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1. Disorder‐Induced Dispersive Magneto‐Electroluminescence of Blue Emitters in Organic Light Emitting Diodes

   https://doi.org/10.1002/adom.202101334  

   Pan, Xin ; Kwon, Ohyun ; Khanal, Dipak Raj ; Choi, Byoungki ; Vardeny, Zeev Valy ( December 2021 , Advanced Optical Materials)

   Disorder‐induced inhomogeneity in blue‐fluorescent‐based organic light‐emitting diodes (OLEDs) based on mixtures of host and guest molecules is studied using magneto‐electroluminescence, MEL(B), response based on the so called “Δgmechanism”, where Δgis the difference in the Landég‐factor of electrons and holes. The disorder in the organic active layer is manifested by a unique non‐Lorentzian MEL(B) response that is analyzed using a distribution of spin lifetimes for the injected electron–hole pairs that is determined by a dispersive parameter, α (<1). The carriers’ inhomogeneous response also influences the free carrier absorption spectrum, which shows characteristic properties described by a dispersive parameter β (<1). From the measured MEL(B) response at various injection conditions it is found that α is robust at increasing current density showing that the inhomogeneity is governed by intrinsic disorder in the device active layer. Also the obtained increase in α at low temperature indicates that the organic layer becomes more ordered, where longer‐lived electron–hole spin pairs are formed.

    

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2. 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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3. Electronic structure calculation of vanadium‐and scandium‐based endohedral fullerenes VSc 2 N@C 2n (2 n = 70, 76, 78, 80)

   https://doi.org/10.1002/qua.25785  

   Bhusal, Shusil ; Baruah, Tunna ; Yamamoto, Yoh ; Zope, Rajendra R. ( September 2018 , International Journal of Quantum Chemistry)

   We present candidate structures for the most stable isomers for the VSc₂N@C₇₀, VSc₂N@C₇₆, VSc₂N@C₇₈, and VSc₂N@C₈₀using a systematic procedure that involves all possible isomers of the host fullerene cages. Subsequently, a detailed investigation of structural and electronic properties of the lowest energy isomers is performed using density functional theory in combination with large polarized Gaussian basis sets. The search correctly identifies the experimentally observed VSc₂N@C₈₀isomer as the most stable structure. The structural analysis shows that only VSc₂N@C₇₀has a non‐IPR cage among the four endohedral fullerenes. Respectively, VSc₂N@C₇₀and VSc₂N@C₇₆have nearly degenerate spin states with total spinS= 0 andS= 1. All the lowest energy cages are energetically stable and show significant electron accepting capacity comparable to C₆₀.

    

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4. Isotope Effect in the Magneto‐Optoelectronic Response of Organic Light‐Emitting Diodes Based on Donor–Acceptor Exciplexes

   https://doi.org/10.1002/adma.202004421  

   Liu, Xiaojie ; Popli, Henna ; Kwon, Ohyun ; Malissa, Hans ; Pan, Xin ; Park, Bumwoo ; Choi, Byoungki ; Kim, Sunghan ; Ehrenfreund, Eitan ; Boehme, Christoph ; et al ( October 2020 , Advanced Materials)

   The isotope effect is studied in the magneto‐electroluminescence (MEL) and pulsed electrically detected magnetic resonance of organic light‐emitting diodes based on thermally activated delayed fluorescence (TADF) from donor–acceptor exciplexes that are either protonated (H) or deuterated (D). It is found that at ambient temperature, the exchange of H to D has no effect on the spin‐dependent current and MEL responses in the devices. However, at cryogenic temperatures, where the reverse intersystem crossing (RISC) from triplet to singlet exciplex diminishes, a pronounced isotope effect is observed. These results show that the RISC process is not governed by the hyperfine interaction as thought previously, but proceeds through spin‐mixing in the triplet exciplex. The observations are corroborated by electrically detected transient spin nutation experiments that show relatively long dephasing time at ambient temperature, and interpreted in the context of a model that involves exchange and hyperfine interactions in the spin triplet exciplex. These findings deepen the understanding of the RISC process in TADF materials.

    

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5. Helicity‐Preserving Metasurfaces for Magneto‐Optical Enhancement in Ferromagnetic [Pt/Co] N Films

   https://doi.org/10.1002/adom.202001420  

   Abendroth, John M. ; Solomon, Michelle L. ; Barton, III, David R. ; El Hadri, Mohammed S. ; Fullerton, Eric E. ; Dionne, Jennifer A. ( September 2020 , Advanced Optical Materials)

   All‐optical control and detection of magnetic states for high‐density recording necessitate nanophotonic approaches to amplify local light intensity below the diffraction limit. Sculpting the near‐field phase and polarization can additionally strengthen magneto‐optical effects that rely on circularly polarized pulses, such as all‐optical helicity‐dependent switching, imaging, and spin‐wave excitation. Here, high‐refractive‐index dielectric nanoantennas illuminated with circularly polarized light resonantly enhance local electric field rotation by more than sixfold within [Pt/Co]_Nthin films. Sub‐wavelength arrays of amorphous Si nanodisks, or metasurfaces, patterned on perpendicularly magnetized films support Mie‐type resonances that modulate reflection and transmission dissymmetry by >±2% in experiments. Spatial and spectral interference between dipolar modes, proximity effects, and gain are evaluated by varying disk aspect ratio, metasurface–metal separation, and magnetic film thickness, respectively. Simulated enhancements in magnetic circular birefringence and differential absorption are correlated with amplified local field rotation at electric dipolar modes. Greater achievable amplifications are shown via simulations with single‐crystalline Si metasurfaces exhibiting lower losses, including a 12‐fold strengthened electric field rotation within ferromagnetic layers. The metasurface design rules established here could enable nanoscale localization of all‐optical magnetic switching with lowered laser fluence thresholds, as well as enhanced magneto‐optical responses for light‐assisted reading in spintronic devices.

    

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