Colloidal Quantum Dot Lasing: Historical Perspective and Recent Progress
Victor Klimov a
a Los Alamos National Laboratory, US, MS-J567, Los Alamos, NM 87545, United States
Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe Fall Meeting 2018 (NFM18)
S3 Fundamental Processes in Semiconductor Nanocrystals
Torremolinos, Spain, 2018 October 22nd - 26th
Organizers: Shannon Boettcher, David Egger, Laura Herz, Joaquim Puigdollers, Arjan Houtepen, Tianquan Lian, Alejandro Perez-Rodriguez, Kevin Sivula, Tze-Chien Sum, Alison Walker, Mischa Bonn, Claudio Quarti and Freddy Rabouw
Keynote, Victor Klimov, presentation 186
DOI: https://doi.org/10.29363/nanoge.nfm.2018.186
Publication date: 6th July 2018

Chemically synthesized quantum dots (QDs) can potentially enable new classes of highly flexible, spectrally tunable lasers processible from solutions [1,2]. Despite a considerable progress over the past years, colloidal-QD lasing, however, is still at the laboratory stage and an important challenge - realization of lasing with electrical injection - is still unresolved. A major complication, which hinders the progress in this field, is fast nonradiative Auger recombination of gain-active multicarrier species such as trions (charged excitons) and biexcitons [3,4]. Recently, we explored several approaches for mitigating the problem of Auger decay by taking advantage of a new generation of core/multi-shell QDs with a radially graded composition that allow for considerable (nearly complete) suppression of Auger recombination by “softening” the electron and hole confinement potentials [5]. Using these specially engineered QDs, we have been able to realize optical gain with direct-current electrical pumping [6], which has been a long-standing goal in the field of colloidal nanostructures. Further, we apply these dots to practically demonstrated the viability of a “zero-threshold-optical-gain” concept using not neutral but negatively charged particles wherein the pre-existing electrons block either partially or completely ground-state absorption [7]. Such charged QDs are optical-gain-ready without excitation and, in principle, can exhibit lasing at vanishingly small pump levels. All of these exciting recent developments demonstrate a considerable promise of colloidal nanomaterials for implementing solution-processible optically and electrically pumped laser devices operating across a wide range of wavelengths and fabricated on virtually any substrate using a variety of optical-cavity designs.

[1] Klimov, V. I.et al., Optical gain and stimulated emission in nanocrystal quantum dots. Science290, 314 (2000).

[2] Klimov, V. I.et al., Single-exciton optical gain in semiconductor nanocrystals. Nature447, 441 (2007).

[3] Klimov, V. I. et al., Quantization of multiparticle Auger rates in semiconductor quantum dots. Science287, 1011 (2000).

[4] Robel, I., et al., Universal Size-Dependent Trend in Auger Recombination in Direct-Gap and Indirect-Gap Semiconductor Nanocrystals. Phys. Rev. Lett.102, 177404 (2009).

[5] Y.-S. Park, et al., Effect of Interfacial Alloying versus “Volume Scaling” on Auger Recombination in Compositionally Graded Semiconductor Quantum Dots. Nano Lett. 17, 5607 (2017).

[6] Lim, J., et al., Optical Gain in Colloidal Quantum Dots Achieved by Direct-Current Charge Injection. Nat. Mater.17, 42 (2018).

[7] Wu, K., et al., Towards zero-threshold optical gain using charged semiconductor quantum dots. Nat. Nanotechnol.12, 1140 (2017).

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