Transparent Oxide Electronics E-Book

Pedro Barquinha

• Herausgeber: John Wiley & Sons
• Kategorie: Fachliteratur
• Sprache: Englisch

Seitenzahl: 616

Veröffentlichungsjahr: 2012

Beschreibung

Transparent electronics is emerging as one of the most promising technologies for the next generation of electronic products, away from the traditional silicon technology. It is essential for touch display panels, solar cells, LEDs and antistatic coatings.

The book describes the concept of transparent electronics, passive and active oxide semiconductors, multicomponent dielectrics and their importance for a new era of novel electronic materials and products. This is followed by a short history of transistors, and how oxides have revolutionized this field. It concludes with a glance at low-cost, disposable and lightweight devices for the next generation of ergonomic and functional discrete devices. Chapters cover:

• Properties and applications of n-type oxide semiconductors
• P-type conductors and semiconductors, including copper oxide and tin monoxide
• Low-temperature processed dielectrics
• n and p-type thin film transistors (TFTs) – structure, physics and brief history
• Paper electronics – Paper transistors, paper memories and paper batteries
• Applications of oxide TFTs – transparent circuits, active matrices for displays and biosensors

Written by a team of renowned world experts, Transparent Oxide Electronics: From Materials to Devices gives an overview of the world of transparent electronics, and showcases groundbreaking work on paper transistors

Leseprobe

Contents

The Impact of Oxides …

Preface

Acknowledgments

1 Introduction

1.1 Oxides and Transparent Electronics: Fundamental Research or Heading Towards Commercial Products?

1.2 The Need for Transparent (Semi)Conductors

1.3 Reaching Full Transparency: Dielectrics and Substrates

2 N-type Transparent Semiconducting Oxides

2.1 Introduction: Binary and Multicomponent Oxides

2.2 Sputtered n-TSOs: Gallium-Indium-Zinc Oxide System

2.3 Sputtered n-TSOs: Gallium-Zinc-Tin Oxide System

2.4 Solution-Processed n-TSOs

3 P-type Transparent Conductors and Semiconductors

3.1 Introduction

3.2 P-type Transparent Conductive Oxides

3.3 Thin Film Copper Oxide Semiconductors

3.4 Thin Film Tin Oxide Semiconductors

4 Gate Dielectrics in Oxide Electronics

4.1 Introduction

4.2 High- κ Dielectrics: Why Not?

4.3 Requirements

4.4 High- κ Dielectrics Deposition

4.5 Sputtered High κ Dielectrics in Oxide TFTs

4.6 Hafnium Oxide

4.7 Tantalum Oxide (Ta2O5)

4.8 Multilayer Dielectrics

4.9 High- κ Dielectrics/Oxide Semiconductors Interface

4.10 Summary

5 The (R)evolution of Thin-Film Transistors (TFTs)

5.1 Introduction: Device Operation, History and Main Semiconductor Technologies

5.2 Fabrication and Characterization of Oxide TFTs

6 Electronics With and On Paper

6.1 Introduction

6.2 Paper in Electronics

6.3 Paper Properties

6.4 Resistivity Behaviour of Transparent Conductive Oxides Deposited on Paper

6.5 Paper Transistors

6.6 Floating Gate Non-volatile Paper Memory Transistor

6.7 Complementary Metal Oxide Semiconductor Circuits With and On Paper – Paper CMOS

6.8 Solid State Paper Batteries

6.9 Electrochromic Paper Transistors

6.10 Paper UV Light Sensors

7 A Glance at Current and Upcoming Applications

7.1 Introduction: Emerging Areas for (Non-)transparent Electronics Based on Oxide Semiconductors

7.2 Active Matrices for Displays

7.3 Transparent Circuits

7.4 Oxide Semiconductor Heterojunctions

7.5 Field Effect Biosensors

Plates

Index

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Library of Congress Cataloging-in-Publication Data

Transparent oxide electronics : from materials to devices / Pedro Barquinha ... [et al.].p. cm.Includes bibliographical references and index.

ISBN 978-0-470-68373-6 (cloth) – ISBN 978-1-119-96700-2 (ePDF) – ISBN 978-1-119-96699-9 (oBook) – ISBN 978-1-119-96774-3 (ePub) –ISBN 978-1-119-96775-0 (Mobi) 1. Semiconductor films. 2. Oxides–Electric properties. 3. Thin film transistors. 4. Transparent semiconductors.I. Barquinha, Pedro. TK7871.15.F5T73 2012621.3815′2–dc23

2011042396

A catalogue record for this book is available from the British Library.

HB ISBN: 9780470683736

Elvira Fortunato and Rodrigo Martins would like to dedicate this book to Catarina, her lovely daughter, for her inestimable stimulus and understanding of ourscientific work, fully supported by the love that unites us!Pedro Barquinha would like to dedicate this book to Martinho and Maria, his parents, and Ana, his wife, for their love, support and comprehension.Luis Pereira would like to dedicate this book to his parents, his wife and his little princess Inês.

The Impact of Oxides …

“The rapid development of semiconductor techniques is requiring an ever greater application of materials of varying physical and physic-chemical properties. This demand cannot be fully met by a handful of elements having semiconducting properties, nor by the few relevant chemical compounds, which are already understood. Therefore increasing attention is being paid to studies on less known chemical compounds able to act as semiconductors.

Among them, compounds of metals or semiconducting elements with oxygen may be considered as most promising.”

Extract from the Introduction of the book: “Oxide Semiconductors”, by Z.M. Jarzebski, Pergamon Press, 1973.

… and the physics behind field effect …

“The particular device … consists of a very thin layer of semiconductor placed on an insulating support. This layer of semiconductor constitutes one plate of a parallel-plate capacitor, the other being a metal plate in close proximity to it. If this capacitor is charged, with the metal plate positive, then the additional charge on the semiconductor will be represented by the increased number of electrons. … Consequently, the added electrons should be free to move and should contribute to the conductivity of the semiconductor. In this way, the conductivity in the semiconductor can be modulated, electronically, by a voltage put on the capacitor plate. Since this input signal requires no power if the dielectric is perfect, power gain will result.”

Extract from the book: “Electrons and Holes in Semiconductors”, by W. Shockley Van Nostrand Reinhold Company Inc., 1950.

Preface

As far as novel materials and devices are concerned, the scientific challenge today is to develop new green materials and technologies that allow both for new product concepts and applications and innovation in terms of physical performance. These materials should be possible to process with low cost and using non-fab conventional manufacturing technologies, away from the dominant field of silicon, the most important material used nowadays to produce electronic devices. These requirements are met by the novel multicomponent amorphous oxides, which can be used in a wide range of applications, as they offer exceptional electronic performance as active semiconductor components or can be tuned for applications where high transparency and electrical conductivity are demanded. Here, one of the most interesting features is related to transparency and the ability to deposit these oxides at low temperatures, giving rise to a plethora of new application opportunities in sectors where the discreetness of the devices as much as their optoelectronic functionality are critical. This is the case, for instance, with thin-film transistors (TFTs) that are fully based on oxides, to which the present authors have been contributing over recent years; or the production of paper electronics, a new area where the authors are world pioneers and which emerge as a key field for research application in the years to come, mainly for the so-called 100 % low cost green disposable electronics.

This book provides an overview of the world of transparent electronics, chiefly the processing of oxide semiconductors and their application to transparent TFTs, being essentially focused on the work developed over recent years in our laboratory. The book is organized into seven chapters as follows. Chapter 1 is a short introduction to transparent electronics and related (semi)conducting materials. Chapter 2 provides some fundamental background regarding the properties and applications of n-type oxide semiconductors (both binary and multicomponent). Special emphasis is then given to the effect of composition and (post-) processing parameters on the structural, electrical and optical properties of the materials. Even though most of the work presented is related to sputtered oxides, recent results obtained with solution-processed (spray pyrolysis and sol-gel spin-coating) oxides are also provided. Chapter 3 gives an overview of the state of the art concerning p-type transparent conductive oxides and describes two of the most promising p-type oxide semiconductors designed to be applied as channel layers of TFTs: copper oxide and tin monoxide. The structural, electrical and optical properties presented by these two materials are highlighted and our results with sputtered thin films are shown. Chapter 4 is devoted to low-temperature processed dielectrics, which are also crucial materials for transparent electronic devices. Besides presenting the generic material requirements that should be met in order to integrate low-temperature dielectrics with oxide semiconductors, results for sputtered tantalum- and hafnium-based oxides are presented and discussed, mostly regarding their structural and electrical properties. Special emphasis is given to amorphous multicomponent and multilayer structures based on the combination of high-κ and high-bandgap materials. Chapter 5 is dedicated to the world of n- and p-type TFTs. After an introduction, where a short historical background and a comparison between existing TFT technologies are provided, a detailed analysis of the devices integrating the oxide semiconductors and dielectrics explored in the previous chapters is presented. Besides the effect of the different compositions and (post-)processing parameters of the active layer, other important aspects are covered, such as contact-resistance analysis, effect of passivation layer and electrical stability. Most of the chapter is related to sputtered n-type oxide TFTs based on the gallium-indium-zinc oxide system; however, sputtered p-type and solution processed n-type oxide TFTs are also presented. Chapter 6 is devoted to the new concept of paper electronics, made possible with semiconductor materials that can be processed at low temperatures and that still exhibit remarkable electrical properties, such as multicomponent amorphous oxides. Special emphasis is given to paper transistors, paper memories and paper batteries, with initial results for CMOS and sensor devices provided. The book concludes with Chapter 7, dedicated to the current and upcoming applications of oxide TFTs, for which transparent circuits including both NMOS and CMOS architectures, active matrices for displays and bio-sensors are highlighted.

When we agreed to write this book, our main purpose was to share our knowledge with the transparent electronics scientific community and simultaneously to attract newcomers by introducing them to this fascinating world. Besides that, we also expect to contribute with a pedagogic tool and a key element to be consulted when material or device concepts are needed, especially for students starting their university degrees.

Acknowledgments

First of all we would like to thank the European Research Council through the Advanced Grant (given to EF) under the project “INVISIBLE” (ERC-2008-AdG 228144) Advanced Amorphous Multicomponent Oxides for Transparent Electronics, directly related to this topic, as well as the support given by the European Commission and the partners involved in the following projects: Multiflexioxides (NMP3-CT-2006-032231), the first fully running project on Transparent Electronics in Europe, and more recently ORAMA (NMP3-LA-2010-246334) and POINTS (NMP3-SL-2011-263042), which are related to multifunctional oxide-based electronic materials and printable organic-inorganic transparent semiconductor devices, respectively. Considerable gratitude is also due to the EU project (262782-2 APPLE CP-TP), dealing with printed paper products for functional labels and electronics, as well as to the project SMART-EC (258203-ICT-2009.3.3) dealing with electrochromic oxides enabling technology applications.

We would like also to thank the fruitful collaborations done directly with companies and institutes such as the SAIT-SAMSUNG project “STABOXI”, related to the passivation of a-GIZO TFTs, the Electronic and Telecommunications Research Institute of South Korea (ETRI) with the project IT R&D program MKE - 2006-S079-03, “Smart window with transparent electronic devices” and to Saint Gobain Recherche France, for the project related to oxides for glazing.

This work was partially funded by the Portuguese Science Foundation (FCT-MCTES) through a multiannual contract with I3N and with projects related to oxide semiconductors such as: POCI/CTM/55945/2004 (Development of transparent and conductive oxide semiconductors p-type: from synthesis to devices); POCI/CTM/55942/2004 (Transparent thin film transistors based on zinc oxide to be used in flexible displays); PTDC/CTM/73943/2006 (Multifunctional Oxides: a novel approach for low temperature integration of oxide semiconductors as active and passive thin films in the future generation of electronic systems); PTDC/EEA-ELC/64975/2006 (High mobility transparent amorphous oxide semiconductors thin film transistors for active matrix displays); PTDC/CTM/103465/2008 (Integrated memory paper using oxide based channel thin film transistors); PTDC/EEA-ELC/099490/2008 (From electronic paper to paper electronic – Paper_@); PTDC/CTM/099124/2008 (Electrochromic thin film transistors for smart windows applications); QREN Nº 3454 (New nanoxide composites for advanced fabrication of targets for passive and active Opto/Micro/Nano-electronics applications); CMU-PT/SIA/0005/2009 (Self-organizing power management for photo-voltaic power plants) and ERA-NET/0005/2009 (Multifunctional zinc oxide-based nanostructures: from materials to a new generation of devices).

We would also like to thank the Calouste Gulbenkian Foundation for the Stimulus to Research Award 2008, “Nanotransistors of oxide semiconductors” (given to PB) and the Luso-American Development Foundation for the project in 2005 “Low-temperature sputter deposition exploration/ optimization of multi-component, amorphous and nanostructure heavy metal cation oxides for TFT and TTFT channel layer applications” and also the several scholarships given to the authors and members of the research team.

The authors also wish to express their gratitude to past deans and especially the present dean of Faculdade de Ciências e Tecnologia da Universidade Nova de Lisboa, Prof. Fernando Santana, who ensured that we enjoyed the excellent working conditions that existed at CENIMAT (FCT-UNL) and CEMOP (UNINOVA), especially the well-equipped laboratories that made this work possible.

We would like to thank Sarah Tilley, Project Editor for Chemistry at John Wiley & Sons, Ltd for her guidance and help during the editorial process.

We finish by acknowledging those who made this work possible, especially the group Microelectronic and Optoelectronic Materials of CENIMAT and CEMOP for their hard work, unlimited patience, dedication, creativity, expertise, knowledge and “emotional support” when the obstacles we faced every day were not so “transparent”. Without them this work would have been impossible.

The Microelectronic and Optoelectronic Materials Team (July 2011).

1

Introduction

1.1 Oxides and Transparent Electronics: Fundamental Research or Heading Towards Commercial Products?

Transparent electronics is emerging as one of the most promising technologies for future electronic products, as distinct from the traditional silicon technology. The fact that circuits based on conventional semiconductors such as silicon and conductors such as copper can be made transparent by using different materials, the so-called transparent semiconducting and conducting oxides (TSOs and TCOs, respectively), is of great importance and allows for the definition of innovative fields of application with high added value. The viability of this technology depends to a large extent on the performance, reproducibility, reliability and cost of the transparent transistors. Transistors are the key components in most modern electronic circuits, and are commonly used to amplify or to switch electronic analog and digital signals. Besides the high-performance silicon transistors used in microprocessors or amplifiers, designated by metal-oxide-semiconductor field-effect transistors (MOSFETs) and requiring processing temperatures exceeding 1000°C, other types of transistors are available for large area electronics, where lower temperatures and costs are required. Perhaps the most relevant are the thin-film transistors (TFTs), which are intimately associated with liquid crystal displays (LCDs), where they allow one to switch each pixel of an image on or off independently.

The most immediate demonstration of transparent electronics would be the realization of a transparent display, something that has been envisaged for a long time, at least from the 1930s when H.G. Wells imagined it in his science fiction novel The Shape of Things to Come (Figure 1.1a, see color plate section). Nowadays, with the advent of TSOs and TCOs, which besides transparency also allow for low temperature, low processing costs and high performance, transparent displays have become truly conceivable. In fact, even if much fundamental research will continue to be required so as to understand all the peculiarities of these materials and improve their performance and stability, the first commercial products within the transparent electronics concept have already started to be mass produced, such as the 22-inch transparent LCD panels by Samsung, in March 2011 (Figure 1.1b).

Figure 1.1Transparent displays: a) early vision, in H.G. Wells’ 1930s novel The Shape of Things to Come [1]; b) Samsung’s 22” transparent LCD panel now being mass-produced in 2011 [2]. Reproduced from [2] Copyright (2011) Samsung Corp.

The market for transparent displays is emerging now and its future looks quite promising, as revealed by the “Transparent Display Technology and Market Forecast” report by Displaybank, which predicts a $ 87.2 biliion market by the year 2025 (Figure 1.2, see color plate section) [3].

Figure 1.2Transparent display technology evolution and global display market. Adapted with permission from [3] Copyright (2011) DisplayBank.

1.2 The Need for Transparent (Semi)Conductors

Materials exhibiting both high optical transparency in the visible range of the electromagnetic spectrum and high electrical conductivity (σ) are not common when considering the categories of conventional materials, such as metals, polymers and ceramics. For instance, metals are generally characterized by having a high σ but being opaque, while ceramics are seen as electrical insulating materials which due to their typically large bandgap (EG) can be optically transparent. However, certain ceramic materials can simultaneously fulfill the requirements of high σ and optical transparency: these are designated by transparent conducting oxides (TCOs), where typically the main free carriers are electrons (n-type materials) [4]. Physically, this can be achieved if the ceramic material has EG > ≈ 3 eV, a free carrier concentration (N) above ≈1019–20 cm−3 and a mobility (μ) larger than ≈1 cm2 V−1 s−1, which can be verified for metallic oxides such as ZnO, In2O3 and SnO2 [5]. Due to the relatively low μ of TCOs when compared with classical semiconductors such as single crystalline silicon, which has μ > 400 cm2 V−1 s−1, TCOs generally need to be degenerately doped if a high σ is envisaged. As with silicon, doping can be achieved by the introduction of extrinsic substitutional elements in the host crystal structure, such as elements with different valences that are introduced in the cationic sites [4, 6, 7]. Doping can also be achieved by intrinsic structural defects, such as oxygen vacancies and/or metal interstitials. This structural imperfection, or in other words the deviation from stoichiometry, which always occurs when TCOs are deposited, is the fundamental reason behind the electrical conduction of these materials: to maintain charge neutrality, in n-type (p-type) materials, the defects give rise to electrons (holes) that depending on the defects’ energy levels within the EG of the oxide can be available for the conduction process, increasing N and consequently σ [6].

The effect of oxygen defining the final properties of materials was readily observed in the early days of this research area. In fact, the first reported TCO, by Badeker in 1907, was obtained after exposing an evaporated cadmium film to an oxidizing atmosphere: the resulting material, CdO, was transparent but maintained a reasonably high σ, resembling a metal [8]. In the 1920–1930s, Cu2O and ZnO were also investigated and researchers found experimentally that a large range of σ, exceeding six orders of magnitude, could be obtained by changing the oxygen partial pressure [9–13]. Oxygen concentration can have more implications than simply changing N and σ. As an example, in tin oxide it is reported that a large oxygen deficiency leads to the change of the tin oxidation state from + 4 to + 2, i.e., SnO2 is transformed into SnO. This can totally change the electrical properties of the resulting material: for instance, as with most of the TCOs, SnO2 is an n-type semiconductor, while SnO can present p-type behavior [4, 14].

However, even if σ can be significantly modulated by the concentration of intrinsic defects, with regard to the objective of obtaining a TCO with a high σ, extrinsic doping has to be used, with aluminum-doped zinc oxide (AZO) or tin-doped indium oxide (ITO) constituting some of the most well-known examples of these n-type materials. Even if optimal doped TCOs present σ values (≈104 Ω−1 cm−1 [15]) which are almost two orders of magnitude lower than those typically obtained in the cooper metal used in integrated circuits, this level of σ signifies that appreciable electrical conduction can be achieved in TCOs, allowing one to target a large range of applications, as will be shown below.

Although work such as that of Badeker was based essentially on pure scientific interest, the continuous advances in the understanding of solid state physics and of processing and characterization tools that occurred during the first half of the 20th century allowed for substantial technological progress in TCOs research. This resulted in the improvement of the properties of materials and soon a large range of applications for them began to be envisaged. The first large-scale use of TCOs occurred during World War II, when antimony-doped tin oxide (SnO2:Sb or ATO) was deposited by spray pyrolysis to be used as a transparent defroster for aircraft windshields [16]. During recent decades, making use of optimized TCO properties such as high σ, high transparency in the visible range, high reflectivity in the infrared, high mechanical hardness or high sensitivity to gas pressure, these materials have been extensively used as transparent electrodes in solar cells, liquid crystal displays (LCDs) and electrochromic windows, heating stages for optical microscopes, transparent heat reflectors in windows, abrasion and corrosion-resistant coatings, antistatic surface layers on temperature control coatings in orbiting satellites, gas sensors, among many other applications [4, 5]. Some examples of these applications are depicted in Figure 1.3 (see colour plate section).

Figure 1.3Some applications of TCOs at CENIMAT: a) electrochromic windows; b) passive matrix LED display; c) see-through solar cell.

In all of the electrical applications mentioned above, the TCO is an electrically passive element, i.e. it works as an electrode. Hence, with regard to electrical properties, most optimization efforts are focused on achieving the maximum possible σ, which requires a large N. However, a new class of applications requiring TCOs with considerably different electrical properties has recently emerged. In fact, the idea of producing ultra-violet (UV) detectors and diodes or even fully transparent TFTs requires the N of TCOs to be substantially decreased, in order to be able to use them as proper semiconductors, i.e. as active elements in devices [5, 17]. For instance, note that the usage of a TCO with a large N as the active layer of a TFT would result in a useless device, because the semiconductor could not be fully depleted, hence it would not be possible to switch-off the TFT. To distinguish these transparent oxides from the highly conducting TCOs, the low σ and N materials can be designated by transparent semiconducting oxides (TSOs). The properties tuning of TSOs can be made using the same principles as those discussed above for TCOs, i.e. either by intrinsic or extrinsic doping. For instance, larger oxygen concentrations during deposition should result in fewer oxygen vacancies, hence less free electrons in an n-type TSO, while extrinsic doping with elements that introduce acceptor-like levels and/or that increase EG can also lead to similar results [6, 18].

Most of the TCOs and TSOs studied so far are n-type. However, p-type oxides are needed to extend the possibilities of transparent electronics, for instance by making possible the fabrication of complementary logic circuits. Besides the early experiments performed with poor-transparency Cu2O in the early 1930s, the first reported p-type oxide was NiO, in 1993 [19]. Although p-type conduction was achieved, poor average visible transmittance (AVT) of 40 % and low σ (≈7 Ω−1 cm−1) were obtained. In 1997 Kawazoe et al. presented a strategy for identifying oxides combining p-type conductivity with good optical transparency [20]. The authors suggested that the candidate materials should have tetrahedral coordination, with cations having a closed shell with comparable energy to those of the 2p levels of oxygen anions, and the dimension of crosslinking of cations should be reduced. They selected CuAlO2 to demonstrate the concept, and p-type conduction and reasonable transparency could in fact be achieved. The paper published by Kawazoe et al. had a significant impact on the research of p-type oxides, with various work being reported during the following years based on similar theoretical principles, mostly employing delafossite structure materials such as SrCu2O2 or CuGaO2 [21–23]. Although the maximum σ and μ achieved with these p-type oxides are at present three to four (σ) and one to two (μ) orders of magnitude lower than the ones of optimized n-type TCOs, the achieved values begin to be suitable for their application as TSOs. Given this, different transparent optoelectronic devices employing both p- and n-type TSOs have been demonstrated, such as near-UV-emitting diodes composed of heteroepitaxially grown TSOs (p-type SrCu2O2 and n-type ZnO) [24] and UV-detectors composed of single crystalline p-type NiO and n-type ZnO [25]. However, to achieve reasonable optical and electrical properties, p-type TSOs generally require larger processing temperatures than n-type oxides, and significant research is still needed in order to surpass the temperature and performance limitations of these materials so as to fabricate transparent p-type materials compatible with the low temperature processed n-type TSOs. However, it will be shown in Chapter 5 that recent research developed at CENIMAT already allows one to obtain good performance p-type oxide TFTs with a maximum processing temperature of 200°C.

1.3 Reaching Full Transparency: Dielectrics and Substrates

To reach the target of fully transparent devices, oxides with very large electrical resistivity (ρ >1010 Ω cm) are also required. In a transparent TFT, for instance, these oxides work as dielectric layers, insulating electrically the gate electrode from the semiconductor. The choice of the appropriate dielectric comprehends both physical requirements, such as the band offsets with the semiconductor and the level of leakage current allowable, as well as process related ones, such as compatibility with the remaining device materials in terms of deposition temperature or etching selectivity. Higher dielectric constant (κ) allows one to preserve a high capacitance with thicker dielectrics, which is especially relevant for low-temperature processed thin films, where leakage currents are normally higher. Moreover, the surface of the dielectric should be highly smooth and the material should have an amorphous structure, since high roughness and polycrystalline structure lead to increased interface defects and grain boundaries can act as paths for carrier flow, increasing leakage current and leading eventually to the dielectrics’ breakdown. Generally, dielectrics with high-κ exhibit low-EG and vice-versa [26]. Hence, to obtain a better match between the desirable structural and electrical properties, amorphous multicomponent dielectrics based on mixtures of high-κ materials, such as Ta2O5 or HfO2, with high-EG materials, such as SiO2 or Al2O3, are proposed by the authors [27, 28].

Finally, substrates also have to be considered and oxides are again a solution, as glass is certainly the most versatile rigid substrate for transparent electronics, combining important properties such as low cost, smooth surface and ability for large area deposition. Moreover, if flexibility is required, polymers or even paper based on nanofibrills should be used.

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