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Advancements in Solution Processable Devices using Metal Oxides For Printed Internet-of-Things Objects

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2019 Electron Devices Technology and Manufacturing Conference (EDTM)

Advancements in Solution Processable Devices using Metal Oxides For Printed Internet-of-Things Objects

Paul R. Berger

1

, Miao Li

2

, Ryan M. Mattei

1

, Maimouna A. Niang

1

, Noah Talisa

1

, Michael Tripepi

1

, Brandon Harris

1

, Sagar R. Bhalerao

2

, Enam A. Chowdhury

1

, Charles H. Winter

3

, and Donald Lupo

2

1Ohio State University, Columbus, OH 43210, USA; 2Tampere University of Technology, FI-33101 Tampere, Finland;

3Wayne State University, Detroit, Michigan, USA Abstract

Internet-of-things (IoT) objects are expected to exceed 75 billion objects by 2020, and a large part of the expansion is expected to be at a finer granularity than existing silicon-based IoT objects (i.e. tablets and cell phones) can deliver [1]. Currently, placing a room light or a thermostat on the internet for remote control is considered progressive. However, if printed electronics can achieve performance increases, then IoT objects could be affixed to almost anything, such as coffee creamer cartons, cereal boxes, or that missing sock. Each of these IoT objects could be driving a sensor, perhaps position, temperature or pressure, essentially a multitude of applications. In order for IoT objects to emulate a simple postage stamp, with self-powering from energy scavenging and local energy storage, all housed in a non-toxic flexible form factor, advances in solution processable devices need to occur.

(Keywords: IoT, energy scavenging, low-power electronics, ALD, NDR, tunnel diodes, Manufacturing, CMOS and SOI)

Introduction

This talk will highlight advances by this collaborative international team in (1) metal oxide rectifying diodes for RF energy harvesting; (2) metal oxide tunnel barriers deposited by atomic layer deposition for negative differential resistance (NDR) devices using post-deposition annealing and novel precursors; and (3) metal oxide channel thin film transistors (TFT) with high mobilities and low operating voltages.

A. Solution Processed In2O3 Diodes

One modality for energy scavenging is the generation of DC power from absorbed RF energy germinated from sources like WiFi networks. Solution processed and organic diodes have shown promise in RFID, energy harvesting, and voltage multiplication applications [2]. Many of these rectifying diodes are based upon printed Schottky diodes. High-frequency air-stable solution processed rectifying diodes based on indium oxides have been successfully fabricated.

The diodes have a vertical structure of Al-In2O3-Au fabricated on an SiO2 coated Si wafer. The diodes offer excellent frequency performance. For an ac input voltage with an amplitude of 10 V, the dc output of a half-wave rectifier stays at 7 V up to at least 50MHz. The cutoff frequency of the diodes has reached 400MHz, entering ultra-high frequency (UHF) range. This is an excellent candidate for RF energy harvesting.

B. Low-Temperature Annealing of ALD Oxides Post-deposition annealing studies on metal oxides deposited by atomic layer deposition (ALD) were conducted using conventional ALD precursors at low deposition temperatures, but above the temperature for organometallic precursor pyrolysis. By carefully shifting the energy level within the metal-oxide bandgap of localized defect states created by oxygen vacancies in the ALD tunneling barrier, a higher peak-to-valley current ratio (PVCR) and lower onset tunneling voltage is expected in our polymer tunnel diodes (PTD) [3-4]. MOS and PTD devices on silicon and ITO coated glass were annealed with varying ultraviolet (UV) and laser irradiation parameters, Fig. 1. UV and laser irradiation have shown to improve the reliability of the film morphology, composition, and leakage current of metal oxides [5-6].

C. Solution Processable In2O3 TFTs

Low voltage operation and low processing temperature of transistors with metal oxide channels remains a challenge. Commonly metal oxide transistors are fabricated at very high processing temperatures (above 500oC) and their operation is not suitable for low power devices [7-8]. Here, thin film transistors (TFT) are reported based upon solution processable indium oxide (In2O3) for channel materials and room temperature processed anodized high-κ aluminum oxide (Al2O3)for gate dielectrics.

Anodization empowers the room temperature deposition of dielectric, bypassing high temperature, high vacuum processes, with the added advantages of nanoscale deposition and denser oxide layers that mitigate leakage current [9-10].

Results and Discussion

Spectroscopic ellipsometry and XRD measurements were used to observe variations in the optical dielectric functions and structural properties of the irradiated oxide samples. Room temperature I-V and C-V (Fig. 2) characteristics of the PTDs and MOS structures are analyzed and the impact of UV and laser annealing on device performance, dielectric properties, and trap states will be reported.

The In2O3 TFTs shown in Fig. 3 operate well below Vds of 3.0 V, with on/off ratio 105, subthreshold swing (S) 160 mV/dec, and low threshold voltage Vth 0.6 V.

The electron mobility (µ) was found to be as high as 3.53 cm2/Vs in the saturation regime and transconductance gm 53 µS. Fig. 4 and 5 show the C- V measurements and low leakage gate current in the TFTs. Additionally, the interface trap density (Dit) in

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2019 Electron Devices Technology and Manufacturing Conference (EDTM)

the oxide/semiconductor interface was quite low i.e.

1.7 × 1012 cm-2 eV-1, indicating good compatibility of In2O3 with anodic Al2O3.

With this report, we have shown advancements in metal-oxide based active devices that are synthesized by solution processing and low-temperature processing to realize the candidate discrete devices that will go into a complete printed IoT system.

Acknowledgments

The authors gratefully acknowledge the contributions of Evan Cornuelle for help in CV and Dit

measurements.

References

[1] D. Lund, C. MacGillivray, V. Turner, and M.

Morales, “Worldwide and regional internet of things (iot) 2014–2020 forecast: A virtuous circle of proven value and demand,” International Data Corporation (IDC), Tech. Rep, 2014.

[2] T. Kraft, P. Berger, D. Lupo, Printed and organic diodes: devices, circuits and applications, Flexible and Printed Electronics, Vol. 2, Number 3, 9/2017.

[3] Paul R. Berger and R. Anisha,“Negative Differential Resistance Devices and Circuits,”

Comprehensive Semiconductor Science and Technology edited by Pallab. Bhattacharya, Roberto Fornari and Hiroshi Kamimura, Elsevier, Volume 5, Chapter 13, pp. 176–241 (2011).

[4] “Negative Differential Resistance in Polymer Tunnel Diodes Using Atomic Layer Deposited, TiO2 Tunneling Barriers at Various Deposition Temperatures,” Jeremy J. Guttman, Conner B.

Chambers, Al Rey Villagracia, Gil Nonato C.

Santos and Paul R. Berger, Organic Electronics, vol. 47, pp. 228-234 (2017).

[5] Carlos, E.; Branquinho, R.; Kiazadeh, A.; Martins, J.; Barquinha, P.; Martins, R.; Fortunato, E.

Boosting electrical performance of high-κ nanomultilayer dielectrics and electronic devices by combining solution combustion synthesis and UV irradiation. ACS Appl. Mater. Interfaces, 2017, 9, 40428–40437.

[6] S. Dellis, I. Isakov, N. Kalfagiannis, K. Tetzner, T.

D. Anthopoulos and D. C. Koutsogeorgis, J. Mater.

Chem. C, 2017, 5, 3673.

[7] Dhananjay, Shiau-Shin Cheng, Chuan-Yi Yang, Chun-Wei Ou, You-Che Chuang, M Chyi Wu and Chih-Wei Chu “Dependence of channel thickness on the performance of In2O3 thin film transistors”

J. Phys. D: Appl. Phys., 41 (2008) 092006.

[8] Xinge Yu, Tobin J. Marks and Antonio Facchetti,

“Metal oxides for optoelectronic applications”, Nature Materials, 15, 2016.

[9] W. Grabinski and T. Gneiting, “Power/HVMOS Devices Compact Modeling,” Springer, ISBN:

978-90-481-3045-0 (2010).

[10] Yiheng Qin, Daniël H. Turkenburg, Ionut Barbu, Wiljan T. T. Smaal, Kris Myny, Wan-Yu Lin, Gerwin H. Gelinck, Paul Heremans, Johan Liu, and Erwin R. Meinders, “Organic Thin-Film Transistors with Anodized Gate Dielectric Patterned by Self-Aligned Embossing on Flexible Substrates”, Adv. Funct. Mater. 2012, 22, 1209–

1214.

Fig. 1: (a) Experimental setup used for Laser Irradiation. (b) Raster of sample with triple-axis stage.

Fig. 2: Impact of UV annealing on the C-V characteristics of Al/Ta2O5/Si structures.

-1.5 -1.0 -0.5 0.0 0.5 1.0 1.5

0 50 100 150 200 250 300 350 400

Capacitance (pF)

Applied Voltage (V) As Deposited

6.5 minute UV Exposure 1.5 minute UV Exposure Furnance Annealed

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2019 Electron Devices Technology and Manufacturing Conference (EDTM)

Fig. 3: Schematic structure of the In2O3 TFT with Al2O3 gate dielectric.

Fig. 4: C-V measurement of the In2O3 TFT.

Fig. 5: Gate leakage current of In2O3 TFT.

-3 -2 -1 0 1 2 3

0.57 0.60 0.63 0.66 0.69 0.72 0.75

Capacitance (µF/cm2)

Voltage (V)

1 Khz

10k 100k 1M

-0.4 -0.2 0.0 0.2 0.4 0.6 0.8 1.0

Capacitance Conductance

Frequency (Hz) Capacitance F/cm2)

0.00 0.02 0.04 0.06 0.08 0.10 0.12 0.14

Gp/ (µF)

0 1 2 3 4 5 6

0.0 2.0 4.0 6.0 8.0 10.0 12.0

Leakage current (mA)

Voltage (V)

Dielectric Breakdown

0.0 0.5 1.0 1.5 2.0 2.5 3.0 3.5 1n

10n 100n 10µ 100µ

Vd = 2.0 V Vd = 2.0 V

Vgate (V)

Idrain (A)

0.0 15.0 30.0 45.0 60.0 75.0

gm (µS)

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