Ultrafast switching of surface plasmonic conditions in nonplasmonic metals

Abstract : We demonstrate that ultrafast carrier excitation can drastically affect electronic structures in nonplasmonic metals and determine a transient, brief surface plasmonic state, potentially creating the conditions for a plasmonic switch. The initial state can be related to d-band partial filling and splitting, with a pseudo-band-gap accommodating the chemical potential. This determines a quasi-resonant-like spectral behavior of the optical constants for pumping carriers across the d-band pseudogap, i.e., visible frequencies. The relation between real and imaginary parts of the refractive index does not fulfill surface plasmonic conditions in the visible photon range. Using first-principles molecular dynamics and Kubo-Greenwood formalism for laser-excited tungsten we show that carrier heating mobilizes d electrons into collective inter-and intraband transitions leading to a sign flip in the imaginary optical conductivity, activating plasmonic properties for the initial nonplasmonic phase. The drive for the laser-induced optical evolution in this case does not rely on a variation of the free electron number but can be visualized as an increasingly damped character of the quasiresonance at visible frequencies. Here laser heating determines an energy-dependent degree of occupation with broadening profiles. The subsequent evolution of optical indices for the excited material is confirmed by time-resolved ultrafast ellipsometry. The large optical tunability extends the existence spectral domain of surface plasmons in ranges typically claimed in laser self-organized nanostructuring. Nonequilibrium heating is thus a strong factor for engineering optical control of evanescent excitation waves, particularly important in laser nanostructuring strategies.