Muonic X-ray Research Articles

Non-destructive Elemental Analysis of Lunar Materials with Negative Muon Beam at J-PARC

In the last decade, non-destructive elemental analysis using negative muon beams advanced significantly. This method can be used to determine the elemental composition of bulk materials without causing damage. In this study, we performed a negative muon irradiation experiment for a Northwest Africa 482 lunar meteorite (NWA482), which was installed in a stainless steel analysis chamber. The analysis chamber was filled with helium gas to suppress the background signals caused by air-scattering muons. The muonic X-rays from Al, Fe, Ca, Mg, Si, and O in the samples were detected using six high-purity germanium semiconductor detectors arranged around the analysis chamber. To correct the X-ray self-absorption effect of the samples, a Monte-Carlo simulation using Geant4 toolkit was used. Based on the quantitative analysis for muonic X-ray measurement with the correction application from the simulation, we successfully investigated the analytical sensitivity of each element in meteorites based on the NWA482 data.

Negative muons for the characterization of thin layers in Cultural Heritage artefacts

Muonic atom X-ray Emission Spectroscopy (µ-XES) is a novel technique based on the detection of high-energy X-rays emitted after the interaction of a negative muon beam with matter. Thanks to the multi-elemental range, negligible self-absorption of the x-rays and the possibility of performing depth profile studies, the technique is a very powerful probe for the analysis of cultural heritage artefacts. By tuning the energy of the incident muon beam, indeed, it is possible to investigate the different layers that constitute a sample. In this work, we report preliminary results of the analysis on two fire-gilded surfaces, in which the data analysis is coupled with Monte Carlo-based simulation software. Here, to perform a depth profile characterization, the samples were analysed at different beam energies (or momentum). Each of the resulting x-ray spectra was then analysed and compared with the output of the simulations software and a remarkably good agreement was reached. The results of the work are promising and with this approach, it will be possible to enhance the capability offered by the technique, both in terms of data analysis and data interpretation.

Developments of muonic X-ray measurement system for historical-cultural heritage samples in Japan Proton Accelerator Research Complex (J-PARC)

Negative muon elemental analysis, which can measure depth-wise elemental composition from 100 nm to several centimeters with a depth resolution of order µm, is a revolutionary technology that enables the nondestructive analysis of materials. In recent years, this technique has begun to apply to understand historical cultural heritage. We have studied the Japanese archaeological heritage to provide new insights into Japanese archaeological research. Here, we report the progress on development of intense (high speed) negative muon X-ray measurement system at KEK Muon Science Laboratory (MSL) in the Japan Proton Accelerator Research Complex (J-PARC). For this purpose, the efficiency of detectors (wide energy range and high resolution) were improved by preparing a high-purity multi-arrayed germanium semiconductor detectors (HP Ge) to detect one photon or less per muon pulse available in J-PARC. In addition, by increasing the number of detectors and suppressing the noise sources, we have succeeded to enhance the detection efficiency by about 10 times compared to conventional systems.

Non-Destructive Composition Identification for Mixtures of Iron Compounds Using a Chemical Environmental Effect on a Muon Capture Process

Abstract The non-destructive investigation of the chemical state of elements within a material is urgently needed in various scientific research fields. In recent years, non-destructive elemental analysis methods using muons have been developed. These methods identify elements by measuring muonic X-rays emitted from muonic atoms formed by the muon irradiation of the material. Interestingly, muonic atom formation processes are slightly influenced by the chemical state of the muon-capturing atom, and as a result, the muon capture probability of each element and the muonic X-ray emission intensity change depending on the chemical state. By utilizing this effect, it may be possible to know the chemical state at the same time as elemental analysis. In this study, the compositions of γ-Fe2O3 and Fe3O4 in an ironsand sample were determined using two approaches: muonic X-ray intensity ratios and muon capture ratios. The mixing ratios obtained from the two approaches were consistent with each other and consistent with results of the Mössbauer technique, a completely different analysis method. In this study, non-destructive chemical state analysis using muons was successfully demonstrated, and this method is promising for applications in various research fields.

Absolute Energy Measurements with Superconducting Transition-Edge Sensors for Muonic X-ray Spectroscopy at 44 keV

Superconducting transition-edge sensor (TES) microcalorimeters have great utility in x-ray applications owing to their high energy resolution, good collecting efficiency and the feasibility of being multiplexed into large arrays. In this work, we develop hard x-ray TESs to measure the absolute energies of muonic-argon ($\mu$-Ar) transition lines around 44 keV and 20 keV. TESs with sidecar absorbers of different heat capacities were fabricated and characterized for their energy resolution and calibration uncertainty. We achieved ~ 1 eV absolute energy measurement accuracy at 44 keV, and < 12 eV energy resolution at 17.5 keV.

Negative muons reveal the economic chaos of Rome’s AD 68/9 Civil Wars

During the AD 68/9 Civil Wars, Galba, Otho, Vitellius and then Vespasian fought for — and gained — control of the Roman Empire. Our textual sources suggest that this was a period of serious and sustained disruption. However, existing analyses of gold coinages produced in AD 68/9 show only a minor reduction in the purity of the gold coinage. Using X-ray fluorescence, we identify a number of heavily debased gold coins issued during the AD 68/9 Civil Wars, and many slightly debased coins issued in their immediate aftermath. We then confirm the interior composition of these coins totally non-destructively using muonic X-ray emission spectroscopy, thus eliminating hypothetical problems of ‘surface enrichment’ or compositional differences between ‘surface’ and ‘core’. Here we show that heavily debased Civil War gold coinages were indeed produced; that copper was used to debase Roman gold coins during this time, c. 185 years earlier than first shown; and that slightly debased gold coins were regularly issued in the years immediately after the Civil Wars. The metallurgical evidence from the gold coinage now allows us to show that the AD 68/9 Civil Wars caused significant and sustained disruption to the Roman economic system. More broadly, we have shown that muonic X-ray emission spectroscopy is a powerful tool for generating important archaeological conclusions from high-value cultural heritage objects that simply cannot be destructively analysed, but need to have their interior compositions sampled.

A study of the feasibility of coded aperture imaging technique for elemental analysis by muonic X-ray measurements based on Geant4 simulations

A novel method of muonic X-ray imaging based on the coded aperture imaging technique is developed. The image quality and detection rate of X-rays can be influenced by the number of detected counts (ND), mask size (thickness t and aperture size d) and sample-to-detector distance (DSD). A figure of merit (FoM) is introduced as an integral and quantitative indicator of these influences. The choice of optimal values of the parameters ND, t, d and DSD is achieved therefore by the comparison of respective FoM values. As compared to the conventional pinhole imaging technique, the coded aperture technique provides slightly better image quality and has a two orders of magnitude higher detection rate. Therefore, the FoM value for the coded aperture imaging technique is higher than that for the pinhole one by a factor not smaller than 1.67. Obtained results demonstrate that the coded aperture imaging technique has significant advantages for the applications for elemental analysis by muonic X-ray measurements.

A Novel Non-Destructive Technique for Cultural Heritage: Depth Profiling and Elemental Analysis Underneath the Surface with Negative Muons

Scientists, curators, historians and archaeologists are always looking for new techniques for the study of archaeological artefacts, especially if they are non-destructive. With most non-destructive investigations, it is challenging to measure beneath the surface. Among the vast board of techniques used for cultural heritage studies, it is difficult to find one able to give information about the bulk and the compositional variations, along with the depth. In addition, most other techniques have self-absorption issues (i.e., only surface sensitive) and limited sensitivity to low Z atoms. In recent years, more and more interest has been growing around large-scale facility-based techniques, thanks to the possibility of adding new and different insights to the study of material in a non-destructive way. Among them, muonic X-ray spectroscopy is a very powerful technique for material characterization. By using negative muons, scientists are able to perform elemental characterization and depth profile studies. In this work, we give an overview of the technique and review the latest applications in the field of cultural heritage.

Non-destructive 3D imaging method using muonic X-rays and a CdTe double-sided strip detector

Elemental analysis based on muonic X-rays resulting from muon irradiation provides information about bulk material composition without causing damage, which is essential in the case of precious or otherwise unreachable samples, such as in archeology and planetary science. We developed a three-dimensional (3D) elemental analysis technique by combining the elemental analysis method based on negative muons with an imaging cadmium telluride double-sided strip detector (CdTe-DSD) designed for the hard X-ray and soft gamma-ray observation. A muon irradiation experiment using spherical plastic samples was conducted at the Japan Proton Accelerator Research Complex (J-PARC); a set of projection images was taken by the CdTe-DSD, equipped with a pinhole collimator, for different sample rotation angles. The projection images measured by the CdTe-DSD were utilized to obtain a 3D volumetric phantom by using the maximum likelihood expectation maximization algorithm. The reconstructed phantom successfully revealed the 3D distribution of carbon in the bulk samples and the stopping depth of the muons. This result demonstrated the feasibility of the proposed non-destructive 3D elemental analysis method for bulk material analysis based on muonic X-rays.

Characterization of a Continuous Muon Source for the Non-Destructive and Depth-Selective Elemental Composition Analysis by Muon Induced X- and Gamma-rays

The toolbox for material characterization has never been richer than today. Great progress with all kinds of particles and interaction methods provide access to nearly all properties of an object under study. However, a tomographic analysis of the subsurface region remains still a challenge today. In this regard, the Muon Induced X-ray Emission (MIXE) technique has seen rebirth fueled by the availability of high intensity muon beams. We report here a study conducted at the Paul Scherrer Institute (PSI). It demonstrates that the absence of any beam time-structure leads to low pile-up events and a high signal-to-noise ratio (SNR) with less than one hour acquisition time per sample or data point. This performance creates the perspective to open this technique to a wider audience for the routine investigation of non-destructive and depth-sensitive elemental compositions, for example in rare and precious samples. Using a hetero-structured sample of known elements and thicknesses, we successfully detected the characteristic muonic X-rays, emitted during the capture of a negative muon by an atom, and the gamma-rays resulting from the nuclear capture of the muon, characterizing the capabilities of MIXE at PSI. This sample emphasizes the quality of a continuous beam, and the exceptional SNR at high rates. Such sensitivity will enable totally new statistically intense aspects in the field of MIXE, e.g., elemental 3D-tomography and chemical analysis. Therefore, we are currently advancing our proof-of-concept experiments with the goal of creating a full fledged permanently operated user station to make MIXE available to the wider scientific community as well as industry.

The muX project

The project is conducting a series of muonic X-ray measurements in medium- and high-Z nuclei at PSI, utilizing a high-purity germanium detector array, in-beam muon detectors, and a modern digital data-acquisition system. A novel hydrogen target for muon transfer was developed, enabling measurements with as little as a few micrograms of target material. First measurements with radioactive Cm and Ra targets were conducted, aimed at determining their nuclear charge radii. These serve as important input for upcoming atomic parity violation experiments. The apparatus is also used to perform a feasibility study of an atomic parity violation experiment with the 2s-1s2s−1s muonic X-ray transition. In addition, the setup has been made available for a wider range of nuclear, particle, and solid-state physics measurements.

Understanding Roman Gold Coinage Inside Out

The true purity of Roman silver coinage was hidden by enriching the surfaces of the coins. The question investigated here is whether Roman gold coins were also surfaced enriched. Two non-destructive techniques were employed to do this: X-ray fluorescence (XRF) and a ‘newer’ technique, muonic X-ray emission spectroscopy (μXES). For the latter, the momentum of the muons is controlled, allowing for the composition of the coin to be determined at various depths. Here we show that there is no surface enrichment of the Roman gold coins analysed. Furthermore, we show that XRF and μXES return congruent results at the near surface. This all supports the integrity of surface level analyses of Roman gold coins. We then discuss the broader applicability of our muon technique to the further study of Roman gold coinage, to the cultural heritage sector and to archaeological scientists more generally.

A novel challenge of nondestructive analysis on OGATA Koan's sealed medicine by muonic X-ray analysis.

OGATA Koan (1810-63) was a physician and the director of Tekijuku, and he contributed to Western medicine in the late Edo period. Osaka University preserves two of his medicine chests. One of the chests, which was used in his last years (the second chest) contained 22 glass bottles and 6 wooden cylinders. These bottles and cylinders contained formulated medicines; however, about half cannot be opened because of the long-term storage. It is necessary to comprehend the physical property of both the containers and their contents for investigation of this adequate preservation method; however, destructive analysis is not allowed. To analyze the medicines sealed in the glass bottles, we focused on muonic X-ray analysis, which has high transmittance. First, we certified the analytical methods using a historical medicinal specimen preserved in Osaka University. Thereafter, we applied the method on the bottles stored in the second chest. X-ray fluorescence identified the glass of those bottles to be lead potash glass. Among these bottles, we chose the bottle with the label "," which contains white powdered medication, for muonic X-ray analysis. We identified the contents of the medication in the glass to be Hg2Cl2. Through this study, we first applied muonic X-ray analysis on the medical inheritances and succeeded to detect the elements contained both in the container and in the contents of the sealed bottle. This would be a new method for nondestructive analysis of such cultural properties.

Transition-Edge Sensor Optimization for Hard X-ray Applications

Arrays of superconducting transition-edge sensor (TES) microcalorimeters are attractive for some X-ray experiments where the combination of higher collection efficiency than crystal spectrometers and much better energy resolution than semiconductor detectors is enabling. For hard X-ray (>2 keV) applications, a TES is often integrated with an extra absorber to extend its dynamic range, quantum efficiency and collecting area. For >100 keV applications, millimeter size absorbers have been manually attached to TES pixels after fabrication. At lower energies, the absorber size needs to be much smaller, because a large heat capacity degrades energy resolution. In that case, the absorber is directly electroplated or evaporated on the TES during the fabrication process. In this work, we present TES microcalorimeters optimized for the intermediate hard X-ray energy region (20 keV ~ 100 keV) that have thick absorbers directly deposited during the TES fabrication process. This microcalorimeter is designed to measure high-resolution muonic atom transition X-ray spectra as a method to study quantum electrodynamics (QED) effects. The absorber is comprised of evaporated gold and electroplated bismuth layers and is designed to optimize dynamic range, collecting efficiency, and energy resolution in the 20 keV to 45 keV energy range. A prototype with pure gold absorbers has been fabricated and characterized, in order to obtain a first experimental reference in the detector development process.

Construction of the Gaseous and Solid-State Targets for the Muon Capture Measuring System in 130Xe, 82Kr, and 24Mg

The description of the muon capture system units with different targets (gas and solid-state) is presented. Using the muon-event selection system and high-purity germanium (HPGe) detectors, precise measurements of the time-energy distributions following ordinary muon capture in the isotopically-enriched $^{130}$Xe, $^{82}$Kr, and $^{24}$Mg nuclei were performed. The optimal parameters of the muon capture measuring system to ensure maximum muon stops in the targets under study and to collect effective statistics during measurements are reported. The system makes it possible to separate muonic X-ray events from gamma radiation with high accuracy, which is critical in such studies, and it is also suitable for future measurements with other targets.

Using the Emission of Muonic X-rays as a Spectroscopic Tool for the Investigation of the Local Chemistry of Elements.

There are several techniques providing quantitative elemental analysis, but very few capable of identifying both the concentration and chemical state of elements. This study presents a systematic investigation of the properties of the X-rays emitted after the atomic capture of negatively charged muons. The probability rates of the muonic transitions possess sensitivity to the electronic structure of materials, thus making the muonic X-ray Emission Spectroscopy complementary to the X-ray Absorption and Emission techniques for the study of the chemistry of elements, and able of unparalleled analysis in case of elements bearing low atomic numbers. This qualitative method is applied to the characterization of light elements-based, energy-relevant materials involved in the reaction of hydrogen desorption from the reactive hydride composite Ca(BH4)2-Mg2NiH4. The origin of the influence of the band-structure on the muonic atom is discussed and the observed effects are attributed to the contribution of the electronic structure to the screening and to the momentum distribution in the muon cascade.

X-ray Spectroscopy of Muonic Atoms Isolated in Vacuum with Transition Edge Sensors

High-resolution X-ray spectroscopy of the highly charged muonic atoms/ions isolated in vacuum is an ideal probe to explore quantum electrodynamics under extremely strong electric fields, which is one of the major topic in fundamental atomic physics. A feasibility test measurement with a low-density neon gas target was performed by observing X-rays emitted by muonic neon via the $$5 \rightarrow 4$$ transition, $$\sim$$ 6.3 keV, using a multi-pixel array of superconducting transition-edge-sensor (TES) microcalorimeters at the J-PARC muon facility. We successfully demonstrated the feasibility of muonic atom X-ray spectroscopy with a gas target at a pressure as low as 0.1 atom using TES array under an intense pulsed muon beam.

Nondestructive High-Sensitivity Detections of Metallic Lithium Deposited on a Battery Anode Using Muonic X-rays.

Metallic Li deposited on the anode is known to induce short circuiting and degradation of the charge capacity of Li-ion batteries. However, no reliable technique is currently available to observe such Li metal without removing the case of the battery. An elemental analysis using muonic X-rays is proposed here because of its unique properties of nondestructive measurement, high sensitivity to light elements, and depth resolution. We demonstrated that this technique can be applied to detection of Li deposited on the surface of an anode containing Li ions, using a fully charged anode with Li deposited due to overcharge in an Al-laminated plastic pouch. The basis for the detection method is the difference in the atomic Coulomb capture ratio of the negative muons between the Li metal and ions. We have found, as a result, that the intensity of the muonic X-rays from metallic Li was approximately 50 times higher than that from Li ions. Consequently, the Li metal on the anode was clearly distinguishable from the intercalated Li ions in the anode. Furthermore, measurements of two overcharged anodes with 1.3 and 2.7 mg of metallic Li deposition, respectively, indicated that this technique is suitable for quantitative analysis. Distribution analysis is also possible, as shown by a preliminary observation on an overcharged anode from the back side. Therefore, this technique offers a new approach to the analysis of Li deposited on the anode of a Li-ion pouch battery.

Innovative amplifiers for muon spectroscopy experiments at RAL

The high intensity pulsed muon beam of ISIS facility at Rutherford Appleton Laboratory (RAL, U.K.) allows to perform high precision muonic X-ray spectroscopy experiments. In particular, FAMU and CHNET_TANDEM projects at RAL are dedicated, respectively, to a precise measurement of the Zemach radius of the proton through the measure of the hyperfine splitting of the ground state of the muonic hydrogen atom and to the optimization of analytical methods based on the muonic atom spectroscopy for non-destructive elementary characterization of archaeological samples. Custom electronic boards dedicated to the detector amplification stages have been designed and prototypized to provide fast high resolution for both experiments. The main features and performance of these custom boards are described in details in this work.

Irradiation Test of 65-nm Bulk SRAMs With DC Muon Beam at RCNP-MuSIC Facility

Negative and positive muon irradiation tests of static random access memories (SRAMs) were performed at Muon Science Innovation Channel (MuSIC) of Research Center for Nuclear Physics (RCNP), Osaka University. The muon-induced single event upset (SEU) cross sections for 65-nm bulk SRAMs were measured. The SRAM device was irradiated by the muon beams with average momenta ranging from 37.8 to 41.0 MeV/c at the beam exit. The incident muon fluence was measured using a one-by-one muon detection system with a plastic scintillator by taking advantage of the direct current (dc) muon beam and reliable absolute values of SEU cross sections were obtained. In addition to the measurement of the SEU cross sections, we measured muonic X-rays from the irradiated device to investigate the relation between the measured SEU cross section and the emission rate of muonic X-rays associated with the stopping position of the muons as a function of incident muon momentum. The result suggested that negative muons have a significant effect on SEUs by the emission of secondary light ions via negative muon capture reaction when negative muons stop near sensitive volumes (SVs) in SRAMs.