X-ray imaging plays an indispensable role in diagnosing and staging disease. Nevertheless, exposure to high doses of X-rays has potential for harm, and much effort is focused towards reducing radiation exposure while maintaining diagnostic function. With this aim, researchers at the King Abdullah University of Science and Technology (KAUST) have shown how interconnecting single-crystal devices can create an X-ray detector with an ultralow detection threshold.
The team created devices using lab-grown single crystals of methylammonium lead bromide (MAPbBr3), a perovskite material that exhibits considerable stability, minimal ion migration and a high X-ray absorption cross-section – making it ideal for X-ray detection. To improve performance further, they used cascade engineering to connect two or more crystals together in series, reporting their findings in ACS Central Science.
X-rays incident upon a semiconductor crystal detector generate a photocurrent via the creation of electron–hole pairs. When exposed to the same X-ray dose, cascade-connected crystals should exhibit the same photocurrent as a single-crystal device (as they generate equal net concentrations of electron–hole pairs). The cascade configuration, however, has a higher resistivity and should thus have a much lower dark current, improving the signal-to-noise ratio and enhancing the detection performance of the cascade device.
To test this premise, senior author Omar Mohammed and colleagues grew single crystals of MAPbBr3. They first selected four identical crystals to evaluate (SC1, SC2, SC3 and SC4), each 3 x 3 mm in area and approximately 2 mm thick. Measuring various optical and electrical properties revealed high consistency across the four samples.
“The synthesis process allows for reproducible production of MAPbBr3 single crystals, underscoring their strong potential for commercial applications,” says Mohammed.
Optimizing detector performance
Mohammed and colleagues fabricated X-ray detectors containing a single MAPbBr3 perovskite crystal (SC1) and detectors with two, three and four crystals connected in series (SC1−2, SC1−3 and SC1−4). To compare the dark currents of the devices they irradiated each one with X-rays under a constant 2 V bias voltage. The cascade-connected SC1–2 exhibited a dark current of 7.04 nA, roughly half that generated by SC1 (13.4 nA). SC1–3 and SC1–4 reduced the dark current further, to 4 and 3 nA, respectively.
The researchers also measured the dark current for the four devices as the bias voltage changed from 0 to -10 V. They found that SC1 reached the highest dark current of 547 nA, while SC1–2, SC1–3 and SC1–4 showed progressively decreasing dark currents of 134, 90 and 50 nA, respectively. “These findings highlight the effectiveness of cascade engineering in reducing dark current levels,” Mohammed notes.
Next, the team assessed the current stability of the devices under continuous X-ray irradiation for 450 s. SC1–2 exhibited a stable current response, with a skewness value of just 0.09, while SC1, SC1–3 and SC1–4 had larger skewness values of 0.75, 0.45 and 0.76, respectively.
The researchers point out that while connecting more single crystals in series reduced the dark current, increasing the number of connections also lowered the stability of the device. The two-crystal SC1–2 represents the optimal balance.
Low-dose imaging
One key component required for low-dose X-ray imaging is a low detection threshold. The conventional single-crystal SC1 showed a detection limit of 590 nGy/s under a 2 V bias. SC1–2 decreased this limit to 100 nGy/s – the lowest of all four devices and surpassing the existing record achieved by MAPbBr3 perovskite devices under near-identical conditions.
Spatial resolution is another important consideration. To assess this, the researchers estimated the modulation transfer function (the level of original contrast maintained by the detector) for each of the four devices. They found that SC1–2 exhibited the best spatial resolution of 8.5 line pairs/mm, compared with 5.6, 5.4 and 4 line pairs/mm for SC1, SC1–3 and SC1–4, respectively.
Finally, the researchers performed low-dose X-ray imaging experiments using the four devices, first imaging a key at a dose rate of 3.1 μGy/s. SC1 exhibited an unclear image due to the unstable current affecting its resolution. Devices SC1–2 to SC1–4 produced clearer images of the key, with SC1–2 showing the best image contrast.
They also imaged a USB port at a dose rate of 2.3 μGy/s, a metal needle piercing a raspberry at 1.9 μGy/s and an earring at 750 nGy/s. In all cases, SC1–2 exhibited the highest quality image.
Could next-generation perovskite detectors improve clinical X-ray imaging?
The researchers conclude that the cascade-engineered configuration represents a significant shift in low-dose X-ray detection, with potential to advance applications that require minimal radiation exposure combined with excellent image quality. They also note that the approach works with different materials, demonstrating X-ray detection using cascaded cadmium telluride (CdTe) single crystals.
Mohammed says that the team is now investigating the application of the cascade structure in other perovskite single crystals, such as FAPbI3 and MAPbI3, with the goal of reducing their detection limits. “Moreover, efforts are underway to enhance the packaging of MAPbBr3 cascade single crystals to facilitate their use in dosimeter detection for real-world applications,” he tells Physics World.
