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At least 631 records · Page 35

Electronic and Geometric effects on Photochemistry of Molecules in Well-Defined Environments

Assemblies of molecular switches at surfaces are of great interest for applications in solar energy conversion, optoelectronic and optomechanical devices. Experimental studies have demonstrated that it is possible to optically probe photoactive molecules in well-defined nanoscale environments. To understand these systems, we have developed a polarizable frozen-density embedding (FDEpol) to model the optical properties of molecules adsorbed on metal clusters. We have demonstrated that the FDEpol method can describe the ground state and linear response properties of strongly coupled systems with results that are in good agreement with exact projection based embedding method.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Investigation of Third Order Optical Nonlinearity and Reverse Saturable Absorption of Octa-alkoxy Metallophthalocyanines

In recent years, there has been a growing interest in the development of passive optical power limiters for the protection of the human eye and solid-state sensors from damage caused by energetic light pulses and also for other switching applications. One of the key issues involved is the search for appropriate materials that show effective reverse saturable absorption. Phthalocyanines seem to be good candidates for such applications because of their higher third order nonlinearity and the unique electronic absorption characteristics. A series of 1,4,8,11,15, 18,22,25-octa-alkoxy metallophthalocyanines containing various central metal atoms such as zinc, copper, palladium, cobalt and nickel were characterized for their third order nonlinearity and for their nonlinear absorptive properties to evaluate their suitability to function as reverse saturable absorbers.

Sanghadasa, Mohan↗

Heralded Multiplexed High-Efficiency Cascaded Source of Dual-Rail Entangled Photon Pairs Using Spontaneous Parametric Down-Conversion

Deterministic sources of high-fidelity entangled qubit pairs encoded in the dual-rail photonic basis, i.e., presence of a single photon in one of two orthogonal modes, are a key enabling technology of many applications of quantum information processing, including high-rate, high-fidelity quantum communications over long distances. The most popular and mature sources of such photonic entanglement, e.g., those that leverage spontaneous parametric down-conversion (SPDC) or spontaneous four-wave mixing, generate an entangled (so-called continuous-variable) quantum state that contains contributions from high-order photon terms that lie outside the span of the dual-rail basis, which is detrimental to most applications. One often uses low pump power to mitigate the effects of those high-order terms. However, that reduces the pair generation rate, and the source becomes inherently probabilistic. We investigate a cascaded source that performs a linear-optical entanglement swap between two SPDC sources, to generate a heralded photonic entangled state that has a higher fidelity (to the ideal Bell state) compared to a free-running SPDC source. Furthermore, with the Bell swap providing a heralding trigger, we show how to build a multiplexed source, which despite reasonable switching losses and detector loss and noise, yields a fidelity versus success probability trade-off of a high-efficiency source of high-fidelity dual-rail photonic entanglement. We find, however, that there is a threshold of 1.5 dB of loss per switch, beyond which multiplexing hurts the fidelity versus success probability trade-off.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Encoding multistate charge order and chirality in endotaxial heterostructures

Abstract High-density phase change memory (PCM) storage is proposed for materials with multiple intermediate resistance states, which have been observed in 1 T -TaS 2 due to charge density wave (CDW) phase transitions. However, the metastability responsible for this behavior makes the presence of multistate switching unpredictable in TaS 2 devices. Here, we demonstrate the fabrication of nanothick verti-lateral H -TaS 2 /1 T -TaS 2 heterostructures in which the number of endotaxial metallic H -TaS 2 monolayers dictates the number of resistance transitions in 1 T -TaS 2 lamellae near room temperature. Further, we also observe optically active heterochirality in the CDW superlattice structure, which is modulated in concert with the resistivity steps, and we show how strain engineering can be used to nucleate these polytype conversions. This work positions the principle of endotaxial heterostructures as a promising conceptual framework for reliable, non-volatile, and multi-level switching of structure, chirality, and resistance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Nanoscale Ferroelectric Control of Novel Electronic States in Layered Two-Dimensional Materials (Final Report)

In this DOE Early Career project “Nanoscale Ferroelectric Control of Novel Electronic States in Layered Two-Dimensional Materials,” the PI’s group has combined ferroelectric field effect with nanoscale domain imaging and writing to design the electronic and optical properties of two-dimensional (2D) van der Waals materials, including graphene and transition metal dichalcogenides MoS2 and ReS2. The van der Waals materials have been prepared into field effect transistor (FET) devices with ferroelectric gates. Through domain patterning in a ferroelectric polymer PVDF-TrEF top-gate via conductive atomic force microscopy, the team has created programmable Schottky junctions in monolayer MoS 2 , where both barrier height and I-V rectifying polarity can be reconfigured. The transport anisotropy of monolayer to few-layer ReS 2 has been mapped out by defining the entire channel into an insulating state and creating nanoscale conducting paths along different directions through domain writing in the ferroelectric top-gate. The result shows that the conductivity along and perpendicular to the Re-chain can differ by >5.5x10 4 . Theoretical modeling points to the band origin of the transport anomaly and reveals the emergence of a flat band in few-layer ReS 2 . The interfacial epitaxial relation between ReS 2 and PVDF-TrFE further promotes the formation of close-packed, highly ordered PVDF-TrFE nanowires with width of 35 nm and 10 nm. Nonvolatile modulation of quantum Hall effect has been achieved in graphene FETs with a ferroelectric oxide Ba 0.4 Sr 0.6 TiO 3 back-gate. Scattering from the remote surface optical phonon in Ba 0.4 Sr 0.6 TiO 3 limits the room temperature mobility of graphene to be about 3x10 4 cm 2 /Vs. Steep-slope switching has been achieved in MoS 2 FETs back-gated by polycrystalline Pb(Zr,Ti)O 3 , which signals a static-state negative capacitance mode without involving an additional dielectric layer. Piezoresponse force microscopy studies show that the sub-threshold swing can be well correlated with the domain wall density in Pb(Zr,Ti)O 3 . The team also observes an unconventional filtering effect of the second harmonic generation response at the MoS 2 /Pb(Zr,Ti)O 3 heterointerface, which can be accounted for by the alignment between one of the polar axes of MoS 2 and the chiral dipole rotation at the surface of domain wall in Pb(Zr,Ti)O 3 . The research supported by this DOE grant has significantly advanced the fundamental understanding and functional design of ferroelectric/2D van der Waals heterostructures for their implementation towards energy applications.

36 MATERIALS SCIENCE↗

Space station tracking requirements feasibility study, volume 2

The objective of this feasibility study is to determine analytically the accuracies of various sensors being considered as candidates for Space Station use. Specifically, the studies were performed whether or not the candidate sensors are capable of providing the required accuracy, or if alternate sensor approaches should be investigated. Other topics related to operation in the Space Station environment were considered as directed by NASA-JSC. The following topics are addressed: (1) Space Station GPS; (2) Space Station Radar; (3) Docking Sensors; (4) Space Station Link Analysis; (5) Antenna Switching, Power Control, and AGC Functions for Multiple Access; (6) Multichannel Modems; (7) FTS/EVA Emergency Shutdown; (8) Space Station Information Systems Coding; (9) Wanderer Study; and (10) Optical Communications System Analysis. Brief overviews of the abovementioned topics are given. Wherever applicable, the appropriate appendices provide detailed technical analysis. The report is presented in two volumes. This is Volume 2, containing Appendices K through U.

Udalov, Sergei↗

Space station tracking requirements feasibility study, volume 1

The objective of this feasibility study is to determine analytically the accuracies of various sensors being considered as candidates for Space Station use. Specifically, the studies were performed whether or not the candidate sensors are capable of providing the required accuracy, or if alternate sensor approaches be investigated. Other topics related to operation in the Space Station environment were considered as directed by NASA-JCS. The following topics are addressed: (1) Space Station GPS; (2) Space Station Radar; (3) Docking Sensors; (4) Space Station Link Analysis; (5) Antenna Switching, Power Control, and AGC Functions for Multiple Access; (6) Multichannel Modems; (7) FTS/EVA Emergency Shutdown; (8) Space Station Information Systems Coding; (9) Wanderer Study; and (10) Optical Communications System Analysis. Brief overviews of the abovementioned topics are given. Wherever applicable, the appropriate appendices provide detailed technical analysis. The report is presented in two volumes. This is Volume 1, containing the main body and Appendices A through J.

Udalov, Sergei↗

Phase-change Tunable Filters (PCTFs) for Hyperspectral Thermal Imaging

In this presentation, we introduce phase-change tunable filters (PCTFs), which are capable of actively tunable spectral filtering as well as continuous tuning (hyperspectral) across multiple IR wavebands (1–10 μm); several orders-of-magnitude faster switching speeds (GHz–MHz) than the state-of-the-art, and narrowband filtering (~50 nm passband). This technology subsystem is based on the unique electro-optics of non-volatile, phase-change materials (PCMs) such as GeSbTe and SbS. PCMs exhibit a large, reversible refractive index shift through applied energetic pulses. By integrating PCMs with established optical filter designs—whose optical properties are strongly dependent on the constituent materials’ refractive indices—we can rapidly and reversibly tune the PCTFs center wavelength (passband).

Tunable filter↗

Beam-steering system based on a MEMS-actuated vertical-coupler array

An integrated-optics MEMS-actuated beam-steering system is disclosed, wherein the beam-steering system includes a lens and a programmable vertical coupler array having a switching network and an array of vertical couplers, where the switching network can energize of the vertical couplers such that it efficiently emits the light into free-space. The lens collimates the light received from the energized vertical coupler and directs the output beam along a propagation direction determined by the position of the energized vertical coupler within the vertical-coupler array. In some embodiments, the vertical coupler is configured to correct an aberration of the lens. In some embodiments, more than one vertical coupler can be energized to enable steering of multiple output beams. In some embodiments, the switching network is non-blocking.

42 ENGINEERING↗

Beam-steering system based on a MEMS-actuated vertical-coupler array

An integrated-optics MEMS-actuated beam-steering system is disclosed, wherein the beam-steering system includes a lens and a programmable vertical coupler array having a switching network and an array of vertical couplers, where the switching network can energize of the vertical couplers such that it efficiently emits the light into free-space. The lens collimates the light received from the energized vertical coupler and directs the output beam along a propagation direction determined by the position of the energized vertical coupler within the vertical-coupler array. In some embodiments, the vertical coupler is configured to correct an aberration of the lens. In some embodiments, more than one vertical coupler can be energized to enable steering of multiple output beams. In some embodiments, the switching network is non-blocking.

Zhang, Xiaosheng↗

Unlocking Electrostrain in Plastically Deformed Barium Titanate

Achieving substantial electrostrain alongside a large effective piezoelectric strain coefficient (d 33 *) in piezoelectric materials remains a formidable challenge for advanced actuator applications. Here, in this work, a straightforward approach to enhance these properties by strategically designing the domain structure and controlling the domain switching through the introduction of arrays of ordered {100}<100> dislocations is proposed. This dislocation engineering yields an intrinsic lock-in steady–state electrostrain of 0.69% at a low field of 10 kV cm -1 without external stress and an output strain energy density of 5.24 J cm -3 in single-crystal BaTiO 3 , outperforming the benchmark piezoceramics and relaxor ferroelectric single-crystals. Additionally, applying a compression stress of 6 MPa fully unlocks electrostrains exceeding 1%, yielding a remarkable d 33 * value over 10 000 pm V -1 and achieving a record-high strain energy density of 11.67 J cm -3 . Optical and transmission electron microscopy, paired with laboratory and synchrotron X-ray diffraction, is employed to rationalize the observed electrostrain. Phase-field simulations further elucidate the impact of charged dislocations on domain nucleation and domain switching. These findings present an effective and sustainable strategy for developing high-performance, lead-free piezoelectric materials without the need for additional chemical elements, offering immense potential for actuator technologies.

36 MATERIALS SCIENCE↗

Hardware Testing for the Optical PAyload for Lasercomm Science (OPALS)

Hardware for several subsystems of the proposed Optical PAyload for Lasercomm Science (OPALS), including the gimbal and avionics, was tested. Microswitches installed on the gimbal were evaluated to verify that their point of actuation would remain within the acceptable range even if the switches themselves move slightly during launch. An inspection of the power board was conducted to ensure that all power and ground signals were isolated, that polarized components were correctly oriented, and that all components were intact and securely soldered. Initial testing on the power board revealed several minor problems, but once they were fixed the power board was shown to function correctly. All tests and inspections were documented for future use in verifying launch requirements.

optical communications↗

XUV-driven plasma switch for THz: new spatio-temporal overlap tool for XUV–THz pump–probe experiments at FELs

A simple and robust tool for spatio-temporal overlap of THz and XUV pulses in in-vacuum pump–probe experiments is presented. The technique exploits ultrafast changes of the optical properties in semiconductors (i.e. silicon) driven by ultrashort XUV pulses that are probed by THz pulses. This work demonstrates that this tool can be used for a large range of XUV fluences that are significantly lower than when probing by visible and near-infrared pulses. This tool is mainly targeted at emerging X-ray free-electron laser facilities, but can be utilized also at table-top high-harmonics sources.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Proximity Ferroelectricity in Compositionally Graded Structures

Proximity ferroelectricity is a novel paradigm for inducing ferroelectricity in a non-ferroelectric polar material, such as AlN or ZnO that are typically unswitchable with an external field below their dielectric breakdown field. When placed in direct contact with a thin switchable ferroelectric layer (such as Al 1-x Sc x N or Zn 1-x Mg x O), they become a practically switchable ferroelectric. Using the thermodynamic Landau-Ginzburg-Devonshire theory, in this work, we perform the finite element modeling of the polarization switching in the compositionally graded AlN-Al 1-x Sc x N, ZnO-Zn 1-x Mg x O, and MgO-Zn 1-x Mg x O structures sandwiched in both a parallel-plate capacitor geometry as well as in a sharp probe-planar electrode geometry. We reveal that the compositionally graded structure allows the simultaneous switching of spontaneous polarization in the whole system by a coercive field significantly lower than the electric breakdown field of unswitchable polar materials. The physical mechanism is the depolarization electric field determined by the gradient of chemical composition “x”. The field lowers the steepness of the switching barrier in the otherwise unswitchable parts of the compositionally graded AlN-Al 1-x Sc x N and ZnO-Zn 1-x Mg x O structures. In the MgO-like regions of the compositionally graded MgO-Zn 1-x Mg x O structure, a shallow double-well free energy potential emerges. Proximity ferroelectric switching of the compositionally graded structures placed in the probe-electrode geometry occurs due to nanodomain formation under the tip. We predict that a gradient of chemical composition “x” significantly lowers effective coercive fields of the compositionally graded AlN-Al 1-x Sc x N and ZnO-Zn 1-x Mg x O structures compared to the coercive fields of the corresponding multilayers with a uniform chemical composition in each layer. A tip-induced switching further lowers the coercive field, enabling control of ferroelectric domains in otherwise unswitchable compositionally graded structures, which can provide nanoscale domain control for memory, actuation, sensing, and optical applications.

36 MATERIALS SCIENCE↗

Tunable Perovskite-Derived Bismuth Halides: Cs 3 Bi 2 (Cl 1– x I x ) 9

Bismuth-based perovskites are of interest as safer alternatives to lead-based optoelectronic materials. Prior studies have reported on the compounds Cs 3 Bi 2 Cl 9 , Cs 3 Bi 2 I 9 , and Cs 3 Bi 2 Cl 3 I 6 . Here we examine a range of compounds of the formula Cs 3 Bi 2 (Cl 1–x I x ) 9 , where x takes values from 0.09 to 0.52. Powder and single-crystal X-ray diffraction were used to determine that all of these compounds adopt the layered vacancy-ordered perovskite structure observed for Cs 3 Bi 2 Cl 3 I 6 , which is also the high-temperature phase of Cs 3 Bi 2 Cl 9 . We find that, even with very small iodine incorporation, the structure is switched to that of Cs 3 Bi 2 Cl 3 I 6 , with I atoms displaying a distinct preference for the capping sites on the BiX 6 octahedra. Optical absorption spectroscopy was employed to study the evolution of optical properties of these materials, and this is complemented by density functional theory electronic structure calculations. Finally, three main absorption features were observed for these compounds, and with increasing x, the lowest-energy features are red-shifted.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

All-optical seeding of a light-induced phase transition with correlated disorder

Ultrafast manipulation of vibrational coherence is an emergent route to control the structure of solids. However, this strategy can only induce long-range correlations and cannot modify atomic structure locally, which is required in many technologically-relevant phase transitions. Here, we demonstrate that ultrafast lasers can generate incoherent structural fluctuations which are more efficient for material control than coherent vibrations, extending optical control to a wider range of materials. We observe that local, non-equilibrium lattice distortions generated by a weak laser pulse reduce the energy barrier to switch between insulating and metallic states in vanadium dioxide by 6%. In conclusion, seeding inhomogeneous structural-fluctuations presents an alternative, more energy efficient, route for controlling materials that may be applicable to all solids, including those used in data and energy storage devices.

36 MATERIALS SCIENCE↗

Broadband electro-optic polarization conversion with atomically thin black phosphorus

Metasurfaces tune polarization In photonic systems, the polarization state of light is typically manipulated with bulky components based on dielectrics and liquid crystals. Active metasurfaces now provide the possibility of shrinking the size of these components to the nanoscale. Biswas et al . demonstrate an active nanophotonic structure capable of versatile electro-optic polarization conversion. Using trilayer black phosphorus sandwiched between electrical gates forming a cavity, they show that the polarization state of light across telecommunication wavelengths can be electrically switched. Such control can be useful for a number of applications in communications, imaging, and beam steering where the wavefront of the propagating light can be actively manipulated. —ISO

Science & Technology - Other Topics↗

Repetitively Q-switched Nd:BeL lasers

The thermal and mechanical characteristics which will ultimately limit the performance of Nd:BeL at high average power levels were investigated. The output beam characteristics (pulse width, peak power, beam dimensions and collimation) were determined at high repetition rates for both Nd:BeL and Nd:YAG. The output of Nd:BeL was shown to exceed that of Nd:YAG by a factor of 2.7 at low Q-switched repetition rates (1 Hz). This result follows from the smaller stimulated emission cross section of x-axis Nb:BeL compared to that of NdYAG by the same factor. At high repetition rates (10 Hz) the output of Nd:Bel falls to a level of three-fifths of its low repetition rate value while under similar tests the output of Nd:YAG remains essentially constant. A comparison of the measured values of the elasto-optic coefficients, the dn/dT values and the linear expansion coefficients for BeL and YAG failed to provide an explanation for the performance of BeL; however, thermal lensing was observed in Nd:BeL. Results imply that the output of a high repetition rate Q-switched Nd:BeL laser (high thermal loading) could be dramatically increased by utilization of a resonator design to compensate for the thermal lensing effects.

Degnan, J.↗