Detection of photoinduced electronic, thermal, and acoustic dynamics of gold film using a transient reflecting grating method under three types of surface plasmon resonance conditions

Abstract

Mechanisms of unusual signal enhancement observed for transient reflecting grating (TRG) experiments are investigated under three types of surface plasmon resonance (SPR) conditions, where two pump beams only, a probe beam only, or two pump beams and a probe beam, excite surface plasmon. A gold thin film deposited on a glass prism is measured in the Kretschmann configuration with a temporal resolution of tens of picoseconds. The signal under each SPR condition exhibits different characteristic features in signal intensity and transient behavior unlike the usual non-SPR TRG experiments. Under SPR with pump beams, high conversion efficiency from light to heat allows detection of a TRG signal 11 times larger in magnitude and much lower in background level than under a non-SPR with them. Under SPR with the probe beam, diffraction caused by heat-induced spatial modulation as described by complex reflection Fresnel coefficients is theoretically proved to enhance the TRG signal and to change transient behavior, which provides a way to get selective observation of heat diffusion near the surface. When both pump and probe beams excite surface plasmons, an additional signal is observed, almost at the same time as the optical pulse, having 100 times larger intensity than the other signals, which is due to electrons excited at the gold surface.