Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

  • Article
  • Published:

An ultrathin organic–inorganic integrated device for optical biomarker monitoring

Abstract

Organic electrochemical transistors can be used in wearable sensors to amplify biological signals. Other wireless communication systems are required for applications in continuous health monitoring. However, conventional wireless communication circuits, which are based on inorganic integrated chips, face limitations in terms of conformability due to the thick and rigid integrated circuit chips. Here, we report an ultrathin organic–inorganic device for wireless optical monitoring of biomarkers, such as glucose in sweat and glucose, lactate and pH in phosphate-buffered saline. The conformable system integrates an organic electrochemical transistor and a near-infrared inorganic micro-light-emitting diode on a thin parylene substrate. The device has an overall thickness of 4 μm. The channel current of the transistor changes according to the biomarker concentration, which alters the irradiance from the light-emitting diode to enable biomarker monitoring. We combine the device with an elastomeric battery circuit to create a wearable patch. We also show that the system can be used for near-infrared image analysis.

This is a preview of subscription content, access via your institution

Access options

Buy this article

Prices may be subject to local taxes which are calculated during checkout

Fig. 1: Wireless optical biomarker monitoring system.
Fig. 2: Electrical and optical characterization of the OECT and μLED integrated device.
Fig. 3: Mechanical stability of the OECT and μLED integrated device.
Fig. 4: Biomarker analysis by the wireless optical monitoring system.

Similar content being viewed by others

Data availability

The data that support the findings of this study are available from the corresponding authors upon reasonable request. Source data are provided with this paper.

References

  1. Kim, D.-H. et al. Epidermal electronics. Science 333, 838–843 (2011).

    Google Scholar 

  2. Nawrocki, R. A. et al. Self-adhesive and ultra-conformable, sub-300 nm dry thin-film electrodes for surface monitoring of biopotentials. Adv. Funct. Mater. 28, 1803279 (2018).

    Google Scholar 

  3. Park, D. Y. et al. Self-powered real-time arterial pulse monitoring using ultrathin epidermal piezoelectric sensors. Adv. Mater. 29, 1702308 (2017).

    Google Scholar 

  4. Cho, H. et al. Real-time finger motion recognition using skin-conformable electronics. Nat. Electron. 6, 619–629 (2023).

    Google Scholar 

  5. Newman, J. D. & Turner, A. P. Home blood glucose biosensors: a commercial perspective. Biosens. Bioelectron. 20, 2435–2453 (2005).

    Google Scholar 

  6. Kim, J., Campbell, A. S., de Avila, B. E. & Wang, J. Wearable biosensors for healthcare monitoring. Nat. Biotechnol. 37, 389–406 (2019).

    Google Scholar 

  7. Lee, H. et al. Wearable/disposable sweat-based glucose monitoring device with multistage transdermal drug delivery module. Sci. Adv. 3, e1601314 (2017).

    Google Scholar 

  8. Sempionatto, J. R. et al. An epidermal patch for the simultaneous monitoring of haemodynamic and metabolic biomarkers. Nat. Biomed. Eng. 5, 737–748 (2021).

    Google Scholar 

  9. Tu, J. et al. A wireless patch for the monitoring of C-reactive protein in sweat. Nat. Biomed. Eng. 7, 1293–1306 (2023).

    Google Scholar 

  10. Zhang, M., Tang, Z., Liu, X. & Van der Spiegel, J. Electronic neural interfaces. Nat. Electron. 3, 191–200 (2020).

    Google Scholar 

  11. Lee, W. et al. Nonthrombogenic, stretchable, active multielectrode array for electroanatomical mapping. Sci. Adv. 4, eaau2426 (2018).

    Google Scholar 

  12. Wang, Z. et al. A flexible and regenerative aptameric graphene–Nafion biosensor for cytokine storm biomarker monitoring in undiluted biofluids toward wearable applications. Adv. Funct. Mater. 31, 2005958 (2020).

    Google Scholar 

  13. Nakatsuka, N. et al. Aptamer–field-effect transistors overcome Debye length limitations for small-molecule sensing. Science 362, 319–324 (2018).

    Google Scholar 

  14. Wang, B. et al. Wearable aptamer-field-effect transistor sensing system for noninvasive cortisol monitoring. Sci. Adv. 8, eabk0967 (2022).

    Google Scholar 

  15. Zhao, C. et al. Implantable aptamer–field-effect transistor neuroprobes for in vivo neurotransmitter monitoring. Sci. Adv. 7, eabj7422 (2021).

    Google Scholar 

  16. Rivnay, J. et al. Organic electrochemical transistors. Nat. Rev. Mater. 3, 17086 (2018).

    Google Scholar 

  17. Diacci, C. et al. Diurnal in vivo xylem sap glucose and sucrose monitoring using implantable organic electrochemical transistor sensors. iScience 24, 101966 (2021).

    Google Scholar 

  18. Pappa, A. M. et al. Direct metabolite detection with an n-type accumulation mode organic electrochemical transistor. Sci. Adv. 4, eaat0911 (2018).

    Google Scholar 

  19. Scheiblin, G., Coppard, R., Owens, R. M., Mailley, P. & Malliaras, G. G. Referenceless pH sensor using organic electrochemical transistors. Adv. Mater. Technol. 2, 1600141 (2017).

    Google Scholar 

  20. Guo, K. et al. Rapid single-molecule detection of COVID-19 and MERS antigens via nanobody-functionalized organic electrochemical transistors. Nat. Biomed. Eng. 5, 666–677 (2021).

    Google Scholar 

  21. Lee, W. et al. Integration of organic electrochemical and field-effect transistors for ultraflexible, high temporal resolution electrophysiology arrays. Adv. Mater. 28, 9722–9728 (2016).

    Google Scholar 

  22. Park, S. et al. Self-powered ultra-flexible electronics via nano-grating-patterned organic photovoltaics. Nature 561, 516–521 (2018).

    Google Scholar 

  23. Ji, X. et al. Mimicking associative learning using an ion-trapping non-volatile synaptic organic electrochemical transistor. Nat. Commun. 12, 2480 (2021).

    Google Scholar 

  24. Khodagholy, D. et al. In vivo recordings of brain activity using organic transistors. Nat. Commun. 4, 1575 (2013).

    Google Scholar 

  25. Kim, D. H. et al. Dissolvable films of silk fibroin for ultrathin conformal bio-integrated electronics. Nat. Mater. 9, 511–517 (2010).

    Google Scholar 

  26. Bariya, M., Nyein, H. Y. Y. & Javey, A. Wearable sweat sensors. Nat. Electron. 1, 160–171 (2018).

    Google Scholar 

  27. Gao, W. et al. Fully integrated wearable sensor arrays for multiplexed in situ perspiration analysis. Nature 529, 509–514 (2016).

    Google Scholar 

  28. Wang, M. et al. A wearable electrochemical biosensor for the monitoring of metabolites and nutrients. Nat. Biomed. Eng. 6, 1225–1235 (2022).

    Google Scholar 

  29. Deng, Y. et al. A flexible and highly sensitive organic electrochemical transistor-based biosensor for continuous and wireless nitric oxide detection. Proc. Natl Acad. Sci. USA 119, e2208060119 (2022).

    Google Scholar 

  30. Matsuhisa, N. et al. High-frequency and intrinsically stretchable polymer diodes. Nature 600, 246–252 (2021).

    Google Scholar 

  31. Kim, Y. et al. Chip-less wireless electronic skins by remote epitaxial freestanding compound semiconductors. Science 377, 859–864 (2022).

    Google Scholar 

  32. Keum, D. H. et al. Wireless smart contact lens for diabetic diagnosis and therapy. Sci. Adv. 6, eaba3252 (2020).

    Google Scholar 

  33. Ku, M. et al. Smart, soft contact lens for wireless immunosensing of cortisol. Sci. Adv. 6, eabb2891 (2020).

    Google Scholar 

  34. Takamatsu, T., Sijie, Y. & Miyake, T. Wearable, implantable, parity‐time symmetric bioresonators for extremely small biological signal monitoring. Adv. Mater. Technol. 8, 2201704 (2023).

    Google Scholar 

  35. Kim, H.-J. et al. Review of near-field wireless power and communication for biomedical applications. IEEE Access 5, 21264–21285 (2017).

    Google Scholar 

  36. Tang, H., Yan, F., Lin, P., Xu, J. & Chan, H. L. W. Highly sensitive glucose biosensors based on organic electrochemical transistors using platinum gate electrodes modified with enzyme and nanomaterials. Adv. Funct. Mater. 21, 2264–2272 (2011).

    Google Scholar 

  37. Kang, X., Mai, Z., Zou, X., Cai, P. & Mo, J. Glucose biosensors based on platinum nanoparticles-deposited carbon nanotubes in sol–gel chitosan/silica hybrid. Talanta 74, 879–886 (2008).

    Google Scholar 

  38. Dutta Gupta, S. & Jatothu, B. Fundamentals and applications of light-emitting diodes (LEDs) in in vitro plant growth and morphogenesis. Plant Biotechnol. Rep. 7, 211–220 (2013).

    Google Scholar 

  39. Jacques, S. L. Corrigendum: optical properties of biological tissues: a review. Phys. Med. Biol. 58, R37–R61 (2013); erratum 58, 5007–5008 (2013).

  40. Jung, D. et al. Sustainably powered, multifunctional flexible feedback implant by the bifacial design and Si photovoltaics. Adv. Healthc. Mater. 10, e2001480 (2021).

    Google Scholar 

  41. Park, S.-I. et al. Printed assemblies of inorganic light-emitting diodes for deformable and semitransparent displays. Science 325, 977–981 (2009).

    Google Scholar 

  42. Khodagholy, D. et al. High transconductance organic electrochemical transistors. Nat. Commun. 4, 2133 (2013).

    Google Scholar 

  43. Canecki Varzic, S. et al. Assessment of FreeStyle Libre flash glucose monitoring system implementation in real life clinical setting: a prospective observational study. Diagnostics 11, 305 (2021).

    Google Scholar 

  44. Grieshaber, D., MacKenzie, R., Vörös, J. & Reimhult, E. Electrochemical biosensors – sensor principles and architectures. Sensors 8, 1400–1458 (2008).

    Google Scholar 

  45. Corrie, S. R., Coffey, J. W., Islam, J., Markey, K. A. & Kendall, M. A. F. Blood, sweat, and tears: developing clinically relevant protein biosensors for integrated body fluid analysis. Analyst 140, 4350–4364 (2015).

    Google Scholar 

  46. Zhang, S. et al. Intrinsically antifouling, soft and conformal bioelectronic from scalable fabrication of thin-film OECT arrays by zwitterionic polymers. Chem. Eng. J. 483, 148980 (2024).

    Google Scholar 

  47. Kaltenbrunner, M. et al. An ultra-lightweight design for imperceptible plastic electronics. Nature 499, 458–463 (2013).

    Google Scholar 

  48. Yang, Y. et al. A laser-engraved wearable sensor for sensitive detection of uric acid and tyrosine in sweat. Nat. Biotechnol. 38, 217–224 (2020).

    Google Scholar 

  49. Min, H. et al. Enhanced biocompatibility and multidirectional wet adhesion of insect-like synergistic wrinkled pillars with microcavities. Chem. Eng. J. 429, 132467 (2022).

    Google Scholar 

  50. Kim, S., Jahandar, M., Jeong, J. H. & Lim, D. C. Recent progress in solar cell technology for low-light indoor applications. Curr. Altern. Energy 3, 3–17 (2019).

    Google Scholar 

  51. Yin, L. et al. A stretchable epidermal sweat sensing platform with an integrated printed battery and electrochromic display. Nat. Electron. 5, 694–705 (2022).

    Google Scholar 

  52. Min, J. et al. An autonomous wearable biosensor powered by a perovskite solar cell. Nat. Electron. 6, 630–641 (2023).

    Google Scholar 

Download references

Acknowledgements

We thank B. Jang (Korea Institute of Machinery & Materials) for advising on the μLED fabrication process. This research was supported by a Korea Institute of Science and Technology project (Grant Nos. 2V09233 to W.L. and J.-H.H., 2E32981 to W.L., 2E33141 to W.L., 2E33150 to W.L. and H.J., 2E32242 to J.-H.H. and 2E33122 to H.J.). This research was supported by the Nano Material Technology Development Program (Grant No. 2021M3H4A1A04092879) through the National Research Foundation of Korea funded by the Ministry of Science and ICT (W.L.). This research was also supported by the Bio & Medical Technology Development Program of the National Research Foundation funded by the Ministry of Science & ICT (Grant No. 2022M3E5E9016506 to W.L.), a grant from the Institute of Information & Communications Technology Planning & Evaluation funded by the Korea government through the Ministry of Science and ICT (Grant No. 2022-0-00208, Infrared long-range multi-devices wireless charging technology, to J.-H.H.), a National Research Foundation of Korea grant funded by the Korean government through the Ministry of Science and ICT (Grant Nos. RS-2023-00302145 to H.J. and 2021R1A2B5B03001691 to S.H.K.), the Graduate School of Converging Science and Technology Program of Korea University and the Korea Institute of Science and Technology (H.J.).

Author information

Authors and Affiliations

Authors

Contributions

K.Y.K. and W.L. designed the project and experiments. K.Y.K. and J.K. developed the biochemical sensor. K.Y.K. and S.S. fabricated the elastomeric battery circuit. K.Y.K., J.-H.H. and W.L. fabricated the μLED and integrated devices. K.L. and H.J. helped with using the glucose assay kit and with data analysis. S.-W.H., S.H.K. and H.J. helped in the data analysis. K.Y.K. and W.L. wrote the manuscript, and all authors revised it. J.-H.H. and W.L. supervised the project.

Corresponding authors

Correspondence to Hojeong Jeon, Jae-Hoon Han or Wonryung Lee.

Ethics declarations

Competing interests

The authors declare no competing interests.

Peer review

Peer review information

Nature Electronics thanks Juliane Sempionatto, Tailin Xu and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

Additional information

Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary information

Supplementary Information

Supplementary Figs. 1–28 and Tables 1 and 2.

Supplementary Data

Supplementary data for Supplementary Figs. 1–28.

Source data

Source Data Fig. 2

Source data for Fig. 2.

Source Data Fig. 3

Source data for Fig. 3.

Source Data Fig. 4

Source data for Fig. 4.

Rights and permissions

Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Kim, K.Y., Kang, J., Song, S. et al. An ultrathin organic–inorganic integrated device for optical biomarker monitoring. Nat Electron 7, 914–923 (2024). https://doi.org/10.1038/s41928-024-01237-6

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue date:

  • DOI: https://doi.org/10.1038/s41928-024-01237-6

This article is cited by

Search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing