Decaying source model: Alternative approach to determination of true counting rates at X and gamma ray counting systems

The counting systems consisting of electronic devices are used for detection of radiation due to X or gamma rays. The dead time of the counting system is based on time limitations of these electronic devices. The dead time causes counting losses. Determination of counting rate losses in quantitative and qualitative analysis become a vital step for correction of analysis. Therefore, compensating for counting rate losses is of great importance. These counting rate losses are due to piled up reject time, paralyzable or non-paralyzable system dead time or a combination of these mechanisms. Paralyzable and non-paralyzable models are well-known and frequently used for correction of counting rate losses dependent on the system dead time. However, these two models do not provide enough correction at medium and high counting rates. Therefore, the new models for corrections of counting rate losses are needed. For this reason, both an alternative approach is proposed and a simulation program is coded for counting rate losses in this study. A good agreement is obtained between theoretical model and simulation program.     

Empirical dead‐time corrections for synchrotron sources

An experimental comparison of models for performing dead‐time corrections of photon‐counting detectors at synchrotron sources is presented. The performance of several detectors in the three operating modes of the Advanced Photon Source is systematically compared, with particular emphasis on asymmetric fill patterns. Several simple and well known correction formulas are evaluated. The results demonstrate the critical importance of detector speed and synchrotron fill pattern in selecting the proper dead‐time correction.     

On the convergence of zero-point vibrational corrections to nuclear shieldings and shielding anisotropies towards the complete basis set limit in water

ABSTRACT

The method and basis set dependence of zero-point vibrational corrections (ZPVCs) to nuclear magnetic resonance shielding constants and anisotropies has been investigated using water as a test system. A systematic comparison has been made using the Hartree–Fock, second-order Møller–Plesset perturbation theory (MP2), coupled cluster singles and doubles (CCSD), coupled cluster singles and doubles with perturbative triples corrections (CCSD(T)) and Kohn–Sham density functional theory with the B3LYP exchange-correlation functional methods in combination with the second-order vibrational perturbation theory (VPT2) approach for the vibrational corrections. As basis sets, the correlation consistent basis sets cc-pVXZ, aug-cc-pVXZ, cc-pCVXZ and aug-cc-pCVXZ with X = D, T, Q, 5, 6 and the polarisation consistent basis sets aug-pc-n and aug-pcS-n with n = 1, 2, 3, 4 were employed. Our results show that basis set convergence of the vibrational corrections is not monotonic and that very large basis sets are needed before a reasonable extrapolation to the basis set limit can be performed. Furthermore, our results suggest that coupled cluster methods and a decent basis set are required before the error of the electronic structure approach is lower than the inherent error of the VPT2 approximation.     

Dead time corrections to photon counting statistics II: Quantum theory

The recent formulation of the quantum theory of photodetection, based on the quantum theory of continuous measurements, is extended to the case of a (nonideal) detector which has non-zero dead time. A general result is proven which expresses the dead time modified counting statistics in terms of the counting statistics of anassociated ideal detector. As an illustration, the dead time corrections to the counting statistics of a single-mode free field are worked out, and these corrections are shown to be identical in form to the dead time corrections for a classical optical field of constant intensity.     

Energy‐dependent dead‐time correction in digital pulse processors applied to silicon drift detector's X‐ray spectra

Dead‐time effects in X‐ray spectra taken with a digital pulse processor and a silicon drift detector were investigated when the number of events at the low‐energy end of the spectrum was more than half of the total, at counting rates up to 56 kHz. It was found that dead‐time losses in the spectra are energy dependent and an analytical correction for this effect, which takes into account pulse pile‐up, is proposed. This and the usual models have been applied to experimental measurements, evaluating the dead‐time fraction either from the calculations or using the value given by the detector acquisition system. The energy‐dependent dead‐time model proposed fits accurately the experimental energy spectra in the range of counting rates explored in this work. A selection chart of the simplest mathematical model able to correct the pulse‐height distribution according to counting rate and energy spectrum characteristics is included.     

~(252)Cf自发裂变中子发射率符合测量的回归分析

~(252)Cf同位素源具有标准的自发裂变中子能谱,但由于其半衰期较短,应用中常需要对源强进行标定修正.随着源年龄增加,来自源中~(250)Cf和~(248)Cm自发裂变的影响愈加凸显,不能简单按~(252)Cf的衰变规律计算源中子发射率,而通过锰浴活化的间接测量方法周期较长,且在源强低于10~4 n/s时误差较大.最近,基于中子多重性计数的源强绝对测量算法已得到验证.本文进一步从点模型假设的测量方程出发,在将符合计数率与总中子计数率关联的基础上,分别对符合计数率随源位置、符合门宽的变化关系进行回归分析,提取变化过程的特征系数,建立了两种避规效率变化的~(252)Cf中子发射率测量方法,并基于JCC-51型中子符合测量装置开展实验验证.结果表明:两种回归分析方法的测量值均与标称值的修正结果在2%的偏差范围内一致;反推求得装置中轴线上的探测效率也与基于MCNPX程序的蒙特卡罗模拟计算值相符.研究结果可为活度信息不明的~(252)Cf源强标定及符合测量装置的效率刻度提供便携准确的实验方法.     

Dead time corrections to photon counting statistics I: Classical theory

A complete solution is given to the problem of calculating the dead time corrections to the counting statistics of an arbitrary doubly stochastic Poisson process with a non-negative random intensity function. It is shown that for the particular case of an optical field with constant intensity, the general dead time modified counting formula leads to a corrected version of results earlier derived by Bedard.     

Experimental characterization of the IRSN long counter for the determination of the neutron fluence reference values at the AMANDE facility

The neutron metrology and dosimetry laboratory has developed a long counter, on the basis of optimization work using Monte-Carlo simulations. The calibration of this new device was performed at the IRSN standard radionuclide source facility. Measurements were also realized at the monoenergetic neutron fields facility, AMANDE, to determine the dead time correction, the effective center and efficiency as a function of neutron energy. A good agreement was observed between the long counter results and the monoenergetic neutron fluence values determined with proton recoil counters. The results of the experimental characterization of the IRSN long counter are presented in this paper.     

Monte Carlo simulation of the decay of neutron resonances to determine resonance spins

The results for two types of experiments which measure the spins of neutron resonances is predicted by means of a Monte Carlo calculation which simulates the γ-cascades following neutron capture. The results are compared with experiment wherever possible. For the method which compares the ratios of γ-lines depopulating low-lying levels, the calculation is performed for ¹⁴³Nd, ¹⁴⁵Nd, ¹⁸⁷Os, and ¹⁸⁷Os. For the method which compares coincidence to singles counting rates, the calculation is performed for the four nuclei mentioned above plus ¹⁸⁵Re, ¹⁸⁷Re, and ¹⁷⁷Hf. The validity of the approximations and assumptions used in the calculation are discussed. Also discussed are proposed improvements in the experiments made on the basis of both experimental data and the calculation. All necessary derivations are given in the appendix.     

A CC2 dielectric continuum model and a CC2 molecular mechanics model

In this paper we present theory and applications for the second-order approximate singles and doubles coupled cluster (CC2) electronic structure method coupled to either a dielectric continuum (the CC2/DC model) or a molecular mechanical intermolecular force field (the CC2/MM model). Calculations of the interaction energy, solvation energy, electric dipole moment and electric quadrupole moment of liquid water are presented using the correlated CC2 approach. The results are compared to the corresponding results using the uncorrelated Hartree-Fock (HF) and the correlated coupled cluster singles and doubles (CCSD) methods. Also, a hierarchy in the coupling between the quantum mechanical (QM) and the molecular mechanical (MM) part of the system is investigated in the QM/MM model for the three different electronic structure methods.     

A local framework for calculating coupled cluster singles and doubles excitation energies (LoFEx-CCSD)

ABSTRACT

The recently developed Local Framework for calculating Excitation energies (LoFEx) is extended to the coupled cluster singles and doubles (CCSD) model. In the new scheme, a standard CCSD excitation energy calculation is carried out within a reduced excitation orbital space (XOS), which is composed of localised molecular orbitals and natural transition orbitals determined from time-dependent Hartree–Fock theory. The presented algorithm uses a series of reduced second-order approximate coupled cluster singles and doubles (CC2) calculations to optimise the XOS in a black-box manner. This ensures that the requested CCSD excitation energies have been determined to a predefined accuracy compared to a conventional CCSD calculation. We present numerical LoFEx-CCSD results for a set of medium-sized organic molecules, which illustrate the black-box nature of the approach and the computational savings obtained for transitions that are local compared to the size of the molecule. In fact, for such local transitions, the LoFEx-CCSD scheme can be applied to molecular systems where a conventional CCSD implementation is intractable.     

Small and efficient basis sets for the evaluation of accurate interaction-induced linear and non-linear electric properties in model hydrogen-bonded complexes

Interaction-induced electric dipole moment, polarisability and first hyperpolarisability are investigated in model hydrogen-bonded clusters built of hydrogen fluoride molecules organised in three linear chains parallel to each other. The properties are evaluated within the finite field approach, using the second order Møller–Plesset method, and the LPol-m (m = ds, dl) and the optical rotation prediction (ORP) basis sets. These bases and correlation method are selected after a systematic basis set and correlation method convergence study carried out on the smallest of the complexes and taking properties obtained with Dunning's bases and the coupled cluster singles and doubles (CCSD) and the CCSD including connected triple corrections (CCSD(T)) methods as reference. Results are analysed in terms of many-body and cooperative effects.     

Electrostatic interactions between molecules from relaxed one-electron density matrices of the coupled cluster singles and doubles model

The influence of electron correlation on the electrostatic interaction between closed shell molecules is studied using the relaxed electron densities of the coupled cluster singles and doubles (CCSD) model. The corresponding CCSD one-electron density matrices are efficiently computed without full four-index transformation by employing the generalized exchange and Coulomb operator technique. Using several representative van der Waals and hydrogen bonded complexes it was found that in most cases the convergence of the M?ller-Plesset expansion of the electrostatic energy, restricted to single, double and quadruple excitations, is satisfactory and the fourth-order triple excitation term is more important than the sum of the fifth- and higher-order contributions from CCSD theory. The importance of the CCSD correlation correction to the electrostatic energy was gauged by comparison of the total interaction energy computed by symmetry-adapted perturbation theory (SAPT) and by the super-molecular CCSD(T) approach (coupled cluster singles and doubles model with a non-iterative inclusion of triple excitations). Except for the CO and N₂ dimers, very good agreement between the two sets of results is observed. For the difficult case of the CO dimer the difference between the SAPT and CCSD(T) results can be explained by the truncation of the SAPT expansion for the dispersion energy at second order in the intramonomer correlation operator.     

Accurate equilibrium inversion barrier of ammonia by extrapolation to the one-electron basis set limit

A scheme based on treating uniform singlet-pair and triplet-pair interactions is suggested to extrapolate electron correlation energy of ammonia, calculated at two basis-set levels of ab initio theory in the infinite one-electron basis-set limit. The dual-level method is tested on the extrapolation of the full correlation in coupled-cluster singles and doubles and in the case also a noniterative perturbative correction for connected triple energies for the C3v and D3h structures of ammonia, with correlation-consistent basis sets of the type cc-pVXZ （X = D, T, Q, 5, 6） and aug-cc-pVXZ （X = D, T, Q, 5）. For testing and comparison purposes, the energies reported by Klopper [J. Comput. Chem. 22 1306 （2001）] have been taken. From a corresponding extrapolation of CCSD（T）/AVXZ energies for X = 4, 5, we obtain total inversion barriers of 1833.87 cm-1/1832.33 cm^-1 for the two/three-parameter extrapolation rules, which are in good agreement with other theoretical extrapolation and empirical values in the literature.     

Dead cell and side leakage correction for a lead-scintillating fiber electromagnetic calorimeter

The electromagnetic calorimeter(ECAL) of the Alpha Magnetic Spectrometer(AMS-02) is one of the key detectors for dark matter searches. It measures the energies of electrons, positrons and photons and seperates them from hadrons. Currently, there are 5 dead cells in the ECAL, which affect the reconstructed energy of 4.2%of total events in the ECAL acceptance. When an electromagnetic shower axis is close to the ECAL border, due to the side leakage, the reconstructed energy is affected as well. In this paper, methods for dead cells and side leakage corrections for the ECAL energy reconstruction are presented. For events with the shower axis crossing dead cells,applying dead cell correction improves the difference in the reconstructed energy from 12% to 1%, while for events near the ECAL border, with side leakage correction it is improved from 4% to 1%.     

主动中子多重性铀质量测量模拟研究

中子多重性技术常用于测量和核查核材料,尤其针对具有较厚屏蔽的对象具有不可替代的优势。钚的自发裂变率较高,可以采用被动测量方法,目前已有多款不同的测量装置。然而铀材料的自发裂变率较低只能采用主动测量方法。现有的主动井型符合计数器（AWCC）能够进行主动中子多重性测量铀材料质量,但依然存在探测效率较低,Am-Li中子源产生偶然符合大等缺点。为提高铀材料测量的效率和精度,对主动中子多重性测量方法开展深入研究非常必要。本文参考AWCC模型,利用Geant4软件对探测器和粒子的输运过程进行建模。研究了多重性移位寄存器的不同符合门宽、不同延迟时间对铀测量结果相对偏差的影响规律。计数器的最佳门宽为44 μs,门宽取值范围在计数器衰减时间的1.5倍左右合适;延迟时间大于3倍计数器衰减时间后,相对偏差显著减少。最后讨论了235U富集度变化对主动中子多重性测量结果的影响。为后续主动中子多重性铀质量测量仪器的设计提供了参考。     

Counting‐loss correction for X‐ray spectroscopy using unit impulse pulse shaping

High‐precision measurement of X‐ray spectra is affected by the statistical fluctuation of the X‐ray beam under low‐counting‐rate conditions. It is also limited by counting loss resulting from the dead‐time of the system and pile‐up pulse effects, especially in a high‐counting‐rate environment. In this paper a detection system based on a FAST‐SDD detector and a new kind of unit impulse pulse‐shaping method is presented, for counting‐loss correction in X‐ray spectroscopy. The unit impulse pulse‐shaping method is evolved by inverse deviation of the pulse from a reset‐type preamplifier and a C‐R shaper. It is applied to obtain the true incoming rate of the system based on a general fast–slow channel processing model. The pulses in the fast channel are shaped to unit impulse pulse shape which possesses small width and no undershoot. The counting rate in the fast channel is corrected by evaluating the dead‐time of the fast channel before it is used to correct the counting loss in the slow channel.