Item

Abstract

Using a mid-infrared emission spectrometer based on a superconducting nanowire single-photon detector (SNSPD), we observe the dynamics of vibrational energy pooling of CO adsorbed at the surface of a NaCl crystal. After exciting a majority of the CO molecules to their first vibrationally excited state (v = 1), we observe infrared emission from states up to v = 27. Kinetic Monte Carlo simulations show that vibrational energy collects in a few CO molecules at the expense of those up to eight lattice sites away by selective excitation of NaCl's transverse phonons. The vibrating CO molecules behave like classical oscillating dipoles, losing their energy to NaCl lattice-vibrations via the electromagnetic near-field. This is analogous to Sommerfeld's description of the Earth's influence on radio transmission by ground waves.