Super-resolution microscopy refers to a powerful set of imaging techniques that overcome the diffraction limit. Some of these techniques, the importance of which was recognized by the 2014 Nobel Prize for chemistry, are based on the concept of image reconstruction by spatially sparse sampling. Here, we introduce the concept of super-resolution spectroscopy based on sparse sampling in the frequency domain, and show that this can be naturally achieved using a random laser source. In its chaotic regime, the emission spectrum of a random laser features sharp spikes at uncorrelated frequencies that are sparsely distributed over the emission bandwidth. These narrow lasing modes probe stochastically the spectral response of a sample, allowing it to be reconstructed with a resolution exceeding that of the spectrometer. We envision that the proposed technique will inspire a new generation of simple, cheap, high-resolution spectroscopy tools with a reduced footprint.
This is a preview of subscription content, access via your institution
Open Access articles citing this article.
Nature Communications Open Access 30 October 2022
Nature Communications Open Access 04 February 2022
Access Nature and 54 other Nature Portfolio journals
Get Nature+, our best-value online-access subscription
$29.99 / 30 days
cancel any time
Subscribe to this journal
Receive 12 print issues and online access
$209.00 per year
only $17.42 per issue
Rent or buy this article
Prices vary by article type
Prices may be subject to local taxes which are calculated during checkout
The data that support the plots within this paper and other findings of this study are available from the corresponding author on reasonable request. Source data for Figs. 1–4 are provided with the paper.
Betzig, E., Trautman, J. K., Harris, T. D., Weiner, J. S. & Kostelak, R. L. Breaking the diffraction barrier: optical microscopy on a nanometric scale. Science 251, 1468–1470 (1991).
Hell, S. W. & Wichmann, J. Breaking the diffraction resolution limit by stimulated emission: stimulated-emission-depletion fluorescence microscopy. Opt. Lett. 19, 780–782 (1994).
Gazit, S., Szameit, A., Eldar, Y. C. & Segev, M. Super-resolution and reconstruction of sparse sub-wavelength images. Opt. Express 17, 23920 (2009).
Szameit, A. et al. Sparsity-based single-shot subwavelength coherent diffractive imaging. Nat. Mater. 11, 455–459 (2012).
Huang, F. M. & Zheludev, N. I. Super-resolution without evanescent waves. Nano Lett. 9, 1249–1254 (2009).
Rust, M. J., Bates, M. & Zhuang, X. Sub-diffraction-limit imaging by stochastic optical reconstruction microscopy (STORM). Nat. Methods 3, 793–796 (2006).
Hess, S. T., Girirajan, T. P. K. & Mason, M. D. Ultra-high resolution imaging by fluorescence photoactivation localization microscopy. Biophys. J. 91, 4258–4272 (2006).
Betzig, E. et al. Imaging intracellular fluorescent proteins at nanometer resolution. Science 313, 1642–1645 (2006).
Kawata, S., Minami, K. & Minami, S. Superresolution of Fourier transform spectroscopy data by the maximum entropy method. Appl. Opt. 22, 3593–3598 (1983).
Sidorenko, P. et al. Super-resolution spectroscopy by compact representation. In Frontiers in Optics 2012/Laser Science XXVIII FM3F.5 (OSA, 2012).
Pedrotti, F. L., & Pedrotti, L. S. Introduction to Optics (Prentice-Hall, 1987).
Blass, W. E. & Halsey, G. W. Deconvolution of Absorption Spectra (Academic, 1981).
Mou-Yan, Z. & Unbehauen, R. A deconvolution method for spectroscopy. Meas. Sci. Technol. 6, 482–487 (1995).
Wiersma, D. S. The physics and applications of random lasers. Nat. Phys. 4, 359–367 (2008).
Liu, J. et al. Random nanolasing in the Anderson localized regime. Nat. Nanotechnol. 9, 285–289 (2014).
Cao, H., Chriki, R., Bittner, S., Friesem, A. A. & Davidson, N. Complex lasers with controllable coherence. Nat. Rev. Phys. 1, 156–168 (2019).
Uppu, R., Tiwari, A. K. & Mujumdar, S. Identification of statistical regimes and crossovers in coherent random laser emission. Opt. Lett. 37, 662–664 (2012).
Araújo, C., Gomes, A. & Raposo, E. Lévy statistics and the glassy behavior of light in random fiber lasers. Appl. Sci. 7, 644 (2017).
Sharma, D., Ramachandran, H. & Kumar, N. Lévy statistics of emission from a novel random amplifying medium: an optical realization of the Arrhenius cascade. Opt. Lett. 31, 1806–1808 (2006).
Bachelard, N., Gigan, S., Noblin, X. & Sebbah, P. Adaptive pumping for spectral control of random lasers. Nat. Phys. 10, 426–431 (2014).
Zhu, L., Zhang, W., Elnatan, D. & Huang, B. Faster STORM using compressed sensing. Nat. Methods 9, 721–723 (2012).
Katz, O., Bromberg, Y. & Silberberg, Y. Compressive ghost imaging. Appl. Phys. Lett. 95, 131110 (2009).
Picqué, N. & Hänsch, T. W. Frequency comb spectroscopy. Nat. Photon. 13, 146–157 (2019).
Liang, H. K. et al. Electrically pumped mid-infrared random lasers. Adv. Mater. 25, 6859–6863 (2013).
Ni, P. N. et al. Fabry-Perot resonance enhanced electrically pumped random lasing from ZnO films. Appl. Phys. Lett. 107, 231108 (2015).
Liu, X.-Y., Shan, C.-X., Wang, S.-P., Zhang, Z.-Z. & Shen, D.-Z. Electrically pumped random lasers fabricated from ZnO nanowire arrays. Nanoscale 4, 2843–2846 (2012).
Yu, S. F. Electrically pumped random lasers. J. Phys. D 48, 483001 (2015).
Chu, S., Olmedo, M., Yang, Z., Kong, J. & Liu, J. Electrically pumped ultraviolet ZnO diode lasers on Si. Appl. Phys. Lett. 93, 181106 (2008).
Ma, X., Chen, P., Li, D., Zhang, Y. & Yang, D. Electrically pumped ZnO film ultraviolet random lasers on silicon substrate. Appl. Phys. Lett. 91, 251109 (2007).
Li, Y., Wang, C., Jin, L., Ma, X. & Yang, D. Electrically pumped random lasing from the light-emitting device based on two-fold-tandem SiO2/ZnO structure. Appl. Phys. Lett. 102, 161112 (2013).
Qiao, Q. et al. Surface plasmon enhanced electrically pumped random lasers. Nanoscale 5, 513–517 (2013).
Poison, R. C., Raikh, M. E. & Vardeny, Z. V. Universal properties of random lasers. IEEE J. Sel. Top. Quant. Electron. 9, 120–123 (2003).
Frolov, S. V., Vardeny, Z. V., Yoshino, K., Zakhidov, A. & Baughman, R. H. Stimulated emission in high-gain organic media. Phys. Rev. B 59, R5284 (1999).
We thank S. Caporali for his assistance with sputter deposition of the FP mirrors and L. Mariani for advice on the optical fibre elements. We thank M. De Pas, A. Montori and M. Giuntini for their assistance with the set-up of the electronics and R. Ballerini and A. Hajeb for the realizations of the mechanical elements. This research was funded by Ente Cassa di Risparmio Firenze (grant 2016-0866), Ministero dell’Istruzione dell’Università e della Ricerca Italiano (grant PRIN2017-2017Z55KCW), European Community by Laserlab-Europe (grant H2020 EC-GA-654148) and PATHOS (grant H2020 FET-OPEN-828946).
The experimental apparatus and the analysis method are currently under patent filing (Italian priority application number 10201900014748).
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
About this article
Cite this article
Boschetti, A., Taschin, A., Bartolini, P. et al. Spectral super-resolution spectroscopy using a random laser. Nat. Photonics 14, 177–182 (2020). https://doi.org/10.1038/s41566-019-0558-4
This article is cited by
Nature Photonics (2023)
Journal of Optics (2023)
Nature Photonics (2022)
Nature Physics (2022)
Nature Communications (2022)