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At least 235 records · Page 13

Probing Coherent States of Light and Matter in Two-Dimensional Semiconductors. Final Report

The ability to enhance light-matter interactions in engineered optical environments is well-established in micro- and nano-photonics. New classes of materials bring new rich correlations between spin, momentum, and light polarization that can be exploited in these photonic systems for information processing and low-power electronics. Interfacing these novel material features with strong optical interactions suggests the compelling capability to create hybrid light-matter systems harnessing low-energy and protected material properties such as spin. The long-term objective of this program was to investigate the interplay between pseudospin in 2D materials and light, revealing new coherent phenomena. The materials studied are the monolayer transition metal dichalcogenides (TMDs), which support polarization-sensitive optical transitions when isolated to a single sub-nanometer crystal layer in thickness. In particular, monolayer TMD semiconductors such as MoS 2 exhibit degenerate valleys in momentum space with distinct spin character. These valleys can be separately addressed by circularly polarized light, providing a tool for manipulation. Integrating this valley pseudospin of excitons in monolayer TMDs with engineered strong optical excitations to create novel coherent phenomena was a key long-term goal of this research. The scope of this research primarily focused on studying light-matter interactions of valley-sensitive excitations in monolayer TMDs. The scope also included the integration of monolayer materials that support valley-polarized emission into photonic devices. This approach extends prior work on exciton-polaritons in 2D materials toward a platform with far more control and improved light input and output characteristics to aid scalability of these polarization-sensitive phenomena to many-body, long-range optical networks. During the course of the five-year Early Career program, the approaches led to successful progress on each proposed aim. Initial successful work seeded additional research that developed from the main themes, while this program focus evolved toward coherent manipulation of valley polaritons and integration with photonics. Both of these advanced topics set the stage for new capabilities in future innovative research. The results of this project provide advances in materials and methods relevant for new visions of opto-electronics and photonics that can improve information processing in an era of increased focus on quantum and coherent phenomena. The research has also contributed to the training of two postdoctoral scholars and five graduate students.

2D Materials↗

Low-energy excitations in type-II Weyl semimetal T d - MoTe 2 evidenced through optical conductivity

Molybdenum ditelluride, MoTe 2 , is a versatile material where the topological phase can be readily tuned by manipulating the associated structural phase transition. The fine details of the band structure of MoTe 2 , key to understanding its topological properties, have proven difficult to disentangle experientially due to the multiband character of the material. Through experimental optical conductivity spectra, we detect two strong low-energy interband transitions. Both are linked to excitations between spin-orbit split bands. The lowest interband transition shows a strong thermal shift, pointing to a chemical potential that dramatically decreases with temperature. Finally, with the help of ab initio calculations and a simple two-band model, we give qualitative and quantitative explanations of the main features in the temperature-dependent optical spectra up to 400 meV.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Femtosecond control of phonon dynamics near a magnetic order critical point

The spin-phonon interaction in spin density wave (SDW) systems often determines the free energy landscape that drives the evolution of the system. When a passing energy flux, such as photoexcitation, drives a crystalline system far from equilibrium, the resulting lattice displacement generates transient vibrational states. Manipulating intermediate vibrational states in the vicinity of the critical point, where the SDW order parameter changes dramatically, would then allow dynamical control over functional properties. Here we combine double photoexcitation with an X-ray free-electron laser (XFEL) probe to control and detect the lifetime and magnitude of the intermediate vibrational state near the critical point of the SDW in chromium. We apply Landau theory to identify the mechanism of control as a repeated partial quench and sub picosecond recovery of the SDW. Our results showcase the capabilities to influence and monitor quantum states by combining multiple optical photoexcitations with an XFEL probe. They open new avenues for manipulating and researching the behaviour of photoexcited states in charge and spin order systems near the critical point.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Quasi-Random Multimetallic Nanoparticle Arrays

Here, this paper describes a nanofabrication procedure that can generate multiscale substrates with quasi-random microregions of nanoparticle arrays having different periodicities and metals. We combine cycles of large-area nanoparticle array fabrication with solvent-assisted wrinkle lithography to mask and etch quasi-random areas of prefabricated nanoparticles to control the fill factors of the arrays. The approach is highly flexible, and parameters, including nanoparticle size and material, array geometry, and fill factor, can be tailored independently. Multimetallic nanoparticle arrays can support surface lattice resonances at fill factors as low as 20% and can function as nanoscale cavities for lasing action with as few as 10% of the nanoparticles in an array. We demonstrated that multimetallic nanoparticle substrates that combine two or three arrays with different periodicities can exhibit lasing responses over visible and near-infrared wavelengths. Our work showcases the robust optical responses of multimetallic and periodic devices for broadband light manipulation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Tunable Broad Light Emission from 3D “Hollow” Bromide Perovskites through Defect Engineering

We report hybrid halide perovskites consisting of corner-sharing metal halide octahedra and small cuboctahedral cages filled with counter cations have proven to be prominent candidates for many high-performance optoelectronic devices. The stability limits of their three-dimensional perovskite framework are defined by the size range of the cations present in the cages of the structure. In some cases, the stability of the perovskite-type structure can be extended even when the counterions violate the size and shape requirements, as is the case in the so-called "hollow" perovskites. In this work, we engineered a new family of 3D highly defective yet crystalline "hollow" bromide perovskites with general formula (FA) 1-x (en) x (Pb) 1-0.7x (Br) 3-0.4x (FA = formamidinium (FA + ), en = ethylenediammonium (en 2+ ), x = 0-0.44). Pair distribution function analysis shed light on the local structural coherence, revealing a wide distribution of Pb-Pb distances in the crystal structure as a consequence of the Pb/Br-deficient nature and en inclusion in the lattice. By manipulating the number of Pb/Br vacancies, we finely tune the optical properties of the pristine FAPbBr 3 by blue shifting the band gap from 2.20 to 2.60 eV for the x = 0.42 en sample. A most unexpected outcome was that at x > 0.33 en incorporation, the material exhibits strong broad light emission (1% photoluminescence quantum yield (PLQY)) that is maintained after exposure to air for more than a year. This is the first example of strong broad light emission from a 3D hybrid halide perovskite, demonstrating that meticulous defect engineering is an excellent tool for customizing the optical properties of these semiconductors.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Improved docking alignment system

Improved techniques are provided for the alignment of two objects. The present invention is particularly suited for 3-D translation and 3-D rotational alignment of objects in outer space. A camera is affixed to one object, such as a remote manipulator arm of the spacecraft, while the planar reflective surface is affixed to the other object, such as a grapple fixture. A monitor displays in real-time images from the camera such that the monitor displays both the reflected image of the camera and visible marking on the planar reflective surface when the objects are in proper alignment. The monitor may thus be viewed by the operator and the arm manipulated so that the reflective surface is perpendicular to the optical axis of the camera, the roll of the reflective surface is at a selected angle with respect to the camera, and the camera is spaced a pre-selected distance from the reflective surface.

Monford, Leo G.↗

Organic crystalline films for optical applications and related methods of fabrication

The present invention provides organic single crystal films of less than 20 .mu.m, and devices and methods of making such films. The crystal films are useful in electro-optical applications and can be provided as part of an electro-optical device which provides strength, durability, and relative ease of manipulation of the mono-crystalline films during and after crystal growth.

Leyderman, Alexander↗

Docking alignment system

Improved techniques are provided for alignment of two objects. The present invention is particularly suited for three-dimensional translation and three-dimensional rotational alignment of objects in outer space. A camera 18 is fixedly mounted to one object, such as a remote manipulator arm 10 of the spacecraft, while the planar reflective surface 30 is fixed to the other object, such as a grapple fixture 20. A monitor 50 displays in real-time images from the camera, such that the monitor displays both the reflected image of the camera and visible markings on the planar reflective surface when the objects are in proper alignment. The monitor may thus be viewed by the operator and the arm 10 manipulated so that the reflective surface is perpendicular to the optical axis of the camera, the roll of the reflective surface is at a selected angle with respect to the camera, and the camera is spaced a pre-selected distance from the reflective surface.

Monford, Leo G.↗

Effects of Quantum Dot Loading on the Radioluminescence Efficiency in Quantum-Dot-Embedded Composites

Nanoparticle-embedded plastic scintillators are an emerging technology for fast, large-area, high-resolution radiation detection and imaging. Here, this study investigates the properties of such composites, focusing on the effects of the quantum dot (QD) concentration on the radioluminescence (RL) intensity, spectra, and dynamics. Experiments using CdSe/CdS QDs in a polymer reveal a superlinear increase in RL with the QD concentration despite optical losses from inner filtering and interparticle interactions. When corrected for inner filtering, RL shows a quadratic concentration dependence, consistent with simple analytical models of improving the secondary electron capture. Practically, the benefits of high QD concentrations are muted by optical losses, but the findings apply to other systems with insulating hosts. In addition to manipulating emission for large effective Stokes shifts, future improvements may come from hosts with higher stopping power and better charge transport, which enable more effective funneling of excitations but without concomitant optical losses associated with high nanoparticle concentrations.

Auger recombination↗

Using the ISS as a Testbed to Prepare for the Next Generation of Space-Based Telescopes

The ISS provides a unique opportunity to develop the technologies and operational capabilities necessary to assemble future large space telescopes that may be used to investigate planetary systems around neighboring stars. Assembling telescopes in space is a paradigm-shifting approach to space astronomy. Using the ISS as a testbed will reduce the technical risks of implementing this major scientific facility, such as laser metrology and wavefront sensing and control (WFSC). The Optical Testbed and Integration on ISS eXperiment (OpTIIX) will demonstrate the robotic assembly of major components, including the primary and secondary mirrors, to mechanical tolerances using existing ISS infrastructure, and the alignment of the optical elements to a diffraction-limited optical system in space. Assembling the optical system and removing and replacing components via existing ISS capabilities, such as the Special Purpose Dexterous Manipulator (SPDM) or the ISS flight crew, allows for future experimentation and repair, if necessary. First flight on ISS for OpTIIX, a small 1.5 meter optical telescope, is planned for 2015. In addition to demonstration of key risk-retiring technologies, the OpTIIX program includes a public outreach program to show the broad value of ISS utilization.

Ess, Kim↗

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↗

A microcontroller-based three degree-of-freedom manipulator testbed

A wheeled exploratory vehicle is under construction at the Mars Mission Research Center at North Carolina State University. In order to serve as more than an inspection tool, this vehicle requires the ability to interact with its surroundings. A crane-type manipulator, as well as the necessary control hardware and software, has been developed for use as a sample gathering tool on this vehicle. The system is controlled by a network of four Motorola M68HC11 microcontrollers. Control hardware and software were developed in a modular fashion so that the system can be used to test future control algorithms and hardware. Actuators include three stepper motors and one solenoid. Sensors include three optical encoders and one cable tensiometer. The vehicle supervisor computer provides the manipulator system with the approximate coordinates of the target object. This system maps the workspace surrounding the given location by lowering the claw, along a set of evenly spaced vertical lines, until contact occurs. Based on this measured height information and prior knowledge of the target object size, the system determines if the object exists in the searched area. The system can find and retrieve a 1.25 in. diameter by 1.25 in. tall cylinder placed within the 47.5 sq in search area in less than 12 minutes. This manipulator hardware may be used for future control algorithm verification and serves as a prototype for other manipulator hardware.

Brown, Robert Michael, Jr.↗

Numerical modeling of a proof-of-principle experiment on optical stochastic cooling at an electron storage ring

Cooling of beams circulating in storage rings is critical for many applications including particle colliders and synchrotron light sources. A method enabling unprecedented beam-cooling rates, optical stochastic cooling (OSC), was recently demonstrated in the Integrable Optics Test Accelerator (IOTA) electron storage ring at Fermilab [J. Jarvis , ]. This paper describes the numerical implementation of the OSC process in the particle-tracking program and discusses the validation of the developed model with available experimental data. The model is also employed to highlight some features associated with different modes of operation of OSC. The developed simulation tool should be valuable in guiding future configurations of optical stochastic cooling and, more broadly, modeling self-field-based beam manipulations. Published by the American Physical Society 2024

43 PARTICLE ACCELERATORS↗

JWST Integrated Science Instrument Module Alignment Optimization Tool

During cryogenic vacuum testing of the James Webb Space Telescope (JWST) Integrated Science Instrument Module (ISIM), the global alignment of the ISIM with respect to the designed interface of the JWST optical telescope element (OTE) will be measured through a series of optical characterization tests. These tests will determine the locations and orientations of the JWST science instrument projected focal surfaces and entrance pupils with respect to their corresponding OTE optical interfaces. If any optical performance non-compliances are identified, the ISIM will be adjusted to improve its performance. In order to understand how to manipulate the ISIM's degrees of freedom properly and to prepare for the ISIM flight model testing, a series of optical-mechanical analyses have been completed to develop and identify the best approaches for bringing a non-compliant ISIM element into compliance. In order for JWST to meet its observatory-level optical requirements and ambitious science goals, the ISIM element has to meet approximately 150 separate optical requirements. Successfully achieving many of those optical requirements depends on the proper alignment of the ISIM element with respect to the OTE. To verify that the ISIM element will meet its optical requirements, a series of cryogenic vacuum tests will be conducted with an OTE Simulator (OSIM). An optical Ray Trace and Geometry Model tool was developed to help solve the multi-dimensional alignment problem. The tool allows the user to determine how best to adjust the alignment of the JWST ISIM with respect to the ideal telescope interfaces so that the approximately 150 ISIM optical performance requirements can be satisfied. This capability has not existed previously.

Bos, Brent↗

Optically addressable molecular spins for quantum information processing

Spin-bearing molecules are promising building blocks for quantum technologies as they can be chemically tuned, assembled into scalable arrays, and readily incorporated into diverse device architectures. In molecular systems, optically addressing ground-state spins would enable a wide range of applications in quantum information science, as has been demonstrated for solid-state defects. However, this important functionality has remained elusive for molecules. Here, we demonstrate such optical addressability in a series of synthesized organometallic, chromium(IV) molecules. These compounds display a ground-state spin that can be initialized and read out using light and coherently manipulated with microwaves. In addition, through atomistic modification of the molecular structure, we vary the spin and optical properties of these compounds, indicating promise for designer quantum systems synthesized from the bottom-up.

99 GENERAL AND MISCELLANEOUS↗

High photon-phonon pair generation rate in a two-dimensional optomechanical crystal

Integrated optomechanical systems are a leading platform for manipulating, sensing, and distributing quantum information, but are limited by residual optical heating. Here, we demonstrate a two-dimensional optomechanical crystal (OMC) geometry with increased thermal anchoring and a mechanical mode at 7.4 GHz, well aligned with the operation range of cryogenic microwave hardware and piezoelectric transducers. The eight times better thermalization than current one-dimensional OMCs, large optomechanical coupling rates, g 0 /2π ≈ 880 kHz, and high optical quality factors, Q opt = 2.4 × 10 5 , allow ground-state cooling (n m = 0.32) of the acoustic mode from 3 K and entering the optomechanical strong-coupling regime. In pulsed sideband asymmetry measurements, we show ground-state operation (n m < 0.45) at temperatures below 10 mK, with repetition rates up to 3 MHz, generating photon-phonon pairs at ≈ 147 kHz. Our results extend optomechanical system capabilities and establish a robust foundation for future microwave-to-optical transducers with entanglement rates exceeding state-of-the-art superconducting qubit decoherence rates.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Continuous operation of a coherent 3,000-qubit system

Neutral atoms are a promising platform for quantum science, enabling advances in areas ranging from quantum simulations and computation to metrology, atomic clocks and quantum networking. Although atom losses typically limit these systems to a pulsed mode, continuous operation could substantially enhance cycle rates, remove bottlenecks in metrology and enable deep-circuit quantum evolution through quantum error correction. Here we demonstrate an experimental architecture for high-rate reloading and continuous operation of a large-scale atom-array system while realizing coherent storage and manipulation of quantum information. Our approach utilizes a series of two optical lattice conveyor belts to transport atom reservoirs into the science region, where atoms are repeatedly extracted into optical tweezers without affecting the coherence of qubits stored nearby. Using a reloading rate of 300,000 atoms in tweezers per second, we create over 30,000 initialized qubits per second, which we leverage to assemble and maintain an array of over 3,000 atoms for more than 2 hours. Furthermore, we demonstrate persistent refilling of the array with atomic qubits in either a spin-polarized or a coherent superposition state while preserving the quantum state of stored qubits. Our results pave the way for the realization of large-scale continuously operated atomic clocks, sensors and fault-tolerant quantum computers.

atomic and molecular physics↗