We describe an optical pump/probe system for sensitive measurements of time-resolved optical measurements of material dynamics. The instrument design is optimized for time-resolved magneto-optic Kerr effect (TR-MOKE) measurements of dynamics in magnetic materials. The system also allows for time-domain thermoreflectance (TDTR) measurements of thermal transport properties and picosecond acoustic measurements of film thickness and/or elastic constants. The system has several advantages over the conventional designs for TR-MOKE and/or TDTR systems. Measurements of pump-induced changes to the probe beam intensity are shot-noise limited. The system’s design allows for MOKE and/or thermoreflectance measurements of both sides of a sample. Pumping and probing the sample on opposite sides allows nanoscale flash diffusivity measurements of transport properties. The wavelengths of the pump and probe beams are straightforward to tune between 350–525 nm and 690–1050 nm. A tunable wavelength allows for optical resonances in a wide array of materials to be excited and/or probed. Finally, the setup is calibrated to allow for the real and imaginary components of Kerr signals to be separately quantified.

To better understand the many effects of temperature on the optical properties of metals, we experimentally and theoretically quantify the electron vs. phonon contributions to the thermoreflectance spectra of gold. We perform a series of pump/probe measurements on nanoscale Pt/Au bilayers at wavelengths between 400 and 1000 nm. At all wavelengths, we find that changes in phonon temperature, not electron temperature, are the primary contributor to the thermoreflectance of Au. The thermoreflectance is most sensitive to the electron temperature at wavelength of ~480 nm due to interband transitions between d-states and the Fermi-level. In the near infrared, the electron temperature is responsible for only ~2% of the total thermoreflectance. We also compute the thermoreflectance spectra of Au from first principles. Our calculations further confirm that phonon temperature dominates thermoreflectance of Au. Most of Au's thermoreflectance is due to the effect of the phonon population on electron lifetime.