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1. Improving Photovoltaic Performance of Light-Responsive Double-Heterojunction Nanorod Light-Emitting Diodes

   https://doi.org/10.1063/5.0147782  

   Huang, C.; Jiang, Y.; Drake, G. A.; Keating, L. P.; Shim, M. (June 2023, Journal of chemical physics)

   Double heterojunction nanorods enable both electroluminescence and light harvesting capabilities within the same device structure, providing a promising platform for energy-scavenging displays and related applications. However, the efficiency of the photovoltaic mode remains modest for useful power conversion and may be challenging to improve without sacrificing performance in electroluminescence. Through a facile on-film partial ligand exchange with benzenethiol integrated into the device fabrication step, we achieve an average of more than threefold increase in power conversion efficiency while maintaining the maximum external quantum efficiency and the maximum luminance in the LED mode. The improved photovoltaic performance is mainly due to the increase in the short circuit current, which we attribute to the enhanced charge separation afforded by the partial ligand exchange. The recovery of the photoluminescence lifetime under the forward bias suggests that the hole traps introduced by benzenethiols are filled prior to reaching the voltage at which light emission begins, allowing LED performance to be maintained and possibly improved. 

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2. Near full light absorption and full charge collection in 1-micron thick quantum dot photodetector using intercalated graphene monolayer electrodes

   https://doi.org/10.1039/c9nr09901h  

   Chen, Wenjun; Ahn, Seungbae; Balingit, Marquez; Wang, Jiaying; Lockett, Malcolm; Vazquez-Mena, Oscar (February 2020, Nanoscale)

   Quantum dots (QDs) offer several advantages in optoelectronics such as easy solution processing, strong light absorption and size tunable direct bandgap. However, their major limitation is their poor film mobility and short diffusion length (<250 nm). This has restricted the thickness of QD film to ∼200–300 nm due to the restriction that the diffusion length imposes on film thickness in order to keep efficient charge collection. Such thin films result in a significant decrease in quantum efficiency for λ > 700 nm in QDs photodetector and photovoltaic devices, causing a reduced photoresponsivity and a poor absorption towards the near-infrared part of the sunlight spectrum. Herein, we demonstrate 1 μm thick QDs photodetectors with intercalated graphene charge collectors that avoid the significant drop of quantum efficiency towards λ > 700 nm observed in most QD optoelectronic devices. The 1 μm thick intercalated QD films ensure strong light absorption while keeping efficient charge extraction with a quantum efficiency of 90%–70% from λ = 600 nm to 950 nm using intercalated graphene layers as charge collectors with interspacing distance of 100 nm. We demonstrate that the effect of graphene on light absorption is minimal. We achieve a time-modulation response of <1 s. We demonstrate that this technology can be implemented on flexible PET substrates, showing 70% of the original performance after 1000 times bending test. This system provides a novel approach towards high-performance photodetection and high conversion photovoltaic efficiency with quantum dots and on flexible substrates. 

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3. RTD Light Emission around 1550 nm with IQE up to 6% at 300 K

   https://doi.org/10.1109/DRC50226.2020.9135175  

   Brown, E. R.; Zhang, W-D.; Fakhimi, P.; Growden, T. A.; Berger, P.R. (June 2020, IEEE Device Research Conference (DRC), Columbus, OH (June 22-24, 2020))

   Resonant tunneling diodes (RTDs) have come full-circle in the past 10 years after their demonstration in the early 1990s as the fastest room-temperature semiconductor oscillator, displaying experimental results up to 712 GHz and fmax values exceeding 1.0 THz [1]. Now the RTD is once again the preeminent electronic oscillator above 1.0 THz and is being implemented as a coherent source [2] and a self-oscillating mixer [3], amongst other applications. This paper concerns RTD electroluminescence – an effect that has been studied very little in the past 30+ years of RTD development, and not at room temperature. We present experiments and modeling of an n-type In0.53Ga0.47As/AlAs double-barrier RTD operating as a cross-gap light emitter at ~300K. The MBE-growth stack is shown in Fig. 1(a). A 15-μm-diam-mesa device was defined by standard planar processing including a top annular ohmic contact with a 5-μm-diam pinhole in the center to couple out enough of the internal emission for accurate free-space power measurements [4]. The emission spectra have the behavior displayed in Fig. 1(b), parameterized by bias voltage (VB). The long wavelength emission edge is at  = 1684 nm - close to the In0.53Ga0.47As bandgap energy of Ug ≈ 0.75 eV at 300 K. The spectral peaks for VB = 2.8 and 3.0 V both occur around  = 1550 nm (h = 0.75 eV), so blue-shifted relative to the peak of the “ideal”, bulk InGaAs emission spectrum shown in Fig. 1(b) [5]. These results are consistent with the model displayed in Fig. 1(c), whereby the broad emission peak is attributed to the radiative recombination between electrons accumulated on the emitter side, and holes generated on the emitter side by interband tunneling with current density Jinter. The blue-shifted main peak is attributed to the quantum-size effect on the emitter side, which creates a radiative recombination rate RN,2 comparable to the band-edge cross-gap rate RN,1. Further support for this model is provided by the shorter wavelength and weaker emission peak shown in Fig. 1(b) around = 1148 nm. Our quantum mechanical calculations attribute this to radiative recombination RR,3 in the RTD quantum well between the electron ground-state level E1,e, and the hole level E1,h. To further test the model and estimate quantum efficiencies, we conducted optical power measurements using a large-area Ge photodiode located ≈3 mm away from the RTD pinhole, and having spectral response between 800 and 1800 nm with a peak responsivity of ≈0.85 A/W at  =1550 nm. Simultaneous I-V and L-V plots were obtained and are plotted in Fig. 2(a) with positive bias on the top contact (emitter on the bottom). The I-V curve displays a pronounced NDR region having a current peak-to-valley current ratio of 10.7 (typical for In0.53Ga0.47As RTDs). The external quantum efficiency (EQE) was calculated from EQE = e∙IP/(∙IE∙h) where IP is the photodiode dc current and IE the RTD current. The plot of EQE is shown in Fig. 2(b) where we see a very rapid rise with VB, but a maximum value (at VB= 3.0 V) of only ≈2×10-5. To extract the internal quantum efficiency (IQE), we use the expression EQE= c ∙i ∙r ≡ c∙IQE where ci, and r are the optical-coupling, electrical-injection, and radiative recombination efficiencies, respectively [6]. Our separate optical calculations yield c≈3.4×10-4 (limited primarily by the small pinhole) from which we obtain the curve of IQE plotted in Fig. 2(b) (right-hand scale). The maximum value of IQE (again at VB = 3.0 V) is 6.0%. From the implicit definition of IQE in terms of i and r given above, and the fact that the recombination efficiency in In0.53Ga0.47As is likely limited by Auger scattering, this result for IQE suggests that i might be significantly high. To estimate i, we have used the experimental total current of Fig. 2(a), the Kane two-band model of interband tunneling [7] computed in conjunction with a solution to Poisson’s equation across the entire structure, and a rate-equation model of Auger recombination on the emitter side [6] assuming a free-electron density of 2×1018 cm3. We focus on the high-bias regime above VB = 2.5 V of Fig. 2(a) where most of the interband tunneling should occur in the depletion region on the collector side [Jinter,2 in Fig. 1(c)]. And because of the high-quality of the InGaAs/AlAs heterostructure (very few traps or deep levels), most of the holes should reach the emitter side by some combination of drift, diffusion, and tunneling through the valence-band double barriers (Type-I offset) between InGaAs and AlAs. The computed interband current density Jinter is shown in Fig. 3(a) along with the total current density Jtot. At the maximum Jinter (at VB=3.0 V) of 7.4×102 A/cm2, we get i = Jinter/Jtot = 0.18, which is surprisingly high considering there is no p-type doping in the device. When combined with the Auger-limited r of 0.41 and c ≈ 3.4×10-4, we find a model value of IQE = 7.4% in good agreement with experiment. This leads to the model values for EQE plotted in Fig. 2(b) - also in good agreement with experiment. Finally, we address the high Jinter and consider a possible universal nature of the light-emission mechanism. Fig. 3(b) shows the tunneling probability T according to the Kane two-band model in the three materials, In0.53Ga0.47As, GaAs, and GaN, following our observation of a similar electroluminescence mechanism in GaN/AlN RTDs (due to strong polarization field of wurtzite structures) [8]. The expression is Tinter = (2/9)∙exp[(-2 ∙Ug 2 ∙me)/(2h∙P∙E)], where Ug is the bandgap energy, P is the valence-to-conduction-band momentum matrix element, and E is the electric field. Values for the highest calculated internal E fields for the InGaAs and GaN are also shown, indicating that Tinter in those structures approaches values of ~10-5. As shown, a GaAs RTD would require an internal field of ~6×105 V/cm, which is rarely realized in standard GaAs RTDs, perhaps explaining why there have been few if any reports of room-temperature electroluminescence in the GaAs devices. [1] E.R. Brown,et al., Appl. Phys. Lett., vol. 58, 2291, 1991. [5] S. Sze, Physics of Semiconductor Devices, 2nd Ed. 12.2.1 (Wiley, 1981). [2] M. Feiginov et al., Appl. Phys. Lett., 99, 233506, 2011. [6] L. Coldren, Diode Lasers and Photonic Integrated Circuits, (Wiley, 1995). [3] Y. Nishida et al., Nature Sci. Reports, 9, 18125, 2019. [7] E.O. Kane, J. of Appl. Phy 32, 83 (1961). [4] P. Fakhimi, et al., 2019 DRC Conference Digest. [8] T. Growden, et al., Nature Light: Science & Applications 7, 17150 (2018). [5] S. Sze, Physics of Semiconductor Devices, 2nd Ed. 12.2.1 (Wiley, 1981). [6] L. Coldren, Diode Lasers and Photonic Integrated Circuits, (Wiley, 1995). [7] E.O. Kane, J. of Appl. Phy 32, 83 (1961). [8] T. Growden, et al., Nature Light: Science & Applications 7, 17150 (2018). 

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4. Si(bzimpy) ₂ – a hexacoordinate silicon pincer complex for electron transport and electroluminescence

   https://doi.org/10.1039/C8CC07681B  

   Kocherga, Margaret; Castaneda, Jose; Walter, Michael G.; Zhang, Yong; Saleh, Nemah-Allah; Wang, Le; Jones, Daniel S.; Merkert, Jon; Donovan-Merkert, Bernadette; Li, Yanzeng; et al (December 2018, Chemical Communications)

   A neutral hexacoordinate silicon complex containing two 2,6-bis(benzimidazol-2′-yl)pyridine (bzimpy) ligands has been synthesized and explored as a potential electron transport layer and electroluminescent layer in organic electronic devices. The air and water stable complex is fluorescent in solution with a λ max = 510 nm and a QY = 57%. Thin films grown via thermal evaporation also fluoresce and possess an average electron mobility of 6.3 × 10 −5 cm 2 V −1 s −1 . An ITO/Si(bzimpy) 2 /Al device exhibits electroluminescence with λ max = 560 nm. 

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5. Ca2+ induced highly fluorescent CsPb(Br/Cl)3 perovskite quantum dots via fast Anion-Exchange & Cation-Doping Inter-Promotion strategy for efficient deep-blue light-emitting diodes

   https://doi.org/10.1016/j.cej.2024.151227  

   Zhou, Jing; Liu, Hongli; Wang, Sisi; Yuan, Longfei; Dridi, Narjes; Wang, Shirong; Mattoussi, Hedi; Li, Xianggao (June 2024, Chemical Engineering Journal)

   Despite the impressive development of perovskite light-emitting diodes (PeLEDs), it is still challenging to achieve high-efficiency deep-blue PeLEDs using colloid perovskite quantum dots (PQDs). The efficiency of PQDs with a wavelength below 460 nm, which meets the requirements for deep-blue emission in the Telecommunication Union UHD television standard (ITU REC. 2020), lags far behind those of their sky-blue counterparts. To address this issue, a novel strategy of fast anion-exchange & cation-doping inter-promotion (FAECDIP) is proposed to achieve highly efficient deep-blue PQDs by introducing CaBr2 into the CsPbCl3 PQDs. Owing to the presence of Ca2+, the speed of ion exchange is increased, driven by the smaller cation, Ca2+, improving the preparation efficiency. Additionally, Ca2+ was doped on the surface of PQDs. Based on studies of fast anion-exchange and theoretical calculations, Ca2+ improves the optical performance by decreasing the number of traps and increasing the crystallinity of target PQDs, facilitating the stability of treated films and PeLEDs by enhancing the formation energy of halogen vacancies. Here, a high PLQY of 80.3 % CaBr2-induced CsPb(Cl/Br)3 deep-blue PQDs (~446 nm) was achieved. The correspondent PeLEDs (~447 nm) achieved a superior EQE of 5.88 %, which is the state-of-the-art among the reported deep-blue PeLEDs. Our strategy provides a potential route to achieve deep-blue PeLEDs, which differs from the previous tedious-complex methods. 

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