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Original Article Open Access
Giant magneto field effect in up-conversion amplified spontaneous emission via spatially extended states in organic-inorganic hybrid perovskites
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Abstract
Up-conversion lasing actions are normally difficult to realize in light-emitting materials due to small multi-photon absorption cross section and fast dephasing of excited states during multi-photon excitation. This paper reports an easily accessible up-conversion amplified spontaneous emission (ASE) in organic-inorganic hybrid perovskites (MAPbBr3) films by optically exciting broad gap states with sub-bandgap laser excitation. The broad absorption was optimized by adjusting the grain sizes in the MAPbBr3 films. At low sub-bandgap pumping intensities, directly exciting the gap states leads to 2-photon, 3-photon, and 4-photon up-conversion spontaneous emission, revealing a large optical cross section of multi-photon excitation occurring in such hybrid perovskite films. At moderate pumping intensity (1.19 mJ/cm2) of 700 nm laser excitation, a significant spectral narrowing phenomenon was observed with the full width at half maximum (FWHM) decreasing from 18 nm to 4 nm at the peak wavelength of 550 nm, simultaneously with a nonlinear increase on spectral peak intensity, showing an up-conversion ASE realized at low threshold pumping fluence. More interestingly, the up-conversion ASE demonstrated a giant magnetic field effect, leading to a magneto-ASE reaching 120%. In contrast, the up-conversion photoluminescence (PL) showed a negligible magnetic field effect (< 1%). This observation provides an evidence to indicate that the light-emitting states responsible for up-conversion ASE are essentially formed as spatially extended states. The angular dependent spectrum results further verify the existence of spatially extended states which are polarized to develop coherent in-phase interaction. Clearly, using broad gap states with spatially extended light-emitting states presents a new approach to develop up-conversion ASE in organic-inorganic hybrid perovskites. -
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References
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Supplementary Information
Supplementary Information for Giant magneto field effect in up-conversion amplified spontaneous emission via spatially extended states in organic-inorganic hybrid perovskites 
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Figure 1.
Morphological and spectral characterizations. (a) SEM image to show large grains with micrometer sizes. (b) Optical absorption spectrum (inset: band edge with PL). (c) Up-conversion ASE under 700 nm excitation wavelength (threshold pumping fluence: 1.19 mJ/cm2). Inset: spectral narrowing with emission intensity simultaneously increasing phenomena. (d) Threshold dependence on excitation wavelength. Inset: luminescence above (the upper left) and below (the bottom right) threshold.
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Figure 2.
Multi-photon up-conversion PL and intensity dependence. (a, d) 2-photon process under 900 nm excitation wavelength. (b),(e) 3-photon process under 1200 nm excitation wavelength. (c, f) 4-photon process under 1500 nm excitation wavelength.
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Figure 3.
ASE measured with and without magnetic field in both up- and down-conversion regions. Magnetic field: 1.2 T. (a) Up-conversion ASE under 800 nm excitation wavelength. (b) Down-conversion ASE under 480 nm excitation wavelength. (c) Orbital order: orbitals are aligned through magnetic dipoles to form cooperative light-emitting states towards developing an ASE.
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Figure 4.
Angle and polarization dependences for ASE and PL. (a) Setup for angle dependence measurement. (b) Spatial distributions of ASE and PL outputs. (c) Setup for polarization measurement. (d) Polarizations of ASE and PL outputs.
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Figure FIG. 1304..
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