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Journal Articles

Visualizing cation vacancies in Ce:Gd$$_{3}$$Al$$_{2}$$Ga$$_{3}$$O$$_{12}$$ scintillators by gamma-ray-induced positron annihilation lifetime spectroscopy

Fujimori, Kosuke*; Kitaura, Mamoru*; Taira, Yoshitaka*; Fujimoto, Masaki*; Zen, H.*; Watanabe, Shinta*; Kamada, Kei*; Okano, Yasuaki*; Kato, Masahiro*; Hosaka, Masahito*; et al.

Applied Physics Express, 13(8), p.085505_1 - 085505_4, 2020/08

 Times Cited Count:1 Percentile:24.67(Physics, Applied)

To clarify the existence of cation vacancies in Ce-doped Gd$$_{3}$$Al$$_{2}$$Ga$$_{3}$$O$$_{12}$$ (Ce:GAGG) scintillators, we performed gamma-ray-induced positron annihilation lifetime spectroscopy (GiPALS). GiPAL spectra of GAGG and Ce:GAGG comprised two exponential decay components, which were assigned to positron annihilation at bulk and defect states. By an analogy with Ce:Y$$_{3}$$Al$$_{5}$$O$$_{12}$$, the defect-related component was attributed to Al/Ga-O divacancy complexes. This component was weaker for Ce, Mg:GAGG, which correlated with the suppression of shallow electron traps responsible for phosphorescence. Oxygen vacancies were charge compensators for Al/Ga vacancies. The lifetime of the defect-related component was significantly changed by Mg co-doping. This was understood by considering aggregates of Mg$$^{2+}$$ ions at Al/Ga sites with oxygen vacancies, which resulted in the formation of vacancy clusters.

Journal Articles

Spin conversion reaction of spin-correlated ${it ortho}$-positronium and radical in liquids

Hirade, Tetsuya

Proceedings of 8th Asia Pacific Symposium on Radiation Chemistry (APSRC 2020) (Internet), 2 Pages, 2020/04

The positrons injected in insulating materials make ionization at the end part of the track, forming excess electrons and radicals. When one of the excess electrons and the incident positron form positronium, the electron in the positronium and the unpaired electron in the radical have a spin correlation. By using this spin correlation, a quantum beat phenomenon that depends on the hyperfine coupling constant of the radical appears in the spin conversion reaction with the positronium. The spin-correlated radical and other radicals can be distinguished by a reaction using the positronium as a probe. It is possible to study the behavior of OH radicals in water and the state of cation radicals in room temperature ionic liquids.

Journal Articles

Temperature dependence of ortho-positronium annihilation in room temperature ionic liquids

Hirade, Tetsuya; Michishio, Koji*; Kobayashi, Yoshinori*; Oshima, Nagayasu*

Acta Physica Polonica A, 137(2), p.109 - 112, 2020/02

 Times Cited Count:0 Percentile:0(Physics, Multidisciplinary)

Recently, it was reported that the positronium (Ps) bubble in Room Temperature Ionic Liquids (RTILs) showed some phenomena that were very different from them observed in other molecular liquids. Now the reason of these interesting phenomena is being understood. The structure caused by the ionic interaction between anions and cations can exist even at the higher temperatures than the melting temperatures. It was the reason why the oscillation of Ps bubble was observed at the temperatures near the melting temperatures in RTILs. The temperature dependence of the Ps bubble size estimated by the triplet Ps ($$ortho$$-Ps) pick-off annihilation lifetime indicated that there was a nano-meter structure remained by ionic interactions even at high temperatures. The $$ortho$$-Ps pick-off annihilation lifetime will be a strong tool to study nano-structure in RTILs.

Journal Articles

Positronium in room temperature ionic liquids

Hirade, Tetsuya

AIP Conference Proceedings 2182, p.030007_1 - 030007_5, 2019/12

 Times Cited Count:1 Percentile:84.1

There are many new application of room temperature ionic liquids (RTILs) for many different fields. One of them is reprocessing spent nuclear fuels and then research of irradiation effects on RTILs are very important. The positron annihilation techniques are very strong tool to investigate fast reactions of excess electrons. Positron annihilation age-momentum correlation (AMOC) experiment was applied to deepen understanding the phenomena occurred at very young positron ages. We clarified that Ps bubble formation in RTILs was very slow and, finally, oscillation of Ps bubble was observed just after the Ps formation at near melting temperatures. These results can indicate that Ps formation occurred in very short time in RTILs. The phenomena observed by Ps just in RTILs will be discussed.

Journal Articles

Hydrogen desorption spectra from excess vacancy-type defects enhanced by hydrogen in tempered martensitic steel showing quasi-cleavage fracture

Saito, Kei*; Hirade, Tetsuya; Takai, Kenichi*

Metallurgical and Materials Transactions A, 50(11), p.5091 - 5102, 2019/11

 Times Cited Count:13 Percentile:85.21(Materials Science, Multidisciplinary)

An attempt was made to separate and identify hydrogen peaks desorbed from lattice defects formed by plastic-strain in the presence of hydrogen in tempered martensitic steel showing quasi-cleavage fracture using thermal desorption spectroscopy from a low temperature (L-TDS) and positron annihilation spectroscopy (PAS). The L-TDS results made it possible to separate two peaks, namely, that of the original desorption and also that of new desorption. The PAS results revealed that the new desorption obtained by L-TDS corresponded to vacancy-type defects. Hydrogen enhanced vacancy-type defect concentration, approximately 10$$^{-5}$$ order in terms of atomic ratio, formed within 1.5 mm from the fracture surface, These results indicate that the accumulation of excess vacancy-type defects enhanced by hydrogen in the local region can lead to nanovoid nucleation and coalescence in plastic deformation, resulting in quasi-cleavage fracture of tempered martensitic steel.

Journal Articles

Detector identification by waveform shape analysis for effective data acquisition; Improvements in time resolution and count rate for positron annihilation age-momentum correlation measurement

Hirade, Tetsuya; Ando, Hirokazu*; Manabe, Kensuke*; Ueda, Daisuke*

Nuclear Instruments and Methods in Physics Research A, 931, p.100 - 104, 2019/07

 Times Cited Count:6 Percentile:81.33(Instruments & Instrumentation)

A detector identification method using waveform-shape analysis is proposed. A method for enabling discrimination of detectors by making a characteristic waveform shape for every detector by each own loop circuit on the detector is shown as an example. This method can be applied in many experimental contexts with detectors, making a high counting rate possible. Moreover, detector identification can be used for other important questions such as detector position. As an example, this detector identification method is used to perform positron-annihilation age-momentum correlation measurement with a high temporal resolution and a high counting rate.

Journal Articles

Structure of nitride layer formed on titanium alloy surface by N$$_{2}$$-gas exposure at high temperatures

Takeda, Yusuke; Iida, Kiyoshi*; Sato, Shinji*; Matsuo, Tadatoshi*; Nagashima, Yasuyuki*; Okubo, Nariaki; Kondo, Keietsu; Hirade, Tetsuya

JPS Conference Proceedings (Internet), 25, p.011023_1 - 011023_3, 2019/03

In this study, we prepared samples under two different conditions, (1) 810$$^{circ}$$C, for 600 min, and (2) 850$$^{circ}$$C, for 720 min. A depth-profile analysis of the surfaces of the samples is conducted through Doppler broadening (DB) measurements of positron annihilation $$gamma$$ rays using a slow positron beam. It was indicated that many of positrons annihilated in defects near the surface. According to the TEM image, there are nano-crystal grains near the surface and then positrons can diffuse in the grains and annihilate in defects at the grain boundaries. Furthermore, DB measurements indicated that there is a depth dependence on the chemical composition where positrons annihilate. EDS spectroscopy measurements also indicated that there is a depth dependence of impurities such as Vanadium. These results indicated change of the chemical composition at the grain boundaries.

Journal Articles

Quantum beats on triplet-positronium reactions in water

Hirade, Tetsuya

JPS Conference Proceedings (Internet), 25, p.011021_1 - 011021_2, 2019/03

Irradiation of water produce some reactive species such as OH radical. OH is formed by the reaction of a water cation and a water molecule just after ionization. On the other hand, a high energy positron injected in water will form cations and excess electrons even at the end part of the track. And hence, some positrons can form Positronium (Ps) with one of the excess electrons. The electrons in OH and Ps used to be in a same orbital in a water molecule before ionization of that water molecule. Therefore they were singlet at the time of the ionization. Every electron have each own hyperfine coupling constant after ionization. In water, reaction between Ps and OH, such as radical reaction or spin conversion, is possible. Therefore, quantum beats on these reaction can occur and the frequency of quantum beats will indicate the hyperfine coupling constant of OH which depends on the structure around OH. Therefore it is becoming possible to discuss the structure of water and reactivity of OH in the structure.

Journal Articles

Reaction between spin-correlated triplet positronium and OH radical in water

Hirade, Tetsuya

JPS Conference Proceedings (Internet), 25, p.011022_1 - 011022_3, 2019/03

OH radicals which are very reactive are formed by radiation decomposition in water. The behavior of OH radicals is important in corrosion of materials and reactions in living bodies. Recently, the reaction occurring between positronium (Ps) formed by OH radicals formed at the end of the positron track when positron is incident and positronium (Ps) formed by reaction of excess electrons formed with OH radical formation with the thermo-positron, it is reported that quantum beat occurs due to spin correlation. This quantum beat seems to have a period depending on the hyperfine coupling constant of OH radical. It is thought that the period and intensity of the quantum beat depends on the temperature, and it seems that it reflects the state around the OH radical. From the temperature dependence of the quantum beat detected by the reaction of this spin-correlated OH radical and triplet positronium we will explain what the liquid structure might be.

Journal Articles

Positronium in room temperature ionic liquids

Hirade, Tetsuya

Yodenshi Kagaku, (11), p.33 - 40, 2018/09

The positron injected in insulating materials thermalizes at the end part of its track and forms Positronium (Ps) with one of excess electrons within $$sim$$ 1 ps. Therefore, Ps formation can be a tool to investigate very fast processes like excess electron solvation in liquids. Many phenomena appeared in radiation chemistry researches for room temperature ionic liquids (ILs) are interesting and important for the application. Positron annihilation lifetime (PAL) measurements in ILs were carried out and anomalously long lifetime values of the shortest lifetime component were found in ILs. PAL and positron annihilation age-momentum correlation (AMOC) measurements were performed to clarify the reason of these anomalously long lifetime values and Ps bubble oscillation was finally discovered. Recent progresses are introduced with showing some results.

Journal Articles

Positron annihilation methods and applied researches for materials such as polymers

Hirade, Tetsuya

Kagaku To Kogyo, 92(2), p.44 - 54, 2018/02

A positron, an anti-particle of an electron, annihilates with an electron and emits energy that is proportional to mass energy as annihilation $$gamma$$-rays. Positron annihilation methods are applied by detecting these $$gamma$$-rays. The information of annihilation time, energy of $$gamma$$-rays, and direction of $$gamma$$-rays emission has been used for materials science. Here, positron annihilation lifetime, doppler broadening of annihilation $$gamma$$-rays and positron annihilation age-momentum correlation are mainly explained by use of research examples for metals and polymers, etc.

Journal Articles

Ortho-positronium annihilation in room temperature ionic liquids

Hirade, Tetsuya

Acta Physica Polonica A, 132(5), p.1470 - 1472, 2017/11

 Times Cited Count:2 Percentile:27.3(Physics, Multidisciplinary)

The positron annihilation lifetime measurements in RTILs showed very strange results. Finally, positron annihilation age-momentum correlation (AMOC) measurements indicated that it was caused by slow bubble formation in RTILs. Then I discovered the oscillation of o-Ps annihilation rates in room temperature ionic liquids (RTILs) which indicated, probably, the oscillation of the Ps bubble. Stepanov et al. calculated change of the bubble size in many liquids and the oscillation of the bubble was not expected except for a liquid He. It means that the structure of RTILs in nanometer scale is very different from usual liquids. Moreover, o-Ps pick-off annihilation rates seems to be too small for the macroscopic surface tension of RTILs. I am going to discuss what you can study by the positron annihilation methods for the structure of RTILs in nanometer scale.

Journal Articles

Modern radiation chemistry (Applications), 24; Radiation chemistry and positron annihilation

Hirade, Tetsuya

Radioisotopes, 66(11), p.587 - 593, 2017/11

Positron, anti-particle of electron, annihilates with the lifetime of 100ps to several ns in condensed matter. The energy of the mass of both particles emits as two $$gamma$$-rays. The annihilation rate of energy of $$gamma$$-rays indicate information just before the annihilation. Positrons have some possibility of reaction with excess electrons to form Positronium (Ps). Ps formation occur within ~ps, therefore Ps formation can be a probe of very fast reactions. Moreover, long lived triplet Ps can have reaction with reactive species until the lifetime of ~ns. Here, methods of positron annihilation research for radiation chemistry and some researches done by positron annihilation methods are introduced.

Journal Articles

Positron annihilation in the near surface of room temperature ionic liquids

Hirade, Tetsuya; O'Rourke, B. E.*; Kobayashi, Yoshinori*

Journal of Physics; Conference Series, 791(1), p.012029_1 - 012029_4, 2017/02

 Times Cited Count:1 Percentile:49.45

We tried to observe the positron annihilation rates near surface of (room temperature ionic liquids) IL's, such as N,N,N-trimethyl-N-propylammonium bis(trifluoromethanesulfonyl)imide (TMPA-TFSI) by use of the perpendicular slow positron beamline installed at AIST. The vaper pressure of TMPA-TFSI is very small and hence it is possible to measure the positron annihilation rate in vacuum chamber directly. This represents the first energy variable experimental results of the positron annihilation rate at the near surface of an IL. The triplet positronium annihilation rate seems to be larger at nearer region to the surface of the IL's.

Journal Articles

Structure of nitride layer formed on titanium alloy surface by N$$_{2}$$-gas exposure at high temperatures

Takeda, Yusuke; Iida, Kiyoshi*; Sato, Shinji*; Matsuo, Tadatoshi*; Nagashima, Yasuyuki*; Okubo, Nariaki; Kondo, Keietsu; Hirade, Tetsuya

Journal of Physics; Conference Series, 791(1), p.012022_1 - 012022_4, 2017/02

 Times Cited Count:1 Percentile:49.45

Titanium alloy is widely used for applications such as golf club heads and structural materials for aircrafts. The surface can be exceedingly hardened by nitriding treatment that initiates defects, but there are some difficulties on use of titanium nitride because the layer can be exfoliated by stress. Therefore, we prepared samples in two different treatment conditions, (1) 810$$^{circ}$$C 600 min and (2) 850$$^{circ}$$C 720 min and performed depth profile analysis of Doppler broadening of positron annihilation $$gamma$$-rays (DB) for these samples. According to a calculation of nitrogen diffusion depth, the nitride layer should be only about 0.05-0.1$$mu$$m. However, the depth profile analysis of the DB measurement indicated that the defects introduced by nitriding treatment extended to a depth of 0.5$$mu$$m.

Journal Articles

Research and application of positronium chemistry

Hirade, Tetsuya

Hoshasen To Sangyo, (139), p.23 - 28, 2015/12

The researches and the applications of the Positronium Chemistry were introduced. The mechanism of Ps formation in low temperature insulators was clarified by Hirade and it is almost the end of the long, more than half century, period for arguments on Ps formation. Hence almost all of the researchers have been accepting the Spur Reaction Model proposed by Mogensen. Therefore, radiation chemistry researches by use of the Spur Reaction Model, especially the study of excess electrons at the time range of pico-to-nano second and electron mobility, were introduced. It was also introduced that the Free Volume Model is not correct and then the sub-nano meter vacant space, such as the microscopic free volume in polymers, can be studied by just the triplet Ps lifetime. As the latest research for the application, it was introduced that Ps bubble shows oscillation especially in ionic liquids and is expected to be a strong tool to investigate nano-scale properties of ionic liquids.

Journal Articles

Enhanced lattice defect formation associated with hydrogen and hydrogen embrittlement under elastic stress of a tempered martensitic steel

Doshida, Tomoki*; Suzuki, Hiroshi*; Takai, Kenichi*; Hirade, Tetsuya; Oshima, Nagayasu*

NanotechJapan Bulletin (Internet), 8(3), 5 Pages, 2015/07

Studying the creation and time evolution of defects is an important issue for interpreting the hydrogen embrittlement mechanism of steels. We have been studied the relationship between hydrogen embrittlement of high strength steel and lattice defects associated with hydrogen by thermal desorption analysis (TDA) and positron probe microanalyzer (PPMA).

Journal Articles

Positronium bubble oscillation in room temperature ionic liquids; Temperature dependence

Hirade, Tetsuya

Journal of Physics; Conference Series, 618(1), p.012004_1 - 012004_5, 2015/06

 Times Cited Count:3 Percentile:78.42

Positronium (Ps; a bound state of positron and electron) has a negative work function in materials and forms a bubble state in liquids. On the way of stable bubble state, the bubble grows and probably oscillates. The usual fast bubble formation has not been observed with the time resolution of the positron annihilation methods that is usually 100-200 pico-seconds. There had been many anomalous phenomena observed in the room temperature ionic liquids (RTIL). Recently it was found that very slow bubble formation caused these anomalous phenomena. And hence the oscillation of the Ps bubble was successfully observed by the change of the annihilation rate of the triplet Ps that is affected by the size of the bubble. The oscillation and the decay of the bubble give the information of the viscoelastic properties at the sub-nano scale. The temperature dependence of the oscillation has been also successfully indicated.

Journal Articles

Measurement method for $$^{134}$$Cs in environment by use of the coincidence method

Hirade, Tetsuya; Katayama, Atsushi; Masaki, Nobuyuki

Radioisotopes, 64(5), p.311 - 318, 2015/05

The quantity of Cesium radioisotopes is estimated with full absorption peaks on the energy spectra measured by $$gamma$$-ray detectors such as Ge semiconductor detector. The heavy shield box made of Lead is needed to obtain reliable data, because the detection efficiency is in inverse proportion to square of the distance between the detectors and the radioactive materials. We have noticed that $$^{134}$$Cs emits two $$gamma$$-rays, 605 keV and 796 keV, with high efficiency, and that there are almost no radio isotopes which emit two $$gamma$$-rays as $$^{134}$$Cs does in environment. In the case of coincidence measurements of two $$gamma$$-rays, the detection efficiency is in inverse proportion to the fourth power of the distance between the detectors and the radioactive materials. Therefore the contamination with radioisotopes around the detectors do not affect to the count of the coincidence events. Hence, it is possible to estimate the quantity of $$^{134}$$Cs by in-situ and nondestructive measurement.

Journal Articles

Positron annihilation age momentum correlation (AMOC) measurement

Hirade, Tetsuya

Yodenshi Kagaku, (4), p.3 - 8, 2015/02

Positron annihilation Age-MOmentum Correlation (AMOC) measurement is the coincidence measurement method of positron injection time, positron annihilation time and positron annihilation $$gamma$$-rays energy. The methods for measurement and analysis of AMOC will be introduced briefly. Some of the interesting researches also will be introduced.

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