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
ci, 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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High Performance Multiwall Carbon Nanotube–Insulator–Metal Tunnel Diode Arrays for Optical Rectification
This work reports important fundamental advancements in multiwall carbon nanotube (MWCNT) rectenna devices by creating and optimizing new diode structures to allow optical rectification with air‐stable devices. The incorporation of double‐insulator layer tunnel diodes, fabricated for the first time on MWCNT arrays, enables the use of air‐stable top metals (Al and Ag) with excellent asymmetry for rectification applications. Asymmetry is increased by as much as 10 times, demonstrating the effectiveness of incorporating multiple dielectric layers to control electron tunneling in MWCNT diode structures. MWCNT tip opening also reduces device resistance up to 75% due to an increase in diode contact area to MWCNT inner walls. This effect is consistent for different oxide materials and thicknesses. A number of insulator layers, including Al2O3, HfO2, TiO2, ZnO, and ZrO2, in both single‐ and then double‐insulator configurations are tested. Resistance increases exponentially with insulator thickness and decreases with electron affinity. These results are used to characterize double‐insulator diode performance. Finally, for the most asymmetric device structure, Al2O3‐HfO2(4/4 nm), optical rectification at a frequency of 470 THz (638 nm) is demonstrated. These results open the door for designing efficient MWCNT rectenna devices with more material flexibility, including air‐stable, transparent, and conductive top electrode materials.
more » « less- Award ID(s):
- 1748413
- NSF-PAR ID:
- 10050254
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Electronic Materials
- Volume:
- 4
- Issue:
- 3
- ISSN:
- 2199-160X
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
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By mimicking biomimetic synaptic processes, the success of artificial intelligence (AI) has been astounding with various applications such as driving automation, big data analysis, and natural-language processing.[1-4] Due to a large quantity of data transmission between the separated memory unit and the logic unit, the classical computing system with von Neumann architecture consumes excessive energy and has a significant processing delay.[5] Furthermore, the speed difference between the two units also causes extra delay, which is referred to as the memory wall.[6, 7] To keep pace with the rapid growth of AI applications, enhanced hardware systems that particularly feature an energy-efficient and high-speed hardware system need to be secured. The novel neuromorphic computing system, an in-memory architecture with low power consumption, has been suggested as an alternative to the conventional system. Memristors with analog-type resistive switching behavior are a promising candidate for implementing the neuromorphic computing system since the devices can modulate the conductance with cycles that act as synaptic weights to process input signals and store information.[8, 9]
The memristor has sparked tremendous interest due to its simple two-terminal structure, including top electrode (TE), bottom electrode (BE), and an intermediate resistive switching (RS) layer. Many oxide materials, including HfO2, Ta2O5, and IGZO, have extensively been studied as an RS layer of memristors. Silicon dioxide (SiO2) features 3D structural conformity with the conventional CMOS technology and high wafer-scale homogeneity, which has benefited modern microelectronic devices as dielectric and/or passivation layers. Therefore, the use of SiO2as a memristor RS layer for neuromorphic computing is expected to be compatible with current Si technology with minimal processing and material-related complexities.
In this work, we proposed SiO2-based memristor and investigated switching behaviors metallized with different reduction potentials by applying pure Cu and Ag, and their alloys with varied ratios. Heavily doped p-type silicon was chosen as BE in order to exclude any effects of the BE ions on the memristor performance. We previously reported that the selection of TE is crucial for achieving a high memory window and stable switching performance. According to the study which compares the roles of Cu (switching stabilizer) and Ag (large switching window performer) TEs for oxide memristors, we have selected the TE materials and their alloys to engineer the SiO2-based memristor characteristics. The Ag TE leads to a larger memory window of the SiO2memristor, but the device shows relatively large variation and less reliability. On the other hand, the Cu TE device presents uniform gradual switching behavior which is in line with our previous report that Cu can be served as a stabilizer, but with small on/off ratio.[9] These distinct performances with Cu and Ag metallization leads us to utilize a Cu/Ag alloy as the TE. Various compositions of Cu/Ag were examined for the optimization of the memristor TEs. With a Cu/Ag alloying TE with optimized ratio, our SiO2based memristor demonstrates uniform switching behavior and memory window for analog switching applications. Also, it shows ideal potentiation and depression synaptic behavior under the positive/negative spikes (pulse train).
In conclusion, the SiO2memristors with different metallization were established. To tune the property of RS layer, the sputtering conditions of RS were varied. To investigate the influence of TE selections on switching performance of memristor, we integrated Cu, Ag and Cu/Ag alloy as TEs and compared the switch characteristics. Our encouraging results clearly demonstrate that SiO2with Cu/Ag is a promising memristor device with synaptic switching behavior in neuromorphic computing applications.
Acknowledgement This work was supported by the U.S. National Science Foundation (NSF) Award No. ECCS-1931088. S.L. and H.W.S. acknowledge the support from the Improvement of Measurement Standards and Technology for Mechanical Metrology (Grant No. 22011044) by KRISS.
References [1] Young
et al. ,IEEE Computational Intelligence Magazine, vol. 13, no. 3, pp. 55-75, 2018.[2] Hadsell
et al. ,Journal of Field Robotics, vol. 26, no. 2, pp. 120-144, 2009.[3] Najafabadi
et al. ,Journal of Big Data, vol. 2, no. 1, p. 1, 2015.[4] Zhao
et al. ,Applied Physics Reviews, vol. 7, no. 1, 2020.[5] Zidan
et al. ,Nature Electronics, vol. 1, no. 1, pp. 22-29, 2018.[6] Wulf
et al., SIGARCH Comput. Archit. News, vol. 23, no. 1, pp. 20–24, 1995.[7] Wilkes,
SIGARCH Comput. Archit. News, vol. 23, no. 4, pp. 4–6, 1995.[8] Ielmini
et al., Nature Electronics, vol. 1, no. 6, pp. 333-343, 2018.[9] Chang
et al., Nano Letters, vol. 10, no. 4, pp. 1297-1301, 2010.[10] Qin
et al. , Physica Status Solidi (RRL) - Rapid Research Letters, pssr.202200075R1, In press, 2022. -
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Ever-increasing demands for energy, particularly being environmentally friendly have promoted the transition from fossil fuels to renewable energy.1Lithium-ion batteries (LIBs), arguably the most well-studied energy storage system, have dominated the energy market since their advent in the 1990s.2However, challenging issues regarding safety, supply of lithium, and high price of lithium resources limit the further advancement of LIBs for large-scale energy storage applications.3Therefore, attention is being concentrated on an alternative electrochemical energy storage device that features high safety, low cost, and long cycle life. Rechargeable aqueous zinc-ion batteries (ZIBs) is considered one of the most promising alternative energy storage systems due to the high theoretical energy and power densities where the multiple electrons (Zn2+) . In addition, aqueous ZIBs are safer due to non-flammable electrolyte (e.g., typically aqueous solution) and can be manufactured since they can be assembled in ambient air conditions.4As an essential component in aqueous Zn-based batteries, the Zn metal anode generally suffers from the growth of dendrites, which would affect battery performance in several ways. Second, the led by the loose structure of Zn dendrite may reduce the coulombic efficiency and shorten the battery lifespan.5
Several approaches were suggested to improve the electrochemical stability of ZIBs, such as implementing an interfacial buffer layer that separates the active Zn from the bulk electrolyte.6However, the and thick thickness of the conventional Zn metal foils remain a critical challenge in this field, which may diminish the energy density of the battery drastically. According to a theretical calculation, the thickness of a Zn metal anode with an areal capacity of 1 mAh cm-2is about 1.7 μm. However, existing extrusion-based fabrication technologies are not capable of downscaling the thickness Zn metal foils below 20 μm.
Herein, we demonstrate a thickness controllable coating approach to fabricate an ultrathin Zn metal anode as well as a thin dielectric oxide separator. First, a 1.7 μm Zn layer was uniformly thermally evaporated onto a Cu foil. Then, Al2O3, the separator was deposited through sputtering on the Zn layer to a thickness of 10 nm. The inert and high hardness Al2O3layer is expected to lower the polarization and restrain the growth of Zn dendrites. Atomic force microscopy was employed to evaluate the roughness of the surface of the deposited Zn and Al2O3/Zn anode structures. Long-term cycling stability was gauged under the symmetrical cells at 0.5 mA cm-2for 1 mAh cm-2. Then the fabricated Zn anode was paired with MnO2as a full cell for further electrochemical performance testing. To investigate the evolution of the interface between the Zn anode and the electrolyte, a home-developed in-situ optical observation battery cage was employed to record and compare the process of Zn deposition on the anodes of the Al2O3/Zn (demonstrated in this study) and the procured thick Zn anode. The surface morphology of the two Zn anodes after circulation was characterized and compared through scanning electron microscopy. The tunable ultrathin Zn metal anode with enhanced anode stability provides a pathway for future high-energy-density Zn-ion batteries.
Obama, B., The irreversible momentum of clean energy.
Science 2017, 355 (6321), 126-129.Goodenough, J. B.; Park, K. S., The Li-ion rechargeable battery: a perspective.
J Am Chem Soc 2013, 135 (4), 1167-76.Li, C.; Xie, X.; Liang, S.; Zhou, J., Issues and Future Perspective on Zinc Metal Anode for Rechargeable Aqueous Zinc‐ion Batteries.
Energy & Environmental Materials 2020, 3 (2), 146-159.Jia, H.; Wang, Z.; Tawiah, B.; Wang, Y.; Chan, C.-Y.; Fei, B.; Pan, F., Recent advances in zinc anodes for high-performance aqueous Zn-ion batteries.
Nano Energy 2020, 70 .Yang, J.; Yin, B.; Sun, Y.; Pan, H.; Sun, W.; Jia, B.; Zhang, S.; Ma, T., Zinc Anode for Mild Aqueous Zinc-Ion Batteries: Challenges, Strategies, and Perspectives.
Nanomicro Lett 2022, 14 (1), 42.Yang, Q.; Li, Q.; Liu, Z.; Wang, D.; Guo, Y.; Li, X.; Tang, Y.; Li, H.; Dong, B.; Zhi, C., Dendrites in Zn-Based Batteries.
Adv Mater 2020, 32 (48), e2001854.Acknowledgment
This work was partially supported by the U.S. National Science Foundation (NSF) Award No. ECCS-1931088. S.L. and H.W.S. acknowledge the support from the Improvement of Measurement Standards and Technology for Mechanical Metrology (Grant No. 22011044) by KRISS.
Figure 1
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The discovery of oxide electronics is of increasing importance today as one of the most promising new technologies and manufacturing processes for a variety of electronic and optoelectronic applications such as next-generation displays, batteries, solar cells, memory devices, and photodetectors[1]. The high potential use seen in oxide electronics is due primarily to their high carrier mobilities and their ability to be fabricated at low temperatures[2]. However, since the majority of oxide semiconductors are n-type oxides, current applications are limited to unipolar devices, eventually developing oxide-based bipolar devices such as p-n diodes and complementary metal-oxide semiconductors. We have contributed to a wide range of oxide semiconductors and their electronics and optoelectronic device applications. Particularly, we have demonstrated n-type oxide-based thin film transistors (TFT), integrating In 2 O 3 -based n-type oxide semiconductors from binary cation materials to ternary cation species including InZnO, InGaZnO (IGZO), and InAlZnO. We have suggested channel/metallization contact strategies to achieve stable and high TFT performance[3, 4], identified vacancy-based native defect doping mechanisms[5], suggested interfacial buffer layers to promote charge injection capability[6], and established the role of third cation species on the carrier generation and carrier transport[7]. More recently, we have reported facile manufacturing of p-type SnOx through reactive magnetron sputtering from a Sn metal target[8]. The fabricated p-SnOx was found to be devoid of metallic phase of Sn from x-ray photoelectron spectroscopy and demonstrated stable performance in a fully oxide-based p-n heterojunction together with n-InGaZnO. The oxide-based p-n junctions exhibited a high rectification ratio greater than 10 3 at ±3 V, a low saturation current of ~2x10 -10 , and a small turn-on voltage of -0.5 V. In this presentation, we review recent achievements and still remaining issues in transition metal oxide semiconductors and their device applications, in particular, bipolar applications including p-n heterostructures and complementary metal-oxide-semiconductor devices as well as single polarity devices such as TFTs and memristors. In addition, the fundamental mechanisms of carrier transport behaviors and doping mechanisms that govern the performance of these oxide-based devices will also be discussed. ACKNOWLEDGMENT This work was supported by the U.S. National Science Foundation (NSF) Award No. ECCS-1931088. S.L. and H.W.S. acknowledge the support from the Improvement of Measurement Standards and Technology for Mechanical Metrology (Grant No. 20011028) by KRISS. K.N. was supported by Basic Science Research Program (NRF-2021R11A1A01051246) through the NRF Korea funded by the Ministry of Education. REFERENCES [1] K. Nomura et al. , Nature, vol. 432, no. 7016, pp. 488-492, Nov 25 2004. [2] D. C. Paine et al. , Thin Solid Films, vol. 516, no. 17, pp. 5894-5898, Jul 1 2008. [3] S. Lee et al. , Journal of Applied Physics, vol. 109, no. 6, p. 063702, Mar 15 2011, Art. no. 063702. [4] S. Lee et al. , Applied Physics Letters, vol. 104, no. 25, p. 252103, 2014. [5] S. Lee et al. , Applied Physics Letters, vol. 102, no. 5, p. 052101, Feb 4 2013, Art. no. 052101. [6] M. Liu et al. , ACS Applied Electronic Materials, vol. 3, no. 6, pp. 2703-2711, 2021/06/22 2021. [7] A. Reed et al. , Journal of Materials Chemistry C, 10.1039/D0TC02655G vol. 8, no. 39, pp. 13798-13810, 2020. [8] D. H. Lee et al. , ACS Applied Materials & Interfaces, vol. 13, no. 46, pp. 55676-55686, 2021/11/24 2021.more » « less
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Abstract Earth‐abundant and air‐stable Cu2BaSnS4−
x Sex (CBTSSe) and related thin‐film absorbers are regarded as prospective options to meet the increasing demand for low‐cost solar cell deployment. Devices based on vacuum‐deposited CBTSSe absorbers have achieved record power conversion efficiency (PCE) of 5.2% based on a conventional device structure using CdS buffer and i‐ZnO/indium tin oxide (ITO) window layers, with open‐circuit voltage (V OC) posing the major bottleneck for improving solar cell performance. The current study demonstrates a >20% improvement inV OC(from 0.62 to 0.75 V) and corresponding enhancement in PCE (from 5.1% to 6.2% without antireflection coating; to 6.5% with MgF2antireflection coating) for solution‐deposited CBTSSe solar cells. This performance improvement is realized by introducing an alternative successive ionic layer adsorption and reaction‐deposited Zn1−x Cdx S buffer combined with sputtered Zn1−x Mgx O/Al‐doped ZnO window/top contact layer, which offers lower electron affinities relative to the conventional CdS/i‐ZnO/ITO stack and better matching with the low electron affinity of CBTSSe. A combined experimental (temperature‐ and light intensity‐dependentV OCmeasurements) and device simulation (SCAPS‐1D) evaluation points to the importance of addressing relative band offsets for both the buffer and window layers relative to the absorber in mitigating interfacial recombination and optimizing CBTSSe solar cell performance.
