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At least 289 records · Page 16

Thickness-Tunable Self-Assembled Colloidal Nanoplatelet Films Enable Ultrathin Optical Gain Media

We propose and demonstrate construction of highly uniform, multilayered superstructures of CdSe/CdZnS core/shell colloidal nanoplatelets (NPLs) using liquid interface self-assembly. These NPLs are sequentially deposited onto a solid substrate into slabs having monolayer-precise thickness across tens of cm(2) areas. Because of near-unity surface coverage and excellent uniformity, amplified spontaneous emission (ASE) is observed from an uncharacteristically thin film having 6 NPL layers, corresponding to a mere 42 nm thickness. Furthermore, systematic studies on optical gain of these NPL superstructures having thicknesses ranging from 6 to 15 layers revealed the gradual reduction in gain threshold with increasing number of layers, along with a continuous spectral shift of the ASE peak (similar to 18 nm). These observations can be explained by the change in the optical mode confinement factor with the NPL waveguide thickness and propagation wavelength. This bottom-up construction technique for thickness-tunable, three-dimensional NPL superstructures can be used for large-area device fabrication.

Erdem, Onur↗

Near-Infrared Optical Gain of Colloidal Quantum Wells via Intraband Transitions

Tunable, unipolar, near-infrared intraband optical gain is demonstrated in semiconductor colloidal quantum wells, expanding the form and optical range for potential infrared applications. Atomically flat colloidal quantum wells of cadmium selenide display photoinduced absorption features in the near-infrared assigned to intraband (alternatively intersubband) transitions from the first to second electron subbands of the quantum wells. Under ultraviolet optical excitation, these same transitions from the first to second electron subbands are shown to exhibit stimulated emission, resulting in optical gain covering the near-infrared spectral region. The modal gain, bandwidth, and lifetime of this intraband gain are manipulated by using excitation energy, fluence, temperature, and surface chemistry. Unlike previous demonstrations of intraband optical gain in epitaxial quantum wells (e.g., quantum cascade lasers), the colloidal quantum wells are undoped. As a result, nearly thresholdless gain is in principle possible and limited in practice by the measurement of small optical losses of the samples in the near-infrared. Furthermore, the observations may be understood as a modified "quantum fountain" employing the valence band, a strategy that may be applied to many other materials.

Optical gain↗

Optically controlled single-valley exciton doublet states with tunable internal spin structures and spin magnetization generation

Manipulating quantum states through light–matter interactions has been actively pursued in two-dimensional materials research. Significant progress has been made toward the optical control of the valley degrees of freedom in semiconducting monolayer transition-metal dichalcogenides, based on doubly degenerate excitons from their two distinct valleys in reciprocal space. Here, we introduce a type of optically controllable doubly degenerate exciton states that come from a single valley, dubbed as single-valley exciton doublet (SVXD) states. They are unique in that their constituent holes originate from the same valence band, making possible the direct optical control of the spin structure of the excited constituent electrons. Combining ab initio GW plus Bethe–Salpeter equation ( GW -BSE) calculations and a theoretical analysis method, we demonstrate such SVXD in substrate-supported monolayer bismuthene—which has been successfully grown using molecular beam epitaxy. In each of the two distinct valleys in the Brillouin zone, strong spin–orbit coupling and C 3 v symmetry lead to a pair of degenerate 1s exciton states (the SVXD states) with opposite spin configurations. Any coherent linear combinations of the SVXD in a single valley can be excited by light with a specific polarization, enabling full manipulation of their internal spin configurations. In particular, a controllable net spin magnetization can be generated through light excitation. Our findings open routes to control quantum degrees of freedom, paving the way for applications in spintronics and quantum information science.

2D materials↗

Magnetically confined surface and bulk excitons in a layered antiferromagnet

The discovery of two-dimensional van der Waals magnets has greatly expanded our ability to create and control nanoscale quantum phases. A unique capability emerges when a two-dimensional magnet is also a semiconductor that features tightly bound excitons with large oscillator strengths that fundamentally determine the optical response and are tunable with magnetic fields. Here, in this study, we report a previously unidentified type of optical excitation-a magnetic surface exciton-enabled by the antiferromagnetic spin correlations that confine excitons to the surface of CrSBr. Magnetic surface excitons exhibit stronger Coulomb attraction, leading to a higher binding energy than excitons confined in bulk layers, and profoundly alter the optical response of few-layer crystals. Distinct magnetic confinement of surface and bulk excitons is established by layer- and temperature-dependent exciton reflection spectroscopy and corroborated by ab initio many-body perturbation theory calculations. By quenching interlayer excitonic interactions, the antiferromagnetic order of CrSBr strictly confines the bound electron-hole pairs within the same layer, regardless of the total number of layers. Our work unveils unique confined excitons in a layered antiferromagnet, highlighting magnetic interactions as a vital approach for nanoscale quantum confinement, from few layers to the bulk limit.

36 MATERIALS SCIENCE↗

Enhanced second-harmonic generation from WS 2 /ReSe 2 heterostructure

Van der Waals stacking presents new opportunities for nonlinear optics with its remarkable tunability and scalability. However, the fundamental role of interlayer interactions in modifying the overall nonlinear optical susceptibilities remains elusive. In this work, we report anisotropic enhancement of second-harmonic generation (SHG) from a WS 2 /ReSe 2 heterobilayer, where the individual composite layers possess distinctive crystal phases. We investigate polarization-resolved response and twist-angle dependence in SHG and reveal that band alignment alone is insufficient to explain the observed anisotropy in the modified SHG response. Spectral shifts in excitonic features highlight band renormalization, supporting the role of hybridization between the two layers. Furthermore, SHG enhancement is highly anisotropic and can even be suppressed in some orientations, suggesting possible intensity-borrowing mechanisms within the heterostructure. Our work demonstrates the ability to tune both the intensity and polarization dependence of nonlinear optical responses with van der Waals stacking of distinctive crystal phases.

2D materials↗

Tunability and synthetic lineshapes in high-Q optical whispering gallery modes

We demonstrate novel techniques to manipulate spectral properties of high quality factor (Q>107) whispering-gallery modes (WGM) in optical dielectric microresonators. These include permanent frequency trimming of WGM frequencies by means of UV photosensitivity of germanium doped silica resonators electro-optical tuning of WGM in lithium niobate resonators, and cascading of microresonators for obtaining second-order filtering function. We present theoretical interpretation of experimental results, and application example of techniques for photonic microwave filtering.

optical filters↗

Structural Diversity and Tunable Emission in Hybrid Organic–Inorganic Copper(I) Bromides

Recently, hybrid organic−inorganic copper(I) metal halides have attracted global attention due to their intriguing optical properties and low-cost solution processability. In this work, we report three hybrid organic−inorganic copper(I) bromides, [TMPA] 2 [Cu 2 Br 4 ], [TMPA] 4 [Cu 6 Br 10 ], and [TMPA] 2 [Cu 4 Br 6 ], synthesized through a slow evaporation method using trimethylphenylammonium (TMPA + ) as the organic cation. By precise control of the CuBr and TMPABr precursors, different copper halide [Cu 2 Br 4 ] 2− , [Cu 6 Br 10 ] 4− , and [Cu 4 Br 6 ] 2− structural units can be obtained. [TMPA] 2 [Cu 2 Br 4 ], [TMPA] 4 [Cu 6 Br 10 ], and [TMPA] 2 [Cu 4 Br 6 ] demonstrate distinct blue, orange, and greenish-yellow light emission, respectively. The first two compounds have zero-dimensional (0D) crystal structures in centrosymmetric triclinic space group P-1 and monoclinic space group P2 1 /n. In contrast, [TMPA] 2 [Cu 4 Br 6 ] features a unique one-dimensional (1D) structure and crystallizes in the centrosymmetric monoclinic space group P2 1 /c. Consequently, the observed greenish-yellow emission of [TMPA] 2 [Cu 4 Br 6 ] is also unique, in contrast to the typical orange-red emission of 0D [Cu 4 Br 6 ]-based compounds. This work provides insights into the design of copper halide light emitters and emphasizes the influence of structural dimensionality on photoluminescence. The tunable optical properties suggest the potential of these materials for multicolor photopatterning, information encryption, and anticounterfeiting applications.

Anions↗

Tunable Filter Made From Three Coupled WGM Resonators

A tunable third-order band-pass optical filter has been constructed as an assembly of three coupled, tunable, whispering-gallery-mode resonators similar to the one described in Whispering-Gallery-Mode Tunable Narrow-Band-Pass Filter (NPO-30896), NASA Tech Briefs, Vol. 28, No. 4 (April 2004), page 5a. This filter offers a combination of four characteristics that are desirable for potential applications in photonics: (1) wide real-time tunability accompanied by a high-order filter function, (2) narrowness of the passband, (3) relatively low loss between input and output coupling optical fibers, and (4) a sparse spectrum. In contrast, prior tunable band-pass optical filters have exhibited, at most, two of these four characteristics. As described in several prior NASA Tech Briefs articles, a whispering-gallery-mode (WGM) resonator is a spheroidal, disklike, or toroidal body made of a highly transparent material. It is so named because it is designed to exploit whispering-gallery electromagnetic modes, which are waveguide modes that propagate circumferentially and are concentrated in a narrow toroidal region centered on the equatorial plane and located near the outermost edge. Figure 1 depicts the optical layout of the present filter comprising an assembly of three coupled, tunable WGM resonators. Each WGM resonator is made from a disk of Z-cut LiNbO3 of 3.3-mm diameter and 50-m thickness. The perimeter of the disk is polished and rounded to a radius of curvature of 40 microns. The free spectral range of each WGM resonator is about 13.3 GHz. Gold coats on the flat faces of the disk serve as electrodes for exploiting the electro-optical effect in LiNbO3 for tuning. There is no metal coat on the rounded perimeter region, where the whispering-gallery modes propagate. Light is coupled from an input optical fiber into the whispering-gallery-modes of the first WGM resonator by means of a diamond prism. Another diamond prism is used to couple light from the whispering-gallery-modes of the third WGM resonator to an output optical fiber. The filter operates at a nominal wavelength of 1,550 nm and can be tuned over a frequency range of plus or minus 12 GHz by applying a potential in the range of plus or minus 150 V to the electrodes. The insertion loss (the loss between the input and output coupling optical fibers) was found to be repeatable at 6 dB. The resonance quality factor (Q) of the main sequence of resonator modes was found to be 5 x 10(exp 6), which corresponds to a bandwidth of 30 MHz. The filter can be shifted from one operating frequency to another within a tuning time less than or equal to 30 micro seconds. The transmission curve of the filter at frequencies near the middle of the passband closely approximates a theoretical third-order Butterworth filter profile, as shown in Figure 2.

Savchenkov, Anatoliy↗

Tunable Antireflection Layers for Planar Bolometer Arrays

It remains a challenge to obtain high-efficiency coupling of far-infrared through millimeter radiation to large-format detector arrays. The conventional approach of increasing detector coupling is to use reflective backshorts. However, this approach often results in excessive systematic errors resulting from reflections off the backshort edge. An alternate approach to both increasing quantum efficiency and reducing systematics associated with stray light is to place an antireflective coating near the front surface of the array. When incorporated with a resistive layer and placed behind the detector focal plane, the AR coating can serve to prevent optical ghosting by capturing radiation transmitted through the detector. By etching a hexagonal pattern in silicon, in which the sizes of the hexes are smaller than the wavelength of incident radiation, it is possible to fabricate a material that has a controllable dielectric constant, thereby allowing for simple tunable optical device fabrication. To this end, we have fabricated and tested tunable silicon "honeycomb" AR layers and AR/resistive layer devices. These devices were fabricated entirely out of silicon in order to eliminate problems associated with differential contraction upon detector cooling.

Brown, Ari-David↗

Develop On-Demand nanoplasmonic Device Concepts in a Semiconductor Compatible Hybrid System. Final Report

This report summarizes the research activities supported by the U.S. Department of Energy grant DE-SC-0010399. The goal of this project is to is to develop an on-demand nanoplasmonic platform that combines emerging oxide nanoelectronics with a low-loss semiconductor-friendly plasmonic materials. Toward this goal, several unique heterostructures formed between complex oxides and 2D layered materials have been developed. Based on these material systems, a set of atomic force microscope (AFM) based techniques have been developed that can allow long-living and reversible material phase transitions to be manipulated in nanoscale at room temperature. Using such technique and through interface coupling, we can effectively tune the plasmon propagations in unconventional plasmonic materials such as graphene and VO 2 . In addition, we also discovered a plethora of novel interface enabled electro-optic effects, including the spatial modulation of light using 2DEG, a giant programmable photothermoelectric effects at room temperature, a light induced superconducting transition, and a tunable giant third order optical nonlinearities. These major results are outlined in this report, along with lists of project participants and products.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Tunable resonator-based devices for producing variable delays and narrow spectral linewidths

Devices with two or more coupled resonators to produce narrow spectral responses due to interference of signals that transmit through the resonators and techniques for operating such devices to achieve certain operating characteristics are described. The devices may be optical devices where optical resonators such as whispering gallery mode resonators may be used. In one implementation, at least one of the coupled optical resonators is a tunable resonator and is tuned to change its resonance frequency to tune the spectral response of the device. The described devices and techniques may be applied in optical filters, optical delays, optical waveform generators, and other applications.

Savchenkov, Anatoliy↗

Concentrated thermal tuner for optical microdisk devices

A thermally tunable microresonator device with enhanced thermal confinement for greater efficiency is provided. A thermal confinement structure is electrically connected in series with the heater element used for tuning the microresonator. The heater element is conformed in a circular arc concentric with the microresonator, the thermal confinement structure comprises two or more tiers, and each tier comprises at least one metal trace conformed in a circular arc concentric with the microresonator.

Martinez, Nicholas Jacob↗

Beam steering at the nanosecond time scale with an atomically thin reflector

Techniques to mold the flow of light on subwavelength scales enable fundamentally new optical systems and device applications. The realization of programmable, active optical systems with fast, tunable components is among the outstanding challenges in the field. Here, we experimentally demonstrate a few-pixel beam steering device based on electrostatic gate control of excitons in an atomically thin semiconductor with strong light-matter interactions. By combining the high reflectivity of a MoSe 2 monolayer with a graphene split-gate geometry, we shape the wavefront phase profile to achieve continuously tunable beam deflection with a range of 10°, two-dimensional beam steering, and switching times down to 1.6 nanoseconds. Our approach opens the door for a new class of atomically thin optical systems, such as rapidly switchable beam arrays and quantum metasurfaces operating at their fundamental thickness limit.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Dynamic motion trajectory control with nanoradian accuracy for multi-element X-ray optical systems via laser interferometry

The past decades have witnessed the development of new X-ray beam sources with brightness growing at a rate surpassing Moore’s law. Current and upcoming diffraction limited and fully coherent X-ray beam sources, including multi-bend achromat based synchrotron sources and high repetition rate X-ray free electron lasers, puts increasingly stringent requirements on stability and accuracy of X-ray optics systems. Parasitic motion errors at sub-micro radian scale in beam transport and beam conditioning optics can lead to significant loss of coherence and brightness delivered from source to experiment. To address this challenge, we incorporated optical metrology based on interferometric length and angle sensing and real-time correction as part of the X-ray optics motion control system. A prototype X-ray optics system was constructed following the optical layout of a tunable X-ray cavity. On-line interferometric metrology enabled dynamical feedback to a motion control system to track and compensate for motion errors. The system achieved sub-microradian scale performance, as multiple optical elements are synchronously and continuously adjusted. This first proof of principle measurement demonstrated both the potential and necessity of incorporating optical metrology as part of the motion control architecture for large scale X-ray optical systems such as monochromators, delay lines, and in particular, X-ray cavity systems to enable the next generation cavity-based X-ray free electron lasers.

47 OTHER INSTRUMENTATION↗

Colloidal Semiconductor Nanocrystal Lasers and Laser Diodes

Lasers and optical amplifiers based on solution-processable materials have been long-desired devices for their compatibility with virtually any substrate, scalability, and ease of integration with on-chip photonics and electronics. These devices have been pursued across a wide range of materials including polymers, small molecules, perovskites, and chemically prepared colloidal semiconductor nanocrystals, also commonly referred to as colloidal quantum dots. The latter materials are especially attractive for implementing optical-gain media as in addition to being compatible with inexpensive and easily scalable chemical techniques, they offer multiple advantages derived from a zero-dimensional character of their electronic states. These include a size-tunable emission wavelength, low optical gain thresholds, and weak sensitivity of lasing characteristics to variations in temperature. Here we review the status of colloidal nanocrystal lasing devices, most recent advances in this field, outstanding challenges, and the ongoing progress toward technological viable devices including colloidal quantum dot laser diodes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Development and Application of Novel Diagnostics for Arc-Jet Characterization

This NASA-Ames University Consortium Project has focused on the design and demonstration of optical absorption sensors using tunable diode laser to target atomic copper impurities from electrode erosion in thc arc-heater metastable electronic excited states of molecular nitrogen, atomic argon, aid atomic oxygen in the arcjet plume. Accomplishments during this project include: 1. Design, construction, and assembly of optical access to the arc-heater gas flow. 2. Design of diode laser sensor for copper impurities in the arc-heater flow. 3 . Diode laser sensor design and test in laboratory plasmas for metastable Ar(3P), O(5S), N(4P), and N2(A). 4. Diode laser sensor demonstration measurements in the test cell to monitor species in the arc-jet plume.

Hanson, R. K.↗

Optical information processing for NASA's space exploration

The development status of optical processing techniques under development at NASA-JPL, NASA-Ames, and NASA-Johnson, is evaluated with a view to their potential applications in future NASA planetary exploration missions. It is projected that such optical processing systems can yield major reductions in mass, volume, and power requirements relative to exclusively electronic systems of comparable processing capabilities. Attention is given to high-order neural networks for distortion-invariant classification and pattern recognition, multispectral imaging using an acoustooptic tunable filter, and an optical matrix processor for control problems.

Chao, Tien-Hsin↗