Exploring Stimulated Emission of 2D Semiconductor Nanoplatelets in Liquid Core Fibers

Dominik Rudolph^a^,^c, Jannika Lauth^a^,^c^,^g^,^h, Veronika Adolfs^b, Artsiom Antanovich^a, Dan Huy Chau^b, Mario Chemnitz^d^,^e, Markus A. Schmidt^d^,^e, Simon Spelthann^b^,^c, Micheal Steinke^a^,^c^,^f

^aLeibniz University Hannover, Institute of Physical Chemistry and Electrochemistry, Callinstraße 3A, D-30167 Hannover, Germany

^bLeibniz University Hannover, Institute of Quantum Optics, Welfengarten 1, D-30167 Hannover, Germany

^cCluster of Excellence PhoenixD (Photonics, Optics, and Engineering – Innovation Across Disciplines), Welfengarten 1A, D-30167 Hannover, Germany.

^dLeibniz- Institute of Photonic Technology, Albert-Einstein-Straße 9, D-07745 Jena, Germany

^eAbbe Center of Photonics, Friedrich-Schiller-University, Albert-Einstein-Straße 6

^fLeibniz University Hannover, QUEST-Leibniz-Research School, Callinstraße 36, D-30167 Hannover, Germany

^gLeibniz University Hannover, Laboratory of Nano and Quantum Engineering (LNQE), Schneiderberg 39, D-30167 Hannover, Germany

^hUniversity Tübingen, Institute of Physical and Theoretical Chemistry, Auf der Morgenstelle 18, D-72076 Tübingen, Germany

Proceedings of MATSUS Fall 2024 Conference (MATSUSFall24)

#PhotoQD - Photophysics of colloidal quantum dots

Lausanne, Switzerland, 2024 November 12th - 15th

Organizers: Philippe Green and Jannika Lauth

Oral, Dominik Rudolph, presentation 187
Publication date: 28th August 2024

Colloidal cadmium chalcogenide-based 2D nanoplatelets (NPLs) display exceptionally narrow absorption and photoluminescence bands, large one- and two-photon absorption cross sections [1] as well as low Auger recombination rates [2] and low gain thresholds [3]. Following the major strides made in the colloidal synthesis of tailored NPLs and related heterostructures, the current research focus has shifted to the incorporation of such NPLs into optical setups and devices, e.g. LEDs and lasing [4]. To date, such application-oriented setups often rely on NPL thin films [5]. Recently, however, an alternative approach using colloidal NPLs in solution gained traction, e.g. in short capillaries with the promise of higher photostability and integration into cavities [6].

Here, we demonstrate optical gain in hollow fused silica liquid-core fibers (LCFs, 20 µm core diameter) filled with a colloidal solution of 4.5 monolayer thick core-crown CdSe/CdS NPLs. The fibers are transversally excited at 480 nm in a stripe geometry (ca. 60 mm) by a 4 ns optical parametric oscillator. Aside from monoexcitonic spontaneous emission, we also observe amplified spontaneous emission (ASE), showing a characteristic bathochromic shift and peak sharpening due to its biexcitonic nature. Importantly, the arising ASE (pump energy threshold of 65 µJ) could only be observed when enabling the LCF waveguiding properties by utilizing a high refractive index solvent, like tetrachloroethylene. If a solvent with a lower refractive index than fused silica is used, e.g. hexane, which suppresses waveguiding, no ASE threshold is reached.

In conclusion, our findings indicate that NPL-filled LCFs offer a viable and efficient approach to achieving visible lasing from fused silica fibers. Incorporating colloidal semiconductor nanostructures into LCFs enables a pathway towards visible-range fiber lasers and offers integrability and flexibility, including tunable optical properties by simple replacement of the lasing medium.

References:

[1] Yeltik, A; Delikanli, S.; Olutas, M.; Kelestemur, Y.; Guzelturk, B.; Demir, H. V. Experimental Determination of the Absorption Cross-Section and Molar Extinction Coefficient of Colloidal CdSe Nanoplatelets. J. Phys. Chem. C 2015, 119, 47, 26768–26775.

[2] Polovitsyn, A.; Dang, Z.; Movilla, J. L.; Martin-Garcia, B.; Khan, A. H.; Betrand, G. H. V.; Brecia, R.; Moreels, I. Synthesis of Air-Stable CdSe/ZnS Core–Shell Nanoplatelets with Tunable Emission Wavelength. J. Chem. Mater. 2017, 29, 13, 5671–5680.

[3] Geuchies, J. J.; Dijkhuizen, R.; Koel, M.; Grimaldie, G.; Fossé, I.; Evers, W. H.; Hens, Z.; Houepen, A. J. Zero-Threshold Optical Gain in Electrochemically Doped Nanoplatelets and the Physics Behind It. ACS Nano 2022, 16, 18777.

[4] Zhang, Q.; Zhu, Y.; Niu, P.; Lao, C.; Yao, Y.; Liu, W.; Yang, Q. F.; Chu, S.; Gao, Y. Low-Threshold Single-Mode Microlasers from Green CdSe/CdSeS Core/Alloyed-Crown Nanoplatelets. ACS Photonics 2023, 10, 5, 1397-1404.

[5] Belitsch, M.; Dirin, D. N.; Kovalenko, M. V.; Pichler, K.; Rotter, S.; Ghalgaoui, A.; Ditlbacher, H.; Hohenau, A.; Krenn, J. R. Gain and lasing from CdSe/CdS nanoplatelet stripe waveguides. Micro and Nano Engineering 2022, 17, 100167.

[6] Delikanli, S.; Erdem, O.; Isik, F.; Baruj, H. D.; Shabani, F.; Yagci, H. B.; Durmusoglu, E. G.; Demir, H. V. Ultrahigh Green and Red Optical Gain Cross Sections from Solutions of Colloidal Quantum Well Heterostructures. The journal physical chemistry letters 2021, 12, 2177.

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