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Linker Contribution toward Stability of Metal–Organic Frameworks under Ionizing Radiation

Here, the effects of radiation on a series of UiO derivative metal–organic frameworks (MOFs) that contain the same zirconium hexamer node and similar organic linkers, UiO-66, UiO-66–NH 2 , UiO-66–OH, and NU-403, were examined using γ-rays and 5 MeV He ions. UiO-66, UiO-66–NH2, and UiO-66–OH contain aromatic linkers and are significantly more stable to radiation than NU-403. Of these, UiO-66 is the most radiation resistant, displaying crystalline features up to 47 MGy of He-ion irradiation. MOFs containing aromatic linkers functionalized by electron-donating groups, UiO-66–NH 2 and UiO-66–OH, retained crystalline features up to 19 MGy. NU-403 contains aliphatic rings and is the least radiation-resistant MOF studied here. NU-403 exhibits small changes in infrared spectra upon 3 MGy of γ-irradiation and significant damage upon 10 MGy of He-ion irradiation. Diffraction data revealed radiation-induced defect formation. Structural locations of radiation-induced breakdown were interrogated experimentally and via density functional theory. The results indicated changes in the carboxylate (-OCO) of the linker and μ 3 -OH vibrational modes, suggesting that introduction of an aliphatic linker into the MOF renders the connection between the linker and metal node most susceptible to radiation damage. This study reveals that the choice of the linker is crucial in designing a radiation-resistant MOF.

36 MATERIALS SCIENCE↗

Detecting ionizing radiation using halide perovskite semiconductors processed through solution and alternative methods

We report the direct detection of high-energy radiation such as X-rays and.-rays by semiconductors at room temperature is a challenging proposition that requires remarkably pure and nearly perfect crystals. The emergence of metal halide perovskites, defect-tolerant semiconductors, is reviving hope for new materials in this field after an almost 20 year hiatus. Metal halide perovskites, which combine exceptional optoelectronic properties, versatile chemistry and simple synthesis, are challenging traditional approaches for the development of novel semiconductors for detecting hard radiation. We discuss the relevant physical properties, promising materials, fabrication techniques and device architectures for high-performance, low-cost detectors by targeting next-generation semiconductors for radiation detection. We also present a perspective on the impact of such advances in future medical imaging applications.

36 MATERIALS SCIENCE↗

Spectroscopic Measurements and Models of Energy Deposition in the Substrate of Quantum Circuits by Natural Ionizing Radiation

Naturally occurring background radiation is a potential source of correlated decoherence events in superconducting qubits that will challenge error-correction schemes. In order to characterize the radiation environment in an unshielded laboratory representative of superconducting qubits’ environments, we performed broadband, spectroscopic measurements of background radiation events inside a millikelvin refrigerator. The spectrometer was designed to mimic the size and composition of a quantum circuit. Specifically, we measured the background radiation spectra in silicon substrates of two thicknesses, 500 and 1500 µm, and one area, 25 mm 2 . The observed spectra span energies from a few kilo-electron-volts up to nearly 10 MeV, are nearly featureless, and decrease in intensity by a factor of 40 000 between 100 keV and 3 MeV for the 500-µm substrate. We integrate the spectra to obtain the average event rates and deposited power levels. These quantities correspond to a rate of 0.023 events per second and a power of 4.9 keV s -1 , when counting events that deposit at least 40 keV for the 500-µm-thick substrate. We find that the cryogenic measurements are in good agreement with predictions based on simple measurements of the terrestrial gamma-ray flux outside the refrigerator, published models of cosmic-ray fluxes, a crude model of the cryostat, and radiation-transport simulations. This model requires no free parameters to predict the background radiation spectra in the silicon substrates. The agreement between measurements and predictions demonstrates that the model we present can be used to assess the relative contributions of terrestrial and cosmic-ray sources to background radiation interactions in silicon substrates of varying thickness. These spectroscopic measurements are performed with a novel combination of superconducting microresonators located on micromachined silicon islands that define the interaction volume with background radiation. The resonators transduce deposited energy to a readily detectable electrical signal. Microresonator readout closely resembles dispersive superconducting qubit readout, so similar devices—with or without micromachined islands—are suitable for integration with superconducting quantum circuits as detectors for background radiation events. For our specific laboratory conditions, we find that gamma-ray emissions from radioisotopes are responsible for the majority of events that deposit E < 1 ⁢Me⁢V. We present results demonstrating that the background radiation spectrum contains relevant contributions from cosmic-ray particles other than muons, particularly a tail of multi-mega-electron-volt events due to protons and neutrons. These observations suggest several paths to reducing the impact of background radiation on quantum circuits, supported by an empirically validated model for generating reliable predictions of radiation interactions with silicon substrates.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Disentangling the sources of ionizing radiation in superconducting qubits

Abstract Radioactivity was recently discovered as a source of decoherence and correlated errors for the real-world implementation of superconducting quantum processors. In this work, we measure levels of radioactivity present in a typical laboratory environment (from muons, neutrons, and $$\gamma $$ γ -rays emitted by naturally occurring radioactive isotopes) and in the most commonly used materials for the assembly and operation of state-of-the-art superconducting qubits. We present a GEANT-4 based simulation to predict the rate of impacts and the amount of energy released in a qubit chip from each of the mentioned sources. We finally propose mitigation strategies for the operation of next-generation qubits in a radio-pure environment.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗