Single-molecule pump-probe detection resolves ultrafast pathways in individual and coupled quantum systems.
We report the first experimental study of individual molecules with femtosecond time resolution using a novel ultrafast single-molecule pump-probe method. A wide range of relaxation times from below 100 up to 400 fs is found, revealing energy redistribution over different vibrational modes and phonon coupling to the nanoenvironment. Addressing quantum-coupled molecules we find longer decay times, pointing towards inhibited intramolecular decay due to delocalized excitation. Interestingly, each individual system shows discrete jumps in femtosecond response, reflecting sudden breakup of the coupled superradiant state.
van Dijk
Erik M H P
EM
Applied Optics Group, MESA+ Institute for Nanotechnology, University of Twente, P.O. Box 217 Enschede, The Netherlands.
Hernando
Jordi
J
García-López
Juan-José
JJ
Crego-Calama
Mercedes
M
Reinhoudt
David N
DN
Kuipers
Laurens
L
García-Parajó
María F
MF
van Hulst
Niek F
NF