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At least 361 records · Page 20

Measuring the Electronic Bandgap of Carbon Nanotube Networks in Non-Ideal p-n Diodes

The measurement of the electronic bandgap and exciton binding energy in quasi-one-dimensional materials such as carbon nanotubes is challenging due to many-body effects and strong electron–electron interactions. Unlike bulk semiconductors, where the electronic bandgap is well known, the optical resonance in low-dimensional semiconductors is dominated by excitons, making their electronic bandgap more difficult to measure. In this work, we measure the electronic bandgap of networks of polymer-wrapped semiconducting single-walled carbon nanotubes (s-SWCNTs) using non-ideal p-n diodes. We show that our s-SWCNT networks have a short minority carrier lifetime due to the presence of interface trap states, making the diodes non-ideal. We use the generation and recombination leakage currents from these non-ideal diodes to measure the electronic bandgap and excitonic levels of different polymer-wrapped s-SWCNTs with varying diameters: arc discharge (~1.55 nm), (7,5) (0.83 nm), and (6,5) (0.76 nm). Our values are consistent with theoretical predictions, providing insight into the fundamental properties of networks of s-SWCNTs. The techniques outlined here demonstrate a robust strategy that can be applied to measuring the electronic bandgaps and exciton binding energies of a broad variety of nanoscale and quantum-confined semiconductors, including the most modern nanoscale transistors that rely on nanowire geometries.

36 MATERIALS SCIENCE↗

Defect Complexes in CrSBr Revealed Through Electron Microscopy and Deep Learning

Atomic defects underpin the properties of van der Waals materials, and their understanding is essential for advancing quantum and energy technologies. Scanning transmission electron microscopy is a powerful tool for defect identification in atomically thin materials, and extending it to multilayer and beam-sensitive materials would accelerate their exploration. Here, we establish a comprehensive defect library in a bilayer of the magnetic quasi-1D semiconductor CrSBr by combining atomic-resolution imaging, deep learning, and calculations. We apply a custom-developed machine learning work flow to detect, classify, and average point vacancy defects. This classification enables us to uncover several distinct Cr interstitial defect complexes, combined Cr and Br vacancy defect complexes, and lines of vacancy defects that extend over many unit cells. We show that their occurrence is in agreement with our computed structures and binding energy densities, reflecting the intriguing layer interlocked crystal structure of CrSBr. Our ab initio calculations show that the interstitial defect complexes give rise to highly localized electronic states. These states are of particular interest due to the reduced electronic dimensionality and magnetic properties of CrSBr and are, furthermore, predicted to be optically active. Our results broaden the scope of defect studies in challenging materials and reveal new defect types in bilayer CrSBr that can be extrapolated to the bulk and to over 20 materials belonging to the same FeOCl structural family.

deep learning↗

Picoseconds-Limited Exciton Recombination in Metal–Organic Chalcogenides Hybrid Quantum Wells

Metal-organic species can be designed to self-assemble in large-scale, atomically defined, supramolecular architectures. Hybrid quantum wells, where inorganic two-dimensional (2D) planes are separated by organic ligands, are a particular example. The ligands effectively provide an intralayer confinement for charge carriers resulting in a 2D electronic structure, even in multilayered assemblies. Air-stable metal organic chalcogenides hybrid quantum wells have recently been found to host tightly bound 2D excitons with strong optical anisotropy in a bulk matrix. Here, we investigate the excited carrier dynamics in the prototypical metal organic chalcogenide [AgSePh] ∞ , disentangling three excitonic resonances by low temperature transient absorption spectroscopy. Our analysis suggests a complex relaxation cascade comprising ultrafast screening and renormalization, inter-exciton relaxation, and self-trapping of excitons within few picoseconds. Finally, the ps-decay provided by the self-trapping mechanism may be leveraged to unlock the material's potential for ultrafast optoelectronic applications.

2D excitons↗

GaN/AlGaN 2DEGs in the quantum regime: Magneto-transport and photoluminescence to 60 tesla

Here, using high magnetic fields up to 60 T, we report magneto-transport and photoluminescence (PL) studies of a two-dimensional electron gas (2DEG) in a GaN/AlGaN heterojunction grown by molecular-beam epitaxy. Transport measurements demonstrate that the quantum limit can be exceeded (Landau level filling factor v <1) and show evidence for the v =2/3 fractional quantum Hall state. Simultaneous optical and transport measurements reveal synchronous quantum oscillations of both the PL intensity and the longitudinal resistivity in the integer quantum Hall regime. PL spectra directly reveal the dispersion of occupied Landau levels in the 2DEG and, therefore, the electron mass. These results demonstrate the utility of high (pulsed) magnetic fields for detailed measurements of quantum phenomena in high-density 2DEGs.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Structural and physical properties of 99 complex bulk chalcogenides crystals using first-principles calculations

Chalcogenide semiconductors and glasses have many applications in the civil and military fields, especially in relation to their electronic, optical and mechanical properties for energy conversion and in enviormental materials. However, they are much less systemically studied and their fundamental physical properties for a large class chalcogenide semiconductors are rather scattered and incomplete. Here, we present a detailed study using well defined first-principles calculations on the electronic structure, interatomic bonding, optical, and mechanical properties for 99 bulk chalcogenides including thirteen of these crytals which have never been calculated. Due to their unique composition and structures, these 99 bulk chalcogenides are divided into two main groups. The first group contains 54 quaternary crystals with the structure composition (A2BCQ4) (A = Ag, Cu; B = Zn, Cd, Hg, Mg, Sr, Ba; C = Si, Ge, Sn; Q = S, Se, Te), while the second group contains scattered ternary and quaternary chalcogenide crystals with a more diverse composition (AxByCzQn) (A = Ag, Cu, Ba, Cs, Li, Tl, K, Lu, Sr; B = Zn, Cd, Hg, Al, Ga, In, P, As, La, Lu, Pb, Cu, Ag; C = Si, Ge, Sn, As, Sb, Bi, Zr, Hf, Ga, In; Q = S, Se, Te; x=1, 2, 3; y=0, 1, 2, 5; z=0, 1, 2 and n=3, 4, 5, 6, 9). Moreover, the total bond order density (TBOD) is used as a single quantum mechanical metric to characterize the internal cohesion of these crystals enabling us to correlate them with the calculated properties, especially their mechanical properties. This work provides a very large database for bulk chalcogenides crucial for the future theoretical and experimental studies, opening opportunities for study the properties and potential application of a wide variety of chalcogenides.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Pressure-stimulus-responsive behaviors of core–shell InP/ZnSe nanocrystals: remarkable piezochromic luminescence and structural assembly

Piezochromic luminescence materials with optical properties can be adjusted (the colors most sensitive to the human eye range from red to green) to provide powerful means for information acquisition in various applications. Inorganic quantum dots, typically based on heavy metals such as cadmium and lead, have congenital advantages as luminescence materials, including strong inoxidizability and excellent photoelectric properties. However, small band-gap shifts under pressure have hindered the development of inorganic-based piezochromic materials. In this study, we combined in situ high-pressure photoluminescence (PL) and absorption measurements with synchrotron X-ray scattering spectra to elucidate the remarkable modulation of optical properties and morphologies by pressure, particularly that of the piezochromic luminescence, in all-inorganic core–shell InP/ZnSe nanocrystals (NCs). We observed a stepwise PL color change from red to green, and an ultrabroad bandgap tunability of 0.46 eV was observed from 1.99 to 2.45 eV in the pressure range of 14.2 GPa for InP/ZnSe NCs. Moreover, two-dimensional (2D) InP/ZnSe nanosheets were synthesized by the stress-driven attachment of nanoparticles. These results demonstrate the ability of the pressure-stimulus response to trigger remarkable piezochromic luminescence and 2D nanosheet assembly in InP/ZnSe NCs, which paves the way for new applications of all-inorganic InP-based semiconductor NCs.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Ligand Desorption and Fragmentation in Oleate-Capped CdSe Nanocrystals under High-Intensity Photoexcitation

Semiconductor nanocrystals (NCs) offer prospective use as active optical elements in photovoltaics, light-emitting diodes, lasers, and photocatalysts due to their tunable optical absorption and emission properties, high stability, and scalable solution processing, as well as compatibility with additive manufacturing routes. Over the course of experiments, during device fabrication, or while in use commercially, these materials are often subjected to intense or prolonged electronic excitation and high carrier densities. The influence of such conditions on ligand integrity and binding remains underexplored. Here, in this study, we expose CdSe NCs to laser excitation and monitor changes in oleate that is covalently attached to the NC surface using nuclear magnetic resonance as a function of time and laser intensity. Higher photon doses cause increased rates of ligand loss from the particles, with upward of 50% total ligand desorption measured for the longest, most intense excitation. Surprisingly, for a range of excitation intensities, fragmentation of the oleate is detected and occurs concomitantly with formation of aldehydes, terminal alkenes, H 2 , and water. After illumination, NC size, shape, and bandgap remain constant although low-energy absorption features (Urbach tails) develop in some samples, indicating formation of substantial trap states. The observed reaction chemistry, which here occurs with low photon to chemical conversion efficiency, suggests that ligand reactivity may require examination for improved NC dispersion stability but can also be manipulated to yield desired photocatalytically accessed chemical species.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A room-temperature polarization-sensitive CMOS terahertz camera based on quantum-dot-enhanced terahertz-to-visible photon upconversion

Detection of terahertz (THz) radiation has many potential applications, but presently available detectors are limited in many aspects of their performance, including sensitivity, speed, bandwidth and operating temperature. Most do not allow the characterization of THz polarization states. Recent observation of THz-driven luminescence in quantum dots offers a possible detection mechanism via field-driven interdot charge transfer. Here, we demonstrate a room-temperature complementary metal–oxide–semiconductor THz camera and polarimeter based on quantum-dot-enhanced THz-to-visible upconversion mechanism with optimized luminophore geometries and fabrication designs. Besides broadband and fast responses, the nanoslit-based sensor can detect THz pulses with peak fields as low as 10 kV cm–1. A related coaxial nanoaperture-type device shows a to-date-unexplored capability to simultaneously record the THz polarization state and field strength with similar sensitivity.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Ultrafast carrier dynamics in terahertz photoconductors and photomixers: beyond short-carrier-lifetime semiconductors

Abstract Efficient terahertz generation and detection are a key prerequisite for high performance terahertz systems. Major advancements in realizing efficient terahertz emitters and detectors were enabled through photonics-driven semiconductor devices, thanks to the extremely wide bandwidth available at optical frequencies. Through the efficient generation and ultrafast transport of charge carriers within a photo-absorbing semiconductor material, terahertz frequency components are created from the mixing products of the optical frequency components that drive the terahertz device – a process usually referred to as photomixing. The created terahertz frequency components, which are in the physical form of oscillating carrier concentrations, can feed a terahertz antenna and get radiated in case of a terahertz emitter, or mix with an incoming terahertz wave to down-convert to DC or to a low frequency photocurrent in case of a terahertz detector. Realizing terahertz photoconductors typically relies on short-carrier-lifetime semiconductors as the photo-absorbing material, where photocarriers are quickly trapped within one picosecond or less after generation, leading to ultrafast carrier dynamics that facilitates high-frequency device operation. However, while enabling broadband operation, a sub-picosecond lifetime of the photocarriers results in a substantial loss of photoconductive gain and optical responsivity. In addition, growth of short-carrier-lifetime semiconductors in many cases relies on the use of rare elements and non-standard processes with limited accessibility. Therefore, there is a strong motivation to explore and develop alternative techniques for realizing terahertz photomixers that do not rely on these defect-introduced short-carrier-lifetime semiconductors. This review will provide an overview of several promising approaches to realize terahertz emitters and detectors without short-carrier-lifetime semiconductors. These novel approaches utilize p-i-n diode junctions, plasmonic nanostructures, ultrafast spintronics, and low-dimensional materials to offer ultrafast carrier response. These innovative directions have great potentials for extending the applicability and accessibility of the terahertz spectrum for a wide range of applications.

36 MATERIALS SCIENCE↗

Magnetic-field-induced Wigner crystallization of charged interlayer excitons in van der Waals heterostructures

Abstract Ever since its inception, coherent excited states of semiconductors have been the focus of semiconductor materials research to evolve into a vibrant field of low-dimensional solid-state physics. The field is gaining new momentum these days due to emerging transdimensional semiconductors such as van der Waals bound layers of transition metal dichalcogenides (TMDs) of controlled thickness. Here, we develop the theory of magnetic-field-induced Wigner crystallization for charged interlayer excitons (CIE) discovered recently in TMD heterobilayers. We derive the ratio of the potential interaction energy to the kinetic energy for the many-particle CIE system in the perpendicular magnetostatic field of an arbitrary strength and predict the crystallization effect in the strong field regime. We show that magnetic-field-induced Wigner crystallization and melting of CIEs can be observed in magneto-photoluminescence experiments with TMD bilayers of systematically varied electron-hole doping concentrations. Our results advance the capabilities of this new generation of transdimensional quantum materials.

36 MATERIALS SCIENCE↗

Ultrafast Spin Crossover in a Room-Temperature Ferrimagnet: Element-Specific Spin Dynamics in Photoexcited Cobalt Ferrite

Transition metal complexes capable of photoinduced spin crossover have been greatly investigated because of their potential to enable ultrafast optical control of information processing. Yet, any real application of photoswitchable molecules requires that spin crossover be paired with additional functionality such as long-range magnetic order. Important advances combining these functions are notably reported for a number of bimetallic Prussian Blue analogues; however, to date, PBA-based magnetic photoswitches can only operate below 150 K due to loss of magnetic order. In contrast, cobalt ferrite is a ferrimagnetic semiconductor with a Curie temperature of 790 K and extremely favorable magnetic properties by comparison to state-of-the-art PBAs. The mixed valence electronic structure of cobalt ferrite is reminiscent of cobalt–iron PBA, which is a well-known photoswitch. To investigate the potential for photoswitching in this material, we employ transient XUV spectroscopy to probe charge and spin dynamics with element-specific resolution on the femtosecond time scale. Results show that 400 nm light excites a metal-to-metal charge transfer transition, which drives the crossover of high-spin Co 2+ to low-spin Co 3+ with a time constant of 405 ± 29 fs and an internal quantum efficiency of unity. This result establishes the existence of efficient photoswitching in a new class of robust ferrimagnetic spinel ferrites.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Screening of hot electrons in the ferroelectric semiconductor In 2 Se 3

We report that in a conventional semiconductor, electrons (e) scatter efficiently with longitudinal-optical phonons (ph LO ) via the Fröhlich interaction, e.g., in polaron formation or hot-electron cooling. Recent studies on lead halide perovskites have suggested that the Fröhlich interaction may be sufficiently screened by the polar lattice. Here we show that hot-electron cooling in a layered ferroelectric semiconductor In 2 Se 3 slows down by 50% as temperature is increased from 115 to 387 K; this decrease is about four times more than that predicted by the Fröhlich model. We suggest that screening of Fröhlich interaction by polar domains or fluctuations in the ferroelectric semiconductor may be responsible for the reduced e-ph LO scattering. Such enhanced screening in polar materials featuring anharmonic lattice instability may also reduce carrier scattering with other charge carriers or with charged defects, leading to improved optoelectronic properties.

36 MATERIALS SCIENCE↗

Vector Electrometry in a Wide-Gap-Semiconductor Device Using a Spin-Ensemble Quantum Sensor

Nitrogen-vacancy (N-V) centers in diamond work as a quantum electrometer. Using an ensemble state of N-V centers, we propose vector electrometry and demonstrate measurements in a diamond electronic device. A transverse electric field applied to the N-V axis under a high voltage is measured, while applying a transverse magnetic field. The response of the energy-level shift against the electric field is significantly enhanced compared with that against an axial magnetic field. Repeating the measurement of the transverse electric field for multiple N-V axes, our team obtains the components of the electric field generated in the device.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Generation of nanosecond THz pulses using a high gain ring resonator with a semiconductor switch

A 250 GHz quasi-optical ring resonator consisting of an input coupler and three mirrors has been designed and tested. A low-loss silicon wafer in the ring provides output coupling of the stored power when irradiated by a pulse from a 532 nm laser. The ring created 5.8 ns, 268 mW output power pulses when excited by a 17 mW, 250 GHz continuously operating input source, achieving a power gain of 16. In a fully tuned ring, higher gain is achievable. If the ring was used with a pulsed input source having a pulse length of several times the fill time, the ring could be used as an efficient pulse compressor with similar high gain. The resonator has a wide range of applications, including, at low power, spectroscopy and, at high power, testing of accelerator structures and materials.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Optically thick GaInAs/GaAsP strain-balanced quantum-well tandem solar cells with 29.2% efficiency under the AM0 space spectrum

GaAs is often used as a multijunction subcell due to its high material quality on GaAs substrates, despite having a non-optimal bandgap. The bandgap can be beneficially reduced using many layers of thin, strain-balanced GaInAs in a superlattice or quantum well device, but achieving excellent carrier collection without increased recombination has proven challenging. Here, we develop and demonstrate high performance, optically thick GaInAs/GaAsP strain-balanced solar cells. Excellent material quality is achieved in thick superlattices by using growth conditions that limit progressive thickness and composition fluctuations. Bandgap-voltage offsets as low as 0.31V are shown in superlattice cells using thin, highly strained GaP barriers. Optically thick superlattice cells with over 2500 nm of total GaInAs in the depletion region are developed, enabling 3.8 mA/cm 2 of extra photocurrent beyond the GaAs band edge under the AM0 space spectrum. Optimized superlattice solar cells are incorporated into two-junction devices that achieve 29.2% efficiency under the AM0 space spectrum due to their improved bandgap combination and high subcell voltages.

14 SOLAR ENERGY↗

Response of CR-39 nuclear track detectors to protons with non-normal incidence

This paper presents data from experiments with protons at non-normal incidence to CR-39 nuclear track detectors, analyzing the properties of detection efficiency, proton track diameter, track contrast, and track eccentricity. Understanding the CR-39 response to protons incident at an angle is important for designing charged particle detectors for inertial confinement fusion (ICF) applications. This study considers protons with incident energies less than 3 MeV. In this regime, an incident angle of 10° has no effect on CR-39 detection efficiency, and >85% detection efficiency is preserved up through 25° in the range of 1.0 MeV–2.1 MeV. For ICF applications, incident angles above 30° are deemed impractical for detector design due to significant drops in proton detection at all energies. We observe significant reductions in detection efficiency compared to theoretical predictions, particularly at low energies where proton tracks are etched away. The proton track diameter measured by the scan system is observed to decrease with higher incident angles. The track diameters are analyzed with two fitting models, and it is shown that the diameter–energy relation can be fit with the existing models at angles up to 30° . The optical contrast of the tracks tends to increase with the angle, meaning that the tracks are fainter, and a larger increase is observed for higher energies. Eccentricity, a measure of how elongated proton tracks are, increases with the incident angle and drops after the critical angle. The lowest energy tracks remain nearly circular even at higher angles.

47 OTHER INSTRUMENTATION↗

AlGaInAs/InP semiconductor lasers with an ultra-narrow waveguide and an increased electron barrier

Semiconductor lasers based on AlGaInAs/InP heterostructures with an ultra-narrow waveguide and an increased electron barrier layer are developed. It is shown that the use of this waveguide in conjunction with profiled doping ensures a balance between internal optical losses and heat resistance. Additional use of strained wide-bandgap layers as blocking barriers limiting electron leakage from the active region makes it possible to increase the output power at the same pump current. The developed lasers with a stripe contact 100 μm wide demonstrate at room temperature an output optical power of 4.0 – 4.4 W (pump current 14 A) in a continuous-wave regime and 15 – 17 W (100 A) in a pulsed regime (100 ns, 1 kHz) at wavelengths of 1450 – 1500 nm. (paper)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗