TY - JOUR
T1 - Coherence spectroscopy in dissipative media
T2 - A Liouville space pathway approach
AU - Ramakrishna, S.
AU - Seideman, Tamar
N1 - Funding Information:
The authors are grateful to Professor R. J. Gordon for helpful discussions about experimental realization of this research. This work was supported in part by the National Science Foundation (Grant No. PHY-0200812).
PY - 2005
Y1 - 2005
N2 - We address the possibility of using coherent control tools to extract useful information about the interaction of a system with a dissipative environment. To that end we extend previous work, which developed a coherence spectroscopy based on two-pathway excitation phase control, from the isolated molecule limit to dense media. Specifically, we explore the properties of the channel phase, an observable of energy-domain two-pathway excitation experiments that was shown in the isolated molecule limit to carry information about the phase properties of the material system. Our analysis is based on the combination of steady state and time-dependent analytical perturbative approaches within the density matrix formalism, complemented by nonperturbative numerical simulations. We find that the channel phase carries significantly richer information in the presence of decoherence mechanisms than in their absence. In particular, rescattering events in the structured continuum introduce new features in the channel phase spectrum, whose structure conveys information about both the molecular continuum and the system bath interaction.
AB - We address the possibility of using coherent control tools to extract useful information about the interaction of a system with a dissipative environment. To that end we extend previous work, which developed a coherence spectroscopy based on two-pathway excitation phase control, from the isolated molecule limit to dense media. Specifically, we explore the properties of the channel phase, an observable of energy-domain two-pathway excitation experiments that was shown in the isolated molecule limit to carry information about the phase properties of the material system. Our analysis is based on the combination of steady state and time-dependent analytical perturbative approaches within the density matrix formalism, complemented by nonperturbative numerical simulations. We find that the channel phase carries significantly richer information in the presence of decoherence mechanisms than in their absence. In particular, rescattering events in the structured continuum introduce new features in the channel phase spectrum, whose structure conveys information about both the molecular continuum and the system bath interaction.
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U2 - 10.1063/1.1850891
DO - 10.1063/1.1850891
M3 - Article
C2 - 15836058
AN - SCOPUS:22944468186
SN - 0021-9606
VL - 122
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
IS - 8
M1 - 084502
ER -