Multilayer graphene structures with enhanced mechanical properties resulting from deterministic control of interlayer twist angles and chemical functionalization

1. An article of manufacture, comprising:

a) a first graphene layer;

b) a second graphene layer over the first graphene layer, the second graphene layer oriented at a first interlayer twist angle with respect to the first graphene layer and bonded by interlayer covalent sp 3 bonds to the first graphene layer; and

c) a third graphene layer over the second graphene layer, the third graphene layer oriented at a second interlayer twist angle with respect to the second graphene layer and bonded by interlayer covalent sp 3 bonds to the second graphene layer.

2. The article of claim 1 , wherein at least one of the first graphene layer, the second graphene layer, and the third graphene layer is a polycrystalline graphene layer.

3. The article of claim 1 , wherein the first and second interlayer twist angles are each separately in a range of between 0° and about 16°.

4. The article of claim 3 , wherein the first and second interlayer twist angles are each equal to 0°, resulting in the formation of a two-dimensional (2D) diamond structure.

5. The article of claim 1 , wherein the first and second interlayer twist angles are each separately in a range of between about 44° and 60°.

6. The article of claim 5 , wherein the first and second interlayer twist angles are each equal to 60°, resulting in the formation of a two-dimensional (2D) diamond structure.

7. A method of making an article, comprising:

a) growing a first graphene layer on a silicon carbide wafer;

b) exfoliating the first graphene layer onto a first transfer layer;

c) disposing the first graphene layer and first transfer layer onto a host substrate, so that the first graphene layer is in contact with the host substrate surface;

d) removing the first transfer layer;

e) growing a second graphene layer on a silicon carbide wafer;

f) exfoliating the second graphene layer onto a second transfer layer;

g) disposing the second graphene layer and second transfer layer over the first graphene layer at a first interlayer twist angle with respect to the first graphene layer, so that the second graphene layer is in contact with the first graphene layer;

h) removing the second transfer layer;

i) covalently bonding the first and second graphene layers, the bonding involving a fraction of carbon atoms of each of the first and second graphene layers;

j) growing a third graphene layer on a silicon carbide wafer;

k) exfoliating the third graphene layer onto a third transfer layer;

l) disposing the third graphene layer and third transfer layer over the second graphene layer at a second interlayer twist angle with respect to the second graphene layer, so that the third graphene layer is in contact with the second graphene layer;

m) removing the third transfer layer; and

n) covalently bonding the third and second graphene layers, the bonding involving a fraction of carbon atoms of each of the second, and third graphene layers.

8. The article of claim 1 , wherein the first graphene layer and the second layer each comprise single crystalline graphene comprising a first unique azimuthal orientation and a second unique azimuthal orientation, respectively, and wherein the first interlayer twist angle comprises an angle between the first unique azimuthal orientation and the second unique azimuthal orientation.