Yes, you can use any material to design and simulate the devices in the Sentaurus TCAD.
There are many materials already listed in the Sentaturs TCAD, but if the required material is not there, then all you need is its key properties (mobility, permittivity, etc.) to use the device in the Sentaurus TCAD.
There is "AnyMaterial" listed in the Structure Editor, use it and change the properties of "AnyMaterial" with the material you are looking for in the parameter file of the "AnyMaterial".