Material, type, method, carrier concentration (
Abstract
Bismuth chalcogenides have been intensively studied for their high-performance thermoelectric properties and their novel topological surface states, which could significantly benefit novel applications in fields such as TE devices, spintronics, and quantum computing. This chapter reports recent advances in pulsed laser deposition (PLD) for the growth of bismuth chalcogenide (e.g., Bi2Te3, Bi2Se3, and Bi3Se2Te) thin films and their novel properties. It covers a wide range of fields such as thin film growth using PLD for fabricating polycrystalline and epitaxial films with different thermoelectric, nanomechanical, and magnetotransport properties as a function of the PLD processing conditions. Moreover, the proximity-induced superconductivities in Bi inclusions/bismuth chalcogenide thin films are also reported and discussed in detail.
Keywords
- pulsed laser deposition
- thermoelectrics
- topological insulators
- bismuth chalcogenides
- superconductivity
- magnetoresistance
1. Introduction
Bismuth chalcogenide thin films are of great interest because of the exciting properties of topological insulators (TIs) and their applications to thermoelectrics (TEs). These materials have been applied in integrated TE cooling devices working at near room temperature [1, 2]. TIs are exotic materials with an insulating bulk and topologically protected states on the surface which could be used in different applications, such as spintronics and quantum computing [3–6]. The topological surface states (TSSs) exhibit Dirac linear energy dispersion inside the bulk gap, spin-polarization by spin-momentum locking nature, and weak anti-localization (WAL) due to the strong spin-orbit coupling [3–6]. Thus, the WAL through magnetotransport studies has been widely used as a signature of TI materials [7–9].
For application purposes, thin film growth techniques for TE and TI materials are required. Among physical vapor deposition techniques, pulsed laser deposition (PLD) offers great versatility in growing polycrystalline and epitaxial thin films with high growth rates, multiple elements, and diverse structural morphologies for both fundamental studies and applications. The purpose of this chapter is to outline recent advances in the PLD growths of bismuth chalcogenide thin films with desired properties for TE/TI applications and fundamental studies.
2. Thin film growth using pulsed laser deposition (PLD)
Thin film growth consists of nucleation, growth, and coalescence (Figure 1a). In a physical vapor deposition, an extremely nonequilibrium process takes place at high supersaturations and at comparatively high concentrations of impure atoms [10]. Nucleation takes place at high supersaturations
2.1. Basic growth modes
For all phase transitions, the formation of thin films is characterized by the formation of nuclei and their growth. Depending on the interaction energies of substrate atoms and film atoms, any of three growth modes in Figure 2a–c can occur:
2D Frank-van der Merwe mode: layer-by-layer growth, in which the interaction between substrate and atoms of film is greater than that between adjacent atoms of film.
3D Volmer-Weber mode: separated islands form on the surface of substrates, in which the interaction between atoms of film is greater than that between a substrate and the adjacent atoms of film.
Stranski-Krastanov mode: layer plus island, in which one or two monolayers form first and then grow individually.
After an initially random nucleation of islands on the surface of the substrates, the deposition on the top of the islands is faster than that in the valleys due to the oblique incident flux (the so-called
2.2. Epitaxy growth
Epitaxy refers to the growth of a single crystal film on top of a single crystal substrate. The deposited film is denoted as an epitaxial film or epitaxial layer. The growth is called homoepitaxy if the film and the substrate are the same material, and it is called heteroepitaxy if they are different materials. Epitaxial relationship is determined as: (
2.3. Factors governing the epitaxy growth
The key factors governing epitaxy growths are structural compatibility, chemical compatibility, and growth temperatures.
Lattice misfit
2.4. Preparation of bismuth chalcogenide films by PLD
PLD is one of the most convenient thin film growth techniques that uses a high-intensity pulsed laser beam as an external energy source to ablate a target, form a plume, and then deposit thin films onto a substrate. Figure 3 shows a typical PLD system for preparing TE and TI thin films. A substrate is heated and maintained at a desired substrate temperature (
The surface of substrates should be atomically clean and free from impurities because the contaminants can interact with the thin films being deposited and substantially degrade its quality and adhesion to the substrates. The presence of unwanted surface contaminants can also influence the growth and orientation of the films in an undesired manner. In the depositions for TE thin films, an approximately 300-nm-thick SiO2 layer was thermally grown on the Si wafers (thickness 525 μm) for electrical isolation purpose. The wafers were cut into 1.5 cm × 1.5 cm substrates. The substrates were cleaned with acetone to dissolve any contaminants adhering to the surface of substrates such as grease and oils. This was followed by rinsing with methanol to remove any residues left behind after cleaning with acetone. Afterward, the substrates were rinsed in distilled water and dried with nitrogen flow. The substrates were then used for the deposition of TE thin films.
Here are some examples of PLD growth of TE films. For Bi2Se3 thin films, the depositions were at
3. Thermoelectric bismuth chalcogenide thin films
3.1. Crystal structures of bismuth chalcogenides
The crystal structures of bismuth chalcogenides (e.g., Bi2Te3, Bi2Se3, and Bi3Se2Te) are usually described by a hexagonal cell consisting of 15 layers of atoms stacking along the
A 5-atomic-layer-thick lamellae of ‐(Te(1)‐Bi‐Te(2)‐Bi‐Te(1))‐ or ‐(Se(1)‐Bi‐Se(2)‐Bi‐Se(1))‐ is called a quintuple layer, QL, in which the Te(1)‐Bi and Bi‐Te(2) or Se(1)‐Bi and Bi‐Se(2) are ionic-covalent bonds. Because of the weak binding (i.e., Van der Waals force) between Te or Se layers, bismuth chalcogenides could be cleaved easily along the plane perpendicular to the
The crystal structures of Bi3Se2Te can be formed by ordered stacking of Bi2Se2Te and Bi2 building blocks, that is, (Bi2)
3.2. Introduction to thermoelectrics and applications
Thermoelectric materials are solid-state energy converters in which the combination of thermal, electrical, and semiconducting properties allows them to be used to convert waste heat into electricity or electrical power directly into cooling and heating [21].
3.2.1. The thermoelectric figure of merit (ZT)
The performance of the thermoelectric materials is often denoted as figure of merit
where
The efficiency of a thermoelectric device is directly related to
and for air-conditioning or refrigeration, the coefficient of performance is [23]
where
3.2.2. Conflicting properties in thermoelectric materials
Maximizing
The electrical conductivity (
The Wiedemann-Franz Law [2] states that the electronic contribution to the thermal conductivity is proportional to the electrical conductivity (
where
The kinetic definition of
The high
Figure 5 shows the compromise between large
3.2.3. Overview of thermoelectric applications
TE devices have unique features: no moving parts, substantially less maintenance, quiet operation, high power density, low environmental impact, and high reliability [26]. Commercial use has been made mostly from Peltier thermoelectric cooling (TEC) effect, such as in small refrigerator devices used for camping and outdoor activities, automotive climate control seats, and localized cooling at the hot spots of chips. Figure 6 gives an overview of the present and potential applications of thermoelectric generators (TEGs) [27]. Indeed, TEGs have been used for the power in miniaturized autarkic sensor systems, automotive waste heat recovery systems, ventilated wood stove, heating systems, water boilers, and heat recovery in industry.
3.3. Thermoelectric properties of polycrystalline Bi2Te3, Bi2Se3, and Bi3Se2Te thin films with controlled structure morphology
Some typical HRTEM images of Bi2Te3, Bi2Se3, and Bi3Se2Te grown using PLD are shown in Figure 7 [14–16]. HRTEM images performed on a high
For a Bi2Se3 film deposited at 300°C and 40 Pa, an HRTEM image taken at the boundary of three platelets (P1, P2, and P3) revealed the granular-polycrystalline structure of the films (Figure 7b). Moreover, P1 and P2 partly overlapped and the corresponding fast Fourier transform (FFT) of this overlapping region indexed by
HRTEM images of a Bi3Se2Te film deposited at 250°C and 40 Pa are shown in Figure 7c and d. Nanocrystallites with sizes of 10–20 nm are clearly observed in Figure 7c, confirming the nanocrystalline type of the Bi3Se2Te films. The interplanar spacing of the Bi3Se2Te (0 0 5) planes in the nanocrystallites is approximately 0.464 nm. Therefore, the
Figure 8a shows the
In order to check the evolution of the
System | Type | Method | (1019 cm−3) |
(cm2/Vs) |
cm−1 K−2) |
References | ||
---|---|---|---|---|---|---|---|---|
Bi2Te3 | Layered smooth film | PLD | 10.1 | 90.6 | 1464 | −186 | 50.6 | [39] |
Bi2Te3 | Layered compact polycrystalline | PLD | 5.0 | 102 | 814.3 | −172.8 | 24.3 | [15] |
Bi2Te3 | Nanoparticle film | PLD | 9.7 | 14.8 | 230 | −91 | 1.9 | [34] |
Bi2Te3 | Super-assembled film | PLD | 4.0 | 12.4 | 79 | −113 | 1.0 | [33] |
Bi2Se3 | Layered hexagonal platelets | PLD | 7.4 | 81.4 | 963.8 | −75.8 | 5.5 | [14] |
Bi3Se2Te | Nanocrystalline film | PLD | 35.5 | 34.4 | 1747.5 | −68.8 | 8.3 | [16] |
Bi2Te3 | Layered structure | Sputtering | 95 | 12.1 | 1840 | −70 | 8.8 | [35] |
Bi2Se3 | Bulk | Melting and hot-pressing |
– | – | 251.9 | −175 | 7.7 | [32] |
Bi2Se0.3Te2.7 | Bulk | Ball milling hot pressing | – | – | 892 | −190 | 32.2 | [36] |
Bi2Se1.5Te1.5 | Bulk | Zone melting | 1.2 | 230 | 441.6 | −193 | 16.5 | [37] |
Bi2Se1.8Te1.2 | Nanoplatelet bulk | Polyol method | – | – | 199.6 | −80.9 | 1.3 | [38] |
Bi2Se2Te | Bulk | Ball milling hot pressing | – | – | 1613 | −60 | 5.8 | [36] |
The
Table 1 summarizes the transport and room-temperature TE properties of bismuth chalcogenides in the literature [14, 15, 32–39]. For PLD growths, the highly (0 0 1)-oriented layered Bi2Te3 films achieved a
Finally, Figure 8d shows the |
4. Nanomechanical properties of Bi2Te3 and Bi3Se2Te thin films
Effects of helium ambient pressure (in PLD) on the nanomechanical properties of Bi2Te3 and Bi3Se2Te thin films have been investigated [9, 40]. The Bi2Te3 thin films were grown at
As shown in Figure 9a, the hardness monotonically increased from 2.92 ± 0.12 to 4.02 ± 0.14 GPa for Bi2Te3 films, and from 2.5 ± 0.2 to 3.0 ± 0.1 GPa for Bi3Se2Te films when
The crystallite sizes (
In contrast, the 200-nm-thick Bi3Se2Te films with
5. Topological insulator bismuth chalcogenide thin films and their novel properties
5.1. The epitaxial growths of bismuth chalcogenide thin films
Topological insulator (TI), a new class of quantum matter, possesses insulating in bulk and robust gapless topological surface states (TSSs) in which the spin of the electron is locked perpendicular to its momentum by strong spin-orbit interaction [6, 50, 51]. TIs have been identified as promising materials for exploiting exciting physics and developing potential applications in optoelectronics, spintronics, and quantum computations [50–54]. Dirac fermions in TIs have also been studied by angle-resolved photoemission spectroscopy [55–57] or scanning tunneling microscopy [58, 59]. In magnetotransport studies, TSS can be studied by weak antilocalization (WAL) [4, 9, 60, 61] and Shubnikov-de Haas oscillations [3, 62].
Topological insulator bismuth chalcogenide thin films have been grown epitaxially on various substrates using PLD. Onose et al. reported the epitaxial growth of Bi2Se3 thin films on InP (1 1 1) substrates (the lattice mismatch of 0.2%) [7]. A designed Se-rich target with an atomic ratio of Bi:Se = 2:8 was used to compensate for the issue of high doping carriers and to avoid unwanted Se-deficient phases. The pulsed laser power and repetition were 140 mJ and 10–20 Hz, respectively. The Bi2Se3 films obtained a small full-width at half-maximum (FWHM) for the XRD rocking curve of (0 0 0 6) peak. The surfaces of the films are composed of triangular pyramids with step-and-terrace structures, reflecting the hexagonal symmetry of Bi2Se3. The epitaxial relationship is Bi2Se3 (0 0 1) || InP (1 1 1) and Bi2Se3
Figure 10 presents the PLD epitaxial growths of Bi2Te3, Bi2Se3, and Bi3Se2Te thin films on large-misfit substrates [9, 53, 64]. The PLD conditions for growing Bi2Te3 films on STO (1 0 0) were as follows: substrate temperature of 300°C; helium ambient pressure of 40 Pa; repetition rate of 2 Hz; pulsed fluence of approximately 3.4 J/cm2. As shown in Figure 10a, a
5.2. Magnetotransport properties of bismuth chalcogenide thin films
The weak antilocalization (WAL) which is a negative quantum correction to classical MR caused by the wave nature of electrons is used as a signature of TSS. In TIs, WAL is induced by both the helicity of the surface state and the spin-orbit coupling of bulk [4, 61, 65, 66]. In a low
where
The typical magnetoresistance (MR) results of some bismuth chalcogenides (i.e., Bi2Te3, Bi2Se3, and Bi3Se2Te) thin films grown by PLD are presented in Figure 11 [9, 64, 67]. The Bi2Te3, Bi2Se3, and Bi3Se2Te thin films were grown on Al2O3 (0 0 0 1) substrates using PLD at
Figure 11b and f also present the –
In Figure 11c, the MR (
5.3. Proximity-induced superconductivities in Bi inclusions/bismuth chalcogenide thin films
Recent studies have shown a two-dimensional interface state between TIs and superconductors resulting from the superconducting proximity effect that supports Majorana fermions [76, 77]. Majorana fermions, novel particles which are their own antiparticles, can potentially be applied to topological quantum computing, which has motivated intense interest in TIs [53]. Koren et al. observed the local superconductivity in Bi2Te2Se and Bi2Se3 films below 2–3 K, which was naturally induced by small amounts of superconducting Bi inclusions or precipitations on the surface [78]. Moreover, Le et al. reported superconductivity at an onset critical temperature of approximately 3.1 K in a topological insulator 200-nm-thick Bi2Te3 thin film grown by pulsed laser deposition [53]. Indeed, Figure 12a shows the normalized resistivity
The detailed investigations of S2 strongly suggest the existence of superconducting Bi nanoclusters on the surface that induce the
The Bi-rich environment on the film surface is confirmed by AES analysis (Figure 12c) [53]. This is because the vapor pressure of Te (at
6. Conclusion
This chapter provides the effects of ambient pressures and substrate temperatures in PLD growths on the structural-morphology, thermoelectric, nanomechanical, and magnetoresistance properties of bismuth chalcogenide thin films. The thermoelectric power factor of the stoichiometric Bi2Te3 films grown in the range of 220–340°C and
Acknowledgments
Financial support from Vietnam National Foundation for Science and Technology Development (NAFOSTED) under Grant number 103.99–2015.17, the Ministry of Science and Technology, Taiwan under Contract Nos.: 103-2923-M-009-001-MY3, 103-2628-M-009-002-MY3, 103-2119-M-009-004-MY3, and the Ministry of Education (MOE-ATU plan at National Chiao Tung University) are gratefully acknowledged.
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