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The role of diamond (Diamond), the raw material of "cultivating diamond", is far from decoration and consumption. It not only plays an irreplaceable role in processing stone, non-ferrous metals and composite materials, but also is called the ultimate semiconductor material by the industry.

As early as 20 years ago, the scientific community set off an upsurge in the study of diamond semiconductors, but today, we have not used the devices made by diamond semiconductors, so that some engineers lament that diamond is always on the edge of the practical use of semiconductors. What are the problems hindering its development, and how will it transform the semiconductor industry?

The tall diamond of the same family as silicon is one of the elemental isomers of carbon (C) and has a face-centered cubic structure. each carbon atom forms a σ-type covalent bond with four other carbon atoms with sp3 hybrid orbitals, the bond length of C is 0.154nm, and the bond energy is 711kJ / mol, forming a regular tetrahedron, which is a typical atomic crystal. It integrates many excellent properties, such as superhardness, wear resistance, heat conduction, radiation resistance, strong acid and alkali corrosion resistance, variable shape (single crystal / polycrystal) and so on. [2]

Graphite, fullerene, carbon nanotubes, graphene and graphyne, which are often mentioned in the industry, are allotropes of carbon. Carbon has three hybrid states: sp3, sp2 and sp. Many kinds of carbon allotropes can be formed by different hybrid states, while diamond is formed by sp3 hybridization. [3]

Structurally speaking, diamond and silicon (Si) and germanium (Ge) which are co-located in the IV group are diamond structures and are born materials for semiconductors [4]. According to rough estimates, the performance of diamond as a semiconductor is 23000 times higher than that of silicon, 120 times higher than that of gallium nitride (GaN), and 40 times higher than that of silicon carbide (SiC). [5]

Since the parameters are excellent, what devices can be made with these parameters?

Diamond is an ultra wide band gap semiconductor material with a band gap as high as 5.5eV, which makes it more suitable for application in extreme environments such as high temperature, high radiation and high voltage. Diamond can be used in high power devices with thermal conductivity up to 22W cm- 1 K-1. Hole mobility is 4500cm2 V-1 s-1 and electron mobility is 3800cm2 V-1 s-1, which makes it suitable for high-speed switching devices. The breakdown field strength is 13MV / cm, which can be used in high voltage devices; the Barrier merit value is as high as 24664, which is much higher than that of other materials (the higher the value, the greater the potential for switching devices) [7]. In addition, because the exciton binding energy of diamond reaches 80meV, diamond can achieve high intensity free exciton emission at room temperature (the luminous wavelength is about 235nm). It has great potential in the preparation of high-power deep ultraviolet light-emitting diodes and the development of extreme ultraviolet, deep ultraviolet and high energy particle detectors. [8]

In addition to the above devices, diamond can also be used in advanced fields such as high power optical lenses of megawatt cyclotron oscillators in nuclear fusion reactors, X-ray optical modules, high power density radiators, Raman laser optical lenses, optoelectronic devices on quantum computers, biochip substrates and sensors, bipolar diamond electronic devices, etc. [9]

Material characteristics of semiconductors [10] Diamond is the fourth generation player of the material revolution.

The first generation is represented by germanium and silicon; the second generation is represented by the successive industrialization of gallium arsenide (GaAs) and indium phosphide (InP) in the 1980s and 1990s; the third generation is represented by gallium nitride (GaN) and silicon carbide (SiC); the fourth generation is the ultra-wide band gap semiconductor materials above 4eV, represented by gallium oxide (Ga2O3), aluminum nitride (AlN) and diamond. (gallium oxide can refer to the fruit shell hard science and technology history article. "after graduating from this year's college entrance examination, can gallium oxide change the world? ")

At present, in the field of semiconductors, the potential of silicon materials has basically been tapped to the extreme, and materials with better properties are needed. As the next generation material of ultra-wide band gap, diamond has attracted global competition, and many countries in the world have included diamond in their key development plans.

Of course, the ultimate function of the new material is not to beat the traditional materials such as silicon and germanium to death on the beach, but to complement each other and play a full role in what they are best at.

Division of semiconductor materials [10] of course, natural diamond has many impurities, small size and high price, so it is difficult to meet the needs of industrialization in the field of electronic devices. Synthetic diamond and natural diamond have the same structure, similar performance and relatively low cost, which can effectively make diamond used by human beings.

Not every kind of diamond can be cored. Diamond growth can be divided into HTHP method (high temperature and high pressure method) and CVD method (chemical vapor deposition). The two growth methods focus on different applications, and they will be complementary for a long time in the future.

For semiconductors, CVD is the main method for the preparation of diamond films, and HPHT diamond single crystals will also serve as the main source of substrates in CVD synthesis. [11]

Comparison of two main diamond growth methods, tabulation, fruit shell hard science and technology, reference materials (Journal of artificial crystals [12], Power Diamond prospectus [13] among them, the CVD method is also divided into four growth methods: HFCVD, DC-PACVD, MPCVD and DC Arc Plasma Jet CVD. Because the MPCVD method adopts electrodeless discharge and pure plasma, it is suitable for the growth of high quality diamond at present, and it is also suitable for the study of high quality diamond epitaxy and doping. [12]

The four main methods and applications of CVD, tabulation, hard science and technology of fruit shell, reference materials, Journal of artificial crystals [14] in fact, HTHP and CVD methods are also used to cultivate diamonds, but diamonds for semiconductor chips are not the same as diamonds and tools: first, they are of different purity, and second, they need to be doped.

The classification of diamond in the early stage of semiconductor can be divided into Ⅰ type and Ⅱ type according to its spectral characteristics. Ⅰ type has high content of impurities, is opaque to ultraviolet light below 300nm, and has strong absorption in the range of 1430~500cm-1, while Ⅱ type diamond is highly pure and completely transparent to the above-mentioned bands. On the basis of Ⅰ type and Ⅱ type, according to the type and quantity of nitrogen (N), boron (B) and other impurities, it is divided into Ⅰ a, Ⅰ b, Ⅱ a, Ⅱ b and other types. [15]

This classification is relatively rough, and it is sufficient for machinery and tools. For example, Ⅰ b type diamond large single crystal (yellow, nitrogen content is about several hundred ppm) is mainly used in heat sink, cutting tools, high precision machining and so on. High quality Ⅱ a type diamond single crystal (colorless, nitrogen content is less than 1ppm) is mainly used as heat sink for high power laser, window material for infrared spectroscopy, diamond anvil, etc. Ⅱ b diamond expands its application space by making use of its semiconductor properties. [11]

However, this classification is obviously not fine enough for semiconductors, until the concept of optical grade CVD appeared in the 1990s, and then the titles such as quantum level, electronic level, optical level, thermal level, mechanical grade and so on appeared one after another. These classifications mainly refer to two parameters: dislocation density and nitrogen content. in essence, the microvoids formed by vacancy and vacancy aggregation and the black structure formed by grain boundary connection in high-speed polycrystal growth are the main factors affecting diamond classification. [14]

The classification and defect requirements of CVD diamond [14] need to emphasize that diamond can be divided into single crystal and polycrystal. Polycrystalline diamond is generally used in heat sink, infrared and microwave windows, wear-resistant coatings, etc., but it can not really give full play to the excellent electrical properties of diamond because of its internal grain boundaries. it will greatly reduce the carrier mobility and charge collection efficiency, and the performance of the electronic devices prepared by it will be seriously suppressed. Single crystal diamond does not have this concern and is generally used in key fields such as detectors (such as ultraviolet detectors, radiation detectors) and power devices (such as field effect transistors, diodes). [16]

For example, the photovoltaic industry once showed a pattern of separation between monocrystalline silicon and polysilicon, but when the cost of monocrystalline silicon dropped sharply, the cost advantage of polysilicon weakened, gradually faded out of the competition and turned to specific areas. Diamond semiconductor is the same truth, single crystal performance is better but the cost will be higher, polycrystal will be valuable in cost-sensitive applications, while some devices can only use single crystal diamond.

Application of different levels of diamond, watchmaking, fruit shell hard science and technology, references (Diamond Manual [17]) requires diamond to conduct electricity to be doped in fact, pure diamond itself is an excellent insulator (resistivity ρ > 1015 Ω cm), only when the introduction of acceptor and donor elements can be changed from insulator to semiconductor.

The doping methods of diamond can be divided into three methods: doping in the growth process of HTHP method, doping in the growth process of CVD method and ion implantation. Among them, HTHP method is mainly used in the growth of single crystal diamond substrate, and there are few studies on doping.

The so-called CVD doping method means that n-type donor elements or p-type acceptor elements are doped in the growth process, and some of the carbon atoms that form semiconductor diamond films will be replaced with corresponding elements, showing electrical conductivity. This method is relatively easy to operate. The ion implantation method, as its name implies, is to accelerate the impurity element ions by accelerating the electric field to obtain large kinetic energy, which can be directly injected into diamond materials. this method can accurately control the implantation concentration of doped atoms and allow selective doping. The degree of freedom of device design is greatly improved, but it will cause damage to the crystal. It is necessary to further carry out high temperature annealing to eliminate the damage and activate the doped atoms. [18]

The main doping methods and current situation of diamond semiconductors, table-making, fruit shell hard science and technology, reference materials: Journal of artificial crystals [18], Research on Electronic Properties of Diamond Semiconductors [19] at present, the p-type doping of diamond semiconductors is more mature, mainly boron (B) doping, while n-type doping is a difficult work, researchers focus on phosphorus doping, nitrogen doping and sulfur doping and so on. In addition, the double or triple doping of multi-elements and the doping of NaN3, h-BN, FeS, NiS, Mn3P2 and other compounds are also being tested. [11]

At present, diamond can be used as both substrate and epitaxy in semiconductors (the process of growing a new single crystal layer on the machined single crystal substrate after cutting, grinding and polishing). Single crystal and polycrystal also have different uses.

With the promotion of CVD growth technology, mosaic splicing technology, homoepitaxial growth technology and heteroepitaxial growth technology, the preparation of large-size single crystal diamond (SCD) is becoming more and more mature. The diameter of single crystal diamond prepared by HTHP method has reached 20mm. The maximum size of independent single crystal wafers grown by homoepitaxy can reach 1 inch; the diamond wafer grown by mosaic splicing technology can reach 2 inches [21]; the wafer grown by diamond heteroepitaxy technology has also reached 4'8 inches; in addition, diamond will also act as a thermal conductive substrate, such as diamond-based GaN wafers have reached 8 inches. [14]

Moreover, in device applications, the application system of diamond is compatible with silicon-based semiconductors [22]. Under such favorable conditions and many breakthroughs, the industry still does not seem to be able to come up with products, where on earth is the problem?

Doping is an obstacle in the way at present, the p-type doping of diamond semiconductors has been relatively mature, but there are still many problems of n-type doping. N-type doping elements have high ionization energy in diamond, so it is difficult to find suitable donor elements.

In n-type doping, the resistivity of nitrogen (N) diamond is higher [23]; the solubility of sulfur (S) in diamond is very low, the quality of the film is not high, and there are more amorphous phases; phosphorus (P) is the most widely used and recognized as the most potential doping element, but the hydrogen atom in diamond will passivate the phosphorus atom and inhibit the ionization of phosphorus atom, resulting in high resistivity. [24]

However, n-type doping has made great progress, and some studies have found that the electrical conductivity of large diamond single crystal obtained by co-doping with boron and nitrogen is 10 ~ 100 times higher than that of single boron-doped diamond. [25]

On the contrary, aluminum nitride (AlN) and gallium oxide (Ga2O3), which belong to the fourth generation semiconductor materials, also have the dilemma of doping: for example, n-type doping of aluminum nitride (AlN) has been realized, but p-type doping only stays in the theoretical stage, gallium oxide (Ga2O3) can not achieve stable p-type doping for the time being. [26]

Core-making pays attention to the manufacture of multi-integrated circuits, there are many individual processes, they all have some special requirements for materials, at the same time, each process will have the problem of compatibility. It has to be said that the road from diamond to wafer to chip is full of difficulties, and it will be a long-term research process to solve these problems one by one.

For example, the PN node is formed by point doping on both sides of diamond [27]; for example, diamond FET is fabricated by surface transfer doping, which makes the design and manufacture of diamond FET different from that of standard devices [28]. In addition, the oxide of diamond is gas and there is no solid-state intrinsic oxide suitable for device applications, which brings difficulties for the design and fabrication of some devices such as MOS, and there are also many inconveniences in lithography mask and other processes. [29]

Although the industry has broken through many problems over the past few decades, no one can tell whether the diamond can withstand the test of the final product when it is really within the industry.

Size and cost are the key. First of all, the larger the wafer size, the more chips can be produced, and the same is true of diamond. Only large wafers can lead the future of commercialization. However, at present, there is a lack of large-size diamond substrate materials, and there are too many internal defects in large-size diamond epitaxial materials commonly used, such as heteroepitaxial substrate and substrate splicing. Taking CVD nitrogen-doped diamond as an example, the dislocation density of 6mm x 7mm single crystal can be as low as 400cm-2, but the dislocation density of 4'8 inch diamond heteroepitaxial wafer is close to 107cm-2. [21]

Second, it is cheap enough to let diamond into the industrial chain. Compared with silicon, the price of silicon carbide (SiC) is 30-40 times that of silicon, the price of gallium nitride (GaN) is 650-1300 times that of silicon, and the price of synthetic diamond used in semiconductor research is almost 10000 times that of silicon. At this price, even if it can effectively improve the efficiency of the chip, TCO (total cost of ownership) will be overwhelmed by the high cost of materials. [28]

Since it is so difficult, does it mean that we have to give up? In fact, diamond is still considered as the most promising material for the preparation of the next generation of high-power, high-frequency, high-temperature and low-power loss electronic devices [27]. But the market will still accept new things.

The countdown to entering the industry chain according to MarketWatch data, the global market size of diamond materials for semiconductors is estimated to reach US $90 million in 2022 and is expected to reach US $365.3 million by 2028, with an annual compound growth rate of 26.3%. [30]

So what is the progress of diamond semiconductors so far?

According to the statistics of fruit shell hard science and technology, at present, the American Akhan company, the British element six (Element Six) company, the Japanese NTT company, the Japanese Industrial Technology Comprehensive Research Institute (AIST), the Japanese Institute of material and Materials Research (NIMS), the American Geophysical Laboratory Carnegie Research Institute, the American Argonne National Laboratory and so on are all promoting the industrialization of diamond semiconductors. Among them, Akhan planned to be the first company to realize the industrialization of diamond semiconductors.

Looking back at the domestic situation, there have been a lot of research and exploration, and achieved phased results, but there are no commercial cases. It should be noted that there is still a lack of autonomy in the acquisition of key process equipment and single crystal diamond substrates in China, as well as in the advanced growth process of large-size single crystal diamond films.

Industrialization actions and landmark events of diamond semiconductors, tabulation? fruit shell hard science and technology, reference materials, "Mechanical and Electrical Information" [31], in terms of device applications, diamond semiconductors are mainly used in power semiconductors. Diamond diodes have representative devices such as p-intrinsic-n diodes (PiND), SBD, metal intrinsic p-diodes (MiPD) and Schottky pn diodes (SPND). [32]

Diamond diode performance [32] the research on diamond switching devices began in the 1980s. Typical switching devices include bipolar junction transistors (BJT), metal semiconductor FET (MESFET), metal oxide semiconductor field effect transistors (MOSFET), junction gate field effect transistors (JFET), H-FET and so on. [32]

The performance of diamond switching devices [32] the research on diamond semiconductors in China is gradually increasing. As a subversive material, our country also includes the direction of diamond semiconductors in strategic advanced electronic materials. According to the "Library and Information Service" paper, among the invention patents before December 31, 2020, diamond has a total of 454 patents in the field of power semiconductors, accounting for 5%. [33]

General situation of Patent Distribution of each Branch (Unit: pieces) [33] from the key research and development direction of each technology branch, the research has focused on subtle technical aspects, such as device gate current leakage, short circuit, anti-surge ability, and the number of related research is on a par with gallium oxide (Ga2O3).

Distribution of key R & D directions for third-and fourth-generation semiconductors [33] from 1990 to 1999, there were fewer patent applications in China, and the total number of applications between the United States and Japan reached 53% of the global total. From 2000 to 2009, the number of patent applications in China increased significantly, and from 2010 to 2020, China became the largest applicant. [33]

The main open countries of patent applications in the field of third-generation and fourth-generation power semiconductors [33] at present, China has become an important player of synthetic diamond. According to the incomplete statistics of Henan Business Daily, the domestic single crystal diamond output in 2020 is about 20 billion carats, with an output value of about 5 billion yuan, with an average of 0.3 yuan per carat. You know, in 1965, the price of synthetic diamond was more than 30 yuan per carat. However, the domestic artificial diamond supply is mainly in the fields of abrasive grinding, optics, electrochemical sensors, sewage treatment and so on. The purity and sheet size of these diamonds are not enough to be used in semiconductors. In order to realize the industrialization of diamond semiconductors, a series of processes such as optimizing process and cost and finding killer applications are needed after successful research and development in the laboratory. It is expected that it will take another 10 to 20 years for research and development to make a breakthrough. [34]

Although diamond semiconductors seem to be far away from the semiconductor industry, the semiconductor industry itself is aimed at the frontier field, and the one who enters the industry first can get the dividend brought by technology.

The phrase "A diamond lasts forever" has made De Beers famous to this day, and for diamond semiconductors, it may be necessary to explore forever to create another kind of brilliance.

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This article comes from the official account of Wechat: fruit Shell hard Technology (ID:guokr233), author: Fu Bin, Editor: Li Tuo

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