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DOE OSTI2025

Crystal Growth of Quaternary Rare Earth Selenosilicates by Using the Flux-Assisted Boron Chalcogen Mixture Method: Investigation of Their Magnetic and Optical Properties

A series of rare earth magnesium selenosilicates, RE3Mg 0.5 SiSe 7 (RE = Ce, Pr, Nd, Sm, Gd, Tb, Dy) were obtained as single crystal using the flux assisted boron chalcogen mixture (BCM) method. The structures of the crystals were determined by single-crystal X-ray diffraction. The RE3Mg 0.5 SiSe 7 series crystallizes in the hexagonal crystal system in the space group P6 3 . Polycrystalline powders were synthesized to perform physical property measurements. Magnetic measurements over the 2–300 K temperature range reveal that Ce 3 Mg 0.5 SiSe 7 and Gd 3 Mg 0.5 SiSe 7 exhibit paramagnetic behavior with negative Weiss constants (θ W = −14.50, θ W = −6.13 K, respectively). The optical properties of RE 3 Mg 0.5 SiSe 7 (RE = Ce, Pr, Nd, Sm, Gd) were measured by ultraviolet–visible (UV–vis) diffuse reflectance. Density functional theory (DFT) electronic structure calculations were performed. Furthermore, a second harmonic generation measurement was performed on a polycrystalline powder of Ce 3 Mg 0.5 SiSe 7 and was found to be SHG active with an efficiency of 0.11 times the standard potassium dihydrogen phosphate (KDP).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Room-Temperature Ferroelectric LiNb 6 Ba 5 Ti 4 O 30 Spinel Phase in a Nanocomposite Thin Film Form for Nonlinear Photonics

Tetragonal tungsten bronze (TTB) materials are one of the most promising classes of materials for ferroelectric and nonlinear optical devices, owing to their very unique noncentrosymmetric crystal structure. In this work, a new TTB phase of LiNb 6 Ba 5 Ti 4 O 30 (LNBTO) has been discovered and studied. A small amount of a secondary phase, LiTiO 2 (LTO), has been incorporated as nanopillars that are vertically embedded in the LNBTO matrix. The new multifunctional nanocomposite thin film presents exotic highly anisotropic microstructure and properties, e.g., strong ferroelectricity, high optical transparency, anisotropic dielectric function, and strong optical nonlinearity evidenced by the second harmonic generation results. An optical waveguide structure based on the stacks of α-Si on SiO 2 /LNBTO–LTO has been fabricated, exhibiting low optical dispersion with an optimized evanescent field staying in the LNBTO–LTO active layer. Lastly, this work highlights the combination of new TTB material designs and vertically aligned nanocomposite structures for further enhanced anisotropic and nonlinear properties.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Roses in the nonperturbative current response of artificial crystals

In two-dimensional artificial crystals with large real-space periodicity, the nonlinear current response to a large applied electric field can feature a strong angular dependence, which encodes information about the band dispersion and Berry curvature of isolated electronic Bloch minibands. Within the relaxation-time approximation, we obtain analytic expressions up to infinite order in the driving field for the current in a band-projected theory with time-reversal and trigonal symmetry. For a fixed field strength, the dependence of the current on the direction of the applied field is given by rose curves whose petal structure is symmetry constrained and is obtained from an expansion in real-space translation vectors. We illustrate our theory with calculations on periodically buckled graphene and twisted double bilayer graphene, wherein the discussed physics can be accessed at experimentally relevant field strengths.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Smooth periodic gauge satisfying crystal symmetry and periodicity to study high-harmonic generation in solids

Intense lasers can easily drive nonadiabatic transitions of excited electron wave packets across the Brillouin zones, thus transition dipole moments (TDM) between energy bands of solids should be continuous, satisfying crystal symmetry, and periodic at zone boundaries. While current ab initio algorithms are powerful in calculating band structures of solids, they all introduced random phases into the eigenfunctions at each crystal momentum k. In this work, we show how to choose a “smooth-periodic” gauge where TDMs can be smooth versus k, preserving crystal symmetry, as well as maintaining periodic at boundaries. The symmetry properties of TDMs with respect to k ensure the absence of even-order harmonics from MgO with inversion symmetry, while the TDM in the “smooth-periodic” gauge for broken-symmetry ZnO is responsible for even harmonics that were underestimated in previous simulations. These results reveal the importance of correctly treating the complex TDMs that satisfy crystal symmetry and continuous across zone boundaries in nonlinear laser-solid interactions, which has been elusive in most theories so far.

36 MATERIALS SCIENCE↗

NASA NTRS1988

Effect of surface tension anisotropy on cellular morphologies

A three-dimensional weakly nonlinear analysis for conditions near the onset of instability at the crystal-melt interface was carried out to second order, taking into account the effects of latent heat generation and surface-tension anisotropy of the crystal-melt interface; particular consideration was given to the growth of a cubic crystal in the 001-, 011-, and 111-line directions. Numerical calculations by McFadden et al. (1987), performed for an aluminum-chromium alloy with the assumption of a linear temperature field and an isotropic surface tension, showed that only hexagonal nodes (and not hexagonal cells) occurred near the onset of instability. The results of the present analysis indicate that the nonlinear temperature field (which occurs when thermal conductivities of the crystal and the melt are different and/or the latent heat effects are not negligible) can modify this result and, for certain alloys and processing conditions, can cause the occurrence of hexagonal cells near the onset of instability.

Mcfadden, G. B.↗

NASA NTRS1989

Recent advances in engineering science; Proceedings of the A. Cemal Eringen Symposium, University of California, Berkeley, June 20-22, 1988

Various papers on recent advances in engineering science are presented. Some individual topics addressed include: advances in adaptive methods in computational fluid mechanics, mixtures of two medicomorphic materials, computer tests of rubber elasticity, shear bands in isotropic micropolar elastic materials, nonlinear surface wave and resonator effects in magnetostrictive crystals, simulation of electrically enhanced fibrous filtration, plasticity theory of granular materials, dynamics of viscoelastic media with internal oscillators, postcritical behavior of a cantilever bar, boundary value problems in nonlocal elasticity, stability of flexible structures with random parameters, electromagnetic tornadoes in earth's ionosphere and magnetosphere, helicity fluctuations and the energy cascade in turbulence, mechanics of interfacial zones in bonded materials, propagation of a normal shock in a varying area duct, analytical mechanics of fracture and fatigue.

Koh, Severino L.↗

NASA NTRS1996

Two-Photon Ghost Image and Interference-Diffraction

One of the most surprising consequences of quantum mechanics is entanglement of two or more distance particles. The two-particle entangled state was mathematically formulated by Schrodinger. Based on this unusual quantum behavior, EPR defined their 'physical reality' and then asked the question: 'Can Quantum-Mechanical Description of Physical Reality Be Considered Complete?' One may not appreciate EPR's criterion of physical reality and insist that 'no elementary quantum phenomenon is a phenomenon until it is a recorded phenomenon'. Optical spontaneous parametric down conversion (SPDC) is the most effective mechanism to generate an EPR type entangled two-photon state. In SPDC, an optical beam, called the pump, is incident on a birefringent crystal. The pump is intense enough so that nonlinear effects lead to the conversion of pump photons into pairs of photons, historically called signal and idler. Technically, the SPDC is said to be type-1 or type-2, depending on whether the signal and idler beams have parallel or orthogonal polarization. The SPDC conversion efficiency is typically on the order of 10(exp -9) to 10(exp -11), depending on the SPDC nonlinear material. The signal and idler intensities are extremely low, only single photon detection devices can register them. The quantum entanglement nature of SPDC has been demonstrated in EPR-Bohm experiments and Bell's inequality measurements. The following two experiments were recently performed in our laboratory, which are more closely related to the original 1935 EPR gedankenezperiment. The first experiment is a two-photon optical imaging type experiment, which has been named 'ghost image' by the physics community. The signal and idler beams of SPDC are sent in different directions, so that the detection of the signal and idler photons can be performed by two distant photon counting detectors. An aperture object (mask) is placed in front of the signal photon detector and illuminated by the signal beam through a convex lens. Surprisingly, an image of this aperture is observed in the idler beam, by scanning the idler photon detector in the transverse plane of the idler beam, if we are sure that the idler photon detector 'catches' the 'twin brother' of the signal, which can be easily performed by a coincidence measurement. This effect is even more striking when we found that the object-lens-image relationship satisfies the Gaussian thin lens equation. The second experiment demonstrates two-photon 'ghost' interference-diffraction. The experimental set up is similar to the image experiment, except that rather than a lens and an aperture it is a Young's double-slit (or a single-slit) inserted into the path of the signal beam. We could not find any interference (or diffraction) pattern behind the slit. Surprisingly, an interference (or diffraction) pattern is observed when scanning the detector in the idler beam, if we are sure that the idler photon detector 'catches' the 'twin brother' of the signal.

Shih, Y. H.↗

DOE OSTI2022

Cascaded Optical Nonlinearities in Dielectric Metasurfaces

Since the discovery of the laser, optical nonlinearities have been at the core of efficient light conversion sources. Typically, thick transparent crystals or quasi-phase matched waveguides are utilized in conjunction with phase-matching techniques to select a single parametric process. In recent years, due to the rapid developments in artificially structured materials, optical frequency mixing has been achieved at the nanoscale in subwavelength resonators arrayed as metasurfaces. Phase matching becomes relaxed for these wavelength-scale structures, and all allowed nonlinear processes can, in principle, occur on an equal footing. This could promote harmonic generation via a cascaded (consisting of several frequency mixing steps) process. However, so far, all reported work on dielectric metasurfaces have assumed frequency mixing from a direct (single step) nonlinear process. In this work, we prove the existence of cascaded second-order optical nonlinearities by analyzing the second- and third-wave mixing from a highly nonlinear metasurface in conjunction with polarization selection rules and crystal symmetries. We find that the third-wave mixing signal from a cascaded process can be of comparable strength to that from conventional third-harmonic generation and that surface nonlinearities are the dominant mechanism that contributes to cascaded second-order nonlinearities in our metasurface.

36 MATERIALS SCIENCE↗

DOE OSTI2026

A Compact Monolithic Electro-Optic Package for Quantum Microwave-to-Optical Transduction

We present a novel quantum transduction package that integrates a macroscopic electro-optic crystal into a compact, monolithic assembly designed for superconducting quantum processors. The device provides an efficient and scalable interface between microwave and optical domains while preserving cryogenic compatibility. We performed full-wave and quantum dynamical simulations to assess the performance of the hybrid system, focusing on the interaction between a transmon-based microwave cavity and the crystal’s and cavity low-frequency microwave mode. The transmon operates both as an ancilla for the QPU and as a nonlinear element enabling four-wave mixing between cavity and electro-optic crystal microwave fields. Our results indicate that this architecture can coherently mediate quantum information transfer from the cavity to the electro-optic mode, offering a promising platform for on-chip quantum transduction within superconducting quantum networks.

Reineri, Alessandro [Fermilab] (ORCID:000000016175↗

DOE OSTI2026

A Compact Monolithic Electro-Optic Package for Quantum Microwave-to-Optical Transduction

Reineri, Alessandro [Fermilab] (ORCID:000000016175↗

DOE OSTI2022

Multifunctional Cu 2 TSiS 4 (T = Mn and Fe): Polar Semiconducting Antiferromagnets with Nonlinear Optical Properties

In this work, Cu 2 TSiS 4 (T = Mn and Fe) polycrystalline and single-crystal materials were prepared with high-temperature solid-state and chemical vapor transport methods, respectively. The polar crystal structure (space group Pmn2 1 ) consists of chains of corner-sharing and distorted CuS 4 , Mn/FeS 4 , and SiS 4 tetrahedra, which is confirmed by Rietveld refinement using neutron powder diffraction data, X-ray single-crystal refinement, electron diffraction, energy-dispersive X-ray spectroscopy, and second harmonic generation (SHG) techniques. Magnetic measurements indicate that both compounds order antiferromagnetically at 8 and 14 K, respectively, which is supported by the temperature-dependent (100–2 K) neutron powder diffraction data. Additional magnetic reflections observed at 2 K can be modeled by magnetic propagation vectors k = (1/2,0,1/2) and k = (1/2,1/2,1/2) for Cu 2 MnSiS 4 and Cu 2 FeSiS 4 , respectively. The refined antiferromagnetic structure reveals that the Mn/Fe spins are canted away from the ac plane by about 14°, with the total magnetic moments of Mn and Fe being 4.1(1) and 2.9(1) μ B , respectively. Both compounds exhibit an SHG response with relatively modest second-order nonlinear susceptibilities. Density functional theory calculations are used to describe the electronic band structures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1974

Unique properties of SBN and their use in a layered optical memory

Holographic storage experiments using crystal Sr(0.75)Ba(0.25)Nb2O6 (SBN 75/25) as a volume-phase holographic medium show that this material is the most sensitive crystalline storage medium yet discovered. An exposure level of 0.003 J/sq cm at 0.488 micron produces a 1% diffraction efficiency in a 5-mm length of crystal. In addition to high recording sensitivity, SBN 75/25 exhibits interesting electric-field induced effects that include electric-field enhanced recording sensitivity and voltage-switchable latent-to-active holographic reconstruction efficiency. These effects are explained in terms of drift and diffusion of photoionized carriers coupled with the nonlinear electrooptic behavior characteristic of this low Curie temperature ferroelectric crystal. A mechanism is proposed that correlates the observed electrically controlled holographic response with the dielectric behavior of the crystal. These interesting effects are used to implement a novel, layered optical memory having no moving parts and having electrical access for writing or reading selected layers.

Thaxter, J. B.↗

NASA NTRS1990

Generating Second Harmonics In Nonlinear Resonant Cavities

Single-axial-mode lasers pump very-low-loss doubling crystals. Important advance in making resonant generation of second harmonics possible for diode-laser-pumped solid-state lasers is recent development of monolithic nonplanar ring geometries in neodymium:yttrium aluminum garnet (Nd:YAG) lasers that produce frequency-stable single-mode outputs. Other advance is development of high-quality MgO:LiNbO3 as electro-optically nonlinear material. Series of experiments devised to improve doubling efficiency of low-power lasers, and particularly of diode-laser-pumped continuous-wave Nd:YAG lasers.

Kozlovsky, William J.↗

DOE OSTI2022

Cubic Crystal Structure Formation and Optical Properties within the Ag–B II –M IV –X (B II = Sr, Pb; M IV = Si, Ge, Sn; X = S, Se) Family of Semiconductors

Quaternary chalcogenide semiconductors are promising materials for energy conversion and nonlinear optical applications, with properties tunable primarily by varying the elemental composition and crystal structure. Here, we first analyze the connections among several cubic crystal structure types, as well as the orthorhombic Ag 2 PbGeS 4 -type structure, reported for select members within the Ag–B II –M IV –X (B II = Sr, Pb; M IV = Si, Ge, Sn; X = S, Se) compositional space. Focusing on the Ag–Pb–Si–S and Ag–Sr–Sn–S systems, we show that one structure type, with the formulas Ag 2 Pb 3 Si 2 S 8 and Ag 2 Sr 3 Sn 2 S 8 , is favored. We have prepared powder and single-crystal samples of Ag 2 Pb 3 Si 2 S 8 and Ag 2 Sr 3 Sn 2 S 8 , showing that each takes on the noncentrosymmetric cubic space group I$\bar{43}$d and is isostructural to the previously reported compound Ag 2 Sr 3 Ge 2 Se 8 . Through hybrid density functional theory calculations, these cubic compounds are demonstrated to be (quasi-)direct band gap semiconductors with high densities of states at the band maxima. Furthermore, the band-gap energies are measured by reflectance spectroscopy as 1.95(3) and 2.66(4) eV for Ag 2 Pb 3 Si 2 S 8 and Ag 2 Sr 3 Sn 2 S 8 , respectively. We further measure the optical properties and show the electronic band structures of three other isostructural A I –B II –M IV –X-type materials, i.e., Ag 2 Sr 3 Si 2 S 8 , Ag 2 Sr 3 Ge 2 S 8 , and Ag 2 Sr 3 Ge 2 Se 8 , showing that the band gaps can be predictably tuned by element substitution. Detailed visual analyses of the different structures and of their relationships with other members of the Ag–B II –M IV –X compositional family provide a basis for a broader understanding of the structure formation and optoelectronic properties within the quaternary chalcogenide semiconductor family.

14 SOLAR ENERGY↗

DOE OSTI2024

Intercalation-Induced Topotactic Phase Transformation of Tungsten Disulfide Crystals

Recent research has demonstrated the potential for topological superconductivity, anisotropic Majorana bound states, optical nonlinearity, and enhanced electrochemical activity for transition metal dichalcogenides (TMDs) with a 2M structure. These unique TMD compounds exhibit metastability and, upon heating, undergo a transition to the thermodynamically stable 2H phase. The 2M phase is commonly made at high temperatures using traditional solid-state methods, and this metastability further complicates the growth of large 2M WS 2 crystals. Herein, a novel synthetic method was developed, focusing on a molten salt reaction to synthesize large 2H crystals and then inducing transformation to the 2M phase through intercalation and thermal treatment. The 2H crystals were intercalated via a room-temperature sodium naphthalenide solution, producing a previously unreported Na-intercalated 2H WS 2 phase. Thermal heating was required to facilitate the phase transition to the intercalated 2M crystal structure. This phase transition was studied by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), selected area electron diffraction (SAED), electron dispersive X-ray spectroscopy (EDS), and Raman spectroscopy, which confirmed the synthesis of the intercalated 2M phase. Upon deintercalation, crystal and powder samples showed superconductivity with a T c of 8.6–8.7 K, similar to previously reported values. The generality of this process was further demonstrated using alkali metal triethyl borohydride to intercalate 2H WS 2 and produced the desired 2M phase. This novel synthetic method has broad implications for discovering metastable phases in other TMD families and layered materials. Furthermore, separation of the intercalation and phase transition also has the potential to allow for large-scale synthesis of this technologically important phase with greater control over each step of the reaction.

36 MATERIALS SCIENCE↗

DOE OSTI2020

An interface-controlled Mott memristor in α -RuCl 3

Memristor devices have history-dependent charge transport properties that are ideal for neuromorphic computing applications. We reveal a memristor material and mechanism in the layered Mott insulator α-RuCl 3 . The pinched hysteresis loops and S-shaped negative differential resistance in bulk crystals verify memristor behavior and are attributed to a nonlinear coupling between charge injection over a Schottky barrier at the electrical contacts and concurrent Joule heating. Direct simulations of this coupling can reproduce the device characteristics.

Physics↗

DOE OSTI2022

Fragmentation of faceted crystalline wires

The reduction of surface energy is a well-known driving force for the fragmentation of nanowires. Fragmentation can limit the service life of those small low-dimensional building blocks or can be controlled to induce beneficial shape changes. For isotropic surface energy, fragmentation is analogous to the classic Rayleigh-Plateau instability of liquid jets. However, commonly synthesized crystalline nanowires have strongly anisotropic surface energies and exhibit facets coinciding with cusps in the Wulff plot. Depending on growth orientation, different fragmentation behaviors have been seen in nanowires. Using phase-field simulations, we show that fragmentation of faceted nanowires with cubic crystal symmetry may occur by a finite-amplitude nonlinear instability, as opposed to a Rayleigh-Plateau-like linear instability, depending on nanowire growth orientation. Here, we carry out a weakly nonlinear analysis based on sharp interface theory to characterize the faceted nanowire shape corresponding to a surface-energy saddle point. The analysis predicts that the minimum amplitude of a periodic shape perturbation to trigger fragmentation increases with cusp strength but decreases inversely proportionally to the perturbation wavelength for long wavelengths, in good quantitative agreement with phase-field predictions. The results provide the theoretical foundation to predict nanowire stability as a function of length and surface energy in diverse applications.

36 MATERIALS SCIENCE↗

NASA NTRS1995

Second Annual Research Center for Optical Physics (RCOP) Forum

The Research Center for Optical Physics (RCOP) held its Second Annual Forum on September 23-24, 1994. The forum consisted of two days of technical sessions with invited talks, submitted talks, and a student poster session. Participants in the technical sessions included students and researchers from CCNY/CUNY, Fisk University, Georgia Institute of Technology, Hampton University, University of Maryland, the Univeristy of Michigan, NASA Langley Research Center, North Caroline A and T University, Steven's Institute of Technology, and NAWC-Warminster. Topics included chaotic lasers, pumped optical filters, nonlinear responses in polythiophene and thiophene based thin films, crystal growth and spectroscopy, laser-induced photochromic centers, raman scattering in phorphyrin, superradiance, doped fluoride crystals, luminescence of terbium in silicate glass, and radiative and nonradiative transitions in rare-earth ions.

Allario, Frank↗