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Detection of X-ray photons by solution-processed lead halide perovskites

Abstract

The evolution of real-time medical diagnostic tools such as angiography and computer tomography from radiography based on photographic plates was enabled by the development of integrated solid-state X-ray photon detectors made from conventional solid-state semiconductors. Recently, for optoelectronic devices operating in the visible and near-infrared spectral regions, solution-processed organic and inorganic semiconductors have also attracted a great deal of attention. Here, we demonstrate a possibility to use such inexpensive semiconductors for the sensitive detection of X-ray photons by direct photon-to-current conversion. In particular, methylammonium lead iodide perovskite (CH3NH3PbI3) offers a compelling combination of fast photoresponse and a high absorption cross-section for X-rays, owing to the heavy Pb and I atoms. Solution-processed photodiodes as well as photoconductors are presented, exhibiting high values of X-ray sensitivity (up to 25 μC mGyair−1 cm−3) and responsivity (1.9 × 104 carriers/photon), which are commensurate with those obtained by the current solid-state technology.

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Figure 1: MAPbI3 perovskite basic properties.
Figure 2: Photovoltaic device.
Figure 3: Visible and X-ray photoconductive devices.

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References

  1. Tegze, M. & Faigel, G. X-ray holography with atomic resolution. Nature 380, 49–51 (1996).

    Article  ADS  Google Scholar 

  2. Shanmugam, M. et al. Alpha particle X-ray spectrometer (APXS) on-board Chandrayaan-2 rover. Adv. Space Res. 54, 1974–1984 (2014).

    Article  ADS  Google Scholar 

  3. Yaffe, M. J. & Rowlands, J. A. X-ray detectors for digital radiography. Phys. Med. Biol. 42, 1–39 (1997).

    Article  Google Scholar 

  4. Kasap, S. O. & Rowlands, J. A. Direct-conversion flat-panel X-ray image sensors for digital radiography. Proc. IEEE 90, 591–604 (2002).

    Article  Google Scholar 

  5. Moy, J. P. Recent developments in X-ray imaging detectors. Nucl. Instrum. Meth. Phys. Res. 442, 26–37 (2000).

    Article  ADS  Google Scholar 

  6. Zhao, W. & Rowlands, J. A. X-ray imaging using amorphous selenium: feasibility of a flat panel self-scanned detector for digital radiology. J. Med. Phys. 22, 1595–1604 (1995).

    Article  Google Scholar 

  7. Oh, K. M. et al. Measurement of the electrical properties of a polycrystalline cadmium telluride for direct conversion flat panel X-ray detector. J. Instrum. 9, P01010 (2014).

    Article  Google Scholar 

  8. Kasap, S. et al. Amorphous and polycrystalline photoconductors for direct conversion flat panel X-ray image sensors. Sensors 11, 5112–5157 (2011).

    Article  Google Scholar 

  9. Halls, J. J. M. et al. Efficient photodiodes from interpenetrating polymer networks. Nature 376, 498–500 (1995).

    Article  ADS  Google Scholar 

  10. Konstantatos, G. et al. Ultrasensitive solution-cast quantum dot photodetectors. Nature 442, 180–183 (2006).

    Article  ADS  Google Scholar 

  11. Keuleyan, S., Lhuillier, E., Brajuskovic, V. & Guyot-Sionnest, P. Mid-infrared HgTe colloidal quantum dot photodetectors. Nature Photon. 5, 489–493 (2011).

    Article  ADS  Google Scholar 

  12. Rauch, T. et al. Near-infrared imaging with quantum-dot-sensitized organic photodiodes. Nature Photon. 3, 332–336 (2009).

    Article  ADS  Google Scholar 

  13. Chung, I., Lee, B., He, J., Chang, R. P. & Kanatzidis, M. G. All-solid-state dye-sensitized solar cells with high efficiency. Nature 485, 486–489 (2012).

    Article  ADS  Google Scholar 

  14. Gratzel, M. The light and shade of perovskite solar cells. Nature Mater. 13, 838–842 (2014).

    Article  ADS  Google Scholar 

  15. Green, M. A., Ho-Baillie, A. & Snaith, H. J. The emergence of perovskite solar cells. Nature Photon. 8, 506–514 (2014).

    Article  ADS  Google Scholar 

  16. Im, J. H., Jang, I. H., Pellet, N., Gratzel, M. & Park, N. G. Growth of CH3NH3PbI3 cuboids with controlled size for high-efficiency perovskite solar cells. Nature Nanotech. 9, 927–932 (2014).

    Article  ADS  Google Scholar 

  17. Jeon, N. J. et al. Compositional engineering of perovskite materials for high-performance solar cells. Nature 517, 476–480 (2015).

    Article  ADS  Google Scholar 

  18. Zhou, H. et al. Interface engineering of highly efficient perovskite solar cells. Science 345, 542–546 (2014).

    Article  ADS  Google Scholar 

  19. Tan, Z. K. et al. Bright light-emitting diodes based on organometal halide perovskite. Nature Nanotech. 9, 687–692 (2014).

    Article  ADS  Google Scholar 

  20. Xing, G. et al. Low-temperature solution-processed wavelength-tunable perovskites for lasing. Nature Mater. 13, 476–480 (2014).

    Article  ADS  Google Scholar 

  21. Dou, L. et al. Solution-processed hybrid perovskite photodetectors with high detectivity. Nature Commun. 5, 5404 (2014).

    Article  ADS  Google Scholar 

  22. Grodstein, G. W. X-ray Attenuation Coefficients from 10 keV to 100 MeV (US Department of Commerce, National Bureau of Standards, 1957).

    Google Scholar 

  23. Stranks, S. D. et al. Electron–hole diffusion lengths exceeding 1 micrometer in an organometal trihalide perovskite absorber. Science 342, 341–344 (2013).

    Article  ADS  Google Scholar 

  24. Wehrenfennig, C., Eperon, G. E., Johnston, M. B., Snaith, H. J. & Herz, L. M. High charge carrier mobilities and lifetimes in organolead trihalide perovskites. Adv. Mater. 26, 1584–1589 (2014).

    Article  Google Scholar 

  25. Xing, G. et al. Long-range balanced electron- and hole-transport lengths in organic–inorganic CH3NH3PbI3 . Science 342, 344–347 (2013).

    Article  ADS  Google Scholar 

  26. Baikie, T. et al. Synthesis and crystal chemistry of the hybrid perovskite (CH3NH3) PbI3 for solid-state sensitised solar cell applications. J. Mater. Chem. A 1, 5628–5641 (2013).

    Article  Google Scholar 

  27. Kasap, S. O. X-ray sensitivity of photoconductors: application to stabilized a-Se. J. Phys. D 33, 2853–2865 (2000).

    Article  ADS  Google Scholar 

  28. Schieber, M. et al. Thick films of X-ray polycrystalline mercuric iodide detectors. J. Cryst. Growth 225, 118–123 (2001).

    Article  ADS  Google Scholar 

  29. Juška, G. & Arlauskas, K. Impact ionization and mobilities of charge carriers at high electric fields in amorphous selenium. Phys. Status Solidi A 59, 389–393 (1980).

    Article  ADS  Google Scholar 

  30. Street, R. A. et al. Comparison of PbI2 and HgI2 for direct detection active matrix X-ray image sensors. J. Appl. Phys. 91, 3345–3355 (2002).

    Article  ADS  Google Scholar 

  31. Kabir, M. Z. & Kasap, S. O. Charge collection and absorption-limited sensitivity of X-ray photoconductors: applications to a-Se and HgI2 . Appl. Phys. Lett. 80, 1664–1666 (2002).

    Article  ADS  Google Scholar 

  32. Masuzawa, T. et al. Development of an amorphous selenium-based photodetector driven by a diamond cold cathode. Sensors 13, 13744–13778 (2013).

    Article  Google Scholar 

  33. Nie, W. et al. High-efficiency solution-processed perovskite solar cells with millimeter-scale grains. Science 347, 522–525 (2015).

    Article  ADS  Google Scholar 

  34. Yakunin, S. et al. High infrared photoconductivity in films of arsenic-sulfide-encapsulated lead-sulfide nanocrystals. ACS Nano 8, 12883–12894 (2014).

    Article  Google Scholar 

Download references

Acknowledgements

The authors acknowledge the Austrian Science Fund FWF for financial support through the SFB project IR_ON. A part of the research was also performed at the Energie Campus Nürnberg and supported by funding through the ‘Aufbruch Bayern’ initiative of the state of Bavaria. M.K. and S.Y. acknowledge partial financial support from the European Union through the FP7 (ERC Starting Grant NANOSOLID, GA no. 306733). The authors thank V. Sassi, S. Roters, E. Nusko, W. Grafeneder and M. Bodnarchuk for technical assistance. S.Y. thanks M. Hardman for assisting with the selection of plants for X-ray imaging. The authors thank N. Stadie for reading the manuscript.

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The manuscript was prepared with contributions from all authors. S.Y., M.S., D.K. and J.S. performed the work with the photoconductors. S.S., H.A., G.M. and M.R. prepared and tested the solar cell devices. W.H., G.M., C.B. and M.K. planned and supervised the work and had major input in the writing of the manuscript.

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Correspondence to Wolfgang Heiss.

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The authors declare no competing financial interests.

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Yakunin, S., Sytnyk, M., Kriegner, D. et al. Detection of X-ray photons by solution-processed lead halide perovskites. Nature Photon 9, 444–449 (2015). https://doi.org/10.1038/nphoton.2015.82

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