Abstract
Light–matter interactions can create and manipulate collective many-body phases in solids1,2,3, which are promising for the realization of emerging quantum applications. However, in most cases, these collective quantum states are fragile, with a short decoherence and dephasing time, limiting their existence to precision tailored structures under delicate conditions such as cryogenic temperatures and/or high magnetic fields. In this work, we discovered that the archetypal hybrid perovskite, MAPbI3 thin film, exhibits such a collective coherent quantum many-body phase, namely superfluorescence, at 78 K and above. Pulsed laser excitation first creates a population of high-energy electron–hole pairs, which quickly relax to lower energy domains and then develop a macroscopic quantum coherence through spontaneous synchronization. The excitation fluence dependence of the spectroscopic features and the population kinetics in such films unambiguously confirm all the well-known characteristics of superfluorescence. These results show that the creation and manipulation of collective coherent states in hybrid perovskites can be used as the basic building blocks for quantum applications4,5.
This is a preview of subscription content, access via your institution
Access options
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
Buy this article
Purchase on Springer Link
Instant access to full article PDF
Prices may be subject to local taxes which are calculated during checkout
Similar content being viewed by others
Data availability
Data that support the plots within this paper and other findings of this study are available from the corresponding author upon reasonable request. Source data are provided with this paper.
References
Torchinsky, D. H., Mahmood, F., Bollinger, A. T., Božović, I. & Gedik, N. Fluctuating charge-density waves in a cuprate superconductor. Nat. Mater. 12, 387–391 (2013).
Li, T. et al. Femtosecond switching of magnetism via strongly correlated spin–charge quantum excitations. Nature 496, 69–73 (2013).
Keeling, J., Marchetti, F., Szymańska, M. & Littlewood, P. Collective coherence in planar semiconductor microcavities. Semicond. Sci. Technol. 22, R1–R26 (2007).
Bergmann, M. & Gühne, O. Entanglement criteria for Dicke states. J. Phys. A 46, 385304 (2013).
Tóth, G. & Apellaniz, I. Quantum metrology from a quantum information science perspective. J. Phys. A 47, 424006 (2014).
Whitfield, J. Synchronized swinging. Nature https://doi.org/10.1038/news020218-16 (2002).
Eastham, P. R. & Rosenow, B. in Universal Themes of Bose–Einstein Condensation (eds Proukakis, N. P. et al.) 462–476 (Cambridge Univ. Press, 2017).
Dicke, R. H. Coherence in spontaneous radiation processes. Phys. Rev. 93, 99–110 (1954).
Li, X. et al. Observation of Dicke cooperativity in magnetic interactions. Science 361, 794–797 (2018).
Scully, M. O. & Svidzinsky, A. A. The super of superradiance. Science 325, 1510–1511 (2009).
Thompson, J. V. et al. Pulsed cooperative backward emissions from non-degenerate atomic transitions in sodium. New J. Phys. 16, 103017 (2014).
Skribanowitz, N., Herman, I. P., MacGillivray, J. C. & Feld, M. S. Observation of Dicke superradiance in optically pumped HF gas. Phys. Rev. Lett. 30, 309–312 (1973).
Ariunbold, G. O. et al. Observation of picosecond superfluorescent pulses in rubidium atomic vapor pumped by 100-fs laser pulses. Phys. Rev. A 82, 043421 (2010).
Florian, R., Schwan, L. O. & Schmid, D. Two-color superfluorescence of O2− centers in KCl. J. Lumin. 31, 169–171 (1984).
Miyajima, K., Kumagai, Y. & Ishikawa, A. Ultrashort radiation of biexcitonic superfluorescence from high-density assembly of semiconductor quantum dots. J. Phys. Chem. C 121, 27751–27757 (2017).
Dai, D. & Monkman, A. Observation of superfluorescence from a quantum ensemble of coherent excitons in a ZnTe crystal: evidence for spontaneous Bose–Einstein condensation of excitons. Phys. Rev. B 84, 115206 (2011).
Noe, G. T. II et al. Giant superfluorescent bursts from a semiconductor magneto-plasma. Nat. Phys. 8, 219–224 (2012).
Rainò, G. et al. Superfluorescence from lead halide perovskite quantum dot superlattices. Nature 563, 671–675 (2018).
Benedict, M. G. Super-Radiance: Multiatomic Coherent Emission (CRC Press, 1996).
Burnham, D. C. & Chiao, R. Y. Coherent resonance fluorescence excited by short light pulses. Phys. Rev. 188, 667–675 (1969).
Gross, M. & Haroche, S. Superradiance: an essay on the theory of collective spontaneous emission. Phys. Rep. 93, 301–396 (1982).
Bonifacio, R. & Lugiato, L. Cooperative radiation processes in two-level systems: superfluorescence. Phys. Rev. A 11, 1507–1521 (1975).
Osherov, A. et al. The impact of phase retention on the structural and optoelectronic properties of metal halide perovskites. Adv. Mater. 28, 10757–10763 (2016).
Jia, Y., Kerner, R. A., Grede, A. J., Rand, B. P. & Giebink, N. C. Continuous-wave lasing in an organic–inorganic lead halide perovskite semiconductor. Nat. Photon. 11, 784–788 (2017).
Chuliá-Jordán, R. et al. Inhibition of light emission from the metastable tetragonal phase at low temperatures in island-like films of lead iodide perovskites. Nanoscale 11, 22378–22386 (2019).
Phuong, L. Q. et al. Free carriers versus excitons in CH3NH3PbI3 perovskite thin films at low temperatures: charge transfer from the orthorhombic phase to the tetragonal phase. J. Phys. Chem. Lett. 7, 2316–2321 (2016).
Milot, R. L., Eperon, G. E., Snaith, H. J., Johnston, M. B. & Herz, L. M. Temperature‐dependent charge‐carrier dynamics in CH3NH3PbI3 perovskite thin films. Adv. Funct. Mater. 25, 6218–6227 (2015).
Malcuit, M. S., Maki, J. J., Simkin, D. J. & Boyd, R. W. Transition from superfluorescence to amplified spontaneous emission. Phys. Rev. Lett. 59, 1189–1192 (1987).
Siegman, A. E. Lasers (University Science Books, 1986).
Miyata, K. et al. Large polarons in lead halide perovskites. Sci. Adv. 3, e1701217 (2017).
Jho, Y. et al. Cooperative recombination of a quantized high-density electron–hole plasma in semiconductor quantum wells. Phys. Rev. Lett. 96, 237401 (2006).
Ariunbold, G. O., Sautenkov, V. A., Rostovtsev, Y. V. & Scully, M. O. Ultrafast laser control of backward superfluorescence towards standoff sensing. Appl. Phys. Lett. 104, 021114 (2014).
Kuan, Y.-H. & Liao, W.-T. Transition between amplified spontaneous emission and superfluorescence in a longitudinally pumped medium by an X-ray free-electron-laser pulse. Phys. Rev. A 101, 023836 (2020).
Vardeny, Z. V. Ultrafast Dynamics and Laser Action of Organic Semiconductors (CRC Press, 2009).
Thouin, F. et al. Phonon coherences reveal the polaronic character of excitons in two-dimensional lead halide perovskites. Nat. Mater. 18, 349–356 (2019).
Ishizaki, A. & Fleming, G. R. Theoretical examination of quantum coherence in a photosynthetic system at physiological temperature. Proc. Natl Acad. Sci. USA 106, 17255–17260 (2009).
Wang, Z. et al. Controllable switching between superradiant and subradiant states in a 10-qubit superconducting circuit. Phys. Rev. Lett. 124, 013601 (2020).
Ariunbold, G. O., Sautenkov, V. A. & Scully, M. O. Temporal coherent control of superfluorescent pulses. Opt. Lett. 37, 2400–2402 (2012).
Acknowledgements
We acknowledge helpful discussions with J. Thomas (NC State University), D. Aspnes (NC State University) and V. Temnov (IMMM Le Mans). We also acknowledge support from the NCSU Imaging and Kinetic Spectroscopy facility and technical support from E. Danilov for the time-resolved absorption experiment. K.G. and F.S. acknowledge support from the National Science Foundation Designing Materials to Revolutionize and Engineer our Future programme (grant 1729383) and the NC State University Research and Innovation Seed Funding (RISF).
Author information
Authors and Affiliations
Contributions
G.F. and M.B. performed the PL and TRPL measurements and pump–probe experiments and analysed the results. D.S. assisted with the pump–probe experiments and H.A. provided help with TRPL experiments. A.B. performed steady-state absorption and PL experiments. L.L., Q.D. and F.S. provided the samples. K.G. conceived the research problems and coordinated the studies. K.G. drafted the manuscript with the help of G.F. and M.B. All authors helped with editing the manuscript.
Corresponding author
Ethics declarations
Competing interests
The authors declare no competing interests.
Additional information
Peer review information Nature Photonics thanks Gombojav Ariunbold and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary information
Supplementary Information
Supplementary Discussion and Figs. 1–15.
Source data
Source Data Fig. 2
Source Data for graphs.
Source Data Fig. 3
Source Data for graphs.
Source Data Fig. 4
Source Data for graphs.
Rights and permissions
About this article
Cite this article
Findik, G., Biliroglu, M., Seyitliyev, D. et al. High-temperature superfluorescence in methyl ammonium lead iodide. Nat. Photon. 15, 676–680 (2021). https://doi.org/10.1038/s41566-021-00830-x
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1038/s41566-021-00830-x
This article is cited by
-
Single-photon superradiance in individual caesium lead halide quantum dots
Nature (2024)
-
Structured air lasing of N2+
Communications Physics (2023)
-
Room-temperature superfluorescence in hybrid perovskites and its origins
Nature Photonics (2022)
-
Room-temperature upconverted superfluorescence
Nature Photonics (2022)