FR3055949B1 - THERMAL CONNECTION FOR LUMINOUS MODULE - Google Patents

Abstract

The invention relates in particular to a light module which comprises a light source, a substrate on a first face which rests the light source, a heat sink having a contact surface with a second face of the substrate, said dissipator comprising graphite. The invention improves the assembly and / or disassembly of the light source of the light module.

Description

THERMAL CONNECTION FOR LUMINOUS MODULE

FIELD OF THE INVENTION

The invention relates to the field of terrestrial vehicle light modules, that is to say modules that can be integrated into a light device of the vehicle and, during use of the vehicle, to project light illuminating the vehicle. road or the cockpit and / or allowing the vehicle to make itself more visible. Examples of such luminous devices are the sidelights or the dipped beam and / or road (commonly called "headlights").

BACKGROUND

A land vehicle is equipped with light devices, including lighting and / or signaling, such as headlights or taillights, intended to illuminate the road in front of the vehicle, at night or in case of reduced brightness. They can also be used to illuminate the cabin of the vehicle. These light devices may comprise one or more light modules. Each lighting function can be provided by one or more modules. Moreover, in these light modules of land vehicles, the light sources are more frequently constituted by light emitting diodes or LEDs (acronym for "Light Emitting Diode"), in particular for the advantages of space and duration of light. life compared to conventional light sources.

Light sources, however, generate heat that must be evacuated so that the light source does not deteriorate under the action of heat. This problem is even more important for LED technology because my components generate a lot of heat that causes a rise in temperature in the components that can degrade components and / or prevent optimal use.

Existing solutions for managing this heat rely on the use of a radiator that is in contact with the substrate on which the light source is placed. The heat is transmitted to the radiator which evacuates it outside the light module which includes the light source.

The contact between the light source and the heat sink may include an interface that promotes heat transfer to the heatsink.

The interface may be for example a copper plate which is a conductive material; but this material is expensive and its use complicates the manufacturing process of the light module.

It is also known to use thermal paste as an interface. However, the use of thermal paste complicates the manufacture and maintenance of the light module. First of all, the management of the stocks of thermal paste in the manufacturing process must be taken into account so that the manufacture of a series of light modules does not lead to the need to eliminate an excessive amount of unused thermal paste which does not occur. not keep. In addition, during the manufacture of the light module, it is necessary to carefully deposit a precise quantity of thermal paste. If it is necessary to rework during the manufacturing process, the thermal paste must be removed and a new precise quantity of pulp re-deposited. Similarly, the disassembly and reassembly of the light module is made complex due to the use of thermal paste. Thus, manufacture / repair is elongated, complicated, and / or expensive.

SUMMARY OF THE INVENTION

For this purpose, a light module is proposed comprising a light source, a substrate on a first face of which the light source rests, a heat sink having a contact surface with a second face of the substrate, said dissipator comprising graphite.

According to various embodiments, the light module may comprise one or more of the following characteristics combined with one another:

the heat sink comprises at least one pyrolytic graphite sheet;

the contact surface of the heat sink with the second face of the substrate is equal to the surface of the second face of the substrate;

the graphite of the heat sink forms the contact surface of the heat sink;

the heat sink further comprises one or more finned radiators;

the fins comprise said at least one pyrolytic graphite sheet;

a heat distribution system integrated into the substrate;

the heat distribution system comprises one or more microcaloducts;

means capable of holding said heat sink fixed against the second face of the substrate;

the means comprise at least one of a spring, a leaf spring, a screw;

the light source is an electroluminescent light source;

the electroluminescent light source comprises electroluminescent elements;

the density of electroluminescent elements is equal to or greater than 500 electroluminescent elements per cm ² .

There is also provided a light device, including lighting and / or signaling preferably land vehicle, comprising the light module above.

BRIEF DESCRIPTION OF THE FIGURES

Various embodiments of the invention will now be described, by way of non-limiting examples, with reference to the appended drawings in which:

Figures 1 to 7 show schematically examples of a light module according to the invention;

Figure 8 shows schematically an example of a 3D monolithic electroluminescent light source.

DETAILED DESCRIPTION

A terrestrial vehicle light module is proposed, as well as a light device comprising one or more versions of such a light module. The light device may constitute or be integrated with a light projector. The light device may be a front projector, a rear light or a luminaire for the passenger compartment. There is also provided a land vehicle comprising one or more versions of such a light device (for example one or more pairs of versions at the front and / or one or more pairs of versions at the rear for a four-wheeled vehicle, or one or more versions at the front and / or one or more versions at the rear for a two or three wheel vehicle).

The light module comprises at least one light source. The light source may be a filament, plasma, or gas light source.

The light source may be a solid-state electroluminescent source (solid-state lighting) which includes electroluminescent elements. The electroluminescent elements are located on the same substrate, and preferably on the same face of the substrate, which may for example be sapphire. The electroluminescent elements are deposited on or extending from at least one face of the substrate.

An electroluminescent element may be, but is not limited to, a light emitting diode (LED), an organic light emitting diode (OLED), a polymeric light emitting diode (PLED). The electroluminescent source is therefore a semiconductor light and has a substrate from which the electroluminescent elements are placed. An electroluminescent element is more generally called a pixel. Therefore, the light source comprises a plurality of pixels deposited on or extending from the first face of the substrate. Pixels (i.e., light-emitting elements) emit light when the semiconductor material is supplied with electricity. We can therefore speak of pixel lit when an electroluminescent element emits light.

The electroluminescent light source may be a high-density light source of light elements, that is to say that it comprises a very large number of electroluminescent elements. By very high number, it is meant that the substrate of the light source comprises at least 500 electroluminescent elements on the same substrate. For example, if the pixels are smaller than 100 μm (micrometers) and the pitch is 200 μm, then the pixel density is 2500 electroluminescent elements per square centimeter (cm ² ).

The pixel density is preferably greater than 500 pixels per cm ² . It is typically between 500 and 2500 pixels per cm ² . It is understood that the pixel density of a light source with a high density of light elements may be greater than 2500 pixels per cm ² .

The electroluminescent elements are each semiconductor, that is to say that they each comprise at least one semiconductor material. The electroluminescent elements may be predominantly of semiconductor material. This semiconductor material may be the same as or different from the semiconductor material of the substrate. The electroluminescent elements may more generally all be made in the same material or materials. The electroluminescent elements may be of the same nature, for example substantially identical or similar. All the electroluminescent elements can be positioned to form a regular pattern, for example a grid.

The electroluminescent light source may be a monolithic electroluminescent source, i.e. each electroluminescent element is electrically independent of the others and emits light independently of the other elements of the matrix. Each element of the matrix is individually controlled by an electronic circuit called "driver" in English. The driver manages the power supply of the monolithic matrix, which is to say that it individually manages the power supply of each electroluminescent element. The driver is therefore an electronic device that is able to control the elements of a monolithic matrix of electroluminescent elements. Several drivers can be used to drive the electroluminescent elements of the matrix.

The light module according to the invention also comprises a substrate on which the light source rests. Depending on the type of light source, the substrate may vary.

In a first example, the substrate may be the material on which the electroluminescent elements of the light source have been deposited on or extending. The light source is therefore a solid state source, for example a high density monolithic electroluminescent source. Other examples will be presented in reference to Figures 7 and 8.

The light module rests on a first face of the substrate. The substrate comprises at least two faces that are flat, or substantially planar. The substrate may have, but is not limited to, a parallelepiped shape; for example, the substrate may be a plate.

The light module also comprises at least one heat sink which is associated with the substrate on which the light source rests. The heat sink allows the heat transfer of the substrate (s) on which the light source rests. The light source and the cooperation between the heat sink and the substrate of the said light source thus make it possible to obtain a land vehicle light module that is simple to produce and to mount in a vehicle light device, inducing a relatively small, compact and having a good ability to dissipate heat.

The heat sink allows heat dissipation via cooperation with the substrate, i.e. the heat sink receives the heat produced by the light module and stored in the substrate. The heat sink is thus in heat communication with the substrate. This means that the second face of the substrate transmits the heat present in the substrate to the heat sink. The heat sink can then dissipate this heat at least partially out of the light module.

In one example, the heat sink is arranged against the second face of the substrate. The heat sink therefore has a contact surface with the second face of the substrate. Preferably, the contact surface of the heat sink is flat; the same for the second face of the substrate. The transmission can be ensured by the fact that the heat sink is in an example arranged directly against the substrate. This means that the heat sink is in physical contact (i.e., material) with the substrate. The contact surface of the heat sink with the second face of the substrate may be equal to the surface of the second face of the substrate; this maximizes heat exchanges between the substrate and the heat sink.

The substrate may have a general shape of plate, having two opposite faces. The light source rests on a first face, and the heat sink can then be arranged against the other face of the plate along a contact surface of the heat sink. This makes it possible to optimize the number of thermal interfaces, the space and the space occupied by the heat dissipation, while keeping a compact light module.

The heat sink comprises graphite. Graphite is a mineral species that is a natural allotrope of carbon. The presence of graphite in the heat sink helps to improve the heat transfer of the substrate (s) on which the light source rests.

Figure 1 shows a first example of the light module 10 according to the invention which comprises a light source 12 resting on a substrate 14. The heat sink 18 comprises graphite in the form of a pyrolytic graphite sheet. Pyrolitic graphite is a material obtained after pyrolysis of graphite. It is in the form of a sheet, that is to say that the material is in the form of a thin layer of sufficiently stable and compact material. For example, a pyrolytic graphite sheet may have a submillimeter thickness, for example 0.025 mm (millimeter). A pyrolytic graphite sheet can be flexible and flexible, and thus can accommodate curved surfaces.

In the example of Figure 1, the graphite of the heat sink forms the contact surface of the heat sink 18. In other words, the pyrolytic graphite sheet 16 is arranged against the substrate 14 is played as an intermediate element, with for example a finned radiator 180. The graphite sheet form is particularly suitable for this role of intermediary. Indeed, the sheet has two opposite faces, one arranged directly against the substrate, the other directly against the dissipator.

In the example of Figure 1, the heat sink 18 (16, 180) is held against the substrate using adhesive fixing means 11 (for example epoxy glue) and / or adhesive glue. For example, the pyrolytic graphite sheet 16 may comprise on each of these faces an adhesive: the intermediate element serves to maintain one of the faces of the substrate 14 against the heat sink 18, while promoting the transfer of heat out of the substrate. The intermediate element serves as a bridge of material between the substrate and, for example, a finned radiator 180. In other words, the intermediate element is constituted such that the heat of the substrate is transmitted to the dissipator by a conduction which follows a path along which material is continuously disposed. The path is devoid of any air barrier. Such a thermal bridge allows better conduction than in the presence of an insulating air barrier. This conduction is all the more effective as the intermediate element comprises pyrolytic graphite which promotes the conduction of heat.

In the example of FIG. 2, the means capable of holding the heat sink 18 fixed against the second face of the substrate 14 are not identical to those of FIG. 1. In this example, the fixing means apply a mechanical force to the substrate and the heat sink so that the pyrolytic graphite sheet 16 only plays its role as a heat conduction promoting element. In other words, the pyrolytic graphite sheet 16 does not participate in maintaining the heat sink 18 (16, 180) against the substrate. The assembly or reassembly of the light module is thus facilitated since the intermediate element 16 of the heat sink can be easily placed, removed, replaced, cut to the right dimensions without particular precautions; unlike thermal interfaces that use thermal paste as known in the state of the art.

The means capable of holding the heatsink fixed against the second face of the substrate may be a leaf spring, as illustrated in FIG. 2. A first part is fixed on the radiator, for example by means of an adhesive or else by welding, and a second portion of the spring bears against the substrate: the latter is therefore held against the heat sink. The use of a leaf spring facilitates the manufacture as well as the disassembly / reassembly of the light module. Other fastening means may be envisaged, for example a strapping ring, a blade, or a screw.

In the examples shown in Figures 1 and 2, the surface of the pyrolytic graphite sheet 16 has dimensions greater than the surface of the second face of the substrate. This ensures that the contact surface of the heat sink covers the entire surface of the second face of the substrate; the heat exchanges between the substrate and the heat sink are thus maximized. In addition, this facilitates assembly or reassembly of the light module because less precision is required; this is particularly the case for repair operations, for example when replacing a faulty light source.

Figure 3 shows another example of a light module according to the invention similar to those of Figures 1 and 2. In this example, the pyrolytic graphite sheet has dimensions greater than those of the substrate for at least one of the sides of the substrate so that the sheet overflows the substrate. In particular, the dimensions of the sheet are chosen such that the overflow of the sheet allows a folding of the sheet along folds 160a, 160b. In Figure 3, the dimensions have been chosen so that the graphite sheet overflows on both sides of the substrate, but also the radiator. The overflow is sufficient so that the folded portion of the sheet covers, at least partially, the radiator. There is preferably no contact between the folded portions 180a, 180b and the fins 180. The two folded portions of the pyrolytic graphite sheet act as radiator fins 180a, 180b and contribute to better heat dissipation. of the light source. Thus, the heat sink comprises graphite, for example in the form of at least one pyrolytic graphite sheet, which forms the contact surface of the dissipator with the substrate and which also forms at least one finned radiator of the dissipator.

The means for fixing the substrate with the heat sink are not shown in FIG. 3. They may be similar to those discussed above. In this example, the folds form an angle 40 with the contact surface substantially equal to 90 °. Preferably, the angle is between 0 ° and 90 °.

In the examples of Figures 1 to 3, a single sheet is in contact with the substrate. Other examples may be envisaged in which at least two sheets of graphite are in contact with the substrate, each sheet belonging to a heat sink.

Figure 4 shows another example of a light module according to the invention similar to that of Figure 3, except that the heat sink 18 includes only a finned radiator 180 formed by the contact surface of the graphite heat sink. In this example too, the angle formed is 90 °.

FIG. 5 shows another example of a light module according to the invention similar to that of FIG. 4, and in which the heat sink 18 comprises several graphite sheets 16a, 16b, 16c, 16d, 16e which are superimposed on each other. others, each having two folded parts. Each folded part forms a fin dissipating the heat of the substrate. The sheet 16a is the single sheet in contact with the substrate. It is therefore both the contact surface of the heat sink with the substrate and a finned radiator of the heat sink. The other sheets 16b-16e serve to evacuate the heat and form finned radiators.

The fold zones and / or the angles formed by the folds of each sheet are chosen so that the fins are not in contact in order to increase the air contact area of each fin. In this example, each sheet comprises a central portion delimited by the two fold zones whose length decreases as one moves away from the contact surface with the substrate. In this configuration example, it is possible to nest the sheets into one another. This makes it possible to optimize the number of fins, the space and the bulk of the heat dissipation, while keeping a compact light module. Still in this example the angle formed by each fold is 90 °, and all the fins are parallel to each other.

Figure 6 shows an example similar to that of Figure 5, in which the sheet 16a is not folded. It extends the surface against which it is possible to come attach 16b-16h fin radiators, to increase the amount of heat evacuated.

The examples of FIGS. 5 and 6 comprise only a single sheet of graphite in contact with the substrate. Other examples may be envisaged in which at least two sheets of graphite are in contact with the substrate, forming as many dissipaters as there are sheets in contact with the substrate.

To improve the heat dissipation, the substrate of the light module can integrate a heat distribution system integrated into the substrate. The heat distribution system distributes the heat substantially homogeneously in the portion of the substrate cooperating with the heat sink. Thus, the heat sink's capabilities are fully utilized, and the heat dissipation is optimized. The heat distribution system may have an area equal to or greater than that of the electroluminescent element bearing areas. The heat distribution system may for example comprise microcalorches. This allows a particularly efficient dissipation, particularly in the configuration where the intermediate element comprises one or more electronic control devices.

The heat distribution system may be configured to distribute the heat to the radiator to maximize its efficiency by integrating one or more micro-heat pipes in the substrate structure, for example silicon. The microcaloducts can be formed of capillary networks which make it possible to drain the liquid from the hot zone of the source and the ASIC towards the cold zone. A micro heat pipe can be etched using standard methods of making chips. This cooling means integrated with the light source and the intelligence makes it possible to better control the thermal by spreading the hot spot towards the heat sink.

A micro-heat pipe consists of networks of a few millimeters in which a fluid evaporates and is transported in the vapor phase to the cold zone. Because of the short length (for example less than 20 cm), the capillary effect makes it possible to operate without the aid of gravity.

The inside of the micro-heat pipe may comprise materials having an irregular structure made by powder sintering or grooves. A flat-shaped microcaloduct may be inserted into a preform defined directly in the substrate, or alternatively in a conductive material to allow the spreading of heat. The micro-heat pipe may include parallel grooves filled with fluid.

Figure 7 shows an example of a light module 10 which includes a light emitting source 12 and a PCB 14 which serves as a substrate. The source 12 rests on a first face of the PCB. The light module further comprises a device 19 which controls the electroluminescent elements of the electroluminescent source 12. Any other support that a PCB can be considered. The light module comprises a heat sink 18 which can be arranged directly or indirectly on the source 12. In this example, the heat sink 18 is arranged indirectly on the source since the PCB 14 and a thermal interface 16 of the heat sink 18 are located between the heat sink 18 and the source 12. The thermal interface may be a graphite sheet, for example a pyrolytic graphite sheet. The heat sink allows the transfer of heat from the light emitting source that it transmits to the PCB when using a light module. The heat sink allows heat dissipation through cooperation with the support 14 of the monolithic electroluminescent source, i.e. the heat sink receives the heat produced by the light emitting source.

The module according to the invention may comprise a monolithic electroluminescent source with a high density of electroluminescent elements called the "3D" electroluminescent source, that is to say that the electroluminescent elements are not only deposited on the substrate of the source: they extending from the source substrate. Items can be grouped into one or more sets. Each set consists of several elements extending from a respective portion of the first face of the substrate. The electroluminescent elements can therefore be distributed in different light emission zones. In one example, these different zones can be activatable selectively. The elements may have a general shape of a stick and thus be called "sticks". The electroluminescent elements can be supplied with electricity via the substrate on one side (eg the substrate forming for example the cathode) and via a layer of electrically conductive material which electrically bonds the electroluminescent elements together on the other side (eg the layer of electrically conductive material forming for example the anode). The contact between the semiconductor material of each electroluminescent element and the semiconductor material of the substrate can therefore be adapted to electrical conduction. The layer of electrically conductive material may cover the electroluminescent elements. The layer of electrically conductive material may also cover each surface portion of the substrate from which the electroluminescent elements extend, or an entire surface or face of the substrate from which the sets of electroluminescent elements extend. The layer of electrically conductive material may be electrically isolated from the semiconductor material of the substrate by any means. This makes it possible to supply the electroluminescent elements with electricity via the substrate. Thus, the electroluminescent elements can be supplied with electricity simply, that is to say by feeding the conductive material of the substrate with a polarity and the layer of electrically conductive material with the other polarity.

The "3D" electroluminescent source may be manufactured by a method comprising at least one step of supplying the substrate, then a step of integrally forming the rods with the substrate, by growth from the substrate. The layer of electrically conductive material may be made by a step of removing a metal finish, for example copper to control rods. This step may also include the creation of aluminum or copper pads on one side of the substrate, suitable for wire wiring between the source and the control component. Wiring by wire or "bridging" (also called "wirebonding" or "wire bonding" of English or ribbon bonding ...) is one of the techniques used to make the electrical connections between the electroluminescent source and the device. supply of the source. The wiring is simply made by a wire (or bridge) welded between the two connection pads provided for this purpose on each of the elements. The welding can be performed by ultrasound. The wire material may be aluminum, gold or copper. The diameter of the wire may be of the order of 20 μm. A rectangular section wire can also be used.

Figure 8 shows an example of such a monolithic electroluminescent light source called "3D". The light source S, here shown in section, comprises a substrate 210 from which extend in a preferred direction sticks 211, 212. This substrate 210 is, in this example, silicon, which represents a much lower cost to that of conventional LEDs, in which the substrates are sapphire. The rods 211, 212 may be obtained by crystalline growth on this substrate 210.

The rods 211, 212 are arranged to form rods of electroluminescent semiconductor material. The rods 211, 212 may for example be formed essentially of gallium nitride.

For example, these rods 211, 212, comprise a semiconductor material core capable of being doped with electrons, around which is formed a first layer of semiconductor material capable of having electron deficits, in which case one speaks of sometimes of doped layer in "holes" or in positive charges. At the interface of this soul and this first layer, an intermediate layer is formed where the electrons and the electron deficits are recombined. Thus, each rod 211, 212, is an electroluminescent semiconductor element.

A nucleation layer 219 is formed on the substrate 210 and around the rods 211, 212.

The rods 211, 212 are here at a distance of about 30 μm and each has a height, taken from the nucleation layer 219 to their apex, of 2.5 μm. Their diameter is 1.5 μm.

The light source S thus essentially comprises a substrate 210 forming a plate bristling with a multitude of small rods 211, 212, electroluminescent and submillimetric, namely whose largest dimension is less than one millimeter.

The light source S is divided into several light zones 201, 202 separated by walls 221, corresponding to a distribution of the set of rods 211, 212.

Between each rod 211, 212 of the same zone 201, 202 is deposited an electrically conductive layer, electrically joining these rods, thus forming a separate anode 225, 226, for each of the light areas 201, 202.

The four anodes 225, 226 thus formed are in contact with the nucleation layer 219, which itself is in contact with the cathode formed by the substrate 210.

Thus, by connecting the anodes 225, 226 and the cathode 210 to a power source, each of the different light zones 201, 202 can be independently supplied with electricity.

In one embodiment, each anode is connected to one or more positive terminals of a connection means 220, intended to be connected to the positive terminal of a power source (not shown) of a vehicle. Similarly, the cathode 210 is connected to the negative terminal of the connection means 220. The activation means therefore allows the power supply of each of these light areas 201, 202.

It is therefore possible to control this light source S, by selective activation of its light areas 201, 202, via the activation means 220.

The control can be achieved by a specific means separate from the light device, or else, as in this example realized by a control device 229 integrated in the light device.

In this example, the control is performed directly by a control device 229. The latter is connected on the one hand to the connection means 220 and on the other hand to the connector C. The connection means 220 is connected to each anode 225 , 226, via electrical conductors.

The control device 229 and the light source S are mounted on the same printed circuit board, not shown. The electrical conductors are formed by electronic tracks of this printed circuit board. Likewise, other electronic tracks connect the connection means 220 to the control device 229.

The luminous efficiency of the light zones 201, 202 can be improved by depositing a reflective layer 217, 218, on the nucleation layer 219. This reflecting layer 217, 218, for example, is deposited on the nucleation layer 219 before growth of the rods, then holes are formed in this reflecting layer 217, 218, as well as in the nucleation layer, before growth of the rods 211, 212, 213, 214, on the substrate 10.

To have a better luminous efficiency, the rods of the luminous zones can have the characteristics below:

a diameter of between 1.4 μm and 1.6 μm, for example 1 μm,

a height of between 2 μm and 10 μm, for example 8 μm,

a distance between each rod of between 3 and 10 μm.

The light source S may comprise a light converter 223 arranged above the rods 211, 212. A light converter comprises at least one luminescent material designed to absorb at least a portion of at least one excitation light emitted by a light emitter. light source and for converting at least a portion of said absorbed excitation light into an emission light having a wavelength different from that of the excitation light. The material may for example be YAG doped with cerium or europium.

Still in the example of FIG. 8, the light source comprises is a high density source, that is to say that it comprises a very large number of sets of electroluminescent elements, at least several hundreds of sets of electroluminescent elements. In practice, the source has more than 1000 sets of electroluminescent elements on the same substrate.

Claims (11)

1. Light module comprising: a light source (12); a substrate (14) on a first face of which the light source rests; a heat sink (18) having a contact surface with a second face of the substrate, said dissipator comprising graphite (16), the light source being an electroluminescent light source comprising electroluminescent elements, the density of electroluminescent elements being equal or greater than 500 electroluminescent elements per cm ² . 2. Light module according to claim 1, wherein the heat sink comprises at least one sheet (16) of pyrolytic graphite. 3. Light module according to one of claims 1 to 2, wherein the contact surface of the heat sink with the second face of the substrate is equal to the surface of the second face of the substrate. 4. Light module according to one of claims 1 to 3, wherein the graphite of the heat sink forms the contact surface of the heat sink. 5. The light module according to one of claims 1 to 4, wherein the heat sink further comprises one or more fins radiators (180). The light module of claim 5 combined with claim 2, wherein the fins comprise said at least one pyrolytic graphite sheet. Light module according to one of claims 1 to 6, further comprising a heat distribution system integrated into the substrate. 8. The light module of claim 7, wherein the heat distribution system comprises one or more micro-heat pipes. 9. Light module according to one of claims 1 to 8, further comprising means (11) adapted to maintain said heat sink fixed against the second face of the substrate. 10. The light module of claim 9, wherein the means comprise at least one of a spring, a leaf spring, a screw. 11. Lighting device, especially lighting and / or signaling preferably land vehicle, comprising a light module according to one of claims 1 to 10.