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At least 19 records

Synthesis and characterization of amorphous Fe2.75Dy-oxide thin films demonstrating room-temperature semiconductor, magnetism, and optical transparency

Recently, amorphous/disordered oxide thin films made from Fe and lanthanides like Dy and Tb have been reported to have a rich set of magnetic, optical, and electronic properties, as well as room-temperature magneto-electric coupling with multiferroics [A. Malasi et al., Sci. Rep. 5, 18157 (2015); H. Taz et al., Sci. Rep. 6, 27869 (2016); and H. Taz et al., Sci. Rep. 10, 1–10 (2020)]. Here, we report the synthesis and detailed characterization of Fe2.75Dy-oxide thin films prepared on various substrates using electron beam co-evaporation. The structure, chemistry, electric, magnetic, and optical properties were studied for the as-prepared and annealed (373 K, in air, 1 h) films of thickness 40 nm. High resolution transmission electron microscopy and electron diffraction study showed that the films were amorphous in both the as-prepared and annealed states. The electron energy-loss spectroscopy studies quantified that metal oxygen stoichiometry changed from Fe2.75Dy-O1.5 to Fe2.75Dy-O1.7 upon annealing. Synchrotron-based x-ray absorption spectroscopy investigation confirmed that the as-prepared films were highly disordered with predominantly metallic Fe and Dy states that became slightly oxidized with annealing in air. The as-prepared amorphous films demonstrated significantly high value of ordinary (∼10 cm2/V s) and anomalous (∼102 cm2/V s) Hall mobility and high electrical conductivity of ∼103 S/cm at room temperature. The cryogenic magnetic property measurement shows two-step magnetization below 200 K, suggesting exchange-spring magnetic interaction. The nature of the field cooled and zero-field cooled curves suggested a spin-glass like transition between 78 K and 80 K, with a characteristic broad peak. The Tauc plot analysis from optical transmission spectra confirms the existence of an optical bandgap of ∼2.42 eV that increased slightly to ∼2.48 eV upon annealing. This rich set of transport, optical, and magnetic properties in these thin films is very exciting and points to potential applicability in low-cost multifunctional devices requiring a combination of transparent, semiconducting, and magnetic responses, such as in spintronics.

Prasad Koirala, Krishna (ORCID:000000029137917X)↗

Role of Selenium in CdZnTeSe as a Defect Engineering Agent

Cadmium zinc telluride (CdZnTe) with 10 atomic % Zn has been the material of choice for room-temperature semiconductor compact X- and gamma-ray detector applications for over three decades. Despite its commercial success as the most desirable room-temperature semiconductor radiation detection material, CdZnTe (CZT) suffers from a lack of compositional homogeneity on both the micro- and macroscales and the presence of high concentrations of performance-limiting defects such as subgrain boundary networks (dislocation walls) and secondary phases (Te-rich inclusions). Random distributions of these defects in the CZT matrix result in the spatial inhomogeneity of the material’s charge-transport properties. The recently discovered quaternary Cd x Zn 1-x Te 1-y Se y (CZTS) has experienced remarkable advances in its material properties, with highly reduced defects and higher compositional homogeneity. This book chapter focuses on the presence of performance-limiting defects in CZT that have thus far hindered the yield and cost of high-quality detectors and restricted their widespread deployment for a variety of potential applications, particularly for their use as large-volume gamma detectors, where the demands on material perfection are significantly greater. This chapter also provides an overview of the recent developments in the quaternary material CZTS, particularly the effects of selenium (Se) in the CZTS matrix on the defect engineering of the quaternary alloy material and the advancement of CZTS as a potential next-generation detector operable at room temperature.

Roy, Utpal N.↗

Impact of substrates and quantum effects on exciton line shapes of 2D semiconductors at room temperature

Exciton resonances in monolayer transition-metal dichalcogenides (TMDs) provide exceptionally strong light–matter interaction at room temperature. Their spectral line shape is critical in the design of a myriad of optoelectronic devices, ranging from solar cells to quantum information processing. However, disorder resulting from static inhomogeneities and dynamical fluctuations can significantly impact the line shape. Many recent works experimentally evaluate the optical properties of TMD monolayers placed on a substrate and the line shape is typically linked directly to the material’s quality. Here, we highlight that the interference of the substrate and TMD reflections can strongly influence the line shape. We further show how basic, room-temperature reflection measurements allow investigation of the quantum mechanical exciton dynamics by systematically controlling the substrate reflection with index-matching oils. By removing the substrate contribution with properly chosen oil, we can extract the excitonic decay rates including the quantum mechanical dephasing rate. The results provide valuable guidance for the engineering of exciton line shapes in layered nanophotonic systems.

2D semiconductor↗

Using 3D position sensitivity to reveal response non-uniformities in CdZnTe, TlBr, and CsPbBr 3 detectors

Position sensitivity enables the correction of response non-uniformities in room-temperature semiconductor detectors caused by crystal defects and other factors. It can also be used to pinpoint the exact location of crystal defects responsible for the response variations. This work describes a technique for revealing and visualizing the detector regions affecting the charge collection efficiency in CdZnTe (CZT), TlBr, and CsPbBr 3 detectors configured as position-sensitive virtual Frisch-grid (VFG) devices. The technique correlates the photopeak events in energy spectra with their spatial distributions inside the detectors using the position information. By selecting the events from narrow energy intervals within a photopeak, we can visualize the detector volumes with particular charge collection efficiencies, which, in turn, correlate with the locations of electrode and crystal defects. Here, we demonstrate this technique in several examples. Columnar structures in the volume plots (position distribution maps) are consistent with signal losses near or at the anode in selected samples of CZT and TlBr. Structures exhibiting a distinct depth dependence are consistent with grain boundaries or other crystal defects.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Ultrafast Waveguiding Quantum Dot Scintillation Detector

Picosecond timing of energetic charged particles and photons is a challenge for many high-energy physics and medical applications. InAs Quantum Dots (QDs) embedded in GaAs matrix are expected to have unsurpassed scintillation properties. The advantages come from highly efficient energy conversion, as well as from fast electron capture and radiative recombination in QDs. Here, we present design considerations and demonstration of an ultrafast, high photon yield room-temperature semiconductor scintillator. Due to the high refractive index of GaAs, the scintillator is fabricated in the form of a20 μm thick planar waveguide with an integrated InGaAs photodiode. QD luminescence of about 60% efficiency at room temperature has been shown, and modal attenuation stabilized at 1 cm -1 . Scintillation responses from 5.5 MeV alpha particles show an extremely fast decay time of 280 ps, a collection efficiency of 11% and a time resolution of 60 ps. This data confirms the unique potential properties of this scintillation detector.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Production-Ready CsPbBr3 Module Fabrication

The purpose of this SBIR was to work on evaluation, development, and testing of CsPbBr3 semiconductors for use in commercial gamma-ray detection. The overarching goal was to demonstrate the capability to fabricate functional detectors through resources available to H3D, Inc in pursuit of an alternative to CdZnTe for room-temperature semiconductor detectors. Throughout the project, CdZnTe crystals from Redlen were used as a control group to demonstrate whether the fabrication processes could produce reasonable results. The CdZnTe crystals were diced into roughly 6 mm x 6 mm x 4.5 mm pieces and electrodes were evaporated onto planar faces. In one case, pixels were patterned through a laser ablation method; in the other, a rudimentary pixel shadow-mask was fabricated, and the pixels were generated in the evaporation process. A 16 mm x 16 mm x 14 mm CsPbBr3 crystal was diced into four smaller crystals. These CsPbBr3 had electrodes applied in a similar way to the CdZnTe samples with a rudimentary mask used for pixels on the cathode. Tested CdZnTe pieces were found to generally function with reasonable, low-energy performance. CsPbBr3 crystals were found to be non-functional under forward bias with a large dark-current. A separate attempt, using reverse bias in a non-H3D, Inc test system, observed a dark current similar to previous observations, and some active pixels but no waveforms were observed.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

CdZnTeSe: Recent advances for radiation detector applications

The quest for cost-effective, high performing room temperature semiconductor detector (RTSD) materials for high energy gamma rays has been continuing for more than three decades. The requirements for RTSD materials, however, are more stringent as compared to other applications unrelated to detection of X- and gamma-rays, mainly due to the requirement of thick detectors for sufficient absorption of high-energy electromagnetic radiation and excellent charge-transport properties. The II-VI compound CdZnTe (CZT) with the composition of 10 atomic % Zn (Cd0.9Zn0.1Te) has been the material of choice over the past several years, and it has dominated the commercial market for RTSD materials and detectors. Despite its commercial success as a room temperature radiation detection material, CZT suffers from a lack of compositional homogeneity on both a micro- and macro-scale and the presence of high concentrations of sub-grain boundary (dislocation walls) networks and secondary phases (Te-rich inclusions). This chapter focuses on the presence of performance-limiting defects in CZT that hinder the yield and elevate the cost of high-quality detectors. The presence of such performance-limiting defects has restricted widespread deployment of CZT for a variety of potential applications, particularly for uses of relatively large detectors where the demands on material perfection are significantly greater. In the recent past, replacing some of the tellurium with selenium in the CZT matrix was found to be very effective in drastically reducing the Te-rich secondary phases and dislocation networks, plus

Roy, Utpal N.↗

Cadmium Magnesium Telluride for Next Generation X-Ray Free Electron Laser, Synchrotron and Many Other Applications

We developed a picosecond photodetector based on our Bridgman grown and specially engineered Cadmium Magnesium Telluride (Cd 1-x Mg x Te) single crystal that is sensitive to both optical and x-ray pulses for coarse timing in Free Electron Laser applications. Cd 1-x Mg x Te is a wide bandgap semiconductor material with potential applications, not only in optoelectronics, but also in particle physics as an intense pulse radiation detector for bremsstrahlung, X-ray/gamma ray radiation, thermal neutrons, and medical imaging. However, for femtosecond optical and x-ray cross correlation, the material has to have very short lifetime, a condition that is opposite to that required for nuclear spectroscopy applications. At the same time, the material also needs to have very low bulk leakage current, in the 0.10 pA range. Hence the ability to tailor or engineer the material is very crucial. In this paper, picosecond response and the crystal growth of this specially engineered cadmium magnesium telluride material will be presented. Other material characterization and transient measurements will also be discussed along with room temperature semiconductor detector performance for other nuclear radiation detection applications.

36 MATERIALS SCIENCE↗

Cadmium Magnesium Telluride for Next-Generation X-Ray Free Electron Laser, Synchrotron, and Many Other Applications

We developed a picosecond photodetector based on our Bridgman-grown and specially engineered cadmium magnesium telluride (Cd 1–x MgxTe) single crystal that is sensitive to both optical and X-ray pulses for coarse timing in free-electron laser applications. Cd 1–x MgxTe is a widebandgap semiconductor with potential applications, not only in optoelectronics, but also in particle physics as an intense pulse radiation detector for bremsstrahlung, X-ray/gamma-ray radiation, thermal neutrons, and medical imaging. For femtosecond optical and X-ray crosscorrelation, the material must have a very short lifetime, a condition that is opposite to that required for nuclear spectroscopy applications. At the same time, the material also needs to have a very low bulk leakage current, in the 10–90 nA range for voltages to even 1000 V. Hence, the ability to tailor or engineer the material is very crucial. Picosecond response and the crystal growth of this specially engineered Cd 1–x MgxTe material are presented. Furthermore, other characterization and transient measurements are discussed along with room-temperature semiconductor detector performance for other nuclear radiation detection applications.

36 MATERIALS SCIENCE↗

Inorganic Halide Perovskitoid TlPbI 3 for Ionizing Radiation Detection

Room temperature semiconductor detector (RTSD) materials for γ-ray and X-ray radiation are in great demand for the nonproliferation of nuclear materials as well as for biomedical imaging applications. Halide perovskites have attracted great attention as emerging and promising RTSD materials. In this contribution, the material synthesis, purification, crystal growth, crystal structure, photoluminescence properties, ionizing radiation detection performance, and electronic structure of the inorganic halide perovskitoid compound TlPbI 3 are reported on. This compound crystallizes in the ABX 3 non-perovskite crystal structure with a high density of d = 6.488 g·cm –3 , has a wide bandgap of 2.25 eV, and melts congruently at a low temperature of 360 °C without phase transitions, which allows for facile growth of high quality crystals with few thermally-activated defects. High-quality TlPbI 3 single crystals of centimeter-size are grown using the vertical Bridgman method using purified raw materials. A high electrical resistivity of ≈10 12 Ω·cm is readily obtainable, and detectors made of TlPbI 3 single crystals are highly photoresponsive to Ag K α X-rays (22.4 keV), and detects 122 keV γ-rays from 57 Co radiation source. The electron mobility-lifetime product µ e τ e was estimated at 1.8 × 10 –5 cm 2 ·V –1 . A high relative static dielectric constant of 35.0 indicates strong capability in screening carrier scattering and charged defects in TlPbI 3 .

36 MATERIALS SCIENCE↗

Extreme γ –Ray Radiation Tolerance of Spectrometer–Grade CsPbBr 3 Perovskite Detectors

The perovskite compound CsPbBr 3 has recently been discovered as a promising room-temperature semiconductor radiation detector, offering an inexpensive and easy-to-manufacture alternative to the current benchmark material Cd 1–x Zn x Te (CZT). The performance of CsPbBr 3 sensors is evaluated under harsh conditions, such as high radiation doses often found in industrial settings and extreme radiation in space. Results show minimal degradation in detector performance after exposure to 1 Mrad of Co-60 gamma radiation, with no significant change to energy resolution or hole mobility and lifetime. Additionally, many of the devices are still functional after being exposed to a 10 Mrad dose over 3 days, and those that do not survive can still be refabricated into working detectors. Notably, these results suggest that the failure mode in these devices is likely related to the interface between the electrode and material and their reaction, or the electrode itself and not the material itself. Overall, the study suggests that CsPbBr 3 has high potential as a reliable and efficient radiation detector in various applications, including those involving extreme fluxes and energies of gamma-ray radiation.

36 MATERIALS SCIENCE↗

Assessment of Blocking Contacts in Suppressing Polarization Effects in CsPbBr 3 Perovskite Detectors

The CsPbBr 3 perovskite has garnered significant attention as a room-temperature semiconductor for hard radiation detection due to straightforward synthesis, scalable crystal growth, low cost, and excellent energy resolution. However, despite these advantages, at ambient temperature, CsPbBr 3 devices may experience performance deterioration and irreversible failure due to “polarization” induced by electromigration of ions to electrical connections on the device. In this study, we tested several contact materials and their optimization deposition techniques to assess the stability of high-performance CsPbBr 3 γ-ray detectors. Metals, with low work functions (Ti, In, Sn, Sb, Pb, Bi, Al, Au, and TiC) and high-work-function (Au or Pt) contacts, were used to form different Schottky junctions using vacuum thermal evaporation, electron-beam evaporation, and sputtering methods. These detectors were tested in intermittent and continuous modes to assess their stability. Among the tested detectors, the Bi/CLB/Pt electrode configuration demonstrated superior stability, operating effectively for 11 months under periodic testing and 16 days under continuous testing. In contrast, other configurations functioned only for a few months under intermittent conditions. Upon incorporating a ~40-nm-thick TiC passivation layer on the anode side (Bi/TiC/CLB/Pt), the CLB device operated continuously for 36 days without degradation. In many cases, the failure mode of the devices was due to the degradation of the anode. Here, the chemical changes in the fresh and deteriorated anodes were characterized using scanning electron microscopy and energydispersive X-ray spectroscopy

CsPbBr3 perovskite↗

Monolayer Vanadium‐Doped Tungsten Disulfide: A Room‐Temperature Dilute Magnetic Semiconductor

Abstract Dilute magnetic semiconductors (DMS), achieved through substitutional doping of spin‐polarized transition metals into semiconducting systems, enable experimental modulation of spin dynamics in ways that hold great promise for novel magneto–electric or magneto–optical devices, especially for two‐dimensional (2D) systems such as transition metal dichalcogenides that accentuate interactions and activate valley degrees of freedom. Practical applications of 2D magnetism will likely require room‐temperature operation, air stability, and (for magnetic semiconductors) the ability to achieve optimal doping levels without dopant aggregation. Here, room‐temperature ferromagnetic order obtained in semiconducting vanadium‐doped tungsten disulfide monolayers produced by a reliable single‐step film sulfidation method across an exceptionally wide range of vanadium concentrations, up to 12 at% with minimal dopant aggregation, is described. These monolayers develop p‐type transport as a function of vanadium incorporation and rapidly reach ambipolarity. Ferromagnetism peaks at an intermediate vanadium concentration of ~2 at% and decreases for higher concentrations, which is consistent with quenching due to orbital hybridization at closer vanadium–vanadium spacings, as supported by transmission electron microscopy, magnetometry, and first‐principles calculations. Room‐temperature 2D‐DMS provide a new component to expand the functional scope of van der Waals heterostructures and bring semiconducting magnetic 2D heterostructures into the realm of practical application.

36 MATERIALS SCIENCE↗

Determination of electron-hole pair creation energy in Cd 0.9 Zn 0.1 Te 0.98 Se 0.02 quaternary semiconductor for room-temperature gamma-ray detection

We report the first-time measurement of the electron-hole pair (ehp) creation energy (W ehp ) in novel Cd 0.9 Zn 0.1 Te 0.98 Se 0.02 (CZTS) quaternary semiconductor. CZTS in single crystalline form is poised to be the future of large-volume room-temperature gamma-ray detectors due to its excellent compositional homogeneity with highly reduced defects, high-Z (atomic number) constituents, wide bandgap (1.6 eV), and superior charge transport properties. Despite a great deal of study of the material and device properties since its inception, the W ehp in CZTS has not been measured experimentally. Accurate determination of W ehp is essential for calibration of the spectrometer and other theoretical calculations. In this study we have used an absolute calibration approach, which is based on an iterative approach that yields the Wehp as the best-fit parameter. Using a 241 Am alpha emitting radioisotope and a planar CZTS detector, the Wehp in CZTS was calculated to be 4.47 eV. The obtained value has been validated by accurately predicting the peak energy for gamma rays emitted by a 137 Cs source and read by a CZTS detector with different dimensions. The dependences of the calculated W ehp value on the detector dimensions, type of interaction, and effect of charge trapping are also discussed.

42 ENGINEERING↗

Semiconductor Behavior and Room Temperature Ferromagnetism in e-Beam Evaporated Co/TiO{sub 2} Multilayer Thin Films

The Co/TiO{sub 2} multilayer thin films have been deposited by e-beam evaporation method on glass substrates in vacuum and annealed in air at 773 K for 1 h. The crystal structure, surface morphology, optical properties, electrical properties and magnetic properties of Co/TiO{sub 2} multilayer thin films have been systematically investigated. The results showed that the particle sizes were significantly reduced when the samples are annealed and the enlargement of particle size occurred when the samples thickness is increased. The spectroscopic analysis exhibited enhanced transmittance and higher optical band gap of annealed sample than the as-deposited one and it was decreased with sample thickness. The resistivity measurement confirmed resistivity decreament with temperature. Furthermore, by investigating the magnetic properties, room temperature ferromagnetism was observed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Electron–hole liquid in a van der Waals heterostructure photocell at room temperature

In semiconductors, photo-excited charge carriers exist as a gas of electrons and holes, bound electron–hole pairs (excitons), biexcitons and trions. At sufficiently high densities, the non-equilibrium system of electrons (e-) and holes (h + ) may merge into an electronic liquid droplet. Here, we report on the electron–hole liquid in ultrathin MoTe2 photocells revealed through multi-parameter dynamic photoresponse microscopy (MPDPM). By combining rich visualization with comprehensive analysis of very large data sets acquired through MPDPM, we find that ultrafast laser excitation at a graphene–MoTe 2 –graphene interface leads to the abrupt formation of ring-like spatial patterns in the photocurrent response as a function of increasing optical power at T = 297 K. The sudden onset to these patterns, together with extreme sublinear power dependence and picosecond-scale photocurrent dynamics, provide strong evidence for the formation of a two-dimensional electron–hole liquid droplet. The electron–hole liquid, which features a macroscopic population of correlated electrons and holes, may offer a path to room-temperature optoelectronic devices that harness collective electronic phenomena.

phonons, thermal conductivity, thermoelectric, spi↗