Terahertz chiral metamaterials with giant and dynamically tunable optical activity
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Zhou, Jiangfeng↗
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Midgap state requirements for optically active quantum defects
Abstract Optically active quantum defects play an important role in quantum sensing, computing and communication. The electronic structure and the single-particle energy levels of these quantum defects in the semiconducting host have been used to understand their optoelectronic properties. Optical excitations that are central for their initialization and readout are linked to transitions between occupied and unoccupied single-particle states. It is commonly assumed that only quantum defects introducing levels well within the band gap and far from the band edges are of interest for quantum technologies as they mimic an isolated atom embedded in the host. In this perspective, we contradict this common assumption and show that optically active defects with energy levels close to the band edges can display similar properties. We highlight quantum defects that are excited through transitions to or from a band-like level (bound exciton) such as the T center and Se S i + in silicon. We also present how defects such as the silicon split-vacancy in diamond can involve transitions between localized levels that are above the conduction band or below the valence band. Loosening the commonly assumed requirement on the electronic structure of quantum defects offers opportunities in quantum defects design and discovery especially in smaller band gap hosts such as silicon. We discuss the challenges in terms of operating temperature for photoluminescence or radiative lifetime in this regime. We also highlight how these alternative type of defects bring their own needs in terms of theoretical developments and fundamental understanding. This perspective clarifies the electronic structure requirement for quantum defects and will facilitate the identification and design of new color centers for quantum applications especially driven by first principles computations.
Xiong, Yihuang (ORCID:0000000178096047)↗
Energetic Performance of Optically Activated Aluminum/Graphene Oxide Composites
Optical ignition of solid energetic materials, which can rapidly release heat, gas, and thrust, is still challenging due to the limited light absorption and high ignition energy of typical energetic materials ( e.g., aluminum, Al). Here, we demonstrated that the optical ignition and combustion properties of micron-sized Al particles were greatly enhanced by adding only 20 wt % of graphene oxide (GO). These enhancements are attributed to the optically activated disproportionation and oxidation reactions of GO, which release heat to initiate the oxidization of Al by air and generate gaseous products to reduce the agglomeration of the composites and promote the pressure rise during combustion. More importantly, compared to conventional additives such as metal oxides nanoparticles ( e.g., WO 3 and Bi 2 O 3 ), GO has much lower density and therefore could improve energetic properties without sacrificing Al content. Finally, the results from Xe flash ignition and laser-based excitation experiments demonstrate that GO is an efficient additive to improve the energetic performance of micron-sized Al particles, enabling micron-sized Al to be ignited by optical activation and promoting the combustion of Al in air.
36 MATERIALS SCIENCE↗
High-resolution, active-optic X-ray fluorescence analyzer
Active optics apparatus and method for aligning active optics are provided for a high-resolution, active optic fluorescence analyzer combining a large acceptance solid angle with wide energy tunability. A plurality of rows of correctors selectively controlled to bend an elongated strip of single crystal material like Si (400) into substantially any precisely defined shape. A pair of pushers engages opposite ends of the silicon crystal strip exert only a force along the long axis of the crystal strip, and does not induce additional bending moments which would result in a torsion of the crystal.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Optically active substituted polyacetylene@carbon nanotube hybrids: Preparation, characterization and infrared emissivity property study
Optically active substituted polyacetylene@multiwalled carbon nanotubes (SPA@MWCNTs) nanohybrids were fabricated by wrapping helical SPA copolymers onto the surface of modified nanotubes through ester bonding linkage. SPA copolymer based on chiral phenylalanine and serine was pre-polymerized by a rhodium zwitterion catalyst in THF, and evidently proved to possess strong optical activity and adopt a predominately one-handed helical conformation. Various characterizations including Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), and transmission electron microscopy (TEM) demonstrated that the SPA had been covalently grafted onto the nanotubes without destroying their original graphite structure. The wrapped SPA was found to exhibit an enhancement in thermal stability and still maintained considerable optical activity after grafting. The infrared emissivity property of the nanohybrids at 8–14 μm was investigated in addition. The results indicated that the SPA@MWCNTs hybrid matrix could possess a much lower infrared emissivity value (ε=0.707) than raw MWCNTs, which might be due to synergistic effect of the unique helical conformation of optically active SPA and strengthened interfacial interaction between the organic polymers and inorganic nanoparticles. - Graphical abstract: Optically active SPA@MWCNTs nanohybrids with low infrared emissivity. - Highlights: • Synthesis of optically active SPA copolymer derived from serine and phenylalanine. • Preparation and characterization of optically active SPA@MWCNTs nanohybrids. • Application study of the SPA@MWCNTs nanohybrids (ε=0.707) in lowering the infrared emissivity.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Preparation, characterization, and infrared emissivity property of optically active polyurethane/TiO{sub 2}/SiO{sub 2} multilayered microspheres
Optically active polyurethane/titania/silica (LPU/TiO{sub 2}/SiO{sub 2}) multilayered core-shell composite microspheres were prepared by the combination of titania deposition on the surface of silica spheres and subsequent polymer grafting. LPU/TiO{sub 2}/SiO{sub 2} was characterized by FT-IR, UV-vis spectroscopy, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), thermogravimetric analysis (TGA), SEM and TEM, and the infrared emissivity value (8-14 {mu}m) was investigated in addition. The results indicated that titania and polyurethane had been successfully coated onto the surfaces of silica microspheres. LPU/TiO{sub 2}/SiO{sub 2} exhibited clearly multilayered core-shell construction. The infrared emissivity values reduced along with the increase of covering layers thus proved that the interfacial interactions had direct influence on the infrared emissivity. Besides, LPU/TiO{sub 2}/SiO{sub 2} multilayered microspheres based on the optically active polyurethane took advantages of the orderly secondary structure and strengthened interfacial synergistic actions. Consequently, it possessed the lowest infrared emissivity value. - Graphical Abstract: Optically active polyurethane/titania/silica (LPU/TiO{sub 2}/SiO{sub 2}) multilayered core-shell composite microspheres were prepared by the combination of titania deposition on the surface of silica spheres and subsequent polymer grafting. Highlights: > Optically active polyurethane based on tyrosine was used for the modification of nanoparticles. > LPU/TiO{sub 2}/SiO{sub 2} multilayered core-shell microspheres were prepared and characterized. > Interfacial interactions and secondary structure affected the infrared emissivity of composite.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Optical activity of chirally distorted nanocrystals
We develop a general theory of optical activity of semiconductor nanocrystals whose chirality is induced by a small perturbation of their otherwise achiral electronic subsystems. The optical activity is described using the quantum-mechanical expressions for the rotatory strengths and dissymmetry factors introduced by Rosenfeld. We show that the rotatory strengths of optically active transitions are decomposed on electric dipole and magnetic dipole contributions, which correspond to the electric dipole and magnetic dipole transitions between the unperturbed quantum states. Remarkably, while the two kinds of rotatory strengths are of the same order of magnitude, the corresponding dissymmetry factors can differ by a factor of 10{sup 5}. By maximizing the dissymmetry of magnetic dipole absorption one can significantly enhance the enantioselectivity in the interaction of semiconductor nanocrystals with circularly polarized light. This feature may advance chiral and analytical methods, which will benefit biophysics, chemistry, and pharmaceutical science. The developed theory is illustrated by an example of intraband transitions inside a semiconductor nanocuboid, whose rotatory strengths and dissymmetry factors are calculated analytically.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Optical activity and defect/dopant evolution in ZnO implanted with Er
The effects of annealing on the optical properties and defect/dopant evolution in wurtzite (0001) ZnO single crystals implanted with Er ions are studied using a combination of Rutherford backscattering/channeling spectrometry and photoluminescence measurements. The results suggest a lattice recovery behavior dependent on ion dose and involving formation/evolution of an anomalous multipeak defect distribution, thermal stability of optically active Er complexes, and Er outdiffusion. An intermediate defect band occurring between the surface and ion-induced defects in the bulk is stable up to 900 °C and has a photoluminescence signature around 420 nm well corresponding to Zn interstitials. The optical activity of the Er atoms reaches a maximum after annealing at 700 °C but is not directly associated to the ideal Zn site configuration, since the Er substitutional fraction is maximal already in the as-implanted state. In its turn, annealing at temperatures above 700 °C leads to dissociation of the optically active Er complexes with subsequent outdiffusion of Er accompanied by the efficient lattice recovery.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Optical activity of solids from first principles
Within the framework of independent particle approximation, the optical activity tensor of solids is formulated as from different contributions: the magnetic dipole, electric quadrupole, and band dispersion terms. The first two terms have similar counterparts in the theory of finite systems, whereas the last term is unique for crystals. Further, the magnetic dipole and electric quadrupole transition moments are calculated with a sum-over-states formulation. We apply the formulation to calculate and analyze the optical rotation of elemental tellurium and the circular dichroism of the (6,4) carbon nanotube. Decomposed optical activity into different contributions is discussed. The calculated spectra agree well with experiments. As a showcase of achiral crystals, we calculate the optical activity of wurtzite GaN.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Entangling unstable optically active matter qubits
In distributed quantum computation, small devices composed of a single or a few qubits are networked together to achieve a scalable machine. Typically, there is an optically active matter qubit at each node, so that photons are exploited to achieve remote entanglement. However, in many systems the optically active states are unstable or poorly defined. We report a scheme to perform a high-fidelity entanglement operation even given severe instability. The protocol exploits the existence of optically excited states for phase acquisition without actually exciting those states; it functions with or without cavities and does not require number-resolving detectors.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Complementary chiral metasurface with strong broadband optical activity and enhanced transmission
We present the design and realization of ultra-thin chiral metasurfaces with giant broadband optical activity in the infrared wavelength. The chiral metasurfaces consisting of periodic hole arrays of complementary asymmetric split ring resonators are fabricated by femtosecond laser two-photon polymerization. Enhanced transmission with strong polarization conversion up to 97% is observed owing to the chiral surface plasmons resulting from mirror symmetry broken. The dependence of optical activity on the degree of structural asymmetry is investigated. This simple planar metasurface is expected to be useful for designing ultra-thin active devices and tailoring the polarization behavior of complex metallic nanostructures.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Organometallic complexes of bulky, optically active, C 3 -symmetric tris(4 S -isopropyl-5,5-dimethyl-2-oxazolinyl)phenylborate (To P *)
A bulky, optically active monoanionic scorpionate ligand, tris(4S-isopropyl-5,5-dimethyl-2-oxazolinyl)phenylborate (To P* ), is synthesized from the naturally occurring amino acid l-valine as its lithium salt, Li[To P* ] (1). That compound is readily converted to the thallium complex Tl[To P* ] (2) and to the acid derivative H[To P* ] (3). Group 7 tricarbonyl complexes To P* M(CO) 3 (M = Mn (4), Re (5)) are synthesized by the reaction of MBr(CO) 5 and Li[To P* ] and are crystallographically characterized. The ν CO bands in their infrared spectra indicate that π back-donation in the rhenium compounds is greater with To P* than with non-methylated tris(4S-isopropyl-2-oxazolinyl)phenylborate (To P ). The reaction of H[To P* ] and ZnEt 2 gives To P* ZnEt (6), while To P* ZnCl (7) is synthesized from Li[To P* ] and ZnCl 2 . The reaction of To P* ZnCl and KOtBu followed by addition of PhSiH 3 provides the zinc hydride complex To P* ZnH (8). In this study, compound 8 is the first example of a crystallographically characterized optically active zinc hydride. We tested its catalytic reactivity in the cross-dehydrocoupling of silanes and alcohols, which provided Si-chiral silanes with moderate enantioselectivity.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Vibrational spectroscopic and non-linear optical activity studies on nicotinanilide : A DFT approach
The molecular structure of nicotinanilide was optimized by the DFT/B3LYP method with cc-pVTZ basis set using Gaussian 09 program. The first order hyperpolarizability of the molecule was calculated, which exhibits the higher nonlinear optical activity. The natural bond orbital analysis confirms the presence of intramolecular charge transfer and the hydrogen bonding interaction, which leads to the higher nonlinear optical activity of the molecule. The Frontier molecular orbitals analysis of the molecule shows that the delocalization of electron density occurs within the molecule. The lower energy gap indicates that the hydrogen bond formation between the charged species. The vibrational frequencies were calculated and assigned on the basis of potential energy distribution calculation using the VEDA 4.0 program and the corresponding vibrational spectra were simulated. Hence, the nicotinanilide molecule can be a good candidate for second-order NLO material.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Exploiting universal nonlocal dispersion in optically active materials for spectro-polarimetric computational imaging
Recent years have seen significant advancements in exploring novel light-matter interactions such as hyperbolic dispersion within natural crystals. However, current studies have predominantly concentrated on local optical response of materials characterized by a dielectric tensor without spatial dispersion. Here, we investigate the nonlocal response in optically-active crystals with screw symmetries, revealing their lossless, super-dispersive properties compared to traditional optical response functions. We leverage this universal nonlocal dispersion, i.e. the dispersion of optical rotatory power, to explore a novel spectral de-multiplexing scheme compared to conventional gratings, prisms and metasurfaces. We design and demonstrate an ‘Nonlocal-Cam’ - a camera that exploits nonlocal dispersion through sampling of polarized spectral states and the application of computational spectral reconstruction algorithms. The Nonlocal-Cam captures information in both laboratory and outdoor field experiments which is unavailable to traditional intensity cameras - the spectral texture of polarization. Merging the fields of nonlocal electrodynamics and computational imaging, our work paves the way for exploiting nonlocal optics of optically active materials in a variety of applications, from biological microscopy to physics-driven machine vision and remote sensing.
Wang, Xueji [Purdue Univ., West Lafayette, IN (Uni↗
Structural, vibrational spectroscopic and nonlinear optical activity studies on 2-hydroxy- 3, 5-dinitropyridine: A DFT approach
The conformational analysis was carried out for 2-Hydroxy- 3, 5-dinitropyridine molecule using potential energy surface scan and the most stable optimized conformer was predicted. The vibrational frequencies and Mulliken atomic charge distribution were calculated for the optimized geometry of the molecule using DFT/B3LYP cc-pVQZ basis set by Gaussian 09 Program. The vibrational frequencies were assigned on the basis of potential energy distribution calculation using VEDA 4.0 program. In the Frontier molecular orbitals analysis, the molecular reactivity, kinetic stability, intramolecular charge transfer studies and the calculation of ionization energy, electron affinity, global hardness, chemical potential, electrophilicity index and softness values of the title molecule were carried out. The nonlinear optical activity of the molecule was studied by means of first order hyperpolarizability, which was computed as 7.64 times greater than urea. The natural bond orbital analysis was performed to confirm the nonlinear optical activity of the molecule.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Infrared-active optical phonons in LiFePO 4 single crystals
Infrared-active optical phonons were studied in olivine LiFePO 4 oriented single crystals by means of both rotating analyzer and rotating compensator spectroscopic ellipsometry in the spectral range between 50 and 1400 cm -1 . The eigenfrequencies, oscillator strengths, and broadenings of the phonon modes were determined from fits of the anisotropic harmonic oscillator model to the data. Optical phonons in a heterosite FePO 4 crystal were measured from the delithiated ab-surface of the LiFePO 4 crystal and compared with the phonon modes of the latter. Good agreement was found between experimental data and the results of solid-state hybrid density functional theory calculations for the phonon modes in both LiFePO 4 and FePO 4 .
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Optically active derivatives of terephthalic acid: synthesis and crystal structures
New optically active derivatives of terephthalic acid, which are of interest as precursors of chiral metal-organic frameworks (MOFs), were synthesized starting from available dimethyl 2-aminoterephthalate, N-Boc-L-alanine, and N-Boc-L-proline. The crystal structures of three samples were determined by powder X-ray diffraction. In all three structures, the acid molecules exist as zwitterions.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗