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WO2025014994A1 - Matériaux d'interface thermique comprenant des particules déformables, ensembles de circuits formés à partir de ceux-ci, et leurs procédés de fabrication - Google Patents

Matériaux d'interface thermique comprenant des particules déformables, ensembles de circuits formés à partir de ceux-ci, et leurs procédés de fabrication Download PDF

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Publication number
WO2025014994A1
WO2025014994A1 PCT/US2024/037294 US2024037294W WO2025014994A1 WO 2025014994 A1 WO2025014994 A1 WO 2025014994A1 US 2024037294 W US2024037294 W US 2024037294W WO 2025014994 A1 WO2025014994 A1 WO 2025014994A1
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WIPO (PCT)
Prior art keywords
thermal interface
microns
interface material
deformable particles
liquid metal
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Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
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PCT/US2024/037294
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English (en)
Inventor
Keyton D. Feller
Alicia CHUA
Dylan S. Shah
Hing Jii Mea
Navid Kazem
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Arieca Inc
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Arieca Inc
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Publication of WO2025014994A1 publication Critical patent/WO2025014994A1/fr
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L23/00—Details of semiconductor or other solid state devices
    • H01L23/34—Arrangements for cooling, heating, ventilating or temperature compensation ; Temperature sensing arrangements
    • H01L23/36—Selection of materials, or shaping, to facilitate cooling or heating, e.g. heatsinks
    • H01L23/373—Cooling facilitated by selection of materials for the device or materials for thermal expansion adaptation, e.g. carbon
    • H01L23/3737—Organic materials with or without a thermoconductive filler
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
    • C09K5/00—Heat-transfer, heat-exchange or heat-storage materials, e.g. refrigerants; Materials for the production of heat or cold by chemical reactions other than by combustion
    • C09K5/08—Materials not undergoing a change of physical state when used
    • C09K5/14—Solid materials, e.g. powdery or granular
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L23/00—Details of semiconductor or other solid state devices
    • H01L23/34—Arrangements for cooling, heating, ventilating or temperature compensation ; Temperature sensing arrangements
    • H01L23/36—Selection of materials, or shaping, to facilitate cooling or heating, e.g. heatsinks
    • H01L23/373—Cooling facilitated by selection of materials for the device or materials for thermal expansion adaptation, e.g. carbon
    • H01L23/3736—Metallic materials

Definitions

  • the present disclosure relates to thermal interface materials comprising deformable particles, circuit assemblies formed therefrom, and methods of manufacture thereof.
  • a thermal interface material can be used to thermally connect two or more layers together.
  • TIMs are often used in CPU packages to thermally connect the integrated heat spreader (IHS) of a CPU package to a heat sink.
  • IHS integrated heat spreader
  • current TIMs present challenges.
  • the present disclosure is directed to a thermal interface material comprising a polymer component, liquid metal droplets dispersed throughout the polymer component, and deformable particles dispersed through the polymer component.
  • the deformable particles exhibit a storage modulus that decreases by at least half responsive to at least one softening event applied to the deformable particles.
  • the softening event is selected from the group consisting of a temperature of at least 30 degrees Celsius and a pressure of at least 20 kPA.
  • the deformable particles can comprise a D90 in a range of 1 micron to 300 microns and/or a polymer, a metal, a metal alloy, or a combination thereof.
  • the thermal interface material comprises 5% to 80% of the polymer component based on a total volume of the thermal interface material, 20% to 95% of the liquid metal droplets based on the total volume of the thermal interface material, and 0.05% to 25% of the deformable particles based on the total volume of the thermal interface material.
  • the liquid metal droplets can comprise a melting point no greater than 30 degrees Celsius, a D90 in a range of 1 micron to 300 microns, and/or at least one of gallium, a gallium alloy, indium, an indium alloy, tin, a tin alloy, mercury, and a mercury alloy.
  • the thermal interface material comprises an additional component, such as, for example, at least one of a catalyst, rigid particles, a coupling agent, and fumed silica.
  • the present disclosure is directed to an assembly comprising a first layer, a second layer, and the thermal interface material according to the present disclosure compressed and disposed in contact with and between the first layer and the second layer.
  • a bondline thickness formed between the first layer and the second layer is less than a D90 of the liquid metal droplets and a D90 of the deformable particles prior to compression of the thermal interface material in the assembly.
  • the present disclosure is directed to a method comprising applying the thermal interface material according to the present disclosure on a first layer of an assembly at a first thickness.
  • the method comprises subjecting the thermal interface material to a softening event and compressing the assembly to decrease the first thickness to a second thickness.
  • the second thickness is no greater than a D90 of the liquid metal droplets and the deformable particles in the thermal interface material prior to compressing the assembly.
  • the present disclosure is directed to a method of manufacture of a thermal interface material.
  • the method comprises mixing a polymer component, a liquid metal, and deformable particles together, thereby forming liquid metal droplets from the liquid metal and dispersing the liquid metal droplets and the deformable particles throughout the polymer component.
  • the deformable particles exhibit a storage modulus that decreases by at least half responsive to at least one softening event applied to the deformable particles.
  • the softening event selected from the group consisting of a temperature of at least 30 degrees Celsius and a pressure of at least 20 kPa.
  • the present invention can provide both a low contact resistance at the material interfaces and a low thermal resistance through the TIM.
  • the low contact resistance can be enabled by the application of the polymer in a conformable state, so that the polymer and liquid metal droplets can adapt to the surface of the layer to achieve a desired contact resistance.
  • the low thermal resistance through the TIM can be enabled by the liquid metal droplets', including the size and/or shape of the liquid metal droplets. Additionally, the TIM and methods described herein can enable enhanced control of manufacturing of assemblies comprising the TIM, thereby enhancing the effective thermal conductivity of the TIM in the assemblies.
  • FIG. l is a perspective view of an assembly according to the present disclosure after deposition of the thermal interface material.
  • FIG. 2 is a side view of an assembly formed by compressing the first and second layer of FIG. 1.
  • Pressure values as used herein refer to gauge pressure unless stated otherwise.
  • a thermal interface material that is applied to a circuit assembly between an integrated heat spreader (IHS) and a heat sink can require balancing the thermal resistance through the TIM and the contact resistance at the material interfaces.
  • a polymeric material may have a low contact resistance at the material interfaces but a high thermal resistance through the material.
  • a solid metal may have a low thermal resistance through the material but a high contact resistance at the material interfaces.
  • the present inventors determined that the speed at which the TIM is compressed can affect the effective thermal conductivity through the TIM in the circuit assembly. In various examples, the speed of compression of the TIM may not be directly controlled by manufacturing equipment. Alternatively, the temperature of the assembly and/or pressure applied during compression may be controlled.
  • a TIM comprising a polymer component, liquid metal droplets dispersed throughout the polymer component, and deformable particles dispersed through the polymer component.
  • the deformable particles exhibit a storage modulus that decreases by at least half responsive to at least one softening event applied to the deformable particles.
  • the softening event selected from the group consisting of a temperature of at least 30 degrees Celsius and a pressure of at least 20 kPa.
  • the deformable particles can be configured to control the speed at which the TIM can be compressed based on the temperature during the compression and/or pressure applied during compression.
  • the thermal interface material according to the present disclosure can achieve a desired distribution of the liquid metal droplets on the circuit assembly, a desired stability of the liquid metal droplet and polymer component emulsion within the TIM, a desired shape of the liquid metal droplets on the circuit assembly, spatial uniformity of the liquid metal droplets packing within the TIM between layers, and/or an enhanced effective thermal conductivity.
  • the terms “on,” “onto,” “over,” and variants thereof mean applied, formed, deposited, provided, or otherwise located over a surface of a substrate but not necessarily in contact with the surface of the substrate.
  • a TIM “deposited on” a substrate or “deposited between” two elements does not preclude the presence of another layer or other layers of the same or different composition located between the applied TIM and the substrate or layers.
  • a second layer “deposited on” a first layer does not preclude the presence of another layer or other layers of the same or different composition located between the deposited second layer and the deposited TIM.
  • polymer and “polymeric” means prepolymers, oligomers, and both homopolymers and copolymers.
  • prepolymer means a polymer precursor capable of further reactions or polymerization by a reactive group or reactive groups to form a higher molecular mass and/or cross-linked state.
  • the polymer component can comprise a polymeric binder, a thermosetting polymer, and/or a thermoplastic polymer.
  • thermosetting refers to polymers that “set” irreversibly upon curing or cross-linking, where the polymer chains of the polymeric components are joined together by covalent bonds, which is often induced, for example, by heat or radiation.
  • curing or a cross-linking reaction can be carried out under ambient conditions. Once cured or cross-linked, a thermosetting polymer may not flow upon the application of heat, may otherwise irreversibly increase in viscosity, and/or can be insoluble in conventional solvents.
  • thermoplastic refers to polymers that include polymeric components in which the constituent polymer chains are not joined (e.g., crosslinked) by covalent bonds and thereby can undergo liquid flow upon heating and are soluble in conventional solvents.
  • the polymer can be elastomeric (e.g., rubbery, soft, stretchy), or rigid (e.g., glassy)
  • the polymer component can be elastomeric and may have a ultimate tensile strain of at least 100%, such as, for example at least 200% or at least 300%. Ultimate tensile strain can be measured according to ASTM D3039.
  • Thermosetting polymers may include at least one of a cross-linking agent that may comprise, for example, aminoplasts, polyisocyanates (including blocked isocyanates), polyepoxides, beta-hydroxyalkylamides, polyacids, anhydrides, organometallic acidfunctional materials, polyamines, polyvinyls, polysilicon hydrides, polyalcohols, polyacid chlorides, polyhalides, and polyamides.
  • a polymer may have functional groups that are reactive with the cross-linking agent.
  • the polymer component in the TIMs described herein may be selected from any of a variety of polymers well known in the art.
  • the thermosetting polymer may comprise at least one of an acrylic polymer (e.g., an acrylate polymer), a vinyl polymer, a polyester polymer, a polyurethane polymer, polybutadiene, a polyamide polymer, a polyether polymer, a polysiloxane polymer (e.g., poly(dimethylsiloxone)), a silicon hydride polymer, a fluoropolymer, a polyisoprene polymer (e.g., rubber), and a copolymer of two or more thereof.
  • an acrylic polymer e.g., an acrylate polymer
  • vinyl polymer e.g., a vinyl polymer
  • a polyester polymer e.g., a polyester polymer, a polyurethane polymer, polybutadiene, a polyamide polymer, a
  • the functional groups on a thermosetting polymer may be selected from any of a variety of reactive functional groups, including, for example, at least one of a carboxylic acid group, an amine group, an epoxide group, a hydroxyl group, a thiol group, a carbamate group, an amide group, a urea group, an isocyanate groups (including a blocked isocyanate group), a vinyl group, a silicon hydride group, an acid chloride group, an acrylate group, a halide group, and a mercaptan group.
  • the thermoplastic polymer can comprise at least one of propylene-ethylene copolymer, styrene-butadiene- styrene, and styrene ethylene butylene styrene.
  • the polymer can comprise a melting point of at least 100 degrees Celsius, such as, for example, at least 120 degrees Celsius, at least 150 degrees Celsius, or at least 200 degrees Celsius.
  • the polymeric binder can be a polyether binder.
  • the polymer component can comprise 0.1% by to 0.5% by weight of a coupling agent based on a total weight of the polymer component.
  • the coupling agent can comprise at least one of 3-Glycidoxypropyltrimethoxysilane, 3- Glycidoxypropyltriethoxysilane, 3 -Aminopropyltrimethoxy silane, and Bis(3- trimethoxysilylpropyl)amine.
  • the polymer component can comprise 0.1% by weight to 5% by weight of a fumed silica based on a total weight of the polymer component.
  • the TIM can comprise at least 5% polymer component by total volume of the TIM, such as, for example, at least 7% polymer component, at least 10% polymer component, at least 15% polymer component, at least 20% polymer component, at least 25% polymer component, at least 30% polymer component, at least 40% polymer component, at least 50% polymer component, or at least 60% polymer component, all based on the total volume of the TIM.
  • the TIM can comprise no greater than 80% polymer component by total volume of the TIM, such as, for example, no greater than 70% polymer component, no greater than 60% polymer component, no greater than 50% polymer component, no greater than 40% polymer component, no greater than 30% polymer component, no greater than 25% polymer component, no greater than 20% polymer component, no greater than 15% polymer component, or no greater than 10% polymer component, all based on the total volume of the TIM.
  • the TIM can comprise a range of 5% to 80% polymer component by total volume of the TIM, such as, for example, 5% to 70% polymer component, 5% to 60% polymer component, 5% to 50% polymer component, 5% to 40% polymer component, 5% to 30% polymer component, 7% to 30% polymer component, 10% to 30% polymer component, 5% to 25% polymer component, or 5% to 20% polymer component, all based on the total volume of the TIM.
  • the amount of the polymer component can be selected while balancing a desired elasticity, adhesiveness, and a desired effective thermal conductivity of the TIM.
  • the polymer component comprises a thermoset
  • the polymer component prior to installation of the TIM on a substrate, at room temperature (e.g., 21 degrees Celsius +/- 2 degrees Celsius)
  • the polymer component may be uncured, liquid, or otherwise flowable and the deformable particles can be solid or semi-solid.
  • the polymer component may have a viscosity at room temperature of no greater than 850,000 cP.
  • the polymer component may have a glass transition temperature, a crystal melting temperature, a thermo-reversible crosslinking temperature, a yield stress, and/or a degradation temperature that is less than a glass transition temperature, a crystal melting temperature, a thermo-reversible crosslinking temperature, and/or a degradation temperature of the deformable particles, such as, for example, at least 10 degrees Celsius less, at least 15 degrees Celsius less, at least 20 degrees Celsius less, at least 30 degrees Celsius less, or at least 50 degrees Celsius less.
  • the polymer component prior to installation of the TIM on a substrate, may have yield stress that is less than a yield stress of the deformable particles, such as, for example, at least 10 kPaless, at least 20 kPa less, at least 50 kPa less, at least 70 kPa less, or at least 100 kPa less.
  • the polymer component can exhibit a storage modulus that is less than a storage modulus of the deformable particles.
  • the storage modulus of the polymer component can be no greater than 1 kPa at room temperature prior to curing.
  • the liquid metal droplets for the TIM can comprise at least one of gallium, a gallium alloy, indium, an indium alloy, tin, a tin alloy, mercury, and a mercury alloy.
  • the liquid metal droplets can comprise a melting point of no greater than 30 degrees Celsius, such as, for example, no greater than 25 degrees Celsius, no greater than 20 degrees Celsius, no greater than 15 degrees Celsius, no greater than 10 degrees Celsius, no greater than 5 degrees Celsius, no greater than 0 degrees Celsius, or no greater than -10 degrees Celsius.
  • the liquid metal droplets can comprise a melting point of at least -40 degrees Celsius, such as, for example, at least -20 degrees Celsius, at least -19 degrees Celsius, at least -10 degrees Celsius, at least 0 degrees Celsius, at least 5 degrees Celsius, at least 10 degrees Celsius, at least 15 degrees Celsius, at least 20 degrees Celsius, or at least 25 degrees Celsius.
  • the liquid metal droplets can comprise a melting point in a range of -40 degrees Celsius to 30 degrees Celsius, such as, for example, -20 degrees Celsius to 30 degrees Celsius, -19 degrees Celsius to 30 degrees Celsius, or -19 degrees Celsius to 25 degrees Celsius.
  • the determination of the melting point can be made at a pressure of 1 atmosphere absolute.
  • the TIM can comprise Gallium Indium Tin (Galinstan) and a melting point of -19 degrees Celsius.
  • the TIM can comprise at least 20% liquid metal droplets by total volume of the TIM, such as, for example, at least 20% liquid metal droplets, at least 25% liquid metal droplets, at least 30% liquid metal droplets, at least 40% liquid metal droplets, at least 50% liquid metal droplets, at least 60% liquid metal droplets, at least 70% liquid metal droplets, at least 80% liquid metal droplets, or at least 90% liquid metal droplets, all based on the total volume of the TIM.
  • the TIM can comprise no greater than 95% liquid metal droplets by total volume of the TIM, such as, for example, no greater than 93% liquid metal droplets, no greater than 90% liquid metal droplets, no greater than 80% liquid metal droplets, no greater than 70% liquid metal droplets, no greater than 60% liquid metal droplets, no greater than 50% liquid metal droplets, no greater than 40% liquid metal droplets, no greater than 30% liquid metal droplets, or no greater than 20% liquid metal droplets, all based on the total volume of the TIM.
  • the TIM can comprise a range of 20% to 95% liquid metal droplets by total volume of the TIM, such as, for example, 20% to 93% liquid metal droplets, 40% to 95% liquid metal droplets, 50% to 95% liquid metal droplets, 50% to 93% liquid metal droplets, 60% to 93% liquid metal droplets, 70% to 95% liquid metal droplets, or 70% to 93% liquid metal droplets, all based on the total volume of the TIM.
  • the amount of liquid metal droplets can be selected while balancing a desired elasticity and a desired effective thermal conductivity of the TIM.
  • the composition and/or mixing techniques can be selected to achieve a desired Dso and/or D90 of the liquid metal droplets in the TIM prior to compressing.
  • the D50 of the liquid metal droplets can be at least 1 micron prior to compressing, such as, for example, at least 5 microns, at least 10 microns, at least 15 microns, at least 20 microns, at least 30 microns, at least 35 microns, at least 40 microns, at least 50 microns, at least 60 microns, at least 70 microns, at least 80 microns, at least 90 microns, at least 100 microns, at least 120 microns, at least 150 microns, or at least 200 microns, all prior to compressing.
  • the D50 of the liquid metal droplets can be no greater than 300 micron, such as, for example, no greater than 250 microns, no greater than 200 microns, no greater than 150 microns, no greater than 120 microns, no greater than 100 microns, no greater than 90 microns, no greater than 80 microns, no greater than 70 microns, no greater than 60 microns, no greater than 50 microns, no greater than 40 microns, no greater than 35 microns, no greater than 30 microns, no greater than 20 microns, no greater than 10 microns, or no greater than 5 microns, all prior to compressing.
  • the D50 of the liquid metal droplets can be in a range of 1 microns to 300 microns, such as, for example, 5 microns to 300 microns, 150 microns to 250 microns, 5 microns to 150 microns, 15 to 150 microns, 35 microns to 150 microns, 35 microns to 70 microns, or 5 microns to 100 microns, all measured prior to compressing.
  • D x can be measured using microscopy (e.g., optical microscopy or electron microscopy).
  • the size can be the diameter of spherical particles or the length along the largest dimension of ellipsoidal or otherwise irregularly shaped particles.
  • Dx of particles refers to the diameter at which X% of the particles have a smaller diameter.
  • the D90 of the liquid metal droplets can be at least 1 micron, such as, for example, at least 5 microns, at least 10 microns, at least 15 microns, at least 20 microns, at least 30 microns, at least 35 microns, at least 40 microns, at least 50 microns, at least 60 microns, at least 70 microns, at least 80 microns, at least 90 microns, at least 100 microns, at least 120 microns, at least 150 microns, or at least 200 microns, all prior to compressing.
  • the D90 of the liquid metal droplets can be no greater than 300 micron, such as, for example, no greater than 250 microns, no greater than 200 microns, no greater than 150 microns, no greater than 120 microns, no greater than 100 microns, no greater than 90 microns, no greater than 80 microns, no greater than 70 microns, or no greater than 50 microns, all prior to compressing.
  • the D90 of the liquid metal droplets can be in a range of 1 microns to 300 microns, such as, for example, 5 microns to 300 microns, 150 microns to 250 microns, 10 microns to 200 microns, 15 to 150 microns, 35 microns to 150 microns, 35 microns to 120 microns, or 50 microns to 100 microns, all measured prior to compressing.
  • the deformable particles can comprise a polymer, a metal, a metal alloy, or a combination thereof.
  • the polymer can comprise a thermoset and/or a thermoplastic as described herein.
  • the thermoset polymer may already be cured.
  • the deformable particles can comprise polyethylene (e.g., semicrystalline polyethylene), polymethyl methacrylate (PMMA) (e.g., amorphous PMMA), polyethylene glycol, polypropylene glycol, polyurethane, polystyrene, polyamide, polyolefin rubber (e.g., polybutadiene, polystyrene, polyisoprene, ethylene propylene diene terpolymer) and/or polysiloxane rubber.
  • PMMA polymethyl methacrylate
  • polyethylene glycol polypropylene glycol
  • polyurethane polystyrene
  • polyamide polyurethane
  • polystyrene polyamide
  • polyolefin rubber e.g., polybutadiene, polystyrene, polyisoprene, ethylene propylene diene terpolymer
  • polysiloxane rubber e.g., polysiloxane rubber
  • the metal or metal alloy can comprise at least one of tin, a tin alloy, silver, a silver alloy, copper, a copper alloy, gallium, a gallium alloy, indium, an indium alloy, lead, a lead alloy, bismuth, a bismuth alloy, a zinc alloy, antimony, and an antimony alloy.
  • the deformable particles can comprise an elasto-plastic filler. The deformable particles may be electrically and/or thermally conductive, or may not be electrically and/or thermally conductive.
  • the deformable particles can exhibit a storage modulus and that storage modulus decreases by half responsive to a softening event applied to the deformable particles. For example, if X is the storage modulus of the deformable particles prior to the softening event, then the storage modulus is less than or equal to 0.5*X after the softening event.
  • the deformable particles comprise a storage modulus in a range of 0.1 MPa to 50 GPa at room temperature.
  • the deformable particles comprise a storage modulus in a range of 0.1 to 100 MPa at a temperature 20 degrees Celsius greater than a glass transition temperature, a crystal melting temperature, a thermo-reversible crosslinking temperature, and/or a degradation temperature of the deformable particles.
  • the storage modulus (G 1 ) can be measured by a parallel plate (40mm) rheometer at 25 degrees Celsius, a frequency of 10 radians per second, and a strain of 5% for a storage modulus of less than 10 kPa.
  • the storage modulus can be measured according to ASTM D413 for rubbers, ASTM D638 for plastics, and ASTM E8 for metals.
  • the storage modulus of the deformable spacers is greater than a storage modulus of the liquid metal droplets at the softening event.
  • the softening event can comprise at least one stimulus selected from the group consisting of a temperature of at least 30 degrees Celsius and a pressure of at least 20 kPa.
  • the softening event can comprise heating the TIM to a temperature of at least 30 degrees Celsius, such as, for example, at least 35 degrees Celsius, at least 40 degrees Celsius, at least 50 degrees Celsius, at least 60 degrees Celsius, at least 70 degrees Celsius, at least 80 degrees Celsius, at least 90 degrees Celsius, at least 100 degrees Celsius, at least 110 degrees Celsius, at least 120 degrees Celsius, or at least 150 degrees Celsius.
  • the softening event can comprise heating the TIM to a temperature no greater than 250 degrees Celsius, such as, for example, no greater than 225 degrees Celsius, no greater than 200 degrees Celsius, no greater than 175 degrees Celsius, no greater than 150 degrees Celsius, no greater than 100 degrees Celsius, no greater than 90 degrees Celsius, or no greater than 80 degrees Celsius.
  • the softening event can comprise heating the TIM to a temperature in a range of 30 degrees Celsius to 250 degrees Celsius, such as, for example, 35 degrees Celsius to 200 degrees Celsius, 40 degrees Celsius to 175 degrees Celsius, 50 degrees Celsius to 175 degrees Celsius, or 80 degrees Celsius to 150 degrees Celsius.
  • the softening event can comprise compressing the TIM with a pressure of at least 20 kilopascals (kPa), such as, for example, at least 35 kPa, at least 50 kPa, at least 70 kPa, at least 100 kPa, at least 200 kPa, at least 250 kPa, at least 300 kPa, at least 400 kPa, at least 1 MPa, at least 2 MPa, or at least 4 MPa.
  • kPa kilopascals
  • the softening event can comprise compressing the TIM with a pressure of no greater than 10 MPa, such as, for example, no greater than 5 MPa, no greater than 4 MPa, no greater than 2 MPa, no greater than 1 MPa, no greater than 500 kPa, no greater than 400 kPa, no greater than 350 kPa, no greater than 300 kPa, no greater than 250 kPa, no greater than 200 kPa, or no greater than 150 kPa.
  • 10 MPa such as, for example, no greater than 5 MPa, no greater than 4 MPa, no greater than 2 MPa, no greater than 1 MPa, no greater than 500 kPa, no greater than 400 kPa, no greater than 350 kPa, no greater than 300 kPa, no greater than 250 kPa, no greater than 200 kPa, or no greater than 150 kPa.
  • the softening event can comprise compressing the TIM with a pressure in a range of 20 kPa to 10 MPa, such as, for example, 20 kPa to 5 MPa, 35 kPa to 2 MPa, 20 kPa to 500 kPa, 50 kPa to 400 kPa, 70 kPa to 350 kPa, or 70 kPa to 200 kPa.
  • the softening event can be related to at least one property of the deformable particles, such as, for example, a glass transition temperature, a crystal melting temperature, a thermo-reversible crosslinking temperature, a yield stress, and a degradation temperature.
  • the deformable particles can comprise a glass transition temperature, a crystal melting point, and/or a reversible crosslinking temperature, of at least 30 degrees Celsius, such as, for example, at least 40 degrees Celsius, at least 50 degrees Celsius, at least 60 degrees, at least 70 degrees Celsius, at least 80 degrees Celsius, at least 90 degrees Celsius, at least 100 degrees Celsius, at least 110 degrees Celsius, at least 120 degrees Celsius, or at least 150 degrees Celsius.
  • the deformable particles can comprise a glass transition temperature, a crystal melting point, and/or a reversible crosslinking temperature of no greater than 250 degrees Celsius, such as, for example, no greater than 225 degrees Celsius, no greater than 200 degrees Celsius, no greater than 175 degrees Celsius, no greater than 150 degrees Celsius, no greater than 100 degrees Celsius, no greater than 90 degrees Celsius, or no greater than 80 degrees Celsius.
  • the deformable particles can comprise a glass transition temperature, a crystal melting point, and/or a reversible crosslinking temperature in a range of 30 degrees Celsius to 250 degrees Celsius, such as, for example, 35 degrees Celsius to 200 degrees Celsius, 40 degrees Celsius to 175 degrees Celsius, 50 degrees Celsius to 175 degrees Celsius, 80 degrees Celsius to 250 degrees Celsius, 100 degrees Celsius to 250 degrees Celsius, or 80 degrees Celsius to 150 degrees Celsius.
  • the deformable particles comprise PMMA
  • the deformable spacer may comprise a degradation temperature of 90 degrees Celsius and the softening event may be a temperature of at least 90 degrees Celsius.
  • the deformable spacer may comprise a glass transition temperature of 65 degrees Celsius and the softening event may be a temperature of at least 65 degrees Celsius.
  • the deformable spacer may comprise a crystal melting temperature of 120 degrees Celsius and the softening event may be a temperature of at least 120 degrees Celsius.
  • the deformable particles comprise a maleimide with furan crosslinking
  • the deformable spacer may comprise a thermo-reversible crosslinking temperature of 110 degrees Celsius and the softening event may be a temperature of at least 110 degrees Celsius.
  • the deformable particles comprise polyurethane
  • the deformable spacer may comprise a yield stress of 15 MPa and the softening event may be a pressure of at least 205 kPa.
  • the melting point of the deformable particles can be at least 10 degrees Celsius greater than the melting point of the liquid metal droplets, such as, for example, at least 15 degrees Celsius, at least 20 degrees Celsius, at least 30 degrees Celsius, at least 40 degrees Celsius, at least 50 degrees Celsius, at least 60 degrees Celsius, at least 70 degrees Celsius, or at least 100 degrees Celsius greater than the melting point of liquid metal droplets.
  • the Dso of the deformable particles can be at least 1 micron prior to compressing, such as, for example, at least 5 microns, at least 10 microns, at least 15 microns, at least 20 microns, at least 30 microns, at least 35 microns, at least 40 microns, at least 50 microns, at least 60 microns, at least 70 microns, at least 80 microns, at least 90 microns, at least 100 microns, at least 120 microns, at least 150 microns, or at least 200 microns, all prior to compressing.
  • at least 5 microns at least 10 microns, at least 15 microns, at least 20 microns, at least 30 microns, at least 35 microns, at least 40 microns, at least 50 microns, at least 60 microns, at least 70 microns, at least 80 microns, at least 90 microns, at least 100 microns, at least 120 microns, at least 150 microns, or
  • the D50 of the deformable particles can be no greater than 300 micron, such as, for example, no greater than 250 microns, no greater than 200 microns, no greater than 150 microns, no greater than 120 microns, no greater than 100 microns, no greater than 90 microns, no greater than 80 microns, no greater than 70 microns, no greater than 60 microns, no greater than 50 microns, no greater than 40 microns, no greater than 35 microns, no greater than 30 microns, no greater than 20 microns, no greater than 10 microns, or no greater than 5 microns, all prior to compressing.
  • the D50 of the deformable particles can be in a range of 1 microns to 300 microns, such as, for example, 5 microns to 300 microns, 150 microns to 250 microns, 5 microns to 150 microns, 15 to 150 microns, 35 microns to 150 microns, 35 microns to 70 microns, or 5 microns to 100 microns, all measured prior to compressing.
  • the D90 of the deformable particles can be at least 1 micron, such as, for example, at least 5 microns, at least 10 microns, at least 15 microns, at least 20 microns, at least 30 microns, at least 35 microns, at least 40 microns, at least 50 microns, at least 60 microns, at least 70 microns, at least 80 microns, at least 90 microns, at least 100 microns, at least 120 microns, at least 150 microns, or at least 200 microns, all prior to compressing.
  • the D90 of the deformable particles can be no greater than 300 micron, such as, for example, no greater than 250 microns, no greater than 200 microns, no greater than 150 microns, no greater than 120 microns, no greater than 100 microns, no greater than 90 microns, no greater than 80 microns, no greater than 70 microns, or no greater than 50 microns, all prior to compressing.
  • the D90 of the deformable particles can be in a range of 1 microns to 300 microns, such as, for example, 5 microns to 300 microns, 150 microns to 250 microns, 10 microns to 200 microns, 15 to 150 microns, 35 microns to 150 microns, 35 microns to 120 microns, or 50 microns to 100 microns, all measured prior to compressing.
  • the TIM can comprise at least 0.05% deformable particles by total volume of the TIM, such as, for example, at least 0.1% deformable particles, at least 0.2% deformable particles, at least 0.3% deformable particles, at least 0.4% deformable particles, at least 0.5% deformable particles, at least 1% deformable particles, at least 2% deformable particles, at least 5% deformable particles, or at least 10% deformable particles, all based on the total volume of the TIM.
  • the TIM can comprise no greater than 25% deformable particles by total volume of the TIM, such as, for example, no greater than 20% deformable particles, no greater than 15% deformable particles, no greater than 10% deformable particles, no greater than 5% deformable particles, no greater than 3% deformable particles, no greater than 2% deformable particles, no greater than 1% deformable particles, or no greater than 0.9% deformable particles, all based on the total volume of the TIM.
  • the TIM can comprise a range of 0.05% to 25% deformable particles by total volume of the TIM, such as, for example, 0.1% to 20% deformable particles, 0.1% to 10% deformable particles, 0.1% to 5% deformable particles, 0.1% to 2% deformable particles, 0.2% to 2% deformable particles, 0.1% to 1% deformable particles, 0.2% to 1% deformable particles, or 0.2% to 0.9% deformable particles, all based on the total volume of the TIM.
  • the amount of the deformable particles can be selected while balancing a desired effective thermal conductivity of the TIM and a desired rate of compression of the TIM.
  • the TIM can optionally comprise other components such as, for example, rigid particles, a catalyst, fumed silica, and a coupling agent.
  • the rigid particles can comprise at least one of iron, an iron alloy (e.g., steel), vanadium, a vanadium alloy, niobium, a niobium alloy, titanium, a titanium alloy, copper, a copper alloy (e.g., bronze), a rigid polymer, a glass, and a ceramic.
  • the rigid particles can be resistant to deformation and/or corrosion by the liquid metal droplets.
  • the rigid particles can comprise a Young’s modulus of at least 100 MPa (megapascals), such as, for example, at least 110 MPa, at least 150 MPa, at least 200 MPa, at least 250 MPa, at least 500 MPa, at least 750 MPa, at least 1 GPa (gigapascals), or at least 2 GPa. Young’s Modulus can be measured according to ASTM El 11-17.
  • the TIM can comprise a range of 0.1% to 30% rigid particles by total volume of the TIM, such as, for example, 0.1% to 10% rigid particles, 0.1% to 5% rigid particles, 1% to 10% rigid particles, or 1% to 5% rigid particles, all based on the total volume of the TIM.
  • the D90 and/or D50 of the rigid particles in the TIM can be selected to achieve a desired bondline thickness in the assembly.
  • the D90 of the rigid particles can be at least 1 micron, such as, for example, at least 5 microns, at least 10 microns, at least 20 microns, at least 30 microns, at least 35 microns, at least 40 microns, at least 50 microns, at least 60 microns, at least 70 microns, at least 80 microns, at least 90 microns, at least 100 microns, at least 120 microns, or at least 125 microns.
  • the D90 of the rigid particles can be no greater than 150 microns, such as, for example, no greater than 125 microns, no greater than 120 microns, no greater than 100 microns, no greater than 90 microns, no greater than 80 microns, no greater than 70 microns, no greater than 60 microns, no greater than 50 microns, no greater than 40 microns, no greater than 35 microns, no greater than 30 microns, no greater than 20 microns, no greater than 10 microns, or no greater than 5 microns.
  • the D90 of the rigid particles can be in a range of 1 microns to 150 microns, such as, for example, 15 to 150 microns, 5 microns to 125 microns, 35 microns to 125 microns, 35 microns to 70 microns, or 50 microns to 70 microns.
  • the D90 of the rigid particles can be less than the D90 of the liquid metal droplets and/or the D90 of the deformable particles.
  • the D90 of the rigid particles can be at least 10% less than the D90 of the deformable particles, such as, for example, at least 15% less, at least 20% less, at least 30% less, at least 40% less, at least 50% less, at least 60% less, at least 70% less, or at least 80% less.
  • the D90 of the rigid particles can be in a range of 1% less to 90% less than the D90 of the deformable particles.
  • the TIM can be manufactured by combining the polymer component and liquid metal to form an intermediate mixture.
  • the method can further comprise dispersing the liquid metal and deformable particles throughout the polymer component in the intermediate mixture.
  • the polymer and bulk liquid metal can be mixed together with at least one of a high shear mixer, low-shear mixing, a centrifugal mixer, by shaking in a container, a mortar and pestle, and sonication to form an emulsion. More details about exemplary ways to form an emulsion of the polymer and the liquid metal droplets are described in (1) published PCT WO/2019/136252, entitled “Method of Synthesizing a Thermally Conductive and Stretchable Polymer Composite”, (2) published U.S.
  • the deformable particles and optional components may be added prior to, during, and/or after forming the liquid metal droplets.
  • the polymer component, the liquid metal, and the deformable particles can be mixed together, thereby forming liquid metal droplets from the liquid metal and dispersing the liquid metal droplets and the deformable particles throughout the polymer component.
  • composition and/or mixing techniques can be chosen such that the viscosity of the TIM is less than 850,000 cP (centipoise), such as, for example, less than 750,000 cP, less than 500,000 cp, less than 250,000 cP, 200,000 cP, less than 150,000 cP, less than 100,000 cP, less than 50,000 cP, less than 15,000 cP, less than 14,000 cP, less than 13,000 cP, less than 12,000 cP, less than 11,000 cP, or less than 10,000 cP.
  • centipoise centipoise
  • the composition and/or mixing techniques can be chosen such that the viscosity of the TIM is at least 1,000 cP, such as, for example, at least 2,000 cP, at least 5,000 cP, or at least 10,000 cP.
  • the composition and/or mixing techniques can be chosen such that the viscosity of the TIM is in a range of 1,000 cP to 850,000 cP, such as, for example, 2,000 cP to 750,000 cP, or 2,000 cP to 500,000 cP.
  • the viscosity of the TIM emulsion can be measured by a parallel plate (40mm) rheometer at 25 degrees Celsius, a frequency of 10 radians per second, and a strain of 5%.
  • Selecting the viscosity can require a balance of installation pressure, which may increase with a high viscosity, an ability to resist undesirably fast spreading during application of the TIM and pump out during operation, viscosity of the polymer component, and the storage modulus of the deformable particles.
  • the method according to the present disclosure comprises depositing a TIM 104 according to the present disclosure between a first layer 106 of an assembly 102 and a second layer 108 of the assembly 102.
  • the thickness of the TIM can be selected based on the desired application.
  • the TIM 104 comprises an emulsion of a polymer component 110, liquid metal droplets 112, deformable particles 114 and optionally rigid particles 116.
  • Depositing the TIM 104 can comprise, for example, at least one of auger or air controlled dispensing, extruding (e.g., through a nozzle, such as, a circular nozzle, a fan nozzle, or other nozzle shape), applying with a utensil (e.g., brush, spatula), stencil printing, 3D printing, and screen printing.
  • the TIM 104 can be deposited in a conformable state such that the TIM 104 can adapt to the surfaces of the first layer 106 and the second layer 108 to achieve a desired level of surface contact therebetween.
  • the TIM 104 can be applied directly to the first layer 106 and, thereafter, the second layer 108 can be applied directly to the TIM 104.
  • the TIM 104 can be applied directly to the second layer 108 and, thereafter, the first layer 106 can be applied directly to the TIM 104. In certain examples, the TIM 104 can be applied to both the first layer 106 and the second layer 108 and then the first layer 106 and the second layer 108 can be applied together. In various examples, after deposition of the TIM 104 and compression of the assembly 102, the TIM 104 can be in direct contact with and between the first layer 106 and the second layer 108. In certain examples, the application of the TIM 104 may be limited to the surfaces of the first layer 106 such that the TIM 104 can be efficiently used.
  • the TIM 104 can be dispensed from a container and applied to a layer in a conformable state.
  • the TIM 104 can be stored in a container prior to use.
  • the TIM 104 can be in a conformable state in the container.
  • the container can comprise at least one of a pillow pack, a syringe, a beaker, a jar, a bottle, and a drum.
  • the container can be a ready to use dispensing device, such as, for example, a pillow pack or a syringe.
  • the TIM 104 may not be stored and can be used after creation of the emulsion without storage.
  • the TIM 104 can be applied to at least 1% of a surface area of an exposed side 106a of the first layer 106 prior to compressing the assembly 102, such as, for example, at least 2%, at least 5%, at least 10%, at least 20%, at least 30%, at least 40%, or at least 50%, all of the surface area of the exposed side 106a of the first layer 106.
  • the TIM 104 can be applied to a range of 1% to 100% of the surface area of an exposed side 106a of the first layer 106 prior to compressing the assembly 102, such as, for example 2% to 100%, 5% to 90%, or 5% to 80%, all of the surface area of the exposed side 106a of the first layer 106.
  • the TIM 104 can be deposited at a first thickness, ti, between a first layer 106 of the assembly 102 and the second layer 108 of the assembly 102.
  • the firstthickness, ti can be selected to enhance the effective thermal conductivity of the TIM 104 and/or spatial uniformity of the liquid metal droplets 112 packing within the TIM 104.
  • the first thickness, ti can be at least 1.1 times a D90 of the liquid metal droplets 112 prior to compression, such as, for example, at least 2.5 times, at least 3 times, at least 4 times, at least 5 times, at least 6 times, at least 10 times, at least 20 times, at least 50 times, or at least 100 times, all of a D90 of the liquid metal droplets 112 prior to compressing the assembly 102.
  • the first thickness, ti can be no greater than 1,000 times a D90 of the liquid metal droplets 112, such as, for example, no greater than 500 times, no greater than 250 times, no greater than 150 times, no greater than 100 times, no greater than 50 times, no greater than 15 times, no greater than 10 times, no greater than 6 times, or no greater than 5 times, all of a D90 of the liquid metal droplets 112 prior to compressing the assembly 102.
  • the first thickness, ti can be in a range of 1.1 times to 1,000 times a D90 of the liquid metal droplets 112 prior to compressing the assembly 102, such as, for example, 2 times to 500 times, 2 times, to 150 times, 2 times to 100 times, 2 times to 50 times, 2 times to 10 times, 3 times to 10 times, or 3 times to 6 times, all of a D90 of the liquid metal droplets 112 prior to compressing the assembly 102.
  • the first thickness, ti can be at least 1.1 times the D90 of the liquid metal droplets 112 prior to compression, a desired distribution of the liquid metal droplets on the assembly 102 and spatial uniformity of the liquid metal droplets 112 packing within the TIM 104 can be achieved, thereby enhancing the effective thermal conductivity of the TIM 104.
  • the first layer 106 can be a heat-generating electronic component (e.g., a battery, memory, a data storage unit, a power inverter, a thermoelectric generator, a motor winding, an integrated circuit) and/or thermally connected to the heat-generating electronic component.
  • the integrated circuit can comprise a processor (e.g., central processing unit(CPU), tensor processing unit (TPU), graphics processing unit (GPU), artificial intelligence focused processor, an ASIC, and/or a system-on-a-chip (SOC)).
  • the second layer 108 can be an upper layer that can be thermally conductive.
  • the first layer 106 and the second layer 108 can be at least one of a battery, a processor, a heat sink (e.g., fins, fan, liquid cooling, cold plate, heat sink, heat wick, heat pipe), an integrated heat spreader, and packaging.
  • the first layer 106 can comprise a processor and the second layer 108 can comprise at least one of a heat sink, an integrated heat spreader, and packaging.
  • the first layer 106 can comprise an integrated heat spreader and the second layer 108 can comprise at least one of a heat sink, an integrated heat spreader, and packaging.
  • the first layer 106 can comprise a battery and the second layer 108 can comprise at least one of a heat sink, an integrated heat spreader, and packaging.
  • the method comprises compressing the assembly 102, thereby deforming the liquid metal droplets 112 and forming an assembly 202.
  • the first layer 106 and the second layer 108 can be urged together.
  • Compressing the assembly 102 can comprise applying a pressure to the first layer 106 and the second layer 108 of at least 3 kPa, such as, for example, at least 10 kPa, at least 70 kPa, at least 100 kPa, or at least 300 kPa.
  • Compressing the assembly 102 can comprise applying a pressure to the first layer 106 and the second layer 108 of no greater than 350 kPa.
  • compressing the assembly 102 comprises a first compression process based on displacement where a pressure is applied to the first layer 106 and the second layer 108 until the TIM 104 is compressed to a desired bondline thickness, tm.
  • the pressure can be applied by a first plate 120 and a second plate 122.
  • the TIM 104 Prior to and/or during the compression, the TIM 104, including the deformable particles 114, can be subjected to a softening event.
  • the softening event can comprise heating the first layer 106 and/or the second layer 108 to at least 30 degrees Celsius, thereby heating the deformable particles 114 to at least 30 degrees Celsius and/or compressing the assembly 102 at a pressure of at least 70 kPa, thereby applying a pressure of at least 70 kPato the deformable particles 114.
  • the first layer 106 and/or the second layer 108 can be heated to a temperature of at least 30 degrees Celsius, such as, for example, at least 35 degrees Celsius, at least 40 degrees Celsius, at least 50 degrees Celsius, at least 60 degrees Celsius, at least 70 degrees Celsius, at least 80 degrees Celsius, at least 90 degrees Celsius, at least 100 degrees Celsius, at least 110 degrees Celsius, at least 120 degrees Celsius, or at least 150 degrees Celsius.
  • the first layer 106 and/or the second layer 108 can be heated to a temperature no greater than 250 degrees Celsius, such as, for example, no greater than 225 degrees Celsius, no greater than 200 degrees Celsius, no greater than 175 degrees Celsius, no greater than 150 degrees Celsius, no greater than 100 degrees Celsius, no greater than 90 degrees Celsius, or no greater than 80 degrees Celsius.
  • the first layer 106 and/or the second layer 108 can be heated to a temperature in a range of 30 degrees Celsius to 250 degrees Celsius, such as, for example, 35 degrees Celsius to 200 degrees Celsius, 40 degrees Celsius to 175 degrees Celsius, 50 degrees Celsius to 175 degrees Celsius, or 80 degrees Celsius to 150 degrees Celsius. As illustrated in FIGs. 1-2, the heating can be applied by the first plate 120 and/or the second plate 122.
  • the softening event can comprise applying a pressure to the first layer 106 and the second layer 108 of at least 20 kPa, such as, for example, at least 50 kPa, at least 70 kPa, at least 100 kPa, at least 150kPa, at least 200 kPa, at least 250kPa, at least 300 kPa, or at least 400 kPa.
  • a pressure can be applied to the first layer 106 and the second layer 108 no greater than 350 kPa, such as, for example, no greater than 300 kPa, no greater than 250 kPa, no greater than 200 kPa, or no greater than 150 kPa.
  • a pressure can be applied to the first layer 106 and the second layer 108 in a range of 20 kPa to 500 kPa, such as, for example, 50 kPa to 400 kPa, 70 kPa to 350 kPa, 70 kPa to 300 kPa, or 70 kPa to 200 kPa.
  • the pressure during compression can be substantially constant and the rate of compression can be controlled with the deformable particles when the first layer 106 and the second layer 108 are in contact with the TIM 104.
  • the compression may occur at a rate of no greater than 50 pm/s when a distance, di, between the first layer 106 and the second layer 108 is less than 200 pm, such as, for example, no greater than 40 pm/s, no greater than 30 pm/s, no greater than 20 pm/s, no greater than 10 pm/s, no greater than 5 pm/s, no greater than 3 pm/s, no greater than 2 pm/s, or no greater than 1 pm/s, all when a distance, di, between the first layer 106 and the second layer 108 is less than 200 pm.
  • the compression may occur at a rate of at least 0.1 pm/s when a distance, di, between the first layer 106 and the second layer 108 is less than 200 pm, such as, for example, at least 0.5 pm/s, or at least 1 pm/s, all when a distance, di, between the first layer 106 and the second layer 108 is less than 200 pm.
  • the compression may occur at a rate in a range of 0.1 pm/s to 50 pm/s when a distance, di, between the first layer 106 and the second layer 108 is less than 200 pm, such as, for example, 0.1 pm/s to 20 pm/s, 0.1 pm/s to 10 pm/s, 0.5 pm/s to 50 pm/s, 1 pm/s to 50 pm/s, 0.5 pm/s to 20 pm/s, 0.5 pm/s to 10 pm/s, or 1 pm/s to 5 pm/s.
  • the use of the deformable particles 114 can enable desirable speed control of the compression of the TIM 104, thereby enabling an enhanced relative thermal conductivity. In various examples, the deformable particles 114 can reduce the rate of compression of the assembly 102.
  • the relative liquid metal surface area coverage between the TIM 104, and the first layer 106 and the second layer 108 can be increased by compression.
  • the relative liquid metal surface area coverage after compression can be in a range of 1% to 100%, such as, for example, 1% to 5%, 5% to 10%, 10% to 30%, 30% to 50%, or increasing until the liquid metal surface area coverage achieves 100%.
  • “relative liquid metal area coverage” is the surface area covered by the liquid metal normalized by the total contact surface area between the TIM 104 and the first layer 106 and second layer 108. Relative liquid metal area coverage can be measured using crosssectioning followed by optical imaging using a ZEISS Axio Zoom.V16 or confocal scanning acoustic microscopy using a Hitachi FineSAT III for CSAM.
  • the bondline thickness, tm, of the assembly 102 can be no greater than 300 microns, such as, for example, no greater than 250 microns, no greater than 200 microns, no greater than 150 microns, no greater than 145 microns, no greater than 140 microns, no greater than 125 microns, no greater than 100 microns, no greater than 80 microns, no greater than 70 microns, no greater than 50 microns, no greater than 40 microns, no greater than 35 microns, or no greater than 30 microns.
  • the bondline thickness, tm, of the assembly 102 can be at least 1 microns, such as, for example, at least 10 microns, at least 15 microns, at least 30 microns, at least 35 microns, at least 40 microns, at least 50 microns, at least 70 microns, at least 75 microns, at least 80 microns, at least 100 microns, at least 120 microns, at least 140 microns, at least 145 microns, or at least 200 microns.
  • the bondline thickness, tBL, of the assembly 102 can be in a range of 1 micron to 300 microns, such as, for example, 1 microns to 250 microns, 10 microns to 300 microns, 10 microns to 250 microns, 1 micron to 200 microns, 15 microns to 200 microns, 15 microns to 150 microns, 30 microns to 150 microns, 50 microns to 120 microns, 75 microns to 125 microns, or 15 microns to 100 microns.
  • the D90 of the liquid metal droplets 112 and/or deformable particles 114 in the TIM 104 prior to applying can be greater than the bondline thickness, tm.
  • the D90 of the liquid metal droplets 112 and/or deformable particles 114 prior to applying and/or a compressing process can be greater than the bondline thickness, tm, such as, for example, 1% greater than the bondline thickness, tm, 2% greater than the bondline thickness, t , 5% greater than the bondline thickness, tm, 10% greater than the bondline thickness, tm, 15% greater than the bondline thickness, tm, 20% greater than the bondline thickness, tm, 30% greater than the bondline thickness, tm, 40% greater than the bondline thickness, tm, 50% greater than the bondline thickness, tm, or 75% greater than the bondline thickness, tm.
  • the D90 of the liquid metal droplets 112 and/or deformable particles 114 prior to applying and/or a compressing process can be no more than 100% greater than the bondline thickness, tm, such as, for example, no more than 75% greater than the bondline thickness, tm, no more than 50% greater than the bondline thickness, tm, no more than 40% greater than the bondline thickness, tm, no more than 30% greater than the bondline thickness, tm, no more than 20% greater than the bondline thickness, tm, no more than 15% greater than the bondline thickness, tm, no more than 10% greater than the bondline thickness, tm, no more than 5% greater than the bondline thickness, tm, or no more than 2% greater than the bondline thickness, tm.
  • the D90 of the liquid metal droplets 112 and/or deformable particles 114 prior to applying and/or a compressing process can be in a range of 1% to 100% greater than the bondline thickness, tm, such as, for example, 1% to 50% greater than the bondline thickness, tm, 1% to 30% greater than the bondline thickness, tm, 2% to 30% greater than the bondline thickness, tm, or 5% to 20% greater than the bondline thickness, tm.
  • the TIM can cover at least 90% of a surface area of an exposed side 106a of the first layer 106 after compressing the circuit assembly, such as, for example, at least 95% of the surface area of the exposed side 106a.
  • the cure time of the TIM 104 can be sufficient to enable the compression to occur and to achieve the bondline thickness, tm.
  • Cure time of the TIM 104 can be in a range of 0.5 minutes to 2 hours, such as, for example, 1 minute to 2 hours, 1 minute to 1 hour, 2 minutes to 1 hour, 2 minutes to 30 minutes, 5 minutes to 1 hour, 10 minutes to 1 hour, 30 minutes to 2 hours, 1 minute to 10 minutes, or 1 hour to 2 hours.
  • Compressing the assembly 102 can apply a force to the TIM 104 and can deform the liquid metal droplets 112 and/or deformable particles 114 dispersed within the polymer component 110 of the TIM 104. Because the polymer component 110 is still liquid and conformable and moveable, the compressing force can deform the liquid metal droplets 112 and/or deformable particles 114.
  • the liquid metal droplets 112 can be in the liquid phase during deformation, such that a lower pressure is required for the compression and a desired deformation can be achieved.
  • the storage modulus of the deformable particles 114 can be reduced such that a lower pressure is required for compression, and a desired deformation can be achieved.
  • the liquid metal droplets 112 and/or deformable particles 114 can be generally spherical as shown in FIG. 1 and thereafter can be generally ellipsoidal as shown in FIG. 2.
  • the concentration of the deformable particles 114 can selected to achieve the desired pressure for compression, resulting velocity of compression, and a desired deformation can be achieved.
  • the liquid metal droplets 112 and/or deformable particles 114 prior to compressing, individually can have a first average aspect ratio and after compressing the liquid metal droplets 112 and/or deformable particles 114, individually, can have a second average aspect ratio.
  • the second average aspect ratio can be different than the first average aspect ratio.
  • the second average aspect ratio can be greater than the first average aspect ratio.
  • the average aspect ratio can be a mean ratio of the width to the height of the liquid metal droplets 112 or the deformable particles 114, as the case may be.
  • the first aspect ratio can be 1 and the second aspect ratio can be greater than 1.
  • the first aspect ratio can be in a range of 1 to 1.5.
  • the second aspect ratio can be at least 0.5 greater than the first aspect ratio, such as, for example, at least 1 greater than the first aspect ratio, at least 2 greater than the first aspect ratio, or at least 5 greater than the first aspect ratio. In certain examples, the second aspect ratio can be at least 2 after compressing the assembly 102, such as, for example, at least 3, or at least 4 after compressing the assembly 102.
  • the width (e.g., longest dimension) of the liquid metal droplets 112 and/or the deformable particles 114 can be substantially aligned with the longitudinal plane of the TIM 104 in the assembly 102 and the height of the liquid metal droplets 112 can be substantially aligned with the thickness of the TIM 104 (e.g., the bondline thickness, dni).
  • the width of the liquid metal droplets 112 and/or deformable particles 114 can increase upon compression of the assembly 102.
  • the diameter of liquid metal droplets 112 prior to compressing can be 200 pm (with a first aspect ratio of 1) and after compression to a bondline thickness of 100 pm, the liquid metal drop can be deformed to an ellipsoidal shape with a 400 pm width (e.g., second aspect ratio of 4).
  • the liquid metal droplets 112, the deformable particles 114, and/or the rigid particles 116 can be aligned substantially in a monolayer as shown in FIG. 2 after compressing.
  • the monolayer can be achieved by selecting the Dso and/or D90 of the liquid metal droplets 112, the deformable particles 114, and/or the rigid particles 116, and the bondline thickness, tni. Configuring the liquid metal droplets 112, the deformable particles 114, and/or the rigid particles 116 in a monolayer can reduce the thermal resistance of the TIM 104.
  • the D50 and/or D90 of the liquid metal droplets 112, the deformable particles 114, and/or the rigid particles 116, deformation of the liquid metal droplets 112, and controlled compression of the TIM 104 can improve the thermal resistance value of the TIM 104.
  • the TIM 104 can comprise a thermal resistance value of at least 0.5 (°K*mm 2 )/W, such as, for example, at least 1 (°K*mm 2 )/W, at least 2 (°K*mm 2 )/W, at least 3 (°K*mm 2 )/W, at least 5 (°K*mm 2 )/W, or at least .
  • the TIM 104 can comprise a thermal resistance value of no greater than , such as, for example, no greater than 20 (°K*mm 2 )/W, no greater than 15 ( greater than 10 (°K*mm 2 )/W, no greater than 9 (°K*mm 2 )/W, no greater than 8 (°K*mm 2 )/W, no greater than 7 (°K*mm 2 )/W, or no greater than 5(°K*mm 2 )/W.
  • the TIM 104 can comprise a thermal resistance value in a range of 0.5 (°K*mm 2 )/W to 30 (°K*mm 2 )/W, such as, for example, 0.5 (°K*mm 2 )/W to 20 (°K*mm 2 )/W, 0.5 (°K*mm 2 )/W to 15 (°K*mm 2 )/W, 1 (°K*mm 2 )/W to 10 (°K*mm 2 )/W, 2 (°K*mm 2 )/W to 10 (°K*mm 2 )/W, or 2 (°K*mm 2 )/W to 8 (°K*mm 2 )/W.
  • the thermal resistance value can be measured using a TIMA 5 instrument from NanoTest (Germany).
  • the D50 and/or D90 of the liquid metal droplets 112, the deformable particles 114, and/or the rigid particles 116, deformation of the liquid metal droplets 112, and controlled compression of the TIM 104 can improve the thermal conductivity value of the TIM 104.
  • the TIM 104 can comprise an effective thermal conductivity value of at least 1 W/m*K, such as, for example, at least 5 W/m*K, at least 10 W/m*K, at least 12 W/m*K, at least 15 W/m*K, at least 17 W/m*K, or at least 20 W/m*K.
  • the TIM 104 can comprise an effective thermal conductivity value in a range of 1 W/m*K to 50 W/m*K, such as, for example, 5 W/m*K to 50 W/m*K, 10 W/m*K to 40 W/m*K or 10 W/m*K to 30 W/m*K.
  • the effective thermal conductivity is a thickness of the TIM divided by a thermal resistance of the TIM.
  • the TIM 104 can be cured or may not be cured, depending on the application. For example, the TIM 104 may be cured to thicken the TIM 104, which may increase the viscosity of the polymer component 110. In certain examples, the TIM 104 may be cured to a solid.
  • the TIM 104 is cured after compressing the first layer 106 and the second layer 108 of the assembly 102. Applying the TIM 104 at a lower viscosity can enable a more efficient installation and ability to wet surfaces of the first layer 106 and the second layer 108. Increasing the viscosity after application can enable the TIM 104 to resist pump out and enhance removal of the TIM 104. In various examples, the TIM 104 may not be cured.
  • the polymer component 110 after curing is elastomeric. Curing the polymer component 110 can inhibit pump out of the liquid metal droplets 112 during thermal cycling of the assembly 102 and can provide a mechanical bond between the first layer 106 and the second layer 108.
  • Curing the TIM 104 can comprise at least one of heating the TIM 104 (e.g., in examples with a thermosetting polymer), adding a catalyst to the TIM 104 (e.g., platinum catalyst, moisture), exposing the TIM 104 to air, cooling the TIM 104 (e.g., in examples with a thermoplastic polymer), applying electromagnetic radiation (e.g., photo-polymerization), and applying pressure to the TIM 104. Curing the TIM 104 can increase the viscosity of the TIM 104.
  • the TIM 104 can comprise a viscosity after curing that is at least double of the TIM prior to curing, such as, for example, at least triple, at least quadrupole, or ten times a viscosity of the TIM prior to curing.
  • the TIM 104 can comprise a viscosity after curing of greater than 15,000 cP, such as, for example, greater than 20,000 cP, greater than 30,000 cP, greater than 50,000 cP, greater than 100,000 cP, greater than 150,000 cP, greater than 200,000 cP, greater than 250,000 cP, greater than 500,000 cP, greater than 750,000 cP, greater than 850,000 cP, greater than 1,000,000 cP, greater than 1,500,000 cP, greater than 2,500,000 cP, greater than 4,000,000 cP, or greater than 5,000,000 cP.
  • the TIM 104 can be an adhesive.
  • the polymer in the TIM 104 can be selected to reduce off-gasing of the TIM 104 during curing.
  • the TIM 104 can be removed with a solvent and/or scrapping.
  • the method of manufacturing the assembly 102 can be a snap-cure process, a reflow oven, a bake process, and/or a high- force magazine.
  • the first plate 120 and the second plate 122 are urged into contact with the first layer 106 and the second layer 108 of the assembly 102.
  • the temperature of the first plate 120 and/or second plate 122 can be in a range of 80 degrees Celsius to 200 degrees Celsius and can be displaced at various rates, which may not be precisely controlled.
  • the pressure applied by the first plate 120 and/or the second plate 122 can be in a range of 35 kPa to 2 MPa for a cure time of the TIM 104 can be in a range of 0.5 minutes to 20 minutes.
  • the deformable spacers in the TIM 104 can be used to control the displacement rate of the compression of the assembly 104 in the snap-cure process.
  • the temperature for the cure can be in a range of 70 degrees Celsius to 150 degrees Celsius, with a compression pressure in a range of 0 kPa to 700 kPa for a cure time of the TIM 104 can be in a range of 30 minutes to 2 hours.
  • cure and “curing” refer to the chemical cross-linking of components in an emulsion or material applied over a substrate, or the increase of viscosity of the components in the emulsion or material applied over the substrate. Accordingly, the terms “cure” and “curing” do not encompass solely physical drying of an emulsion or material through solvent or carrier evaporation.
  • thermosetting polymer refers to the condition of an emulsion or material in which a component of the emulsion or material has chemically reacted to form new covalent bonds in the emulsion or material (e.g., new covalent bonds formed between a binder resin and a curing agent).
  • cured refers to the condition of an emulsion or material in which the temperature of the thermoplastic polymer decreases below the melting point of the thermoplastic polymer such that the viscosity of the emulsion or material increases.
  • cured refers to one of or both of the polymers curing as described herein.
  • the TIM according to the present disclosure can be used in a system on a package.
  • a single horizontal TIM layer can be in contact with multiple dies on one side (e.g., the integrated circuit can comprise multiple dies, or multiple integrated circuits can be in contact with the same side of the TIM) and an upper layer or layers on a different side.
  • a thermal interface material comprising: a polymer component; liquid metal droplets dispersed through the polymer component; and deformable particles dispersed through the polymer component, such that the deformable particles exhibit a storage modulus that decreases by at least half responsive to at least one softening event applied to the deformable particles, the softening event selected from the group consisting of a temperature of at least 30 degrees Celsius and a pressure of at least 20 kPa.
  • thermo interface material of clause 1 wherein the thermal interface material comprises: 5% to 80% of the polymer component based on a total volume of the thermal interface material; 20% to 95% of the liquid metal droplets based on the total volume of the thermal interface material; and 0.05% to 25% of the deformable particles based on the total volume of the thermal interface material.
  • thermo interface material of any of clauses 1-2, wherein the thermal interface material comprises: 5% to 30% of the polymer component based on a total volume of the thermal interface material; 50% to 95% of the liquid metal droplets based on the total volume of the thermal interface material; and 0.2% to 1% of the deformable particles based on the total volume of the thermal interface material.
  • Clause 7 The thermal interface material of any of clauses 1-6, wherein the deformable particles comprise polyethylene, polymethyl methacrylate, polyethylene glycol, polypropylene glycol, polyurethane, polystyrene, polyamide, polyolefin rubber, polysiloxane rubber, or a combination thereof.
  • Clause 8 The thermal interface material of any of clauses 1-7, wherein the deformable particles comprise tin, a tin alloy, silver, a silver alloy, copper, a copper alloy, gallium, a gallium alloy, indium, an indium alloy, lead, a lead alloy, bismuth, a bismuth alloy, a zinc alloy, antimony, an antimony alloy, or a combination thereof.
  • Clause 13 The thermal interface material of any of clauses 1-12, wherein the polymer component comprises at least one of an acrylic polymer, an acrylate polymer, a vinyl polymer, a polyester polymer, a polyurethane polymer, a polybutadiene polymer, a polyamide polymer, a polyether polymer, a polysiloxane polymer, a silicon hydride polymer, a fluoropolymer, a polyisoprene polymer, and a copolymer of any two or more thereof.
  • the polymer component comprises at least one of an acrylic polymer, an acrylate polymer, a vinyl polymer, a polyester polymer, a polyurethane polymer, a polybutadiene polymer, a polyamide polymer, a polyether polymer, a polysiloxane polymer, a silicon hydride polymer, a fluoropolymer, a polyisoprene polymer, and a copolymer of any
  • Clause 14 The thermal interface material of any of clauses 1-13, wherein the deformable particles comprise a D90 in a range of 1 micron to 300 microns and the liquid metal droplets comprise a D90 in a range of 1 micron to 300 microns.
  • Clause 15 The thermal interface material of any of clauses 1-14, wherein the deformable particles comprise a D90 in a range of 15 microns to 150 microns and the liquid metal droplets comprise a D90 in a range of 15 microns to 150 microns.
  • Clause 17 The thermal interface material of any of clauses 1-16, further comprising at least one of a catalyst, rigid particles, a coupling agent, and fumed silica.
  • Clause 18 The thermal interface material of any of clauses 1-17, wherein the deformable particles comprise a storage modulus in a range of 0.1 MPa to 100 MPa when measured at a temperature 20 degrees Celsius greater than the glass transition temperature of the deformable particles.
  • Clause 19 An assembly comprising: a first layer; a second layer; and the thermal interface material of any of clauses 1-18 compressed and disposed in contact with and between the first layer and the second layer, wherein a bondline thickness formed between the first layer and the second layer is less than a D90 of the liquid metal droplets and a D90 of the deformable particles prior to compression of the thermal interface material in the assembly.
  • Clause 20 The assembly of clause 19, wherein a width of the liquid metal droplets and a width of the deformable particles are substantially aligned with a longitudinal plane of the thermal interface material.
  • Clause 21 The assembly of any of clauses 19-20, wherein the bondline thickness formed between the first layer and the second layer is no greater than 300 microns.
  • Clause 22 The assembly of any of clauses 19-21, wherein the first layer and the second layer, individually, comprise at least one of a battery, a processor, a heat sink, an integrated heat spreader, and packaging.
  • Clause 23 The assembly of any of clauses 19-22, wherein the thermal interface material is cured.
  • Clause 25 A method comprising: applying the thermal interface material of any of clauses 1-18 on a first layer of an assembly at a first thickness; subjecting the thermal interface material to at least one softening event; and compressing the assembly to decrease the first thickness to a second thickness, wherein the second thickness is no greater than a D90 of the liquid metal droplets and a D90 of the deformable particles in the thermal interface material prior to compressing the assembly.
  • Clause 26 The method of clause 25, wherein the at least one softening event comprises heating at least one of the first layer and a second layer of the assembly to at least 30 degrees Celsius, thereby heating the deformable particles to at least 30 degrees Celsius.
  • Clause 27 The method of any of clauses 25-26, wherein the at least one softening event comprises comprising the assembly at a pressure of at least 20 kPa, thereby applying a pressure of at least 20 kPa to the deformable particles.
  • Clause 28 The method of any of clauses 25-27, further comprising, after compressing the assembly, curing the thermal interface material thereby forming a cured assembly.
  • Clause 29 The method of any of clauses 25-28, wherein the compressing occurs at a rate of less than 50 pm/s when a distance between the first layer and the second layer is less than 200 pm.
  • Clause 30 The method of any of clauses 25-29, wherein the first thickness is at least 1.1 times a D90 of the liquid metal droplets in the thermal interface material prior to compressing the assembly.
  • Clause 31 An assembly produced by the method of any of clauses 25-29.
  • a method of manufacture of a thermal interface material comprising: mixing a polymer component, liquid metal, and deformable particles together, thereby forming liquid metal droplets from the liquid metal and dispersing the liquid metal droplets and the deformable particles throughout the polymer component, wherein the deformable particles exhibit a storage modulus that decreases by at least half responsive to at least one softening event selected from the group consisting of a temperature of at least 30 degrees Celsius and a pressure of at least 20 kPa.
  • At least one of’ a list of elements means one of the elements or any combination of two or more of the listed elements.
  • at least of A, B, and C means A only; B only; C only; A and B; A and C; B and C; or A, B, and C.
  • any numerical range recited in this specification describes all sub-ranges of the same numerical precision (z.e., having the same number of specified digits) subsumed within the recited range.
  • a recited range of “1.0 to 10.0” describes all sub-ranges between (and including) the recited minimum value of 1.0 and the recited maximum value of 10.0, such as, for example, “2.4 to 7.6,” even if the range of “2.4 to 7.6” is not expressly recited in the text of the specification.
  • the Applicant reserves the right to amend this specification, including the claims, to expressly recite any sub-range of the same numerical precision subsumed within the ranges expressly recited in this specification. All such ranges are inherently described in this specification such that amending to expressly recite any such sub-ranges will comply with the written description, sufficiency of description, and added matter requirements.

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Abstract

L'invention concerne des matériaux d'interface thermique comprenant des particules déformables, des ensembles circuits formés à partir de ceux-ci, et leurs procédés de fabrication. Le matériau d'interface thermique comprend un composant polymère, des gouttelettes de métal liquide dispersées à travers le composant polymère, et des particules déformables dispersées à travers le composant polymère. Les particules déformables présentent un module de conservation qui diminue d'au moins de moitié en réponse à au moins un événement de ramollissement appliqué aux particules déformables. Les particules déformables sont choisies dans le groupe consistant à une température d'au moins 30 degrés Celsius et une pression d'au moins 20 kPa.
PCT/US2024/037294 2023-07-12 2024-07-10 Matériaux d'interface thermique comprenant des particules déformables, ensembles de circuits formés à partir de ceux-ci, et leurs procédés de fabrication Pending WO2025014994A1 (fr)

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US202363513229P 2023-07-12 2023-07-12
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Citations (6)

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Publication number Priority date Publication date Assignee Title
US20040124526A1 (en) * 2002-12-30 2004-07-01 Matayabas James C. Gel thermal interface materials comprising fillers having low melting point and electronic packages comprising these gel thermal interface materials
US20050228097A1 (en) * 2004-03-30 2005-10-13 General Electric Company Thermally conductive compositions and methods of making thereof
US20170218167A1 (en) 2016-02-02 2017-08-03 Carnegie Mellon University, A Pennsylvania Non-Profit Corporation Polymer Composite with Liquid Phase Metal Inclusions
WO2019136252A1 (fr) 2018-01-05 2019-07-11 Carnegie Mellon University Procédé de synthèse d'un composite polymère thermiquement conducteur et étirable
US10777483B1 (en) 2020-02-28 2020-09-15 Arieca Inc. Method, apparatus, and assembly for thermally connecting layers
WO2022204689A1 (fr) 2021-03-25 2022-09-29 Arieca Inc. Procédé, appareil et ensemble pour relier thermiquement des couches avec des matériaux d'interface thermique comprenant des particules rigides

Patent Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20040124526A1 (en) * 2002-12-30 2004-07-01 Matayabas James C. Gel thermal interface materials comprising fillers having low melting point and electronic packages comprising these gel thermal interface materials
US20050228097A1 (en) * 2004-03-30 2005-10-13 General Electric Company Thermally conductive compositions and methods of making thereof
US20170218167A1 (en) 2016-02-02 2017-08-03 Carnegie Mellon University, A Pennsylvania Non-Profit Corporation Polymer Composite with Liquid Phase Metal Inclusions
WO2019136252A1 (fr) 2018-01-05 2019-07-11 Carnegie Mellon University Procédé de synthèse d'un composite polymère thermiquement conducteur et étirable
US10777483B1 (en) 2020-02-28 2020-09-15 Arieca Inc. Method, apparatus, and assembly for thermally connecting layers
WO2022204689A1 (fr) 2021-03-25 2022-09-29 Arieca Inc. Procédé, appareil et ensemble pour relier thermiquement des couches avec des matériaux d'interface thermique comprenant des particules rigides

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