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Indentation is a versatile method to assess the hardness of different materials along with their elastic properties. Recently, powerful approaches have been developed to determine further material properties, like yield strength, ultimate tensile strength, work-hardening rate, and even cyclic plastic properties, by a combination of indentation testing and computer simulations. The basic idea of these approaches is to simulate the indentation with known process parameters and to iteratively optimize the initially unknown material properties until just a minimum error between numerical and experimental results is achieved. In this work, we have developed a protocol for instrumented indentation tests and a procedure for the inverse analysis of the experimental data to obtain material parameters for time-dependent viscoplastic material behavior and kinematic and isotropic work-hardening. We assume the elastic material properties and the initial yield strength to be known because these values can be determined independently from indentation tests. Two optimization strategies were performed and compared for identification of the material parameters. The new inverse method for spherical indentation has been successfully applied to martensitic steel.