonal tellurium, a small-gap semiconductor with pronounced magneto-electric and magneto-optical responses, is among the simplest realizations of a chiral crystal. We have studied by spin- and angle-resolved photoelectron spectroscopy its unconventional electronic structure and unique spin texture. We identify Kramers-Weyl, composite, and accordionlike Weyl fermions, so far only predicted by theory, and show that the spin polarization is parallel to the wave vector along the lines in k space connecting high-symmetry points. Our results clarify the symmetries that enforce such spin texture in a chiral crystal, thus bringing new insight in the formation of a spin vectorial field more complex than the previously proposed hedgehog configuration. Our findings thus pave the way to a classification scheme for these exotic spin textures and their search in chiral crystals.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2025

Group Conductivity and Nonadiabatic Born Effective Charges of Disordered Metals, Warm Dense Matter, and Hot Dense Plasma

The average ionization state is a critical parameter in plasma models for charged particle transport, equations of state, and optical response. The dynamical or nonadiabatic Born effective charge (NBEC), calculated via first principles time-dependent density-functional theory, provides exact ionic partitioning of bulk electron response for both metallic and insulating materials. The NBEC can be transformed into a “group conductivity,” i.e., the electron conductivity ascribed to a subset of ions. We show that for disordered metallic systems, such as warm dense matter (WDM) and hot dense plasma, the static limit of the NBEC is different from the average ionization states, but that the ionization state can be extracted from the group conductivity even in mixed systems. Here we demonstrate this approach using a set of archetypical examples, including cold and warm aluminium, low- and high-density WDM carbon, and a WDM carbon-beryllium-hydrogen mixture.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Correlating dynamic microstructure to observed color in electrophoretic displays via in situ small-angle x-ray scattering

Electrophoretic deposition (EPD) is an industrially relevant and scalable technique used to form particle deposits from colloidal suspensions. Highly concentrated particle suspensions generally prevent real-time in situ microscopy observations which limit the characterization of EPD films to ex situ, or postprocessed, laboratory techniques. For dynamic systems, such as tunable amorphous photonic crystals (APCs), only reversible deposits are formed during the EPD process. Since reversible deposits cannot be characterized with standard ex situ methods, the particle-particle and particle-field interactions that govern the displayed color and crystallinity of these systems are not well understood. In this paper, we present in situ small-angle x-ray scattering and UV-Vis techniques for measuring both the structural and optical response of an APC under applied electric fields. Furthermore, we also develop a computational model based on colloidal interactions to explain the observed change in the interparticle spacing of APCs due to the applied electric field which correlates to displayed color. Ultimately, this work provides a new in situ characterization method that could be expanded for other dynamic, tunable colloidal systems.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Metamagnetism of few-layer topological antiferromagnets

MnBi 2 Te 4 (MBT) materials are a promising class of antiferromagnetic topological insulators whose films provide access to novel and technologically important topological phases, including quantum anomalous Hall states and axion insulators. MBT device behavior is expected to be sensitive to the various collinear and noncollinear magnetic phases that are accessible in applied magnetic fields. Here, we use classical Monte Carlo simulations and electronic structure models to calculate the ground state magnetic phase diagram as well as topological and optical properties for few-layer films with up to six septuple layers. Using magnetic interaction parameters appropriate for MBT, we find that it is possible to prepare a variety of different magnetic stacking sequences, some of which have sufficient symmetry to disallow nonreciprocal optical response and Hall transport coefficients. Other stacking arrangements do yield large Faraday and Kerr signals, even when the ground state Chern number vanishes.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Semi-Dirac Fermions in a Topological Metal

Topological semimetals with massless Dirac and Weyl fermions represent the forefront of quantum materials research. In two dimensions, a peculiar class of fermions that are massless in one direction and massive in the perpendicular direction was predicted 16 years ago. These highly exotic quasiparticles—the semi-Dirac fermions—ignited intense theoretical and experimental interest but remain undetected. Using magneto-optical spectroscopy, we demonstrate the defining feature of semi-Dirac fermions— B 2 / 3 scaling of Landau levels—in a prototypical nodal-line metal ZrSiS. In topological metals, including ZrSiS, nodal lines extend the band degeneracies from isolated points to lines, loops, or even chains in the momentum space. With calculations and theoretical modeling, we pinpoint the observed semi-Dirac spectrum to the crossing points of nodal lines in ZrSiS. Crossing nodal lines exhibit a continuum absorption spectrum but with singularities that scale as B 2 / 3 at the crossing. Our work sheds light on the hidden quasiparticles emerging from the intricate topology of crossing nodal lines and highlights the potential to explore quantum geometry with linear optical responses. Published by the American Physical Society 2024

Shao, Yinming (ORCID:0000000228910028)↗