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In this article, we report the growth of Cd0.9Zn0.1Te0.97Se0.03 (CZTS) wide bandgap semiconductor single crystals for room temperature gamma-ray detection using a modified vertical Bridgman method. Charge transport properties measured in the radiation detectors, fabricated from the grown CZTS crystals, indicated signs of hole trapping. Hole traps inhibit high-resolution radiation detection especially for energetic gamma rays. Machine learning (ML) applications are gaining tremendous impetus in improving device and sensor performance by compensating for limitations arising from such intrinsic material properties. In this article, we describe a deep convolutional neural network (CNN) that has demonstrated remarkable efficiency in identifying the energy of a gamma photon detected by a CZTS detector. The CNN has been trained using simulated data that resemble output pulses from actual CZTS detectors when exposed to 662-keV gamma photons. The device properties required for the simulation have been derived from radiation detection measurements on a real Cd0.9Zn0.1Te0.97Se0.03 detector fabricated in our laboratory. The CNN has been trained with detector pulses arising through photoelectric (PE) and Compton scattering (CS) separately. The percentage error in predicting the detected energies, within an extremely small duration of 0.28 ms, was found to be lower than 0.1% for gamma energies above 50 keV and for training datasets containing PE and CS events separately. The CNN was also validated for a mixed PE and CS dataset to obtain a prediction error of 1%. The effect of detector resolution on the efficiency of the CNN was also explored. [ABSTRACT FROM AUTHOR]

We report a modified vertical Bridgman method to grow Cd0.9Zn0.1Te0.97Se0.03 (CZTS) single crystals using in-house zone-refined 7 N (99.99999%) purity elemental precursors for room-temperature radiation detection. CZTS is an economic yet high performance alternative to expensive CdZnTe (CZT) detectors for room-temperature gamma-ray detection. Radiation detector in planar geometry has been fabricated on an 11.0 × 11.0 × 3.0 mm3 CZTS single crystal. A bulk resistivity of 1010 Ω.cm has been achieved without using any compensating dopant. The elemental composition of the grown crystal has been examined using energy-dispersive X-ray (EDX) analysis. Powder X-ray diffraction (XRD) showed formation of zincblende phase with a lattice constant of 6.447 Å, and sharp peaks confirmed the formation of highly crystalline single-phase CZTS crystals. A modified Vegard's law has been applied to calculate the atomic percentage of Se in the grown crystals from the XRD patterns and compared with the intended and the measured stoichiometry. The electron mobility-lifetime (μτ) product and the drift mobility have been calculated to be 1.5 × 10–3 cm2/V and 710 cm2/V.s, respectively, using alpha spectroscopy. The presented vertical Bridgman growth method uses a single pass through the controlled heating zone in contrast to the previously reported multiple pass growth techniques, thus, reducing the growth duration by two third which would help to further reduce the cost of production of CZTS-based room-temperature detectors. [ABSTRACT FROM AUTHOR]

Quaternary Cd0.9Zn0.1Te1–ySey (CZTS) single crystals, a novel room-temperature nuclear radiation detector semiconductor material, have been grown using a modified vertical Bridgman method (VBM) and a traveling heater method (THM). The percentage concentration of selenium in the VBM-grown crystal was 3% and that in the THM-grown crystal was 2%. While the THM Frisch collar detector ($4.4\times 4.4\times10.7$ mm $^{3}$) produced a highly resolved pulse height spectra (PHS) with a resolution of ~1.06% for 662-keV gamma rays without any correction, the VBM-grown detector ($10\times 10\times 2$ mm $^{3}$) offered a high-energy resolution of ~2% after the application of a digital bi-parametric correction. The high-resolution performance of these detectors has been attributed to the addition of Se in the Cd0.9Zn0.1Te (CZT) matrix. Ab-initio calculations based on density functional theory (DFT) also confirmed that the addition of Se in the CZT matrix helps to reduce the formation of TeCd and the TeZn antisites. The VBM-grown crystals were characterized using powder X-ray diffraction (XRD) and energy dispersive X-ray spectroscopy (EDS). While the XRD results revealed sharp diffraction peaks confirming the crystalline nature of the grown crystal, the EDS results confirmed the targeted stoichiometry of the elemental composition. The bulk resistivity of the grown crystal was calculated to be $\sim 3\times 10^{10}\,\,\Omega$ -cm from the current–voltage characteristics recorded at room temperature in a planar configuration, ensuring that the grown CZTS crystals have low dark current as required for detector-grade crystals. [ABSTRACT FROM AUTHOR]

Large-volume detector-grade Cd0.9Zn0.1Te (CZT) single crystals were grown using a vertical Bridgman technique. The bulk resistivity of the as-grown crystal was found to be ~ 5 × 1010 Ω-cm from current–voltage measurements. A 19.0 ×19.0 × 5.0 mm3 block of the crystal was used to fabricate a detector with 10 × 10 pixelated anode configuration integrated with interpixel guard rings. The detector was tested for its radiation detection properties using 662-keV gamma rays from a 137Cs source. The pixels exhibited well-resolved gamma pulse-height spectra (PHS) with percentage energy resolution ~1.6% at 662 keV. A few pixels exhibited tailing of the photopeak on the lower energy side indicating the presence of hole traps. Biparametric plots (BPs) were obtained from digitally recorded preamplifier pulses. The BPs showed anomalous behavior, which was correlated with the gamma interactions in the active region of the detector in virtual Frisch grid configuration. The BPs also enabled to extract PHS free from the extensive tailing of the photopeak. [ABSTRACT FROM AUTHOR]

The application of Cd0.9Zn0.1Te (CZT) single crystals, the primary choice for high-resolution, room-temperature compact gamma-ray detectors in the field of medical imaging and homeland security for the past three decades, is limited by the high cost of production and maintenance due to low detector grade crystal growth yield. The recent advent of its quaternary successor, Cd0.9Zn0.1Te1−ySey (CZTS), has exhibited remarkable crystal growth yield above 90% compared to that of ~33% for CZT. The inclusion of Se in appropriate stoichiometry in the CZT matrix is responsible for reducing the concentration of sub-grain boundary (SGB) networks which greatly enhances the compositional homogeneity and growth yield. SGB networks also host defect centers responsible for charge trapping, hence their reduced concentration ensures minimized charge trapping. Indeed, CZTS single crystals have shown remarkable improvement in electron charge transport properties and energy resolution over CZT detectors. However, our studies have found that the overall charge transport in CZTS is still limited by the hole trapping. In this article, we systematically review the advances in the CZTS growth techniques, its performance as room-temperature radiation detector, and the role of defects and their passivation studies needed to improve the performance of CZTS detectors further. [ABSTRACT FROM AUTHOR]

• Crystal growth of CZTS crystals using a vertical gradient freeze (VGF) method. • Significant reduction in crystal growth duration. • 100 % charge collection efficiency has been obtained for 5486 keV alpha particles. • Significant improvement in electron drift mobility and mobility-lifetime product. We report the growth of detector grade Cd 0.9 Zn 0.1 Te 0.97 Se 0.03 (CZTS) single crystals, a recently discovered quaternary semiconductor for room temperature radiation detection, by a vertical gradient freeze (VGF) method. VGF is a comparatively low-temperature growth method and avoids relative motion between the heater and the ampoule containing the precursor materials which minimizes any thermal drift or temperature fluctuations. As a result, CZTS single crystals with superior charge transport properties has been obtained. Growth of detector-grade CZTS single crystals using VGF method has not been reported yet. X-ray spectroscopy based elemental analysis showed that the grown crystals demonstrated the desired stoichiometry required for high resolution radiation detection. Planar detectors fabricated by deposition of gold contacts (∼0.07 cm2) demonstrated high bulk resistivity ∼1010 Ω-cm and a very low leakage current density of 2.8 × 10−8 A/cm2 at a bias of 100 V when measured at room temperature. The detectors showed excellent radiation response with 100 % charge collection efficiency when exposed to 5486 keV alpha particles. The electron mobility-lifetime (μ τ) product was measured to be 3 × 10−3 cm2/V using a single polarity Hecht analysis which is at par with the recently reported values measured in CZTS grown using conventional Bridgman or travelling heater method. The electron mobility has been calculated to be 964 cm2V−1s−1 using a time-of-flight (TOF) method, a substantial improvement over that obtained from conventionally grown CZTS single crystals. [ABSTRACT FROM AUTHOR]