Browsing by Author "Sharma, A."
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Item Open Access All-optical control of exciton flow in a colloidal quantum well complex(Springer Nature, 2020) Yu, J.; Sharma, Manoj; Sharma, A.; Delikanlı, Savaş; Demir, Hilmi Volkan; Dang, C.Excitonics, an alternative to romising for processing information since semiconductor electronics is rapidly approaching the end of Moore’s law. Currently, the development of excitonic devices, where exciton flow is controlled, is mainly focused on electric-field modulation or exciton polaritons in high-Q cavities. Here, we show an all-optical strategy to manipulate the exciton flow in a binary colloidal quantum well complex through mediation of the Förster resonance energy transfer (FRET) by stimulated emission. In the spontaneous emission regime, FRET naturally occurs between a donor and an acceptor. In contrast, upon stronger excitation, the ultrafast consumption of excitons by stimulated emission effectively engineers the excitonic flow from the donors to the acceptors. Specifically, the acceptors’ stimulated emission significantly accelerates the exciton flow, while the donors’ stimulated emission almost stops this process. On this basis, a FRET-coupled rate equation model is derived to understand the controllable exciton flow using the density of the excited donors and the unexcited acceptors. The results will provide an effective all-optical route for realizing excitonic devices under room temperature operation.Item Open Access Blue-emitting CdSe nanoplatelets enabled by sulfur-alloyed heterostructures for light-emitting diodes with low turn-on voltage(American Chemical Society, 2021-12-28) İzmir, M.; Sharma, A.; Shendre, S.; Durmuşoğlu, E. G.; Sharma, V. K.; Shabani, Farzan; Baruj, Hamed Dehghanpour; Delikanlı, Savaş; Sharma, M.; Demir, Hilmi VolkanColloidal nanoplatelets (NPLs) have emerged as the last class of semiconductor nanocrystals for their potential optoelectronic applications. The heterostructures of these nanocrystals can achieve high photoluminescence quantum yield and enhanced photostability, along with color purity. Such advantages make them a promising candidate for solution-processable light-emitting diodes (LEDs). However, to date, blue-emitting CdSe nanoplatelets (NPLs) exhibit poor photoluminescence quantum yield and also typically suffer from a rolled-up morphology. To mitigate these problems in this work, we propose and demonstrate efficient alloyed 4 ML CdSe1–xSx nanoplatelets having a CdS crown with enhanced photoluminescence quantum yields (up to 60%) in the blue region (462–487 nm). We successfully used these NPLs as an electrically driven active emitter in the blue-emitting NPL-LEDs with a low turn-on voltage of ∼4 V. The Commission Internationale de L’Eclairage (CIE) coordinates of (0.23, 0.14) were obtained for these blue-emitting NPL-LEDs. These emitters could potentially open up the opportunity for full-color displays using these NPL-based blue LEDs in conjunction with the red and green ones.Item Open Access Ligand exchange and impurity doping in 2d cdse nanoplatelet thin films and their applications(Wiley-VCH Verlag GmbH & Co. KGaA, 2021-09-23) Lee, W, S.; Kang, Y-G.; Lee, Y. M.; Jean, S.; Sharma, A.; Demir, Hilmi Volkan; Han, M. J.; Koh, W-K.; Oh, S. J.The effects of halide-ligand exchange and Cu and Ag doping are studied on structural, optical, and electrical properties of four monolayer CdSe nanoplatelet (NPL) and NPL thin films. Combinational study shows that NH4Cl-treatment on CdSe NPL and NPL thin films show tetragonal lattice distortion of NPL, side-to-side attachment between NPLs, bathochromic shift in absorption spectra, and complete quenching of band-edge and dopant-induced emissions. First-principle calculations reveal that Cl creates states below valence band maximum while Ag and Cu dopants create acceptor-like states, explaining the change of their optical property. Field-effect transistors are fabricated to investigate the effect of doping and reduced interplatelet distance on electrical properties of CdSe NPL thin films, demonstrating Cu and Ag dopants mitigate n-type character of CdSe NPL thin films. Temperature-dependent electrical characterization is conducted to further understand charge transport behavior depending on the existence of dopants. This work provides scientific information on the influence of surface chemistry and impurity doping on quantum confined semiconductors and new directions for the design of high-performance nanomaterial-based electronic and optoelectronic devices.Item Open Access Light-induced paramagnetism in colloidal Ag+-doped CdSe nanoplatelets(American Chemical Society, 2021-03-25) Najafi, A.; Sharma, Manoj; Delikanlı, Savaş; Bhattacharya, A.; Murphy, J. R.; Pientka, J.; Sharma, A.; Quinn, A. P.; Erdem, Onur; Kattel, S.; Kelestemur, Y.; Kovalenko, M. V.; Rice, W. D.; Demir, Hilmi Volkan; Petrou, A.We describe a study of the magneto-optical properties of Ag+-doped CdSe colloidal nanoplatelets (NPLs) that were grown using a novel doping technique. In this work, we used magnetic circularly polarized luminescence and magnetic circular dichroism spectroscopy to study light-induced magnetism for the first time in 2D solution-processed structures doped with nominally nonmagnetic Ag+ impurities. The excitonic circular polarization (PX) and the exciton Zeeman splitting (ΔEZ) were recorded as a function of the magnetic field (B) and temperature (T). Both ΔEZ and PX have a Brillouin-function-like dependence on B and T, verifying the presence of paramagnetism in Ag+-doped CdSe NPLs. The observed light-induced magnetism is attributed to the transformation of nonmagnetic Ag+ ions into Ag2+, which have a nonzero magnetic moment. This work points to the possibility of incorporating these nanoplatelets into spintronic devices, in which light can be used to control the spin injection.Item Open Access Low-threshold lasing from copper-doped CdSe colloidal quantum wells(Wiley, 2021-05-04) Yu, J.; Sharma, M.; Li, M.; Delikanlı, Savaş; Sharma, A.; Taimoor, M.; Altintas, Y.; McBride, J. R.; Kusserow, T.; Sum, T.; Demir, Hilmi VolkanTransition metal doped colloidal nanomaterials (TMDCNMs) have recently attracted attention as promising nano-emitters due to dopant-induced properties. However, despite ample investigations on the steady-state and dynamic spectroscopy of TMDCNMs, experimental understandings of their performance in stimulated emission regimes are still elusive. Here, the optical gain properties of copper-doped CdSe colloidal quantum wells (CQWs) are systemically studied with a wide range of dopant concentration for the first time. This work demonstrates that the amplified spontaneous emission (ASE) threshold in copper-doped CQWs is a competing result between the biexciton formation, which is preferred to achieve population inversion, and the hole trapping which stymies the population inversion. An optimum amount of copper dopants enables the lowest ASE threshold of ≈7 µJ cm−2, about 8-fold reduction from that in undoped CQWs (≈58 µJ cm−2) under sub-nanosecond pulse excitation. Finally, a copper-doped CQW film embedded in a vertical cavity surface-emitting laser (VCSEL) structure yields an ultralow lasing threshold of 4.1 µJ cm−2. Exploiting optical gain from TMDCNMs may help to further boost the performance of colloidal-based lasers.Item Open Access Modulating emission properties in a host–guest colloidal quantum well superlattice(Wiley-VCH Verlag GmbH & Co. KGaA, 2021-12-19) Yu, J.; Sharma, Manoj; Wang, Y.; Delikanlı, S.; Baruj, Hamed Dehghanpour; Sharma, A.; Demir, Hilmi VolkanSelf-assembly of colloidal nanocrystals into ordered superlattices is a powerful approach to enable novel collective properties which are not available in individual colloids. However, to date, it remains a major challenge to develop a practical route to modulate such collective properties for potential photonic applications. Herein, it is shown that the collective emission properties in colloidal quantum well (CQW) superlattices, including emission color and anisotropy, can be effectively modulated in a binary host–guest architecture. The experimental and theoretical results reveal that excitons of the host (i.e., the undoped CQWs) generated by photoexcitation can be controllably harvested by the guest (i.e., the Cu-doped CQWs) for light emission, owing to an exciton hopping assisted exciton trapping process. Such a nano-building block with tunable collective optical properties may enlighten novel colloidal material-based photonic applications, including optical anti-counterfeiting, next-generation liquid crystal displays, and multifunctional biological markers.Item Open Access Spectrally resolved nonlinear optical properties of doped versus undoped quasi-2D semiconductor nanocrystals: copper and silver doping provokes strong nonlinearity in colloidal CdSe nanoplatelets(American Chemical Society, 2022-01-04) Nawrot, K. C.; Sharma, M.; Cichy, B.; Sharma, A.; Delikanli, Savas; Samoć, M.; Demir, Hilmi Volkan; Nyk, M.Nonlinear optical processes are crucial for emerging applications including multiphoton-excited fluorescence microscopy and optical power limiting. Therefore, searching for materials of high multiphoton absorption cross sections is essential for the development of these techniques. We present synthesis of 4.5 monolayer CdSe nanoplatelets (NPLs) doped with silver and copper ions along with the evaluation of their two-photon absorption (TPA) and three-photon absorption (3PA) cross sections. Doping significantly increases the TPA cross section of each NPL sample, which reaches up to 1.33 × 107 GM for the most absorbing copper-doped ones. We also detected 1–2 orders of magnitude-enhanced 3PA cross sections for the doped NPLs in comparison with their undoped counterparts. As TPA and 3PA peaks appear, in the first and the second biological transmission windows, respectively, doped NPLs are promising candidates for multiphoton fluorescence microscopy as bioimaging agents. Moreover, the strong nonlinear response suggests application as active optoelectronic materials in optical sensors.