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At least 19 records

Broad Distribution of Local Polar States Generates Large Electrothermal Properties in Pb-Free Relaxor Ferroelectrics

Electrothermal energy conversion provides attractive solutions for global energy management, such as energy harvesting from waste heat using pyroelectric energy conversion (PEC) and efficient cooling of portable electronics or data servers using the electrocaloric effect. Relaxor ferroelectrics are attractive for electrothermal energy conversion because of their large pyroelectric coefficients over a wide temperature range. Although Pb-based relaxors are well-known, toxicity concerns have mandated the intense search for Pb-free alternatives. Here, we engineered (Ba,Ca)TiO 3 -based relaxors based on a multisite doping strategy, which show promising electrothermal performance, viz. a maximum PEC efficiency of 14% and electrocaloric refrigeration capacity of 115 J/kg. Using local-scale structural analysis, we provide an atomistic model for large electrothermal properties in the newly designed Pb-free ferroelectrics, whereby a temperature-independent continuous distribution of cation displacement directions creates easy pathways for microscopic polarization reorientation. This research provides key structural insight for future atomic-scale engineering of environmentally sustainable ferroelectrics in energy applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Metasurface‐Based Mueller Matrix Microscope

In conventional optical microscopes, image contrast of objects mainly results from the differences in light intensity and/or color. Muller matrix optical microscopes (MMMs), on the other hand, can provide significantly enhanced image contrast and rich information about objects by analyzing their interactions with polarized light. However, state-of-the-art MMMs are fundamentally limited by bulky and slow polarization state generators and analyzers. Here, the study demonstrates a metasurface-based MMM, i.e., Meta-MMM, which is equipped with a chip-integrated, single-shot metasurface polarization state analyzer (Meta-PSA). The Meta-MMM is featured with high-speed measurement (≈2s per Muller matrix (MM) image), superior operation stability, dual-color operation, and high measurement accuracy (measurement error 1–2%) for MM imaging. The Meta-MMM is applied to nanostructure characterization, surface morphology analysis, and discovering birefringent structures in honeybee wings. As a result, the Meta-MMMs hold the promise to revolutionize various applications from biological imaging, medical diagnosis, and material characterization to industry inspection and space exploration.

36 MATERIALS SCIENCE↗

Polarimetric calibration of the Multi-Angle Imager for Aerosols (MAIA)

NASA’s Multi-Angle Imager for Aerosols (MAIA) mission, under development at the Jet Propulsion Laboratory, is designed to study the adverse health effects of different types of particulate air pollution. Planned for launch in 2023 for a 3-year mission, the MAIA satellite instrument will focus on a selected set of metropolitan target areas, where air quality monitors and health data are available. Aerosol concentration and speciation are inferred from multi-angle measurements of backscattered sunlight in 14 spectral bands from 350-2200 nm, with bands near 442, 645 and 1040 nm measuring the degree (DoLP) and angle of linear polarization (AoLP) in addition to radiance. The pushbroom camera has a ~240-km cross-track field of view with a nadir resolution of ~200 m, and is mounted onto a biaxial gimbal to provide along-track view angles within ±60°, to extend the field of regard to ±48°, and to view the instrument’s onboard calibrator (OBC) and dark target. The OBC consists of a sunlit transmissive diffuser, followed by 12 polarizers at different orientations. MAIA’s polarimetry is implemented using miniature wire grid polarizers on the focal plane array, and dual photoelastic modulators (PEMs) and achromatic quarter-wave plates to rapidly rotate the polarization. The resulting ~26-Hz intensity modulation encodes the linearly polarized and total radiance in each pixel, leaving the DoLP and AoLP insensitive to gain calibration. We report on the polarimetric calibration of the MAIA camera using a vacuum-compatible polarization state generator, consisting of a 1600W Xenon lamp, 12-inch integrating sphere, and rotating high-extinction polarizer. Mueller-matrix-based calibration coefficients for each detector pixel are derived from measurements at multiple polarizer angles, and are used to correct the measurements for instrumental polarization aberrations. Prior to flight, the calibrated MAIA camera is panned across the OBC to characterize its output, using uniform illumination with an irradiance similar to the Sun.

Werne, Thomas↗

Near-circularly polarized isolated attosecond pulse generation from coherent superposition state by a circularly polarized laser field

We theoretically investigate high-order harmonic generation (HHG) from a coherent superposition state of hydrogen atom in a circularly polarized (CP) laser field. The results show that, driven by the CP field, HHG from the coherent superposition state is enhanced by 4 to 5 orders of magnitude compared to that from the ground state. The enhanced intensity is comparable to that of the ground state in a linearly polarized laser field. Based on the classical and quantum analyses, we demonstrate that HHG in the CP laser field mainly arises from the recombination of electrons ionized at non-zero initial positions. The enhancement of HHG from the coherent superposition state is due to the higher ionization rate and also the larger probability density of electrons located far from the nucleus of the involved excited state. The obtained harmonic spectra support the generation of intense isolated attosecond pulses (IAPs) with the ellipticity as high as 0.93. Moreover, we show that the generation of IAPs with large ellipticity is robust against the variation of the carrier envelope phase (CEP) of the laser field. Our results provide a new route toward generating near-CP IAPs, which will be beneficial for ultrafast detection of chiral-sensitive light-matter interactions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Kilohertz generation of high contrast polarization states for visible femtosecond pulses via phase-locked acousto-optic pulse shapers

We present a detailed analysis of a setup capable of arbitrary amplitude, phase, and polarization shaping of broadband visible femtosecond pulses at 1 kHz via a pair of actively phase stabilized acousto-optic programmable dispersive filters arranged in a Mach-Zehnder interferometer geometry. The setup features phase stability values around λ/225 at 580 nm as well as degrees of polarization of at least 0.9 for any polarization state. Both numbers are important metrics to evaluate a setup's potential for applications based on polarization-shaped femtosecond pulses, such as fully coherent multi-dimensional electronic spectroscopy.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Experimental generation of tripartite polarization entangled states of bright optical beams

The multipartite polarization entangled states of bright optical beams directly associating with the spin states of atomic ensembles are one of the essential resources in the future quantum information networks, which can be conveniently utilized to transfer and convert quantum states across a network composed of many atomic nodes. In this letter, we present the experimental demonstration of tripartite polarization entanglement described by Stokes operators of optical field. The tripartite entangled states of light at the frequency resonant with D1 line of Rubidium atoms are transformed into the continuous variable polarization entanglement among three bright optical beams via an optical beam splitter network. The obtained entanglement is confirmed by the extended criterion for polarization entanglement of multipartite quantized optical modes.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Robotic calibration of the motional Stark effect diagnostic on Alcator C-Mod

The capability to calibrate diagnostics, such as the Motional Stark Effect (MSE) diagnostic, without using plasma or beam-into-gas discharges will become increasingly important on next step fusion facilities due to machine availability and operational constraints. A robotic calibration system consisting of a motorized three-axis positioning system and a polarization light source capable of generating arbitrary polarization states with a linear polarization angle accuracy of <0.05° has been constructed and has been used to calibrate the MSE diagnostic deployed on Alcator C-Mod. The polarization response of the complex diagnostic is shown to be fully captured using a Fourier expansion of the detector signals in terms of even harmonics of the input polarization angle. The system's high precision robotic control of position and orientation allow it to be used also to calibrate the geometry of the instrument's view. Combined with careful measurements of the narrow bandpass spectral filters, this system fully calibrates the diagnostic without any plasma discharges. The system's high repeatability, flexibility, and speed has been exploited to quantify several systematics in the MSE diagnostic response, providing a more complete understanding of the diagnostic performance.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Ellipsometry

Ellipsometry is a technique often used to measure the thickness and properties of a thin film. This article covers the instrumental, theoretical, and practical aspects of this technique. Notably, different types of instruments including nulling ellipsometer, rotating compensator ellipsometer, and photoelastic modulator ellipsometer designs are presented. Elements of proper data analysis are also included, such as the use of an error-based figure of merit.

Complex reflection coefficients↗

Manipulating Triplet Yield through Control of Symmetry-Breaking Charge Transfer

The efficiency of an organic solar cell depends on the efficacy of exciton diffusion and dissociation processes, and this can be enhanced by reducing the exciton binding energy and increasing the exciton lifetime. Zinc chlorodipyrrin (ZCl) complexes exhibit reduced exciton binding energy due to ultrafast generation of intramolecular charge transfer (ICT) states via symmetry breaking charge transfer in polar media. This paper explores the fate of the ICT states using nanosecond transient absorption. In cyclohexane, ZCl undergoes intersystem-crossing to produce triplets with ~8 ns time constant (~30% yield) and no ICT states are generated. However, in more polar solvents, triplets are generated within 1 ns via ICT state recombination with ~3 times higher yield than produced via ISC. Furthermore, this high triplet yield in toluene (89%) and acetonitrile (76%) via ICT state recombination is a beneficial pathway to spin-protect the excited state decay for additional charge generation from triplet excited states.

14 SOLAR ENERGY↗

Quantum filter of spin polarized states: Metal–dielectric–ferromagnetic/semiconductor device

Highlights: • Development of a new spintronics device. • Development of quantum spin polarized filters. • Development of theory of quantum spin polarized filter. - Abstract: Recently we proposed a model for the Quantum Spin-Polarized State Filter (QSPSF). The magnetic moments are transported selectively in this model, detached from the electric charge carriers. Thus, transfer of a spin-polarized state between two conductors was predicted in a system of two levels coupled by exchange interaction. The strength of the exchange interaction between the two conductive layers depends on the thickness of the dielectric layer separating them. External magnetic fields modulate spin-polarized state transfer, due to Zeeman level shift. Therefore, a linearly growing magnetic field generates a series of current peaks in a nearby coil. Thus, our spin-state filter should contain as least three nanolayers: (1) conductive or ferromagnetic; (2) dielectric; and (3) conductive or semiconductive. The spectrum of spin-polarized states generated by the filter device consists of a series of resonance peaks. In a simple case the number of lines equals S, the total spin angular momentum of discrete states in one of the coupled nanolayers. Presently we report spin-polarized state transport in metal–dielectric–ferromagnetic (MDF) and metal–dielectric–semiconductor (MDS) three-layer sandwich devices. The exchange-resonance spectra in such devices are quite specific, differing also from spectra observed earlier in other three-layer devices. The theoretical model is used to interpret the available experimental results. A detailed ab initio analysis of the magnetic-field dependence of the output magnetic moment averaged over the surface of the device was carried out. The model predicts the resonance structure of the signal, although at its present accuracy it cannot predict the positions of the spectral peaks.

36 MATERIALS SCIENCE↗

ZnO quantum dot–molecule conjugates: Chemical interactions, charge dynamics, and spin polarization

Conjugates between molecules and quantum dots (QDs) have been explored for a range of potential applications from photocatalysis and photovoltaics to quantum information science technologies. A particularly ubiquitous material in many of these applications are ZnO QDs since they can accept and transport electrons and can also act as hosts for unique spin states. Conjugates between molecular light absorbers and ZnO QDs have been explored for decades as components in dye-sensitized solar cells. Recently, these materials have also attracted interest for their ability to produce spin-polarized states upon photoexcitation. The current paper employs a series of light absorbing perylene molecules with different ZnO QD sizes to explore key features of these QD–molecule conjugates: (1) chemical interactions, (2) charge dynamics, and (3) spin polarization. The chemical interactions between the molecules and QDs are determined with binding equilibria and reveal dramatic impact of ligand size. The charge transfer dynamics from photoexcited perylenes to ZnO QDs were found to depend exponentially on the linker length. Finally, time-resolved electron paramagnetic resonance experiments reveal that these conjugates generate spin-polarized states in the form of radical pairs and triplets. These spin states hold promise as potential qubits and also offer an avenue to efficiently sensitize molecular triplets.

Hernandez, Frida S. [Amherst College, MA (United S↗

Electrical detection of current generated spin in topological insulator surface states: Role of interface resistance

Current generated spin polarization in topological insulator (TI) surface states due to spin-momentum locking has been detected recently using ferromagnet/tunnel barrier contacts, where the projection of the TI spin onto the magnetization of the ferromagnet is measured as a voltage. However, opposing signs of the spin voltage have been reported, which had been tentatively attributed to the coexistence of trivial two-dimensional electron gas states on the TI surface which may exhibit opposite current-induced polarization than that of the TI Dirac surface states. Models based on electrochemical potential have been presented to determine the sign of the spin voltage expected for the TI surface states. However, these models neglect critical experimental parameters which also affect the sign measured. Here we present a Mott two-spin current resistor model which takes into account these parameters such as spin-dependent interface resistances, and show that such inclusion can lead to a crossing of the voltage potential profiles for the spin-up and spin-down electrons within the channel, which can lead to measured spin voltages of either sign. These findings offer a resolution of the ongoing controversy regarding opposite signs of spin signal reported in the literature, and highlight the importance of including realistic experimental parameters in the model.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Direct comparison of current-induced spin polarization in topological insulator Bi2Se3 and InAs Rashba states

Three-dimensional topological insulators (TIs) exhibit time-reversal symmetry protected, linearly dispersing Dirac surface states with spin–momentum locking. Band bending at the TI surface may also lead to coexisting trivial two-dimensional electron gas (2DEG) states with parabolic energy dispersion. A bias current is expected to generate spin polarization in both systems, although with different magnitude and sign. Here we compare spin potentiometric measurements of bias current-generated spin polarization in Bi2Se3(111) where Dirac surface states coexist with trivial 2DEG states, and in InAs(001) where only trivial 2DEG states are present. We observe spin polarization arising from spin–momentum locking in both cases, with opposite signs of the measured spin voltage. We present a model based on spin dependent electrochemical potentials to directly derive the sign expected for the Dirac surface states, and show that the dominant contribution to the current-generated spin polarization in the TI is from the Dirac surface states.

36 MATERIALS SCIENCE↗

Spin selective charge recombination in chiral donor-bridge-acceptor triads

In this paper, we outline a physically motivated framework for describing spin-selective recombination processes in chiral systems, from which we derive spin-selective reaction operators for recombination reactions of donor–bridge–acceptor molecules, where the electron transfer is mediated by chirality and spin–orbit coupling. In general, the recombination process is selective only for spin-coherence between singlet and triplet states, and it is not, in general, selective for spin polarization. We find that spin polarization selectivity only arises in hopping-mediated electron transfer. We describe how this effective spin-polarization selectivity is a consequence of spin-polarization generated transiently in the intermediate state. Furthermore, the recombination process also augments the coherent spin dynamics of the charge separated state, which is found to have a significant effect on the recombination dynamics and to destroy any long-lived spin polarization. Although we only consider a simple donor–bridge–acceptor system, the framework we present here can be straightforwardly extended to describe spin-selective recombination processes in more complex systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

FREQUENCY DEPENDENCE OF POLARIZATION OF ZEBRA PATTERN IN TYPE-IV SOLAR RADIO BURSTS

We investigated the polarization characteristics of a zebra pattern (ZP) in a type-IV solar radio burst observed with AMATERAS on 2011 June 21 for the purpose of evaluating the generation processes of ZPs. Analyzing highly resolved spectral and polarization data revealed the frequency dependence of the degree of circular polarization and the delay between two polarized components for the first time. The degree of circular polarization was 50%–70% right-handed and it varied little as a function of frequency. Cross-correlation analysis determined that the left-handed circularly polarized component was delayed by 50–70 ms relative to the right-handed component over the entire frequency range of the ZP and this delay increased with the frequency. We examined the obtained polarization characteristics by using pre-existing ZP models and concluded that the ZP was generated by the double-plasma-resonance process. Our results suggest that the ZP emission was originally generated in a completely polarized state in the O-mode and was partly converted into the X-mode near the source. Subsequently, the difference between the group velocities of the O-mode and X-mode caused the temporal delay.

79 ASTRONOMY AND ASTROPHYSICS↗

Bell-State Bootstrapping via Spot-Checking

We present a spot-checking method to monitor and mitigate errors in imperfect entangled photon sources from semi-trusted third parties. We demonstrate that our method effectively mitigates polarization drifts and yields high-fidelity polarization-entangled Bell-state generation.

Zhang, Yanbao [ORNL] (ORCID:0000000245530561)↗

Lidar Electro-Optic Beam Switch with a Liquid Crystal Variable Retarder

A document discusses a liquid crystal variable retarder, an electro-optic element that changes the polarization of an optical beam in response to a low-voltage electronic signal. This device can be fabricated so that the element creates, among other states, a half-wave of retardance that can be reduced to a very small retardance. When aligned to a polarized source, this can act to rotate the polarization by 90 in one state, but generate no rotation in the other state. If the beam is then incident on a polarization beam splitter, it will efficiently switch from one path to the other when the voltage is applied. The laser beam switching system has no moving parts, improving reliability over mechanical switching. It is low cost, tolerant of high laser power density, and needs only simple drive electronics, minimizing the required system resources.

Baer, James↗

Quantum Pair Generation in Nonlinear Metasurfaces with Mixed and Pure Photon Polarizations

Metasurfaces are highly effective at manipulating classical light in the linear regime; however, effectively controlling the polarization of nonclassical light generated from nonlinear resonant metasurfaces remains a challenge. Here, in this study, we present a solution by achieving polarization engineering of frequency-nondegenerate biphotons emitted via spontaneous parametric down-conversion in GaAs metasurfaces, utilizing quasi-bound states in the continuum (qBIC) resonances to enhance biphoton generation. Through comprehensive polarization tomography, we demonstrate that the emitted photons’ polarization directly reflects the qBIC mode’s far-field properties. Furthermore, we show that both the type of qBIC mode and the symmetry of the meta-atoms can be tailored to control each single-photon polarization state, and that the subsequent two-photon polarization states are nearly separable, offering potential applications in the heralded generation of single photons with adjustable polarization. This work provides a significant step toward utilizing metasurfaces to generate quantum light and engineer their polarization, a critical aspect for future quantum technologies.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗