Résumé des cours

Lecture 1 & 2

Coherent phonon photogeneration processes in solids

Speaker: Pascal Ruello

Keywords:

Laser-matter interaction, electron-phonon coupling, optoacoustics; picosecond acoustics.

Summary:

In this lecture, we will discuss the generation processes of coherent phonons with ultrafast light pulses. This will be the core of the lectures. Some more recent research directions will be discussed at the end.

We will mainly discuss the coherent phonon frequency ranging from GHz to THz. The basics of optical properties of solids will be briefly reminded first. Then we will discuss the different electron-phonon coupling mechanisms for both optical and acoustic phonons photogeneration with a particular focus on acoustic phonon. For that, the out-of-equilibrium carriers dynamics will be described (two-temperature model, Boltzmann equation). We will discuss, for instance, the generation of coherent phonons with visible light (NIR-VIS-NUV), i.e. eV photon [1,3]. This will include the deformation potential mechanism (for both optical and acoustic phonons), the thermoelastic process (for acoustic phonon), the inverse-piezoelectric effect (for acoustic phonon) and the stimulated Raman-Brillouin process (optical-acoustic phonon). Different situations will be discussed in semiconductors [4], topological insulators [5], and ferroic materials [6], to cite a few. As a more recent research direction, we will also discuss the generation of coherent phonon with ultrashort THz pulses  i.e. meV photon) leading to optical phonon generation (IR active mode) and acoustic phonons [7]. Finally, by combining time-resolved optical methods and time-resolved X-ray diffraction [8], we will illustrate how it is possible to disentangle the photogeneration and the photodetection processes, and then how it is possible to evaluate more precisely the efficiency of the conversion of the light energy into the mechanical energy (optoacoustics), that we cannot access with full optical method only.


References:

1. C. Thomsen, H. T. Grahn, H. J. Maris, and J. Tauc, Surface generation and detection of phonons by picosecond light pulses, Phys. Rev. B 34, 4129 (1986).

2. P. Ruello and V.E. Gusev, Physical mechanisms of coherent acoustic phonons generation by ultrafast laser action. Ultrasonics, 2015. 56: p. 21-35.  doi.org/10.1016/j.ultras.2014.06.004.

3.  V. Gusev and A. Karabutov, Laser Optoacoustics (AIP, New York, 1993).

4. Baldini, E.; Dominguez, A.; Palmieri, T.; Cannelli, O.; Rubio, A.; Ruello, P.; Chergui, M. Exciton control in a room temperature bulk semiconductor with coherent strain pulses Science Advances, 2019, 5, eaax2937, DOI:10/ggq6zb

5. Weis, M., K. Balin, R. Rapacz, A. Nowak, M. Lejman, J. Szade, and P. Ruello, Ultrafast light-induced coherent optical and acoustic phonons in few quintuple layers of the topological insulator Bi2Te3. Phys. Rev. B, 2015. 92(1). doi.org/10.1103/PhysRevB.92.014301

6. Lejman, M., G. Vaudel, I.C. Infante, I. Chaban, T. Pezeril, M. Edely, G.F. Nataf, M. Guennou, J. Kreisel, V.E. Gusev, B. Dkhil, and P. Ruello, Ultrafast acousto-optic mode conversion in optically birefringent ferroelectrics. Nature Communications, 2016. 7. doi.org/10.1038/ncomms12345

7. A. Levchuk, B. Wilk, G. Vaudel, F. Labbé, B. Arnaud, K. Balin, J. Szade, P. Ruello, and V. Juvé, Coherent acoustic phonons generated by ultrashort terahertz pulses in nanofilms of metals and topological insulators, Phys. Rev. B 101, 180102(R) (2020)  doi.org/10.1103/PhysRevB.101.180102

8. V Juvé, R Gu, S Gable, T Maroutian, G Vaudel, S Matzen, N Chigarev, S Raetz, VE Gusev, M Viret, A Jarnac, C Laulhé, AA Maznev, B Dkhil, P. Ruello, Ultrafast light-induced shear strain probed by time-resolved x-ray diffraction: Multiferroic  as a case study, Phys. Rev. B, 102, 220303(R), (2020).

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LECTURE 3

(I)Time-domain Brillouin scattering: theoretical backgrounds and applications for nanoscale imaging and materials characterization

Speaker: Vitali E. Gusev

Keywords:

photoacoustics; optoacoustics; laser ultrasound; time-domain Brillouin scattering; picosecond acoustic interferometry; imaging; microscopy; vibrations of nanolayers and nanostructures 

Summary:

Time-domain Brillouin scattering (TDBS), also known as picosecond acoustic interferometry, is an experimental technique that uses ultrafast lasers for generation and detection of nanometer-scale coherent acoustic pulses with picosecond scale time duration. Detection involves interfering two weak probe light pulses: one scattered by the acoustic nanopulse propagating in transparent materials, and one reflected from various interfaces of the sample. Transient optical reflectivity recorded by a photodetector, as the acoustic nanopulse propagates, contains information on local acoustical, optical, and acousto-optical parameters of the material. TDBS imaging is based on Brillouin scattering and has potential to provide all information that researchers in materials science, physics, chemistry, biology etc., could get with classic frequency-domain Brillouin scattering. It can be viewed as a replacement for Brillouin microscopy in all investigations where nanoscale spatial resolution is required. TDBS has been already applied for imaging of nanoporous films, ion-implanted semiconductors/dielectrics, grain boundaries, metal-epoxy interfaces, vegetable and animal cells, texture in polycrystalline materials, temperature distributions in liquids, and for monitoring the transformation of nanosound caused by absorption, diffraction, nonlinearity and focusing. The first applications of shear acoustic waves in TDBS-based imaging have been recently reported. The theory of TDBS-based imaging suggests multiple perspectives for its further development.

 

References:

1. V. E. Gusev and P. Ruello, Advances in applications of time-domain Brillouin scattering for nanoscale imaging, Appl. Phys. Rev. 5, 031101 (2018); https://doi.org/10.1063/1.5017241.

2. J. D. G. Greener, E. de Lima Savi, A. V. Akimov, S. Raetz, Z. Kudrynskyi, Z. D. Kovalyuk, N. Chigarev, A. Kent, A. Patanè, and V. Gusev, High frequency elastic coupling at the interface of van der Waals nanolayers imaged by picosecond ultrasonics, ACS Nano 13 (10) 11530-11537 (2019); https://doi.org/10.1021/acsnano.9b05052

3. Y. Wang, D. H. Hurley, Z. Hua, T. Pezeril, S. Raetz, V. E. Gusev, V. Tournat & M. Khafizov, Imaging grain microstructure in a model ceramic energy material with optically generated coherent acoustic phonons, NATURE COMMUNICATIONS 11, 1597 (2020) ; https://doi.org/10.1038/s41467-020-15360-3

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LECTURE 4

(I)Picosecond Acoustics: from lab to fab

Speaker: Arnaud Devos

Keywords: picosecond acoustics,thickness control, thin-film, elasticity, adhesion, RFfilters

Summary :

The main goal of this lecture is to give an outlook of the numerous and various applications that the picosecond acoustic technique has met in the industrial world. The story started a few years after its invention by Prof. H. Maris. Indeed, Rudolph Technologies (now ONTO) rapidly realized that such a technique was the missing one in the industrial world for controlling the thickness of thin metal films. That was the beginning of the Metapulse® story, a full automatized tool dedicated to microelectronics applications and that can be found in any production company worthy of the name. More recently, picosecond acoustics and especially its variant based on laser-tuning, the so-called Colored Picosecond Acoustics or APiC, have been shown to be very useful for many other industrial applications in topics as different as space mirror, radio-frequency filtering, flat and smart glass, solar cells,…

References:

 [1].         A. DEVOS, “Colored Ultrafast Acoustics: from fundamentals to applications”, Ultrasonics 56, pp. 90-97  (2015) DOI 10.1016/j.ultras.2014.02.009

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LECTURE 5

(II)Time-domain Brillouin scattering: theoretical backgrounds and applications for nanoscale imaging and materials characterization

Speaker: Vitali E. Gusev

Keywords:

photoacoustics; optoacoustics; laser ultrasound; time-domain Brillouin scattering; picosecond acoustic interferometry; imaging; microscopy; vibrations of nanolayers and nanostructures 

Summary:

Time-domain Brillouin scattering (TDBS), also known as picosecond acoustic interferometry, is an experimental technique that uses ultrafast lasers for generation and detection of nanometer-scale coherent acoustic pulses with picosecond scale time duration. Detection involves interfering two weak probe light pulses: one scattered by the acoustic nanopulse propagating in transparent materials, and one reflected from various interfaces of the sample. Transient optical reflectivity recorded by a photodetector, as the acoustic nanopulse propagates, contains information on local acoustical, optical, and acousto-optical parameters of the material. TDBS imaging is based on Brillouin scattering and has potential to provide all information that researchers in materials science, physics, chemistry, biology etc., could get with classic frequency-domain Brillouin scattering. It can be viewed as a replacement for Brillouin microscopy in all investigations where nanoscale spatial resolution is required. TDBS has been already applied for imaging of nanoporous films, ion-implanted semiconductors/dielectrics, grain boundaries, metal-epoxy interfaces, vegetable and animal cells, texture in polycrystalline materials, temperature distributions in liquids, and for monitoring the transformation of nanosound caused by absorption, diffraction, nonlinearity and focusing. The first applications of shear acoustic waves in TDBS-based imaging have been recently reported. The theory of TDBS-based imaging suggests multiple perspectives for its further development.

 

References:

1. V. E. Gusev and P. Ruello, Advances in applications of time-domain Brillouin scattering for nanoscale imaging, Appl. Phys. Rev. 5, 031101 (2018); https://doi.org/10.1063/1.5017241.

2. J. D. G. Greener, E. de Lima Savi, A. V. Akimov, S. Raetz, Z. Kudrynskyi, Z. D. Kovalyuk, N. Chigarev, A. Kent, A. Patanè, and V. Gusev, High frequency elastic coupling at the interface of van der Waals nanolayers imaged by picosecond ultrasonics, ACS Nano 13 (10) 11530-11537 (2019); https://doi.org/10.1021/acsnano.9b05052

3. Y. Wang, D. H. Hurley, Z. Hua, T. Pezeril, S. Raetz, V. E. Gusev, V. Tournat & M. Khafizov, Imaging grain microstructure in a model ceramic energy material with optically generated coherent acoustic phonons, NATURE COMMUNICATIONS 11, 1597 (2020) ; https://doi.org/10.1038/s41467-020-15360-3

 

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LECTURE 6

Low frequency Raman scattering to probe nano-objects

 

Speaker: Alain Mermet

Keywords: Raman, Brillouin, nanoparticles, nanoplates

Summary :Halfway between Brillouin scattering and conventional Raman spectroscopy, low frequency Raman scattering allows to probe nano-objects through localized acoustic modes (also called Lamb modes) [1]. Initially uncovered as an original technique to evaluate the size of nanoparticles, low frequency Raman scattering has proved over the past two decades, thanks to continuous spectroscopic improvements and increased control of nanoparticle synthesis methods, to be able to probe fine details of nanostructures with diverse morphologies.

After discussing the specificity of low frequency Raman scattering with respect to Brillouin and conventional Raman spectroscopies, we will illustrate from recent examples how the low-frequency Raman probe allows to assess crystallinity in metallic nanocrystals [2], probe the elastic coupling in a nanoparticle dimer [2] and sense nanomass loads in semiconductor nanoplates [3].

 

References:

[1] L. Saviot, A. Mermet & E. Duval, "Nanoparticles and Quantum Dots, Handbook of Nanophysics", edited by K. D. Sattler (CRC Press, 2010) Chap. 11, pp. 11.1-11.17

[2] H. Portales; N. Goubet, L. Saviot, S. Adichtchev, DB  Murray, A.  Mermet, E. Duval, MP Pileni, PNAS, 14874 (2008)

[3] A. Girard, H. Gehan, A. Crut, A. Mermet, L.  Saviot, J. Margueritat, Nanoletters 6, 3843 (2016)

[3] A. Girard, L.  Saviot, S. Pedetti, MD Tessier, J. Margueritat, H. Gehan, B. Mahler, B. Dubertret, A.  Mermet, Nanoscale, 13251 (2016)

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LECTURE 7

Part I: Current understanding and unsolved problems in thermal transport at the nanoscale

Speaker: David Cahill

Keywords: Nanoscale thermal transport; time-domain thermoreflectance

Summary :

On length scales large compared to the mean-free-paths and equilibration lengths of the excitations that carrier heat, the diffusion equation is an accurate description of the relationship between temperature fields and heat fluxes. On small spatial and temporal scales, this simple description fails due to scattering of excitations by boundaries and the out-of-equilibrium distributions of heat carriers that are induced by heat flow across material interfaces.  In this lecture, I will provide an overview of what is known and not known in the physics of thermal transport at the nanoscale with an emphasis on experimental studies of dielectric and metallic crystals and their interfaces at temperatures near ambient.  I will also introduce the emerging area of thermally-driven generation and transport of spin in magnetic materials on ultrafast time-scales.

 

References:

Cahill et al., Nanoscale thermal transport II, Applied Physics Reviews 1, 011305 (2014).

Choi et al., Thermal spin-transfer torque driven by the spin-dependent Seebeck effect in metallic spin-valves, Nature Physics 11, 576-581 (2015).

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LECTURE 8

Part II: Measurement of thermal transport coefficients at the nanoscale

Speaker: David Cahill

Keywords: Nanoscale thermal transport; time-domain thermoreflectance

Summary :

I will discuss the use of time-domain thermoreflectance (TDTR) for measurements of thermal transport properties of materials and material interfaces and compare the capabilities and limitations of TDTR to other methods that are widely used in studies of nanoscale thermal transport: the 3-omega method, transient thermal gratings, frequency domain thermoreflectance, and microfabricated test platforms.  I will discuss the basic implementation of the TDTR method, the analysis of the data based on the diffusion equation and radiative boundary conditions at interfaces, and evaluation of uncertainties.  I will then discuss extensions of TDTR to include lateral heat flow, two-channel modeling of non-equilibrium effects, spot size and frequency dependence of the apparent value of the transport coefficients and the use of the time-resolved magneto-optic Kerr effect as an alternative to thermoreflectance for sensing temperature changes at the surface of a sample.

References:

Cahill, Analysis of heat flow in layered structures for time-domain thermoreflectance, Review of Scientific Instruments 75, 5119-5122 (2004).

Jiang et al., Tutorial: Time-domain thermoreflectance (TDTR) for thermal property characterization of bulk and thin film materials, Journal of Applied Physics 124, 161103 (2018).

 

 

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LECTURE 9

(II)Picosecond Acoustics: from lab to fab

Speaker: Arnaud Devos

Keywords: picosecond acoustics,thickness control, thin-film, elasticity, adhesion, RFfilters

Summary :

The main goal of this lecture is to give an outlook of the numerous and various applications that the picosecond acoustic technique has met in the industrial world. The story started a few years after its invention by Prof. H. Maris. Indeed, Rudolph Technologies (now ONTO) rapidly realized that such a technique was the missing one in the industrial world for controlling the thickness of thin metal films. That was the beginning of the Metapulse® story, a full automatized tool dedicated to microelectronics applications and that can be found in any production company worthy of the name. More recently, picosecond acoustics and especially its variant based on laser-tuning, the so-called Colored Picosecond Acoustics or APiC, have been shown to be very useful for many other industrial applications in topics as different as space mirror, radio-frequency filtering, flat and smart glass, solar cells,…

References:

 [1].         A. DEVOS, “Colored Ultrafast Acoustics: from fundamentals to applications”, Ultrasonics 56, pp. 90-97  (2015) DOI 10.1016/j.ultras.2014.02.009

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LECTURE 10

High-Brightness Ultrafast Transmission Electron Microscopy: Applications to Nano-optics and Nanomechanics

Speaker: Arnaud Arbouet

Keywords: Ultrafast Transmission Electron Microscopy, nano-optics, electron energy gains, acoustic vibrations

Summary (5 to 10 lines):

Nanosized systems have optical properties that can differ significantly from their bulk counterpart due to the existence of optical resonances such as surface plasmons in metallic nanoparticles or Mie modes in high refractive index nanostructures. These excitations have extremely short lifetimes (fs-ns) and pattern the optical near-field on subwavelength scales.

Ultrafast Transmission Electron Microscopes (UTEM) combining sub-picosecond temporal resolution and nanometer spatial resolution have emerged as unique tools for investigations at ultimate spatio-temporal resolution [1,2]. In this talk, I will report on the development of a high-brightness UTEM and discuss its potential in nano-optics and nanomechanics [3,4]. In particular, I will report on Electron Energy Gain Spectroscopy experiments performed in a UTEM that allow mapping the optical near-field at the nanometer scale and discuss the potential of electron diffraction and holography experiments performed with femtosecond electron pulses to explore the vibrational dynamics of nanoscale systems.

 References:

[1] 4D Electron Microscopy, Imaging in Space and Time, 2009 Ahmed H Zewail and John M Thomas (Cambridge)

 [2] Ultrafast Transmission Electron Microscopy : fundamentals, instrumentation and applications
Arnaud Arbouet, Giuseppe M. Caruso, Florent Houdellier
Advances in Imaging and Electron Physics, Advances in Electronics and Electron Physics, 207, Elsevier, 2018, 1076-5670, 2018

 [3] Development of a high brightness ultrafast Transmission Electron Microscope based on a laser-driven cold field emission source
F. Houdellier, Giuseppe Mario Caruso, Sébastien Weber, Mathieu Kociak and Arnaud Arbouet
Ultramicroscopy, 186, 128-138, 2018

 [4] High brightness ultrafast transmission electron microscope based on a laser-driven cold-field emission source: principle and applications
G.M. Caruso, F Houdellier, S Weber, M Kociak, A Arbouet
Advances in Physics: X 4 (1), 1660214, 2019

 


 

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LECTURE 11

An introduction to nanomechanics

Speaker: Eva Weig

Keywords: mechanical resonators, nanomechanical systems, flexural modes

Summary (5 to 10 lines):

Nano- or micromechanical resonators are freely suspended structures with discrete vibrational eigenmodes, such as, e.g., the flexural modes of a string or a membrane. These resonators are receiving an increasing amount of attention for a broad range of possible applications, ranging from practical sensing to fundamental challenges addressing the foundations of quantum mechanics. This lecture will review the basics of nanomechanical resonators, and present some fields of use, including the thriving field of cavity optomechanics.

References:

M. Poot & H. S. J. van der Zant, Mechanical systems in the quantum regime, Phys. Rep. 511, 273 (2012).

M. Aspelmeyer, T. J. Kippenberg & F. Marquardt, Cavity optomechanics, Rev. Mod. Phys. 86, 1391 (2014).

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LECTURE 12

Biosensors based on optonanomechanical systems

Speaker: Monserrat Calleja

Keywords: biosensors, nanomechanics, optomechanics

Summary :

We will be discussing the application of optomechanics to biology and biomedicine, as well as how strategies inspired by these phenomena can be applied to microscale devices for cancer cell characterization, for the detection of attogram per mililliter concentrations of protein biomarkers in the exploration of the deep plasma proteome and for the identification of pathogens through their intrinsic mechanical properties.

References:

[1] Biosensors based on nanomechanical systems, J Tamayo at al, Chemical Society Reviews 42 (3), 1287 (2013)

[2]Mass and stiffness spectrometry of nanoparticles and whole intact bacteria by multimode nanomechanical resonators

O Malvar, JJ Ruz, PM Kosaka, CM Domínguez, E Gil-Santos, M Calleja, J Tamayo, Nature communications 7, 13452 (2016)

[3]Silicon nanowires: where mechanics and optics meet at the nanoscale, D Ramos, E Gil-Santos, O Malvar, JM Llorens, V Pini, A San Paulo, M Calleja, J Tamayo, Scientific reports 3, 3445 (2013)

[4] Optomechanics with silicon nanowires by harnessing confined electromagnetic modes, D Ramos, E Gil-Santos, V Pini, JM Llorens, M Fernández-Regúlez, A San Paulo, M Calleja, J Tamayo, Nano letters 12 (2), 932-937 (2012)

[5]Mechano-optical analysis of single cells with transparent microcapillary resonators, A Martín-Pérez, D Ramos, E Gil-Santos, S García-López, ML Yubero, PM Kosaka, A San Paulo, J Tamayo, M Calleja, ACS sensors 4 (12), 3325-3332, 2019

 [6]Detection of cancer biomarkers in serum using a hybrid mechanical and optoplasmonic nanosensor, PM Kosaka, V Pini, JJ Ruz, RA Da Silva, MU González, D Ramos, M Calleja, J Tamayo, Nature nanotechnology 9 (12), 1047 (2014)

 [7]Optomechanical devices for deep plasma cancer proteomics, PM Kosaka, M Calleja, J Tamayo, Seminars in cancer biology 52, 26-38 (2018)

 [8] Gil-Santos, E., Ruz, J.J., Malvar, O. et al. Optomechanical detection of vibration modes of a single bacterium. Nat. Nanotechnol. 15, 469–474 (2020). https://doi.org/10.1038/s41565-020-0672-y

 [9] Juan Molina, Daniel Ramos, Eduardo Gil-Santos, Javier E. Escobar, José J. Ruz, Javier Tamayo, Álvaro San Paulo, and Montserrat Calleja. Optical Transduction for Vertical Nanowire Resonators. Nano Letters 2020 20 (4), 2359-2369. DOI: 10.1021/acs.nanolett.9b04909

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LECTURE 13

Stimulated Brillouin scattering microscopy for mechanical imaging of cells and organisms

Speaker: Alberto Bilenca

Keywords: Stimulated Brillouin scattering, microscopy, biomechanics

Summary: The mechanical properties of biological systems, such as cells and organisms, play a major role in their function and development. One established technique for assessing biomechanics is atomic-force microscopy, but it requires contact with the sample. Recently, Brillouin microscopy has been developed for biomechanical imaging with no sample contact or external mechanical stimulus. Whereas most of the development efforts in Brillouin microscopy have used spontaneous Brillouin scattering as the contrast mechanism, I will introduce here a new approach for high sensitivity and specificity, noncontact, biomechanical-contrast imaging based on stimulated Brillouin scattering (SBS). The physical working principles of the method and its use in biological settings will be described and discussed in detail.

 References:

Itay Remer, Roni Shaashoua, Netta Shemesh, Anat Ben-Zvi, Alberto Bilenca, “High-sensitivity and high-specificity biomechanical imaging by stimulated Brillouin scattering microscopy,” Nat Methods 17, 913-916 (2020).

Itay Remer, Lear Cohen, Alberto Bilenca, “High-speed continuous-wave stimulated Brillouin scattering spectrometer for material analysis,” J Vis Exp 127, 55527 (2017).

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LECTURE 14

Picosecond Acoustics: a Laser Pump-Probe Technique for the Determination of Thermo-Elastic Properties of Solids and Liquids at High Pressure and High Temperature

Speaker: Silvia Boccato

Keywords: picosecond acoustics, elastic constants, sound velocity, high pressure, high temperature

Summary :Picosecond acoustics is a time-resolved optical pump-probe technique that allows studying the propagation of acoustic echoes in a large variety of samples at different pressure and temperature conditions. With this technique we can access melting curves, the complete set of elastic moduli for single crystals and longitudinal velocities for polycrystalline samples.

I will illustrate the importance of these experiments for Earth and planetary science, providing examples of studies with a direct interest in these fields, including measurements on iron and iron alloys, metallic liquids, hydrogen and deuterium.

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LECTURE 15

 

 

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LECTURE 16

 

 

 

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LECTURE 17

Measurements of sound absorption and phonon lifetimes with picosecond ultrasonics technique

Speaker: Bernard Perrin (Sorbonne Université, CNRS, Institut des NanoSciences de Paris, INSP, F-75005 Paris, France.)

Keywords:Picosecond ultrasonics, acoustic attenuation, phonon mean free path, phonon lifetime

Summary

Attenuation of acoustic waves can be a limiting factor in many areas such as high frequency acoustic imaging, surface wave devices or very high quality factor resonators. Picosecond ultrasonics technique offers a very good opportunity to perform attenuation measurements over a wide frequency and temperature range. This lecture will start with a brief discussion of the different regimes of sound absorption which occur according to the frequency and temperature domains. The second part will be devoted to the different configurations which can be used to measure this parameter in pump probe experiments. The many artefacts that can interfere with the measurements will be discussed in detail. At the end, a review of experimental results, obtained on different systems (thin films bulk materials, membranes, resonators) and different materials (crystals, amorphous systems, quasi-crystals), will be given.

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LECTURE 18

Vibrational and Cooling Dynamics of Metal Nanoparticles:

Optical Investigations and Modeling

Speaker: Aurelien Crut

Keywords: metal nanoparticles, time-resolved spectroscopy, vibration modes, single-particle spectroscopy, interfacial phonon transfer, plasmonics

Summary:

Nano-objects exhibit discrete vibrational modes, which can be monitored in the time domain using ultrafast optical pump-probe spectroscopy. This enables both the design of artificial nanoresonators with frequencies reaching the THz domain and fundamental investigations of the laws governing acoustics at the nanoscale. In particular, measuring the frequencies of the vibrational modes of small nanoparticles (with sizes down to few atoms) allows one to test the accuracy of their description using continuum elasticity theory. Their damping is usually dominated by energy transfer from the nano-objects to their environment (a mechanism also ruling nano-object cooling), its investigation ideally requiring measurements at the single-particle level to avoid the inhomogeneous broadening effects affecting ensemble experiments.

In this talk, after discussing the vibrational and cooling dynamics of nano-objects, I will present their investigation by time-resolved pump-probe spectroscopy of ensembles of nano-objects and single ones, as well as their modeling using analytical and numerical approaches.

References:

 1)     A. Crut, P. Maioli, N. Del Fatti and F. Vallée Optical absorption and scattering spectroscopies of single nano-objects Chem. Soc. Rev. 43, 3921 (2014).

2)     A. Crut, P. Maioli, N. Del Fatti and F. Vallée Acoustic vibrations of metal nano-objects: time-domain investigations Phys. Rep. 549, 1 (2015).

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LECTURE 19 & 20

Raman Imaging

Speaker: Hervé Rigneault

Keywords: Vibrational imaging, Raman imaging, Coherent Raman Imaging

Summary :

I will review and present the basics and technical implementations of Raman imaging and coherent Raman imaging. I will exemplify the methods in compressive spontaneous Raman for fast chemical spectroscopy and imaging. To reach higher frame rate, I will present the latest development in coherent Raman both in the high and low frequency ranges.  Finally I will present our effort to push Raman imaging in endoscopes.

References:

TUTORIALS:

H. Rigneault, and P. Berto, "Tutorial: Coherent Raman light matter interaction processes," APL Photonics 3, 091101 (2018). https://doi.org/10.1063/1.5030335

X. Audier, S. Heuke, P. Volz, I. Rimke, and H. Rigneault, "Noise in stimulated Raman scattering measurement: From basics to practice," APL Photonics 5, 011101 (2020).https://doi.org/10.1063/1.5129212

X. Audier, N. Forget, and H. Rigneault, "High-speed chemical imaging of dynamic and histological samples with stimulated Raman micro-spectroscopy," Optics Express 28, 15505-15514 (2020). https://doi.org/10.1364/OE.390850_________________________________________________________________________________

LECTURE 21

Sensing with plasmons and Raman scattering

Speaker: Nathalie Lidgi-Guigui

Keywords: Plasmons, Raman scattering, Surface Enhanced Raman Scattering, biosensing, sensing

Summary :

During this course I will start by briefly presenting the physics of surface and localised plasmons. I will then present how these localized surface plasmons can be used to enhance Raman scattering. In a second part I will discuss the notion of molecular detection based on plasmons and Raman spectroscopy. I will consider in particular the detection of biomolecules in complex media such as blood or urine. For this I will introduce very basics notions of molecular biology and surface chemistry.

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LECTURE 22

Brillouin and Raman spectroscopy to investigate metastable water

Speaker: Frédéric Caupin

Keywords: Brillouin spectroscopy, Raman spectroscopy, water, metastability, equation of state

Summary :

As any liquid, water can be prepared in a metastable liquid state: supercooled below the ice-liquid equilibrium temperature, or stretched below the liquid-vapor equilibrium pressure, down to negative pressure. The properties of water in these states is key to understanding the origin of its anomalies. However, measuring these properties is challenging because external perturbations can easily nucleate the more stable phase. Non-intrusive optical measurements are thus a tool of choice. This lecture will describe two examples: accurate size measurement of supercooled evaporating droplets with Raman spectroscopy [1], and equation of state at negative pressure with Brillouin spectroscopy [2,3,4].

References:

[1] C. Goy et al. Shrinking of rapidly evaporating water microdroplets reveals their extreme supercooling. Phys. Rev. Lett., 2018, 120, 015501.

[2] G. Pallares et al. Anomalies in bulk supercooled water at negative pressure. Proc. Natl. Acad. Sci. USA, 2014, 111, 7936-7941.

[3] G. Pallares et al. Equation of state for water and its line of density maxima down to
-120 MPa. Phys. Chem. Chem. Phys. 2016, 18, 5896-5900.

[4] V. Holten et al. Compressibility anomalies in stretched water and their interplay with density anomalies. J. Phys. Chem. Lett., 2017, 8, 5519–5522.

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LECTURE 23

Picosecond ultrasonic microscopy to image the cell mechanics and probe its nanostructure

 

Speaker: Bertrand Audouin

Summary: This presentation will review the current state of the art solutions offered by the picosecond ultrasonic technique to achieve single cell microscopy. Among them is the time domain Brillouin spectroscopy that allows probing ultrasound propagation along the cell depth. When coupled with convenient scanning devices and fast acquisition systems the technique allows for imaging several mechanical properties with an in-plane resolution equal to that provided by standard optics. The current and foreseen applications in biology and medicine will be discussed.

 

References:

C. Rossignol et al. Appl. Phys. Lett. 93,123901, 2008

T. Dehoux et al., Scient. Rep. 5, 8650, 2015

S. Danworaphong et al. Appl. Phys. Let. 106, 163701, 2015

F. Perez-Cota et al. Scient. Rep. 6, 39326, 2016

A. Viel et al. Appl. Phys. Let. 115, 213701, 2019

L. Liu et al. J. of Biophot. 201900045, 2019

L. Liu et al. Scient. Rep. 9, 6409, 2019

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LECTURE 24

Vibrational spectroscopy in the acoustic band:
from Gravitational Waves to relaxations in amorphous materials

Speaker: Gianpietro Cagnoli

Keywords: Vibrational spectroscopy, mechanical response, thermal noise, interferometry, gravitational waves, glasses, relaxations

Summary: Thanks to the combined non-linear response of the interferometer and its photodetector the space-time ripples known as Gravitational Waves are able to phase modulate the light. Details about this interaction of light with that special sound of the space-time will be presented and the advantages of using this new probe to study the Universe will be shown.

One of the main limit to the detection of GW comes from the thermally driven relaxations inside the materials that are able to randomly change the shape of the objects like the mirrors used in the GW detectors. The interaction of light with matter is able to detect the vibrations of both the proper modes of the solid body and that of the molecular structure. Detail of how this two types of light-sound interaction will give information on the structural relaxations inside an amorphous material will be given.

 

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LECTURE 25

Extreme Nanocavities

Speaker: Jeremy Baumberg

Keywords: nanocavity, picocavity, nanoparticle-on-mirror, MIM dispersion, nano-optics

 

Summary :

The properties of now-routinely-available nano-optical cavities will be discussed, and their use in various experiments reviewed. In particular, we will focus on nanoparticle-on-mirror and similar nanogap metal-insulator-metal architectures, to discuss field confinement, cavity volume, input/output coupling, and scaling. We will use this to describe enhancements in SERS, light emission, two-photon-absorption and their application to various societal challenges.

References:

Extreme nanophotonics from ultrathin metallic gaps, Nature Materials 18, 668 (2019); DOI: 10.1038/s41563-019-0290-y

Plasmonic nanocavity modes: from near-field to far-field radiation, ACS Phot. (2020); DOI: 10.1021/acsphotonics.9b01445

Breaking the selection rules of spin-forbidden molecular absorption in plasmonic nanocavities, ACS Photonics (2020);  DOI: 10.1021/acsphotonics.0c00732

Cascaded Nano-Optics to Probe Microsecond Atomic Scale Phenomena, PNAS (2020);  DOI 10.1073/pnas.1920091117

Efficient generation of two-photon excited phosphorescence from molecules in plasmonic nanocavities, Nano.Lett. (2020); DOI: 10.1021/acs.nanolett.0c01593

Optical probes of molecules as nano-mechanical switches, Nature Comm 11:5905 (2020); DOI: 10.1038/s41467-020-19703-y
Real-Time In-Situ Optical Tracking of Oxygen Vacancy Migration in Memristors, Nature Electronics (2020); DOI: 10.1038/s41928-020-00478-5

Mechanistic study of immobilised molecular electrocatalyst by in-situ gap plasmon assisted spectro-electrochemistry, Nature Catalysis (2020); DOI: 10.1038/s41929-020-00566-x

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LECTURE 26

The Physics and Applications of high Q optical microcavities: Cavity Quantum Optomechanics

Speaker: Tobias J. Kippenberg

Keywords:quantum optomechanics, microresonator

In this talk, I will describe a range of optomechanical phenomena that we observed using high Q optical microresonators. Radiation pressure back-action of photons is shown to lead to effective cooling(1, 2, 10, 11) of the mechanical oscillator mode using dynamical backaction. Sideband resolved cooling, combined with cryogenic precooling enables cooling the oscillators such that it resides in the quantum ground state more than 1/3 of its time(1,2). Increasing the mutual coupling further, it is possible to observe quantum coherent coupling(1,2) in which the mechanical and optical mode hybridize and the coupling rate exceeds the mechanical and optical decoherence rate (7). This regime enables a range of quantum optical experiments, including state transfer from light to mechanics using the phenomenon of optomechanically induced transparency(1,3). Moreover, the optomechanical coupling can be exploited for measuring the position of a nanomechanical oscillator in the timescale of its thermal decoherence(1,4), a basic requirement for preparing its ground-state using feedback as well as (Markovian) quantum feedback.

References:

1.V. B. Braginsky, S. P. Vyatchanin, Low quantum noise tranquilizer for Fabry-Perot interferometer. Physics Letters A 293, 228 (Feb 4, 2002).
2. V. B. Braginsky, Measurement of Weak Forces in Physics Experiments. (University of Chicago Press, Chicago, 1977).
3. T. J. Kippenberg, H. Rokhsari, T. Carmon, A. Scherer, K. J. Vahala, Analysis of Radiation-Pressure Induced Mechanical Oscillation of an Optical Microcavity. Physical Review Letters 95, 033901 (2005).
4. T. J. Kippenberg, R. Holzwarth, S. A. Diddams, Microresonator-based optical frequency combs. Science 332, 555 (Apr 29, 2011).
5. P. Del'Haye et al., Optical frequency comb generation from a monolithic microresonator. Nature 450, 1214 (Dec 20, 2007).
6. T. Herr et al., Temporal solitons in optical microresonators. Nature Photonics 8, 145 (2013).
7. V. Brasch et al., Photonic chip–based optical frequency comb using soliton Cherenkov radiation. Science 351, 357 (2016).
8. M. Aspelmeyer, T. J. Kippenberg, F. Marquardt, Cavity optomechanics. Reviews of Modern Physics 86, 1391 (2014).
9. T. J. Kippenberg, K. J. Vahala, Cavity optomechanics: back-action at the mesoscale. Science 321, 1172 (Aug 29, 2008).
10. A. Schliesser, P. Del'Haye, N. Nooshi, K. J. Vahala, T. J. Kippenberg, Radiation pressure cooling of a micromechanical oscillator using dynamical backaction. Physical Review Letters 97, 243905 (Dec 15, 2006).
11. A. Schliesser, R. Rivière, G. Anetsberger, O. Arcizet, T. J. Kippenberg, Resolved-sideband cooling of a micromechanical oscillator. Nature Physics 4, 415 (2008).

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LECTURE 27

Brillouin Imaging:
application to the mechanical characterization of cells and tissues

 

Speaker: Maurizio Mattarelli

Keywords:Brillouin spectroscopy, Elastography, Phonons.

Summary :Brillouin imaging is an emerging optical elastography technique that is able to generate maps of the mechanical properties at microscale with great potential in biophysical and biomedical fields. In this lecture I will review the fundamentals of the technique and show some applications to biological matter. In particular I will present few examples where, the combined use of Raman and Brillouin complementary techniques provided mechanical and chemical functional maps of inherently heterogeneous biological samples.

 

References:

1)    Relevant length scales in Brillouin imaging of biomaterials: the interplay between phonons propagation and light focalization, M Mattarelli, M Vassalli, S Caponi,
ACS Photonics 7 (9), 2319-2328, 2020

2)    On the actual spatial resolution of Brillouin Imaging,
S Caponi, D Fioretto, M Mattarelli, Optics Letters 45 (5), 1063-1066, 2020

3)    Non-contact mechanical and chemical analysis of single living cells by microspectroscopic techniques, S Mattana et al
Light: Science & Applications 7 (2), 17139, 2018

4)    Mechano-chemistry of human femoral diaphysis revealed by correlative Brillouin–Raman microspectroscopy, MA Cardinali et al, Scientific Reports 10 (1), 1-11, 2020

 

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LECTURE 28

Phonons in biology: from phenotyping to design

Speaker: Thomas Dehoux

Summary : The mechanics of cells and tissues are key players in many biological processes, such as embryogenesis or differentiation. Alteration of inherent mechanical properties or abnormal mechanical cues can lead to the development of degenerative diseases, including cancer. In the first part of this lecture I will show how phonons can be used to probe the mechanical phenotype of biological sample and monitor their fate.  In the second part, I will show the phenotype of cells can be hijacked to manipulate phonons. I will describe how such approaches can be used to create innovative acoustic materials, and fuel a new type of bioeconomy.

 

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LECTURE 29

Brillouin Scattering of Novel Materials: From the Solid State to the Biological

Speaker: Kristie Koski

Keywords: Brillouin scattering

Summary :

Brillouin scattering spectroscopy is an extraordinarily powerful technique to measure acoustic phonons of a vast array of materials ranging from the biological to the solid state.  In this talk, I will show application of Brillouin spectroscopy to a wide variety of problems including 2D nanomaterials, biological materials, and topological insulators. Often the complex nature of these materials, coupled with their small size and hierarchical nature, makes studying elasticity and acoustic phonons difficult. Specifically, I will show how it is possible to use Brillouin scattering to determine mechanical properties of lightweight nacre and sea sponges - marine biomaterials whose remarkable mechanical properties were shaped by environmental pressures. I will demonstrate solid state application including chemically tunable acoustic phonons in 2D materials such as Bi2Se3 and MoO3. Finally, I will show how Brillouin light scattering can be used to obtain the complete stiffnesses, sound velocities, acoustic phonon dispersion relations, refractive indices, and linear elastic properties of novel materials to address a diverse array of physical problems.

References:

B.W. Reed, D.R. Williams, B.P. Moser, and K.J. Koski, Chemically tuning quantized acoustic phonons in 2D layered MoO3 nanoribbons. Nano Letters 19, 4406-4412 (2019)

B.W. Reed, V. Huynh, C. Tran, and K.J. Koski, Brillouin scattering of V2O5 and Sn-intercalated V2O5. Physical Review B 102, 054109 (2020)

D. Radhakrishnan, M. Wang, K. J. Koski, Correlation between color and elasticity in Anomia ephippium shells: Biological design to enhance the mechanical properties, ACS Applied Bio Materials, 3, 9012-9018 (2020).

Y. Zhang, B.W. Reed, F.R. Chung, K.J. Koski, Mesoscale elastic properties of marine sponge spicules. J. Struct. Biol. 193, 67-74 (2016).

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LECTURE 30

From phonons to lattice thermal conductivity

 

Speaker: Stéphane Pailhès

Keywords:phonon, inelastic spectroscopy, neutrons, X-rays, lattice thermal conductivity

Summary : The understanding of the lattice thermal conductivity requires the knowledge of the phonon energies and lifetimes in the whole phase space in momentum and in energy (q,ħω). In this lecture, I will present the neutrons and X-rays inelastic spectroscopy techniques currently used for mapping the phonon spectrum, specifically illustrating their technical limitations [1-2]. We will follow the cases of the phonon dynamics in some complex thermoelectric crystalline phases and show how the structural complexity led to very low and almost temperature independent lattice thermal conductivity [2-5]. After going through the experimental measurements, we will see the link between the microscopic description and the macroscopic heat conduction using simple models and comparing with state-of-the-art ab initio simulations [2,6].  

 

References:

[1]X-Rays and Neutrons Spectroscopy for the Investigation of Individual Phonons Properties in Crystalline and Amorphous Solids” S. Pailhès et al., chapter 19, p. 517 in the book “Nanostructured Semiconductors: Amorphization and Thermal Properties” Ed. by K. Termentzidis, CRC Press  (2017)

[2]«Direct measurement of individual phonon lifetimes in the clathrate compound Ba7.81Ge40.67Au5.33 », P.-F. Lory, S. Pailhès et al.  Nat. Comm. 8,491 (2017)

[3]« Impact of temperature and mode polarization on the acoustic phonon range in complex crystalline phases: A case study on intermetallic clathrates » S. Turner Phys. Rev. Res. 3, 013021 (2021)

[4]« Reduced phase space of heat-carrying acoustic phonons in single-crystalline InTe » Shantanu M et al. Phys. Rev. Res. 2, 043371 (2020)

[5] « Anisotropic low-energy vibrational modes as an effect of cage geometry in the binary barium silicon clathrate Ba24Si100 » R Viennois et al., Phys. Rev. B 101 (22), 224302 (2020)

[6]« Understanding lattice thermal conductivity in thermoelectric clathrates: A density functional theory study on binary Si-based type-I clathrates », H. Euchner et al., Phys. Rev. B 97, 014304 (2018)

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LECTURE 31

Nanocomposites and nanophononic materials: the role of interfaces on phonon propagation and thermal transport

Speaker: Valentina Giordano

Keywords:phonons, disorder, nanostructure, nanocomposites

Summary :

In the last decades, nanocomposites and nanophononic materials, made of the random or periodic intertwining at the nanoscale of materials with different elastic properties, have arisen as major players in applications where thermal management is needed. Indeed, depending on the properties of the constituents, thermal conductivity can be greatly enhanced or drastically reduced, with almost no effect on other functional properties1. At this day, a microscopic understanding of phonon propagation and thermal transport in such materials is still partial. In this lecture, I will present the state of the art of such understanding, as can be achieved by coupling macroscopic thermal transport measurements and microscopic investigation of phonon dynamics.

References:

[1] Y. Nakamura et al. Nano Energy 12, 845 (2015) ; L. Zhang et al., Composites Comm. 8,74 (2018)

 

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