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Engineering solar cells based on correlative X-ray microscopy

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Abstract

In situ and operando measurement techniques combined with nanoscale resolution have proven invaluable in multiple fields of study. We argue that evaluating device performance as well as material behavior by correlative X-ray microscopy with <100 nm resolution can radically change the approach for optimizing absorbers, interfaces and full devices in solar cell research. In this article, we thoroughly discuss the measurement technique of X-ray beam induced current and point out fundamental differences between measurements of wafer-based silicon and thin-film solar cells. Based on reports of the last years, we showcase the potential that X-ray microscopy measurements have in combination with in situ and operando approaches throughout the solar cell lifecycle: from the growth of individual layers to the performance under operating conditions and degradation mechanisms. Enabled by new developments in synchrotron beamlines, the combination of high spatial resolution with high brilliance and a safe working distance allows for the insertion of measurement equipment that can pave the way for a new class of experiments. Applied to photovoltaics research, we highlight today’s opportunities and challenges in the field of nanoscale X-ray microscopy, and give an outlook on future developments.

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Notes

  1. Although multiple exciton generation (MEG) by single photons has been demonstrated e.g., in Ref. 161 for quantum-dot solar cells, solar cells with internal quantum efficiencies above 1 are of no practical relevance so far beyond fundamental research.

  2. Although experimentally not confirmed, there may be cases, where layers adjacent to the absorber layer could contribute to the X-ray beam induced photocurrent as discussed in Ref. 65.

  3. One can think of a device and measurement architecture, where more electrons leave the back surface than the front surface, e.g., with a front that is transparent for X-rays but absorbs heavily electrons, and a back that absorbs X-rays efficiently. However, we have in practice never encountered such a case, in which the grounding scheme would need to be inverted.

  4. “Front” and “back” side of a device denotes here the side exposed to or turned away from the incident X-rays. Obviously, this does not have to be the side of a solar cell that is exposed to the sun. As demonstrated in Fig. 2, for standard operation, the sun light enters this type of perovskite solar cell through the glass, but its high absorption of X-rays forced us to shine the X-rays through the other side.

  5. In most cases, the fraction of photons transmitted through the solar cell is not directly measurable by a down-stream detector, as most of them will be absorbed in the cell substrate.

  6. We used the attenuation coefficients included in the Penelope package for Beer–Lambert’s law and Monte–Carlo simulations, which justifies a direct comparison. Note that different databases for element-specific X-ray coefficients are available. A relatively recent database is presented in Ref. 162, and online80,163 as well as offline sources68,86 are available.

  7. Another common tool for fitting XRF data is PyMCA, described in Ref. 164 and available from Ref. 165.

  8. All absorption length values reported in this section were calculated using the functions “material.f” and “tables.f”, both being part of the Monte-Carlo simulation software package Penelope.68 For broader discussion of absorption length of different solar cell absorber layers, we refer to our publication in prep.69

  9. Note that the discrete layers do not need to correspond to physically distinct layers. In most cases, we use max. 1 nm thick layers for the calculation of the correction, which allows to take into account depth-dependent composition gradients as they are standard in many solar cell architectures. Whereas such depth-dependent composition variations are not accessible in plan view XRF measurements, they can be determined by other means (secondary ion mass spectroscopy, glow-discharge optical emission spectroscopy, cross-section XRF, etc.), and be taken into account for the calculation of the correction.

  10. Although I0 represents the intensity of the incoming photon beam as in Beer–Lambert’s law, I does not represent the intensity of the outgoing photon beam in Eq. (9)—in contrast to Eq. (10). Instead, I represents the outgoing photon beam intensity if there was no angular scattering or reemission of photons (fluorescence probability 100%).

  11. For the quantification of raw XRF counts into area concentrations by fitting of the reference and sample spectra, we typically use the MAPS software package developed at APS.79

  12. Poly{[N,N-9-bis(2-octyldodecyl)naphthalene-1,4,5,8-bis(dicarboximide)-2,6-diyl]-alt-5,59-(2,29-bithiophene)}.

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ACKNOWLEDGMENTS

We greatly acknowledge Jérémie Werner, Bjoern Niesen, Christophe Ballif (all EPFL, Switzerland), Harvey Guthrey, Mowafak Al-Jassim (all NREL, USA), Lei Chen, William Shafarman (all U. of Delaware, USA) for providing solar cells; Rupak Chakraborty, Jim Serdy, Tonio Buonassisi (all MIT, USA) for their contributions building the heating stage, David Fenning (UC San Diego, USA) for fruitful discussions, Chris Roehrig and Martin Holt (both ANL, USA) for practical help with XBIC measurements, Yanqi Luo (UC San Diego, USA) for measurement of the PbI2 reference, and Genevieve Hall, Sebastian Husein, Srikanth Gangam, and April Jeffries (all ASU, USA) for their contribution to measurements and discussions.

We acknowledge funding from the U.S. Department of Energy under contract DEEE0005848. Use of the Center for Nanoscale Materials and the Advanced Photon Source, both Office of Science user facilities, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. This material is based upon work supported in part by the National Science Foundation (NSF) and the Department of Energy (DOE) under NSF CA No. EEC-1041895. Any opinions, findings and conclusions or recommendations expressed in this material are those of the author(s) and do not necessarily reflect those of NSF or DOE.

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Authors and Affiliations

  1. Defect Lab, School of Electrical, Computer and Energy Engineering, Arizona State University, Tempe, AZ, 85287, USA

    Michael Stuckelberger, Bradley West, Tara Nietzold & Mariana I. Bertoni

  2. Advanced Photon Source, Argonne National Laboratory, Argonne, IL, 60439, USA

    Barry Lai, Jörg M. Maser & Volker Rose

  3. Center for Nanoscale Materials, Argonne National Laboratory, Argonne, IL, 60439, USA

    Volker Rose

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  1. Michael Stuckelberger
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  2. Bradley West
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Correspondence to Michael Stuckelberger.

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Stuckelberger, M., West, B., Nietzold, T. et al. Engineering solar cells based on correlative X-ray microscopy. Journal of Materials Research 32, 1825–1854 (2017). https://doi.org/10.1557/jmr.2017.108

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