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Observation of Lorentzian lineshapes in the room temperature optical spectra of strongly coupled Jaggregate/metal hybrid nanostructures by linear two-dimensional optical spectroscopy

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Title Observation of Lorentzian lineshapes in the room temperature optical spectra of strongly coupled Jaggregate/metal hybrid nanostructures by linear two-dimensional optical spectroscopy
 
Creator WANG, W
VASA, P
SOMMER, E
DE SIO, A
GROSS, P
VOGELGESANG, R
LIENAU, C
 
Subject nano-optics
coherent optical spectroscopy
two-dimensional optical spectroscopy
exciton-plasmon-coupling
line broadening
SEMICONDUCTOR QUANTUM DOTS
SYNTHETIC HETERODIMER SYSTEMS
SURFACE-PLASMON POLARITONS
NEAR-FIELD SPECTROSCOPY
ENGINEERING COHERENCE
EXCITED-STATES
FLUORESCENCE INTERMITTENCY
PARA-TERPHENYL
SHAPES
DYNAMICS
 
Description We analyze the linear optical reflectivity spectra of a prototypical, strongly coupled metal/molecular hybrid nanostructure by means of a new experimental approach, linear two-dimensional optical spectroscopy. White-light, broadband spectral interferometry is used to measure amplitude and spectral phase of the sample reflectivity or transmission with high precision and to reconstruct the time structure of the electric field emitted by the sample upon impulsive excitation. A numerical analysis of this time-domain signal provides a two-dimensional representation of the coherent optical response of the sample as a function of excitation and detection frequency. The approach is used to study a nanostructure formed by depositing a thin J-aggregated dye layer on a gold grating. In this structure, strong coupling between excitons and surface plasmon polaritons results in the formation of hybrid polariton modes. In the strong coupling regime, Lorentzian lineshape profiles of different polariton modes are observed at room temperature. This is taken as an indication that the investigated strongly coupled polariton excitations are predominantly homogeneously broadened at room temperature. This new approach presents a versatile, simple and highly precise addition to nonlinear optical spectroscopic techniques for the analysis of line broadening phenomena.
 
Publisher IOP PUBLISHING LTD
 
Date 2014-12-29T04:43:57Z
2014-12-29T04:43:57Z
2014
 
Type Article
 
Identifier JOURNAL OF OPTICS, 16(11)
2040-8978
2040-8986
http://dx.doi.org/10.1088/2040-8978/16/11/114021
http://dspace.library.iitb.ac.in/jspui/handle/100/17107
 
Language English