Search

Diluted magnetic semiconductor (DMS) colloidal nanocrystals demonstrate remarkable magneto-optical properties. However, the behavior of circular polarization of their emission in high magnetic fields remains unclear. We measure magneto-optical properties of colloidal CdSe/CdMnS nanoplatelets in high magnetic fields up to 30 T and at cryogenic temperatures. The degree of circular polarization of photoluminescence demonstrates non-monotonous behavior in a magnetic field. In low magnetic fields, the polarization degree is positive, due to an exchange interaction of excitons with localized spins of magnetic Mn ions. The exchange interaction is strong enough to overcome the intrinsic Zeeman splitting, which provides negatively polarized emission in nonmagnetic CdSe/CdS nanoplatelets. After reaching a maximum the polarization degree starts to decrease and reverses the sign to negative in high magnetic fields. The critical magnetic field, in which the sign is reversed, increases when temperature is elevated. We develop a model, which explains this behavior by an interplay of bright and dark exciton recombination.

Semiconductor colloidal quantum wells (CQWs) make an exciting quasi-2D class of nanocrystals thanks to their unique properties including their highly anisotropic optical transition dipole moment (TDM). Thus, employing a film of CQWs with face-down orientation as an emissive layer (EML) in an electroluminescent device is expected to substantially boost photon outcoupling efficiency. Here, we show all-solution-processed colloidal quantum well light-emitting diodes (CQW-LEDs) using a single all-face-down oriented self-assembled monolayer (SAM) film of CQWs that enables a high level of in-plane (IP) TDMs of 92%. This SAM film significantly enhances the outcoupling efficiency from 22% (of standard randomly-oriented emitters) to 34% (of face-down oriented emitters) and charge injection efficiency. This SAM-CQW-LED architecture enables a record high level of external quantum efficiency of 18.1% for the solution-processed type of CQW-LEDs, putting their efficiency performance on par with the hybrid organic-inorganic evaporation-based CQW-LEDs and all other best solution-processed LEDs. In addition, this architecture provides a high maximum brightness of 19,800 cd/m2 with a long operational lifetime of 247 h at 100 cd/m2 along with saturated deep-red emission (651 nm). These findings indicate the effectiveness of oriented self-assembly of CQWs as electrically-driven emissive layers in improving outcoupling and external quantum efficiencies in the CQW-LEDs.

Optical gain in solution, which provides high photostability as a result of continuous regeneration of the gain medium, is extremely attractive for optoelectronic applications. Here, we propose and demonstrate amplified spontaneous emission (ASE) in solution with ultralow thresholds of 30 mikroJ/cm2 in red and of 44 mikroJ/cm2 in green from engineered colloidal quantum well (CQW) heterostructures. For this purpose, CdSe/CdS core/crown CQWs, designed to hit the green region, and CdSe/CdS/CdxZn1-xS core/crown/gradient-alloyed shell CQWs, further tuned to reach the red region by shell alloying, were employed to achieve high-performance ASE in the visible. The net modal gain of these CQWs reaches 530 cm-1 for the green and 201 cm-1 for the red, two orders of magnitude larger than those of colloidal quantum dots (QDs) in solution owing to intrinsically larger gain cross-sections of these CQWs. To explain the root cause for ultrahigh gain coefficient in solution, we show that for the first time that the gain cross-sections of these CQWs is 3.3x10-14 cm2 in the green and 1.3x10-14 cm2 in the red which are two orders magnitude larger compared to those of CQDs. These findings confirm the extraordinary prospects of these solution-processed CQWs as solution-based optical gain media in lasing applications.

In this work, we report the first account of monolithically-fabricated vertical cavity surface emitting lasers (VCSELs) of densely-packed, orientation-controlled, atomically flat colloidal quantum wells (CQWs) using a self-assembly method and demonstrate single-mode lasing from a record thin colloidal gain medium with a film thickness of 7 nm under femtosecond optical excitation. We used specially engineered CQWs to demonstrate these hybrid CQW-VCSELs consisting of only a few layers to a single monolayer of CQWs and achieved the lasing from these thin gain media by thoroughly modeling and implementing a vertical cavity consisting of distributed Bragg reflectors with an additional dielectric layer for mode tuning. Accurate spectral and spatial alignment of the cavity mode with the CQW films was secured with the help of full electromagnetic computations. While overcoming the long-pending problem of limited electrical conductivity in thicker colloidal films, such ultra-thin colloidal gain media can help enabling fully electrically-driven colloidal lasers.

Colloidal semiconductor quantum wells have emerged as a promising material platform for use in solution-processable light-generation including colloidal lasers. However, application relying on their optical gain suffer from a fundamental complication due to multi-excitonic nature of light amplification in common II-VI semiconductor nanocrystals. This undesirably increases the optical gain threshold and shortens the net gain lifetime because of fast nonradiative Auger decay. Here, we demonstrate sub-single exciton level of optical gain threshold in specially engineered CdSe/CdS@CdZnS core/crown@gradient alloyed shell colloidal quantum wells. This sub-single exciton ensemble-averaged gain threshold of Ng = 0.80 (per particle) resulting from impeded Auger recombination along with a large absorption cross-section of quantum wells enables us to observe the amplified spontaneous emission starting at a low pump fluence of 800 nJ cm-2, at least three-folds better than the previously best reported values among all colloidal semiconductor nanocrystals. Moreover, long optical gain lifetimes of 800 ps accompanied with modal gain coefficients of 2,000 cm-1 are achieved. Finally, using these gradient shelled quantum wells, we show a vertical cavity surface-emitting colloidal laser operating at an ultralow lasing threshold of 7.5 micro-joule cm-2. These results represent a significant step towards the realization of solution-processable electrically-driven colloidal lasers.

Biexcitons have been considered as one of the fundamental building blocks for quantum technology because of its overwhelming advantages in generating entangled photon pairs. Although many-body complexes have been demonstrated recently in mono-layer transition metal dichalcogenides (TMDs), the low emission efficiency and scale up capability hinder their applications. Colloidal nanomaterials, with high quantum efficiency and ease of synthesis/processing, are regarded to be an appealing complement to TMDs for biexciton sources. However, a progress towards biexciton emission in colloidal nanomaterials has been challenging largely by small binding energy and ultrafast non-radiative multiexciton recombination. Here, we demonstrate room-temperature biexciton emission in Cu-doped CdSe colloidal quantum wells (CQWs) under continuous-wave excitation with intensity as low as ~10 W/cm2. The characteristics of radiative biexciton states are investigated by their super linear emission with respect to excitation power, thermal stability and transient photophysics. The interaction between the quantum confined host carriers and the dopant ions increases biexciton binding energy by two folds compared to the undoped CQWs. Such strong binding energy together with suppressed Auger recombination and efficient, spectrally narrow photoluminescence in a quasi-2D semiconductor enables sustained biexciton emission at room temperature, providing a potential solution for efficient, scalable and stand-alone quantum devices., Comment: 11 pages, 5 Figures

We demonstrate high quantum yield broad photoluminescence emission of ultrathin sub-nanometer CdSe nanoplatelets (two-monolayer). They also exhibit polarization-characterized lateral size dependent anomalous heavy hole and light/split-off hole absorption intensities., Comment: Published in Conference on Lasers and Electro-Optics (CLEO): Science and Innovations 2017, San Jose, CA, USA, 14-19 May 2017 (2 pages, 3 figures)

Carrier-dopant exchange interactions in Mn-doped PbS colloidal quantum dots were studied by circularly polarized magneto-photoluminescence. Mn substitutional doping leads to paramagnetic behavior down to 5 K. While undoped quantum dots show negative circular polarization, Mn doping changes its sign to positive. A circular polarization value of 40% was achieved at T=7 K and B=7 tesla. The results are interpreted in terms of Zeeman splitting of the band edge states in the presence of carrier-dopant exchange interactions that are qualitatively different from the s,p-d exchange interactions in II-VI systems., Comment: 4 pages, 4 figures; To appear in Applied Physics Letters 101 (2012)