Optical gain in colloidal quantum dots achieved with direct-current electrical pumping
Source abstract
Abstract
Chemically synthesized semiconductor quantum dots (QDs) can potentially enable solution-processable laser diodes with a wide range of operational wavelengths, yet demonstrations of lasing from the QDs are still at the laboratory stage. An important challenge-realization of lasing with electrical injection-remains unresolved, largely due to fast nonradiative Auger recombination of multicarrier states that represent gain-active species in the QDs. Here we present population inversion and optical gain in colloidal nanocrystals realized with direct-current electrical pumping. Using continuously graded QDs, we achieve a considerable suppression of Auger decay such that it can be outpaced by electrical injection. Further, we apply a special current-focusing device architecture, which allows us to produce high current densities (j) up to ∼18 A cm-2 without damaging either the QDs or the injection layers. The quantitative analysis of electroluminescence and current-modulated transmission spectra indicates that with j = 3-4 A cm-2 we achieve the population inversion of the band-edge states.
Source: europepmc · Quality: candidate unverified · Source record ↗
Research context
OpenAlex topics: Quantum Dots Synthesis And Properties · Chalcogenide Semiconductor Thin Films · Nanocluster Synthesis and Applications
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (27)
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1. Svelto, O. Principles of Lasers Vol. 1, 5 edn (Springer, 2010).10.1007/978-1-4419-1302-9 ↗
2. Klimov, V. I. et al. Optical gain and stimulated emission in nanocrystal quantum dots. Science 290, 314–317 (2000).10.1126/science.290.5490.314 ↗
3. Landsberg, P. T. Recombination in Semiconductors (Cambridge Univ. Press, 1991).
4. Robel, I., Gresback, R., Kortshagen, U., Schaller, R. D. & Klimov, V. I. Universal size-dependent trend in Auger recombination in direct-gap and indirect-gap semiconductor nanocrystals. Phys. Rev. Lett. 102, 177404 (2009).10.1103/PhysRevLett.102.177404 ↗
5. García-Santamaría, F. et al. Suppressed Auger recombination in “Giant” nanocrystals boosts optical gain performance. Nano Lett. 9, 3482–3488 (2009).10.1021/nl901681d ↗
6. Nasilowski, M., Spinicelli, P., Patriarche, G. & Dubertret, B. Gradient CdSe/CdS quantum dots with room temperature biexciton unity quantum yield. Nano Lett. 15, 3953–3958 (2015).10.1021/acs.nanolett.5b00838 ↗
7. Htoon, H., Hollingsworth, J. A., Dickerson, R. & Klimov, V. I. Effect of zero- to one-dimensional transformation on multiparticle Auger recombination in semiconductor quantum rods. Phys. Rev. Lett. 91, 227401 (2003).10.1103/PhysRevLett.91.227401 ↗
8. Rabouw, F. T. et al. Reduced Auger recombination in single CdSe/CdS nanorods by one-dimensional electron delocalization. Nano Lett. 13, 4884–4892 (2013).10.1021/nl4027567 ↗
9. Lutich, A. A. et al. Multiexcitonic dual emission in CdSe/CdS tetrapods and nanorods. Nano Lett. 10, 4646–4650 (2010).10.1021/nl1028057 ↗
10. Cragg, G. E. & Efros, A. L. Suppression of Auger processes in confined structures. Nano Lett. 10, 313–317 (2010).10.1021/nl903592h ↗
11. Bae, W. K. et al. Controlled alloying of the core–shell interface in CdSe/CdS quantum dots for suppression of Auger recombination. ACS Nano 7, 3411–3419 (2013).10.1021/nn4002825 ↗
12. Bae, W. K. et al. Controlling the influence of Auger recombination on the performance of quantum-dot light-emitting diodes. Nat. Commun. 4, 3661 (2013).
13. Park, Y.-S., Bae, W. K., Baker, T., Lim, J. & Klimov, V. I. Effect of Auger recombination on lasing in heterostructured quantum dots with engineered core/shell interfaces. Nano Lett. 15, 7319–7328 (2015).10.1021/acs.nanolett.5b02595 ↗
14. Vaxenburg, R., Rodina, A., Lifshitz, E. & Efros, A. L. Biexciton Auger recombination in CdSe/CdS core/shell semiconductor nanocrystals. Nano Lett. 16, 2503–2511 (2016).10.1021/acs.nanolett.6b00066 ↗
15. Park, Y.-S., Bae, W. K., Pietryga, J. M. & Klimov, V. I. Auger recombination of biexcitons and negative and positive trions in individual quantum dots. ACS Nano 8, 7288–7296 (2014).10.1021/nn5023473 ↗
16. Efros, A. L. et al. Band-edge exciton in quantum dots of semiconductors with a degenerate valence band: dark and bright exciton states. Phys. Rev.B 54, 4843–4856 (1996).10.1103/PhysRevB.54.4843 ↗
17. Norris, D. J. & Bawendi, M. G. Measurement and assignment of the size-dependent optical spectrum in CdSe quantum dots. Phys. Rev. B 53, 16338–16346 (1996).10.1103/PhysRevB.53.16338 ↗
18. Klimov, V. I. Multicarrier interactions in semiconductor nanocrystals in relation to the phenomena of Auger recombination and carrier multiplication. Annu. Rev. Condens. Matter Phys. 5, 285–316 (2014).10.1146/annurev-conmatphys-031113-133900 ↗
19. Vanmaekelbergh, D. et al. Shape-dependent multiexciton emission and whispering gallery modes in supraparticles of CdSe/multishell quantum dots. ACS Nano 9, 3942–3950 (2015).10.1021/nn507310f ↗
20. Gollner, C. et al. Random lasing with systematic threshold behavior in films of CdSe/CdS core/thick-shell colloidal quantum dots. ACS Nano 9, 9792–9801 (2015).10.1021/acsnano.5b02739 ↗
21. Diaconescu, B., Padilha, L. A., Nagpal, P., Swartzentruber, B. S. & Klimov, V. I. Measurement of electronic states of PbS nanocrystal quantum dots using scanning tunneling spectroscopy: the role of parity selection rules in optical absorption. Phys. Rev. Lett. 110, 127406 (2013).10.1103/PhysRevLett.110.127406 ↗
22. Dai, X. et al. Solution-processed, high-performance light-emitting diodes based on quantum dots. Nature 515, 96–99 (2014).10.1038/nature13829 ↗
23. Kwak, J. et al. Bright and efficient full-color colloidal quantum dot light-emitting diodes using an inverted device structure. Nano Lett. 12, 2362–2366 (2012).10.1021/nl3003254 ↗
24. Lim, J. et al. Influence of shell thickness on the performance of light-emitting devices based on CdSe/Zn1−XCdXS core/shell heterostructured quantum dots. Adv. Mater. 26, 8034–8040 (2014).10.1002/adma.201403620 ↗
25. Klimov, V. I. Optical nonlinearities and ultrafast carrier dynamics in semiconductor nanocrystals. J. Phys. Chem. B 104, 6112–6123 (2000).10.1021/jp9944132 ↗
26. Crooker, S. A., Barrick, T., Hollingsworth, J. A. & Klimov, V. I. Multiple temperature regimes of radiative decay in CdSe nanocrystal quantum dots: intrinsic limits to the dark-exciton lifetime. Appl. Phys. Lett. 82, 2793–2795 (2003).10.1063/1.1570923 ↗
27. Joshi, A., Narsingi, K. Y., Manasreh, M. O., Davis, E. A. & Weaver, B. D. Temperature dependence of the band gap of colloidal CdSe/ZnS core/shell nanocrystals embedded into an ultraviolet curable resin. Appl. Phys. Lett. 89, 131907 (2006).10.1063/1.2357856 ↗