Single nano-objects:
linear and ultrafast optical properties

Nano-objets individuels :
propriétés optiques linéaires et ultrarapides

Understanding and modeling the impact of size, shape and environment on the optical properties of nano-objects is an intense field of research with both fundamental and technological motivations. However, most of the optical studies on nano-scale materials are performed on ensembles, where thousands or more nano-objects are simultaneously studied. Only an average response is measured, making difficult identification of the mechanisms responsible for the specific physical properties and their comparison with theoretical models, in systems where the characteristics of the nano-objects and of their local environment present fluctuations. This limitation can be overcome by studying single nano-objects, but this constitutes an important difficulty.

Our group pioneered single nanoparticle spectroscopy activities by introducing the “Spatial Modulation Spectroscopy” (SMS) technique [*], which yields access to the quantitative absorption cross-section spectra and amplitude of a single nano-object with size down to a few nanometers. Its morphology being also independently determined by electron microscopy, this open the way to precise comparison with theoretical models.

We have investigated single nano-objects deposited on a transparent or opaque substrate (by using SMS in transmission or reflexion, respectively), as monometallic nanoparticles (Au, Ag), bimaterial nano-objects (Ag@SiO2, Au@Ag, …), metal dimers (Au-Ag@SiO2), single-wall carbon nanotubes and more complex nanosystems. These studies led to an increased comprehension of the physical processes governing the optical response of nanosystems, of dielectric and quantum confinements effects in metals and, more generally, of electromagnetic interactions at the nanoscale.

Understanding and modeling the impact of size, shape and environment on the optical properties of nano-objects is an intense field of research with both fundamental and technological motivations. However, most of the optical studies on nano-scale materials are performed on ensembles, where thousands or more nano-objects are simultaneously studied. Only an average response is measured, making difficult identification of the mechanisms responsible for the specific physical properties and their comparison with theoretical models, in systems where the characteristics of the nano-objects and of their local environment present fluctuations. This limitation can be overcome by studying single nano-objects, but this constitutes an important difficulty.

Our group pioneered single nanoparticle spectroscopy activities by introducing the “Spatial Modulation Spectroscopy” (SMS) technique [*], which yields access to the quantitative absorption cross-section spectra and amplitude of a single nano-object with size down to a few nanometers. Its morphology being also independently determined by electron microscopy, this open the way to precise comparison with theoretical models.

We have investigated single nano-objects deposited on a transparent or opaque substrate (by using SMS in transmission or reflexion, respectively), as monometallic nanoparticles (Au, Ag), bimaterial nano-objects (Ag@SiO2, Au@Ag, …), metal dimers (Au-Ag@SiO2), single-wall carbon nanotubes and more complex nanosystems. These studies led to an increased comprehension of the physical processes governing the optical response of nanosystems, of dielectric and quantum confinements effects in metals and, more generally, of electromagnetic interactions at the nanoscale.

 

By combining SMS linear extinction measurements with a femtosecond pump-probe setup, we can characterize the ultrafast optical response of single isolated nanosystems, thus yielding novel information on the internal dynamical processes (ultrafast electron thermalization, electron-phonon energy transfer, acoustic dynamics, thermal coupling between nanoparticle and the external environment, origin of plasmonic nonlinearities in confined metal, …).

 

[*] SMS technique was developed in 2004 in collaboration between Bordeaux (using a laser source, N. Del Fatti & F. Vallée) and Lyon (using a white lamp source, J.R.Huntzinger & M.Broyer) research groups.

By combining SMS linear extinction measurements with a femtosecond pump-probe setup, we can characterize the ultrafast optical response of single isolated nanosystems, thus yielding novel information on the internal dynamical processes (ultrafast electron thermalization, electron-phonon energy transfer, acoustic dynamics, thermal coupling between nanoparticle and the external environment, origin of plasmonic nonlinearities in confined metal, …).

 

[*] SMS technique was developed in 2004 in collaboration between Bordeaux (using a laser source, N. Del Fatti & F. Vallée) and Lyon (using a white lamp source, J.R.Huntzinger & M.Broyer) research groups.

 

 

Selection of publications on the single nanoparticle spectroscopy

Selection of publications on the single nanoparticle spectroscopy

 

E. Pertreux, A. Lombardi, I. Florea, M. Spuch-Calvar, S. Gómez-Graña, D. Ihiawakrim, C. Hirlimann, O. Ersen, J. Majimel, M. Tréguer-Delapierre, M. Hettich, P. Maioli, A. Crut, F. Vallée, and N. Del Fatti

"Surface Plasmon Resonance of an Individual Nano-Object on an Absorbing Substrate: Quantitative Effects of Distance and 3D Orientation"

Advanced Optical Materials 4, 567 (2016)

 

A. Crut, P. Maioli, N. Del Fatti, and F. Vallée

"Optical absorption and scattering spectroscopies of single nano-objects"

Chemical Society Reviews 43, 3921-3956 (2014) (review)

 

 A. Lombardi, M. P. Grzelczak, A. Crut, P. Maioli, I. Pastoriza-Santos, L. M. Liz-Marzán, N. Del Fatti, and F. Vallée

"Optical Response of Individual Au-Ag@SiO2 Heterodimers"

ACS Nano 7, 2522–2531 (2013)

 

V. Juvé, M.F. Cardinal, A. Lombardi, A. Crut, P. Maioli, J. Pérez-Juste, L.M. Liz-Marzán, N. Del Fatti, and F. Vallée

"Size-Dependent Surface Plasmon Resonance Broadening in Nonspherical Nanoparticles: Single Gold Nanorods"

Nano Letters 13, 2234–2240 (2013)

 

J.-C. Blancon, M. Paillet, H. Nam Tran, X. Tinh Than, S. Aberra Guebrou, A. Ayari, A. San Miguel, N.-M. Phan, A.-A. Zahab, J.-L. Sauvajol, N. Del Fatti, and F. Vallée

"Direct measurement of the absolute absorption spectrum of individual semiconducting single-wall carbon nanotubes"

Nature Communications 4, 2542 (2013)

 

Y.R. Davletshin, A. Lombardi, M.F. Cardinal, V. Juvé, A. Crut, P. Maioli, L.M. Liz-Marzán, F. Vallée, N. Del Fatti, and J.C. Kumaradas

"A Quantitative Study of the Environmental Effects on the Optical Response of Gold Nanorods"

ACS Nano 8, 8183-8193 (2012)

 

H. Baida, D. Mongin, D. Christofilos, G. Bachelier, A. Crut, P. Maioli, N. Del Fatti, and F. Vallée

"Ultrafast nonlinear optical response of a single gold nanorod near its surface plasmon resonance"

Physical Review Letters 107, 057402 (2011)

 

O.L. Muskens, N. Del Fatti, and F. Vallée

"Femtosecond response of a single metal nanoparticle"

Nano Letters 6, 552 (2006)

 

A. Arbouet, D. Christofilos, N. Del Fatti, F. Vallée, J. R. Huntzinger, L. Arnaud, P. Billaud, and M. Broyer

"Direct Measurement of the Single-Metal-Cluster Optical Absorption"

Physical Review Letters 93, 127401 (2004)

 

 

Full list of publications of the FemtoNanoOptics group

Liste complète des publications de l'équipe FemtoNanoOptics

 

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