Method for producing SiC single crystal

Abstract

A method for producing a SiC single crystal, including flowing a high-frequency current at a first frequency to an induction heating coil disposed around a graphite crucible to heat raw material Si to a predetermined temperature, thereby while melting the raw material Si, dissolving out C from said graphite crucible to form a SiC solution, and after heating to the predetermined temperature, lowering the frequency from the first frequency to a second frequency to warm and hold the SiC solution.

Claims

1. A method for producing a SiC single crystal by a solution method of bringing a seed crystal into contact with a Si solution of C to grow a SiC single crystal, the production method of a SiC single crystal comprising: flowing a high-frequency current at a first frequency to a spiral induction heating coil disposed around a graphite crucible to heat raw material Si to a predetermined temperature, thereby while melting said raw material Si, dissolving out C from said graphite crucible to form a SiC solution, and after heating to said predetermined temperature, lowering the frequency from the first frequency to a second frequency, thereby while inducing convection of the SiC solution, warming and holding said SiC solution at the predetermined temperature from 1900 degrees Celsius to 2200 degrees Celsius and maintaining a temperature gradient at a depth of up to 3 centimeters from the SiC solution surface from 10 degrees Celsius per centimeter to 20 degrees Celsius per centimeter, wherein the frequency of the high-frequency current is alternately switched between the first frequency and the second frequency a plurality of times during warming and holding of said SiC solution to obtain a balance between recovery of warming and holding temperature of the SiC solution and maintenance of a C-supersaturated part.

2. The method according to claim 1, wherein said first frequency is from 4 to 6 kHz.

3. The method according to claim 1, wherein said second frequency is from 0.5 to 2 kHz.

4. The method according to claim 2, wherein said second frequency is from 0.5 to 2 kHz.

Description

BRIEF DESCRIPTION OF THE DRAWINGS

(1) FIG. 1 A view illustrating an example of the outline of the apparatus used for carrying out the present invention.

(2) FIG. 2 A view illustrating the frequency switching timing in a first embodiment of the present invention.

(3) FIG. 3 A view illustrating an example of the frequency switching circuit used for carrying out the present invention.

(4) FIG. 4 A view illustrating the frequency switching timing in a second embodiment of the present invention.

MODE FOR CARRYING OUT THE INVENTION

(5) The embodiments of the production method of a SiC single crystal according to the present invention are described below by referring to the drawings. The present invention is not limited to the following embodiments.

(6) FIG. 1 is a view illustrating an example of the outline of the apparatus used for carrying out the present invention.

(7) The SiC single crystal production apparatus 100 comprises a graphite crucible 1, an induction heating coil 2, and a high-frequency power source 6.

(8) The induction heating coil 2 is disposed around the graphite crucible 1. The induction heating coil 2 and the high-frequency power source 6 are connected, and a high-frequency current is flowed to the induction heating coil 2, whereby raw material Si (not illustrated) is heated to a predetermined temperature. By this heating, while melting the raw material Si, C is dissolved out from the graphite crucible 1 to form a SiC solution 3. The SiC solution as used herein means a Si solution of C.

(9) Subsequently, a high-frequency current is flowed to the induction heating coil whereby the SiC solution 3 is warmed and held at the above-described predetermined temperature. A seed crystal 5 is put into contact with this warmed and held SiC solution 3 to grow a SiC single crystal 4.

(10) The predetermined temperature is a temperature in the portion where the temperature is highest inside the graphite crucible 1. The predetermined temperature is not particularly limited as long as it is a temperature at which a SiC single crystal can be grown, but the temperature is preferably from 1,900 to 2,200 C. When the predetermined temperature is 1,900 C. or more, not only the raw material Si is melted but also C can be dissolved out raw material Si is melted but also C cars be dissolved out from the graphite crucible 1 to form a SiC solution 3. On the other hand, when the predetermined temperature is 2,200 C. or less, a temperature gradient from the lower part toward the upper part can be maintained in the vicinity of the SiC solution surface 3a.

(11) The vicinity of the SiC solution surface 3a means a depth of up to 3 cm at the deepest from the SiC solution surface 3a. When a temperature gradient is established to such a depth, a SiC single crystal 4 can be grown starting from the seed crystal 5.

(12) The temperature gradient is preferably from 10 to 20 C./cm. When the temperature gradient is 10 C./cm or more, a SiC single crystal 4 can be grown, and on the other hand, when the temperature gradient is 20 C./cm or less, the convection of the SiC solution 3 is not inhibited.

(13) A stirring force acts on the solution dissolved by high-frequency heating, and a convection exceeding natural convection is generated in the solution by the stirring force. When a high-frequency current is flowed to the induction heating coil 2, an eddy current is generated in a to-be-heated material. The eddy current is larger closer to the surface of the to-be-heated material and smaller closer to the inside. An indicator indicating the degree thereof is the penetration depth. When the frequency of the high-frequency current is high, the penetration depth is shallow and the heating capability is high, but the stirring force is small. On the other hand, when the frequency of the high-frequency current is low, the penetration depth is deep and the heating capability is low, but the stirring force is large.

(14) In other words, the high-frequency current has high heating capability but low capability of cresting convection in a solution when the frequency is high, and has low healing capability but high capability of creating convection in a solution when the frequency is low.

(15) Therefore, in the present invention, the frequency of the high-frequency current flowed to the induction heating coil 2 is switched between when the raw material Si is heated to a predetermined temperature to form a SiC solution 3 by dissolving out C from the graphite crucible 1 while melting the raw material Si and when the SiC solution 3 is warmed and held.

(16) FIG. 2 is a view illustrating the frequency switching timing in a first embodiment of the present invention.

(17) After charging raw material Si into the graphite crucible 1, a high-frequency current is caused to start flowing to the induction heating coil 2. The frequency is a first frequency. The first frequency is not particularly limited as long as it can efficiently heat the raw material Si and is higher than a second frequency. The frequency capable of efficiently heating the raw material Si varies depending on the diameter and depth of the graphite crucible 1, the amount of raw material Si charged, and the spiral pitch of the induction heating coil 2. Accordingly, the first frequency may be appropriately determined by taking into account these factors. The first frequency is preferably from 4 to 6 kHz. When the frequency is 4 kHz or more, the raw material Si can be heated in a short time, and this is efficient. On the other hand, when the frequency is 6 kHz or less, a special high-frequency power source is not needed.

(18) At the point when the SiC solution 3 reaches a predetermined temperature, the frequency of the high-frequency current is decreased to a second frequency from the first frequency. As described above, the predetermined temperature is the temperature in which a SiC single crystal is growing. When the temperature of the SiC solution 3 reached the predetermined temperature, the predetermined temperature need not be raised any more and may be sufficient if the solution can be warmed and held.

(19) On the other hand, in order to form a C-supersaturated part on the SiC solution surface 3a, C dissolved out from the graphite crucible 1 in a high-temperature part at the bottom of the graphite crucible 1 needs to be elevated to the vicinity of the SiC solution surface 3a by generating convention in the SiC solution 3.

(20) More specifically, after the SiC solution 3 reaches the predetermined temperature, the hearing capability is not so required, but the capability of creating convection in the SiC solution 3 is required.

(21) Therefore, in the present invention, the second frequency is specified to be a frequency lower than the first frequency. The high-frequency current at the second frequency may be sufficient if it has heating capability high enough to warm and hold the SiC solution 3 and has capability of sufficiently inducing convection of the SiC solution 3.

(22) The second frequency is not particularly limited as long as it is lower than the first frequency, but the frequency is preferably from 0.3 to 2 kHz. A frequency of 0.5 kHz or more is less likely to lack the warming and holding capability. On the other hand, a frequency of 2 kHz or less is less likely to lack the capability of inducing convection in the SiC solution 3.

(23) Therefore, by switching the frequency of the high-frequency current, a SiC solution 3 can be rapidly formed from the raw material Si with a small power source capacity, and the SiC solution 3 can undergo sufficient convection.

(24) The circuit for switching the frequency of the high-frequency current is not particularly limited as long as switching between desired first frequency and second frequency can be achieved while watching the impedance of a high-frequency current generation source to that of a to-be-heated material.

(25) FIG. 3 is a view illustrating an example or the frequency switching circuit used for carrying out the present invention.

(26) The high-frequency current is generated by an inverter 7. In order to match the impedance of the inverter 7 to that of the raw material Si as a to-be-heated material, a transformer 8 and capacitors 9a and 9b are connected between the induction heating coil 2 and the inverter 7. That is, the transformer 8, the capacitors 9 and 9b, and a selector switch 10 constitute a matching box 11.

(27) In the example illustrated in FIG. 3, capacitors 9a and 9b are connected in parallel. In addition, the selector switch 10 is provided in order to select connecting only the capacitor 9a or connecting both the capacitor 9a and the capacitor 9b.

(28) As for the capacitor, the amount of its capacitance, the quantities of capacitor, and the connection method (in series and/or in parallel) may be appropriately selected according to the selection of the frequency of the first frequency and second frequency, and matching of the impedance of the inverter 7 to that of the raw material Si as a to-be-heated material. The same applies to the selector switch.

(29) At the time of growing a SiC single crystal 4 by warming and holding the SiC solution 3, depending on the growth conditions, the temperature of the warmed and held SiC solution 3 may be lowed. In such a case, the second embodiment described below is effective.

(30) FIG. 4 is a view illustrating the frequency switching timing in a second embodiment of the present invention.

(31) Charging raw material Si into a graphite crucible 1 and then flowing a high-frequency current at a first frequency to an induction heating coil 2 until a SiC solution 3 reaches a predetermined is the same as the first embodiment. In addition, switching the first frequency of the high-frequency current to the second frequency when the SiC solution 3 reaches a predetermined temperature is the same as the first embodiment.

(32) After switching to the second frequency, when the temperature of the SiC solution 3 lowers during warming and holding of the SiC solution 3, the frequency of the high-frequency current is again switched to the first frequency. By this switching, the lowered warming/holding temperature can be recovered to the predetermined temperature by the high-frequency current at the first frequency excellent in the heating capability. However, if the current is continuously kept at the first frequency, the convection of the SiC solution 3 becomes insufficient to reduce the C concentration in the C-supersaturated part. Therefore, the frequency is again switched to the second frequency.

(33) Therefore, as illustrated in FIG. 4, after the temperature of the SiC solution 3 reaches a predetermined temperature, the frequency of the high-frequency current is alternately switched between the first frequency and the second frequency a plurality of times. The time for which the first frequency is selected and the time for which the second frequency is selected may be appropriately determined according to the balance between the recovery of the warming and holding temperature and the maintenance of the C-supersaturated part.

EXAMPLES

(34) Production of a SiC single crystal was performed by setting the first frequency to 5 kHz and the second frequency to 1 kHz.

(35) For the switching of the high-frequency current, the circuit illustrated in FIG. 3 was used. The capacitance of the capacitor 9a was 2 F, the capacitance of the capacitor 9b was 44 F, and the capacitor 9a and the capacitor 9b were connected in parallel.

(36) At the time of switching of the frequency of the high-frequency current to 5 kHz (first frequency), the selector switch 10 was opened to actuate only the capacitor 9a. At the time of switching of the frequency of the high-frequency current to 1 kHz (second frequency), the selector switch 10 was closed to actuate both the capacitor 9a and the capacitor 9b.

(37) As a result, a high-frequency current of 5 kHz flowed in an amount of 120 A to the induction heating coil 2, and a SiC solution 3 at 2,000 C. could be obtained. Thereafter, the frequency of the high-frequency current was switched to 1 kHz, and the solution could be warmed and held at the same temperature as above.

INDUSTRIAL APPLICABILITY

(38) According to the present invention, a production method of a SiC single crystal, in which a SiC solution can undergo sufficient convection without upsizing the production apparatus, can be provided. Hence, there is great industrial applicability in the present invention.

DESCRIPTION OF NUMERICAL REFERENCES

(39) 1 Graphite crucible 2 Induction heating coil 3 SiC Solution 3a SiC Solution surface 4 SiC Single crystal 5 Seed crystal 6 High-frequency power source 7 Inverter 8 Transformer 9a, 9b Capacitor 10 Selector switch 11 Matching box 100 SiC Single crystal production apparatus