Cadmium chalcogenide nanoplatelets (NPLs) and their heterostructures have been reported to have low gain thresholds and large gain coefficients, showing great potential for lasing applications. However, the further improvement of the optical gain properties of NPLs is hindered by a lack of models that can account for their optical gain characteristics and predict their dependence on the properties (such as lateral size, concentration, and/or optical density). Herein, we report a systematic study of optical gain (OG) in 4-monolayer thick CdSe NPLs by both transient absorption spectroscopy study of colloidal solutions and amplified spontaneous emission (ASE) measurement of thin films. We showed that comparing samples with the same optical density at the excitation, the OG threshold is not dependent of the NPL lateral area, while the saturation gain amplitude is dependent on the NPL lateral area when comparing samples with the same optical density at the excitation wavelength. Both the OG and ASE thresholds increase with the optical density at the excitation wavelength for samples of the same NPL thickness and lateral area. We proposed an OG model for NPLs that can successfully account for the observed lateral area and optical density dependences. The model reveals that OG originates from stimulated emission from the bi-exciton states and the OG threshold is reached when the average number of excitons per NPL is about half the occupation of the band-edge exciton states. The model can also rationalize the much lower OG thresholds in the NPLs compared to QDs. This work provides a microscopic understanding of the dependence of the OG properties on the morphology of the colloidal nanocrystals and important guidance for the rational optimization of the lasing performance of NPLs and other 1- and 2-dimensional nanocrystals.
more »
« less
Gain roll-off in cadmium selenide colloidal quantum wells under intense optical excitation
Abstract Colloidal quantum wells, or nanoplatelets, show among the lowest thresholds for amplified spontaneous emission and lasing among solution-cast materials and among the highest modal gains of any known materials. Using solution measurements of colloidal quantum wells, this work shows that under photoexcitation, optical gain increases with pump fluence before rolling off due to broad photoinduced absorption at energies lower than the band gap. Despite the common occurrence of gain induced by an electron–hole plasma found in bulk materials and epitaxial quantum wells, under no measurement conditions was the excitonic absorption of the colloidal quantum wells extinguished and gain arising from a plasma observed. Instead, like gain, excitonic absorption reaches a minimum intensity near a photoinduced carrier sheet density of 2 × 10 13 cm −2 above which the absorption peak begins to recover. To understand the origins of these saturation and reversal effects, measurements were performed with different excitation energies, which deposit differing amounts of excess energy above the band gap. Across many samples, it was consistently observed that less energetic excitation results in stronger excitonic bleaching and gain for a given carrier density. Transient and static optical measurements at elevated temperatures, as well as transient X-ray diffraction of the samples, suggest that the origin of gain saturation and reversal is a heating and disordering of the colloidal quantum wells which produces sub-gap photoinduced absorption.
more »
« less
- Award ID(s):
- 1808590
- NSF-PAR ID:
- 10378351
- Date Published:
- Journal Name:
- Scientific Reports
- Volume:
- 12
- Issue:
- 1
- ISSN:
- 2045-2322
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
more » « less
Abstract A type-II InAs/AlAs
$$_{0.16}$$ $$_{0.84}$$ $$>100$$ $$E{_g}$$ $$E{_g}$$ $$ $$>E{_g}$$ -
Razeghi, Manijeh ; Khodaparast, Giti A. ; Vitiello, Miriam S. (Ed.)Band structure, strain, and polarization engineering of nitride heterostructures open unparalleled opportunities for quantum sensing in the infrared. Intersubband absorption and photoluminescence are employed to correlate structure with optical properties of nonpolar strain-balanced InGaN/AlGaN nanostructures grown by molecular-beam epitaxy. Mid-infrared intersubband transitions in m-plane (In)AlxGa1-xN/In0.16Ga0.84N (0.19x0.3) multi-quantum wells were observed for the first time in the range of 3.4-5.1 μm (244-360 meV). Direct and attenuated total-reflection infrared absorption measurements are interpreted using structural information revealed by high-resolution x-ray diffraction and transmission electron microanalysis. The experimental intersubband energies are better reproduced by calculations using the local-density approximation than the Hartree-Fock approximation for the exchange-correlation correction. The effect of charge density, quantum well width, and barrier alloy composition on the intersubband transition energy was examined to evaluate the potential of this material for practical infrared applications. Temperature-dependent continuous-wave and time-resolved photoluminescence (TRPL) measurements are also investigated to probe carrier localization and recombination in m-plane InGaN/AlGaN quantum wells. Average localization depths of 21 meV and 40 meV were estimated for the undoped and doped structures, respectively. Using TRPL, dual localization centers were identified in undoped structures, while a single type of localization centers was found in doped structures. At 2 K, a fast decay time of approximately 0.3ns was measured for both undoped and doped structures, while a longer decay time of 2.2 ns was found only for the undoped sample. TRPL in magnetic field was explored to examine the effect of doping sheets on carrier dynamics.more » « less
-
The magnitude and temporal evolution of the quantum-state renormalization (QSR), or the energetic shifting of the quantum-confinement states caused by photoexcitation and changes in electron screening, were probed in transient absorption (TA) spectroscopy measurements of colloidal semiconductor nanoparticles. Experiments were performed on high- and lower-quality wurtzite CdTe quantum wires (QWs) with photoluminescence quantum yields of 8.8% and ∼0.2% using low-excitation fluences. The QSR shifts the spectral features to lower energies in both samples, with larger shifts measured in the high-quality QWs. The TA spectral features measured for both samples shift uniquely with time after photoexcitation, illustrating dynamic QSR that depends on the quantum-confinement states and on the states occupied by carriers. The higher fraction of carriers that reach the band-edge states in the high-quality QWs results in larger renormalization, with the energies of the band-edge states approaching the Stokes shift of the steady-state photoluminescence feature below the band-edge absorption energy. The intraband relaxation dynamics of charge carriers photoexcited in semiconductor nanoparticles was also characterized after accounting for contributions from QSR in the TA data. The intraband relaxation to the band-edge states was slower in the high-quality QWs than in the lower-quality QWs, likely due to the reduced number of trap states accessible. The contrasting relaxation time scales provide definitive evidence for a dependence of the photoluminescence efficiency on excitation energy. These studies reveal the complicated interplay between the energetics and relaxation mechanisms of carriers within semiconductor nanoparticles, even those with the same dimensionality.more » « less
-
Abstract High-precision placement of rare-earth ions in scalable silicon-based nanostructured materials exhibiting high photoluminescence (PL) emission, photostable and polarized emission, and near-radiative-limited excited state lifetimes can serve as critical building blocks toward the practical implementation of devices in the emerging fields of nanophotonics and quantum photonics. Introduced herein are optical nanostructures composed of arrays of ultrathin silicon carbide (SiC) nanowires (NWs) that constitute scalable one-dimensional NW-based photonic crystal (NW-PC) structures. The latter are based on a novel, fab-friendly, nanofabrication process. The NW arrays are grown in a self-aligned manner through chemical vapor deposition. They exhibit a reduction in defect density as determined by low-temperature time-resolved PL measurements. Additionally, the NW-PC structures enable the positioning of erbium (Er 3+ ) ions with an accuracy of 10 nm, an improvement on the current state-of-the-art ion implantation processes, and allow strong coupling of Er 3+ ions in NW-PC. The NW-PC structure is pivotal in engineering the Er 3+ -induced 1540-nm emission, which is the telecommunication wavelength used in optical fibers. An approximately 60-fold increase in the room-temperature Er 3+ PL emission is observed in NW-PC compared to its thin-film analog in the linear pumping regime. Furthermore, 22 times increase in the Er 3+ PL intensity per number of exited Er ions in NW-PC was observed at saturation while using 20 times lower pumping power. The NW-PC structures demonstrate broadband and efficient excitation characteristics for Er 3+ , with an absorption cross-section (~2 × 10 −18 cm 2 ) two-order larger than typical benchmark values for direct absorption in rare-earth-doped quantum materials. Experimental and simulation results show that the Er 3+ PL is photostable at high pumping power and polarized in NW-PC and is modulated with NW-PC lattice periodicity. The observed characteristics from these technologically friendly nanophotonic structures provide a promising route to the development of scalable nanophotonics and formation of single-photon emitters in the telecom optical wavelength band.more » « less
- Free Publicly Accessible Full Text
-
Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1038/s41598-022-11882-6
