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1.1 The response function of metals to an optical excitation : intraband and interband transitions, transverse dielectric function of metals. Scattering of light by small metallic particles : theory of Mie, the effective medium response, surface plasmons. 1.2 General motivations, Magneto-optics of metals : Kerr and Faraday magneto-optical responses; Superparamagnetism of nanoparticles : Nel and Brown models

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Lycurgus Cup (Roman period : 4th century) exhibited at the British Museum.

Reflection

Transmission

Seoul - 2009 - Jean-Yves Bigot - Winter_school_IPCMS-QMMRC

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Gold and silver salts were used in medieval times to color glass used in church windows. For example, silver particles were used to stain glass yellow, while gold particles were used to stain glass red.

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planar X-ray imaging: Kidneys in live mouse 60 minutes after intravenous injection

Au nanoparticles Iodine contrast medium

Ureter : 100 nm

70 mm

Courtesy : www.nanoprobes.com

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Optimizing chemical reactions over an energy barrier Energy

Without catalyst

Au

Reactants

with catalyst

Products

Au nanoparticle on oxide substrate. CO and CO2 molecules react on the surface of the nanoparticle

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What is the effect of 2D and 3D self-organization on optical and magneto-optical properties ?

Electron microscopy image : mono-layer of self organized cobalt nanoparticules Fourier transform : hexagonal order

Collaboration : LM2N - Universit Pierre et Marie Curie Paris ; (I. Lisiecki, C. Petit, M.-P. Pilni)

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Faraday was the first to report what later came to be called metallic nanoparticles. In 1847 he discovered that the optical properties of gold colloids differed from those of the corresponding bulk metal. This was probably the first reported observation of the effects of size, and might be considered to be the birth of nanoscience

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1.1 The response function of metals to an optical excitation : intraband and interband transitions, transverse dielectric function of metals. Scattering of light by small metallic particles : theory of Mie, the effective medium response, surface plasmons. 1.2 General motivations, Magneto-optics of metals : Kerr and Faraday magneto-optical responses; Superparamagnetism of nanoparticles : Nel and Brown models

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Consider N nanoparticles in an external electric field E, with a dielectric function . It is an effective medium with dielectric function eff

-P

Then the polarization Pind, induced in the medium and the local field Eloc are:

ind,

Eloc

+ + + +

( 0 ) E Pind = 3N 0 ( + 2 0 ) loc

Pind = 0E + 3 0

( 0 ) eff = 0 + 3N 0 ( + 2 0 )

y s n e d l a i t p O c

Resonance if :

e ( ) = 2 0

IP

CM

When does the condition for resonance occur ? and what is its effect on the optical properties ?

e ( ) = 2 0

Consider n electrons of mass m in an external field Ecos(t)

d x dx m 2 + m = eE dt dt

P = nex

(polarization)

D( ) P( ) metal ( ) = = 1 + 4 E ( ) E ( )

2 p

4ne 2 1 metal ( ) = 1 = 1 m ( + i ) ( + i )

2 p

4ne 2 = m

p : Volume

Plasmon resonance

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for metals (1/) = ~10-14 s, so typically for h ~ 2 eV (wavelength ~ 600 nm) : 22 >> 1

2 p e ( ) 1 2

2 2 p p m ( ) 3 = 3

10

Absorption of nanoparticles

absorption (a.u.)

5 0

2 1

0 2 4 6 8

1.0

0.5

- 20 -5

-10

= p

10 12

0.0

h (eV)

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e [ ( )] = 2 0

h (eV)

Au Ag Cu

Ag : 6.5 nm Au : 25 nm Cu : 10 nm

400

500

600

700

Wavelength (nm)

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from : Materials Chemistry and Physics 113 (2009) 276282 Au mole fraction max (nm) Particle size (nm) Zeta-potential (mV) Conductance (S) Emission peak

29 27 32 26 26 44

12 2 7 13 17 28

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What are the important parameters for the surface plasmon peak position and width of the resonance :? () is more complicated than just Drude theory Even with Drude theory, what is the meaning of damping ? What is the role of the size and shape of the particles ? What does self - organization do ?

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Classical model of conduction electrons : DRUDE model of non-interacting electrons Based on kinetic equation for n electrons (e, m) in a field E (Ecost).

p 4ne 2 1 = 1 D ( ) = 1 m ( + i ) ( + i )

2

2 p

4 ne 2 = m

100

100 10

e |D| m (D) -m (1/D)

50

1

0

0.1

0.0 0.5 1.0

-50

/ p

1.5

0.01

0.0

0.5

1.0 / 1.5

p

e (D) = 0 for = p

- for 0 1 for

m (D) ~ 0 for = p

for 0 0 for

Optical absorption

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ih

= [H , ] ; H = H 0 + H int (r, t) t e H int (r, t) = p(r ).A (r ) Coulomb Gauge (.A = 0) 2mc

H o kl = Ekl kl and o kl = f o ( Ekl ) kl k: wave vector, l : band kl eigenstates Ekl E F k BT f o ( Ekl ) = 1 / 1 + e EF : Fermi energy

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ih

kl 1 k + q, l ' t

For an adiabatic field excitation : A(q,t) is harmonic : A(q,t) = A(q) exp(-i+)t then the matrix elements are :

Note the damping parameter , which assures that A 0 when t -

kl 1 k + q, l ' =

S

[ f o ( Ek + q ,l ' ) f o ( Ekl )]

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Diamagnetic response Paramagnetic response

J ( q, ) =

i ( - 1) : conductivity ( q, ) A ( q ) ; = c 4i

4e 2 0 4e 2 lim ( q, ) = 1 { 2 2 2 m 0 m

k ,l ,l '

kl p k + q, l '

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Advantages of the theory : 1) Dispersion is included ( depends on and q) 2) Two contributions : intraband (l = l) and interband l l 3) Temperature can be included via Fermi-Dirac f(Ekl, kbT) instead of f0(Ekl) * However the theory is not complete : in principle one should consider the Liouville equation to higher order perturbation theory ! * The theory is OK for multi-level systems but it does not solve the problem of the many-body electron gaz. Still one can grasp some physics !

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E intraband transition !

interband transition

kl p k + q, l '

2

l = d band

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( q, ) 1 +

4i

h =

( q, )

h 2 (q + 2qk F ) 2m

2 3vF 2 h P ( q ) = h P ( 1 + q ) 2 10 P

Re() = 0

h =

Re() = 0

h 2 (q 2qk F ) 2m

2kF

Fermi surfaces of radius kF kF+q

I

M S PC IC M P S

Interband transitions

e 2h 2 int er ( ) = 2 2 m

E kl' h2k 2 = Eg + 2m

2hl 'l [(h ) 2 (hl 'l ) 2 (h ) 2 2ihh ] ' dk (h ) 2 [ f o ( Ekl ) f o ( Ekl ' )] [(h ) 2 (h ) 2 (h ) 2 ]2 + 4(h ) 2 (h ) 2 l ,l l 'l l 'l

3

Pll '

In general Pll is assumed independant of k For parabolic p band and flat d band :

( ) = K dx

Eg

hx E g x

2 x 2 2 2i 2 (1 f o ( x )) 2 ( x 2 2 ) 2 + 4 2 2

Interband effects are most spectacular in noble metals They are are responsible for the colors of copper, gold and silver

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Copper

interband

Silver

Ag

Dielectric function e ()

experimental (Ehrenreich)

Dielectric function e ()

-5

Drude

-10 2 4 6 8 10

energy (eV)

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In real life one has to take into account the complexity of the bands in the Brillouin Zone

For silver

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Dielectric confinement results from the optical index matching at the surface of a nano-structure (boundary conditions for the EM field) Unlike the refraction at a dielectric surface, the light scattering from such nanostructure can display a complex mode structure. Simple case : metallic spheres. Plane wave has to be projected in spherical coordinates

E + ( q0 )2 E = 0 H + ( q0 )2 H = 0

Helmoltz equations :

: dielectric function inside or outside the sphere

q0 =

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Mie scattering theory (exact solution for a sphere): Write equation in spherical coordinates r, ,

1 2(r ) 1 1 2 2 + 2 (sin )+ 2 2 + q0 2 = 0 r r 2 r sin r sin 2

(a) (b)

r tm

2 = 2 0 2 k ( 2 )

l =1

(a) (b)

2 r = 2 0 2 k d ( 2)

m d

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l =1

S = c Re E H 8

W=

sphere

S ds

2 Wa + Wscat Qext = = 02 2nd Si

Qscat

Re[(i)

l =1

l +1

l +1

l (l + 1)(al + bl )

2 Wscat = = 02 2nd Si

(1)

l =1

l 2 (l + 1) 2 2 2 [ al + bl ] 2l + 1

To first order in l :

a1 = i d d

d 3 x + 2 d

p0 = a 3 d

for small spheres (d << ), the scattered light is the same as the one of a dipole centered on the sphere p=p0exp(it) and :

d + 2 d

(u.a)

0.6

0.4

Silver

0.4 0.2 0.2

0.0

2 3 nergie (eV)

d=50nm,lmax=1 d=50nm,lmax=5

0.0

nergie (eV)

d=80nm,lmax=1 d=80nm,lmax=5 d=80nm,lmax=7

(u.a)

2 2 1 1 0

Copper

-1

3.0

2.0

nergie (eV)

2.5

3.0

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1.1 The response function of metals to an optical excitation : intraband and interband transitions, transverse dielectric function of metals. Scattering of light by small metallic particles : theory of Mie, the effective medium response, surface plasmons. 1.2 General motivations, Magneto-optics of metals : Kerr and Faraday magneto-optical responses; Superparamagnetism of nanoparticles : Nel and Brown models

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Tunnel Magneto Resistance

R

MRT = R

R

R

writing

35,7 Mb/s on a theoretical bus of 1 data bit ~10 / 1 MB compare to ~10 / 1GB for RAM or flash memories (USB)

S

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Modify and study magnetization dynamics with light pulses Technology and fundamental physical processes

Relevant physical scales : 100-10 nm; 100 ps 100 fs

-20 10 0 20

50

M (u.a)

-50x10

-6

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-10

In 1845 Michael Faraday discovered that the polarization of light propagating through a magnetized substance is rotated. This magneto-optical (M.O.) effect, first observed in a sample of glass placed in an intense magnetic field and later in the reflectivity of metals by John Kerr, is now a widely used physical method to explore the properties of magnetic materials. The magneto-optical Kerr and Faraday effects are due to an asymmetric absorption and refraction for the left and right helicities of circularly polarized light due to the spin-orbit interaction.

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In the linear response theory these M.O. effects are well described by the off-diagonal complex dielectric tensor element xy For example, the Kerr rotation K and ellipticity K acquired by a linearly polarized light reflected from a ferromagnet is given, in the polar geometry, by :

n+ n n+ n K = m n n - 1 ; K = e n n - 1 + - + -

with n = = xx ixy

2

Refractive index for (+) and (-) circularly polarized light Simple case :

xx xy 0

H E E = 0 ; H = 0 t t D = 0 ( M , ) E

xy xx

0

0 0 zz

Onsager relation

2 D+ = 0 n+ ( E x + iE y ) 2 D = 0 n ( E x iE y )

ij (M, ) = ji (M, )

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if M = 0 : e n+= e nm n+= m n-

if M = 0 : e n+ e nm n+= m n-

if M = 0 : e n+= e nm n+ m n-

(j,k) : sample plane

elliptic non-rotated

k j

b ent ncid I eam

M

Re

fle cte d

Polar : M // i ; Longitudinal : M // j ; Transverse : M // k

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B v

f = e(E + v B )

Lorentz force

Working out the extended Drude model with a Lorentz force gives :

xy () = yx () =

2 p

2

+ i

2 2

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Magnetic material with magnetization M, Polarization P excited by a monochromatic wave E(r,) with frequency

P (r, ) = P L (r, ) + P NL (r, ) M (r, ) = M L (r, ) + M NL (r, )

Linear :

(1) Pi(1) () = ij () E j () j

(1)MO M i(1) () = ij () E j () j

jkl

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J.-Y. Bigot, C. R. Acad. Sci. Ser. IV (Paris) 2, 1483-1504 (2001).

So far in our approach to the optical response of metals we Have neglected the spins. But we need to introduce them and in addition a coupling with the polarization. For this, we introduce the spin-orbit interaction : Since we dont know how to handle properly the Coulomb correlations in full, let us consider a sum of one body hamiltonians H0n , where the Coulomb interaction e 2/r nm between the electrons is replaced by an effective one body operator Veff (rn):

H 0n

Pn : General momentum of electron n. Amag(rn) : vector potential of the applied magnetic field

e Pn = p n + A mag (rn ) c

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H Rn =

n = Pn + s n V(rn )

s n V(rn )

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N P = e * E * E i = N h W ij j 2 ij

W per unit time at energy h between the states |> and | > separated by the energy h. The Fermi golden rule gives :

2 EE * e 2 = 2 2 h 4m

[(h - h) + (h + h)]

= ( x y )

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Real and imaginary parts of the conductivity tensor : (allow to calculate the Kerr and Faraday rotation and ellipticity)

2 2 N e + e xy = - 2 2 2 2 hm ( ) ( 2 )

2

Ne 2 m xy = ( ) 2 2hm

- +

They include the spin-orbit coupling and the level separation which depends on the Zeeman splitting for uncorrelated systems and on the exchange interaction in ferromagnetic systems For ferromagnets it is admitted that the spin-orbit coupling is the most important contribution !!!

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Super-paramagnetism

Thermal fluctuations of magnetization

Nanoparticle with volume V

E = KV sin 2 H cos

Anisotropy K dipolar

E

KV

+H H

2 KV

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KV (1 H / H K ) 2 k BT

with : H K =

Fluctuations : (V, T, K)

K

0.5

Example:

d = 2 nm = 0 ~ 10-10 s d = 8 nm ~ 1017 s !

E / KV

Gyroscopic behavior : 0

M

0.5

E / KV

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dM dM V + h(t ) = 0M dt dt M

usual damping : Gilbert Fluctuating field : Stationnary Gaussian stochastic process

hi (t ) = 0 ;

hi t )h j (t + ) = ij (t )

The magnetic moment for a single particle is distributed on a sphere with a density of probabilty W(,,t) which obeys a Fokker-Planck equation

with : H c 2K 0 M S

2M S H c 2 (M S ) 2 + 0

0 VM S H c 2 k BT

Coherent term

IP CM S

Incoherent term

C. DOrlans, C. Estourns

Si02

Si wafer

SiO2, diameter ~8 nm (ferromagnetic at 295K) Al2O3, diameter ~4 nm (superparamagnetic at 295 K)

S

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Concentration profile

2x10 2x10

22

Co in Sapphire

22

16 14 12

At / cm

1x10 8x10

22

10 8 6 4 2

-5

21

4x10

21

Blocking temperature Tb ~ 80 K

Co (~4 nm) / Sapphire

50

100

150

200

250

2.0x10 1.5x10

Depth (nm)

-5

FC

2 M (emu.cm )

1.0x10 5.0x10

-5

-6

ZFC

0.0 0

100b T

200

300

400

T (K)

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2.1 A rapid overview of femtosecond laser optics. 2.2 The dynamics of the electron gas : Landau damping, electronelectron interaction and the Fermi liquid approximation, two temperatures model, non-thermal electron dynamics. 2.3 Time resolved studies of metallic films and nanoparticles. .

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The detection of primary events in the time evolution of many physical, chemical or biological systems require a femtosecond temporal resolution

Example : chloration of methane

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Estimates of the typical timescales associated with the energies involved in molecular systems

M1

r0

eM2

Electronic energy : Ee = p2/2me ~ h2/me r02 in SI units : me ~ 10-30 ; h ~ 10-34; r0 ~ 3x10-10 : Ee ~ 10-19 J ~ 1 eV The corresponding timescale is : T ~ h/E 1eV 10-15 s = 1 femtosecond Energy of vibration stretch : The force binding the two nuclei is comparable to the one of the electron bound to the molecule. Considering classical oscillators :

E vib = k/M ; E e = k/m e ; E vib = E e m e /M with : 1 1 1 = + M M1 M 2

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A. Zewail, 1999 Nobel price in chemistry for his studies of the transition states of chemical reactions using femtosecond spectroscopy

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C=C

23 fs C=C stretch

CC

6 5 0 -4 0 0 6 0 0 4 0

Time (f s)

Chem. Phys. Lett., 259, 469-474 (1996)

S

8 0

5 5 0 1 2 0

gth len e av W

m) (n

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Appl. Phys. Lett., 87, 192104 (2005)

E1

Piezoelectric CdTe QW

HH1 HH2

2.5

2.0

retard (ps)

1.5

1.0

0.5

0.0

rd ta re

0.0 790

780 785

775

770

765

790 785 780 775 770 765

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s) (p

) (nm

(nm)

Structure of rod rhodopsin Okada et al., JMB 2004

11-cis

all-trans

Retinal increases dipole moment when distorted (<200 fs) Electrostatic interaction with protein drives isomerization. Schenkl et al., Science 2005

All-trans form shows up as increased absorption at > 570 nm Isomerization occurs in 200 fs Wang et al., Science 1994

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* A sound wave propagating over a distance x = 100 in a metal : v ~104 m/s T = x/v ~ 10-12 s (acoustic waves : 1 picosecond) * Optical phonons in dielectric and semiconductors : ~100 fs) * Light interferometry : = 1 m ; c = 3 108 m/s T = /c ~ 3 femtoseconds * Electron-hole pair breaking in a semiconductor : Binding energy of excitons Eb ~ 10 meV (T~ 100 fs) Ultrafast spectroscopy performed with femtosecond pulses allows studying the dynamics of chemical and biological molecules as well as a variety of materials in condensed matter physics

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1 (t) = 2

e - i t d

An ideal -function pulse contains an infinite spectrum ! Typically : 2 C (if equality : Fourier transform pulse)

Pulse duration

12 fs pulse

Spectrum

exp[4 ln 2(t / ) 2 ] C = 0.441 1/[1 + (2t / ) 2 ] C = 0.221 1/[cosh (1.76t / )]2 C = 0.315

-80 -40

Time ( fs )

40

80

550

600

650

700

Wavelength ( nm )

time dependent spectroscopy is accessible in a very large bandwidth of the optical spectrum

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Typical energy of a low power CW laser (beam pointer): 1 mW The same energy in 10 fs : 1011 Watt (still only 1 mJ / pulse) Power density focused on a spot of 10 m diameter : 1017 Watt/cm2 Actual high power laser facilities : 1-10 J / pulse 1020 1021 Watt/cm2

109-1012 W/cm2 : Conventional Nonlinear Optics + Time resolved spectroscopy Material processing (electron plasma) + medical applications New laser design : self phase modulation, self focusing

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fluorescence

fluorescence

h/2

S

Application to bio-imaging : Maybe one of the largest success of femtosecond Titanium Sapphire laser !

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Nanosecond

Femtosecond

Laser fabrication of 100 m hole made in steel with nanosecond and femtosecond pulses

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If n2 > 0 : when I increases (leading part of pulse) decreases red colors are generated when I decreases (falling part of pulse) increases blue colors generated

I(t)

Kerr medium

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1012-1016 W/cm2 : High intensity Nonlinear Optics High harmonic generation Xrays sources Attosecond lasers ?

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2.1 A rapid overview of femtosecond laser optics. 2.2 The dynamics of the electron gas : Landau damping, electronelectron interaction and the Fermi liquid approximation, two temperatures model, non-thermal electron dynamics. 2.3 Time resolved studies of metallic films and nanoparticles. .

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4e 2 0 4e 2 lim ( q, ) = 1 { 2 2 2 m 0 m

k ,l ,l '

kl p k + q, l '

* Temperature can be obtained from f0 : Fermi-Dirac distribution at finite temperature * Spins can be included (with temperature) Stoner model at finite temperature

What is missing ?

* Time is absent : theory of linear response function in the frequency domain. * We do not have a good description of damping: is simply there for causality.

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i

W( r,r; Ei Ef )

f E Fermi

Conduction electrons

1 dq 1 =2 Vq m (2) 3 (q, )

requires a model for (q, )

Random Phase Approximation (RPA) or (q, ) = RPA(q, ) G(q, )(RPA(q, ) -1) (G : local field factor)

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For a Fermi liquid with temperature e quasiparticles near the Fermi level scatter according to (Pines & Nozires) :

( k Be ) 2 + (E - E F ) 2 E - EF 1 + exp( ) k Be 1

Good for interband processes specially if interested in the electron dynamics at the threshold of interband transitions 2. Density functional theory

* TDLDA: Time dependent local density approximation * TDLSDA: with spins (both can be performed at finite temperature : even if rigorously exact only for the ground state)

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(E)

athermal Distribution

EF

(E)

3

(E)

* lattice vibrations (coherent) : t < 100 ps * Relaxation of lattice Exchange with environment : t > 1 ns

EF

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Tl 10 - 3 Kfs 1 t Te 10 Kfs 1 t

C e (T e ) Cl dT l dt

r r r e T e (t, r ) r r)

1200

Temperature (K)

Laser pulse

Telectrons TLattice

0 5 10 (ps) 15

IP

CM

Time

dN = N N + P(t) dt r r r dT e C e (T e ) = G el (T l (t) T e (t) ) e T e (t, r ) + N dt r r r dT l Cl = G el (T e (t) T l (t) ) l T l (t, r ) + N dt

temperature (K)

N : Volume density of non-thermal electrons = 1/th : coupling between the non thermalized and thermalized electrons 650 : coupling to phonons.

600 550 500 450 400 350 -2 0

(electrons)

(lattice)

laser

n(t)

0.0 0.5 1.0 time (ps)

10

time (ps)

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(r,t) [r,Te(t)]

2) Suppose that we are in the adiabatic regime (the temperature changes slowly enough so that the medium respond instantaneous OK for electrons) D(r,t)=E(r,t) and B(r,t)=M(r,t) P(r,t)=eE(r,t) and M(r,t)=mH(r,t)

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2.1 A rapid overview of femtosecond laser optics. 2.2 The dynamics of the electron gas : Landau damping, electronelectron interaction and the Fermi liquid approximation, two temperatures model, non-thermal electron dynamics. 2.3 Time resolved studies of metallic films and nanoparticles. .

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Optical density

0.8

Cu : 10 nm

0.4

0 1.8

Edp

2.2 2.6 (eV)

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0

Delay (picoseconds)

1.8 2.0 2.2 2

Energy (eV)

J.-Y. Bigot, J.-C. Merle, O. Crgut, A. Daunois

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F. Valle - Bordeaux

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T/T (normalized)

1 ,0

Cu: 10 nm

0 ,5

0 ,0 -1 0 1 2 3

eff

= +

or + F g ( ) R

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V (r , r ') = Vbulk e2 + a 1 4 r r ' 1 lm ( , )lm ( ' , ') 2l + 1 a a l ( ) ( ) l ,m

l l

h (E d , e ) =

A 1 f o (E c ) Im 2 (E E ) 3 a [E c E d ] d s c

A d hole can decay by emitting a plasmon : Excitation with photons of energy h leads to a resonant scattering of the holes created by the probe. This effect increases with the electron temperature (via f0(Ec)) and when the particle size decreases (via 1/a3).

h f o (E c ) Im

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s ( ) 1

J.-Y. Bigot, V. Halt, J.-C. Merle, A. Daunois - Chem. Phys., 251, 181-203 (2000).

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t = 2 ps

1.00 1.00 0.75 0.50 0.25 0.00 -0.25 2.4 2.8 3.2 3.6

T / T normalized

0.15 0.10 0.05 0.00 -0.05 3.6

T / T

(eV)

(eV)

Experiments

Phys. Rev. B, 60, 11738-11746 (1999). Chem. Phys., 251, 181-203 (2000).

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Theory (TDLDA)

Eur. Phys. J. D 24, 185 (2003) Phys. Rev. Lett., 92, 177402 (2004).

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3.1 Ultrafast Magnetization Dynamics of thin ferromagnetic films

3.2 Ultrafast magnetization dynamics of nanostructures

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Laser field Photons (E, V; A, ) Electrons Charges, plasmons Electrons Spins, magnons

Photons : TeraHertz emission (spins) ; Brillouin scattering Micro-magnetic interactions : Internal Vibrational Relaxat Heat propagation (internal & to environment : substrate ) Precession and damping; Spin torque; Nucleation propagation & pinning of domain walls Fluctuations : Superparamagnetic fluctuations Domain fluctuations

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Photons : High Harmonics & Xrays TeraHertz emission (charges); Raman scattering Luminescence

1.0

M

0.5

C T Tc

Pierre Weiss

0.0

300

600

900

1200

Temperature (K)

TC

700 500 300 700 500 300

E(r,t)

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Kerr configuration: , reflection

, transmission

Pump pulse

t

Probe pulse: linear polarization

The rotation (K, F) and ellipticity (K, F) of the probe polarization are proportional to the Magnetization M

Seoul - 2009 - Jean-Yves Bigot - Winter_school_IPCMS-QMMRC

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h

M

h

M

CoPt3 Kerr Signal (a.u.)

No pump

t =500 fs

-4

-2

0 2 H (kOe)

time

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H S E(r,t)

e, p, V(r)

Dirac relatisvistic

ih

Development in 1/c2

(central potential)

eh 2 1 dV l.s 2 2 2m c r dr

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Heff

Co/Al2O3

M H0

Gilbert damping:

Pump :P(t)

damp

M PC

600

Field ( Gauss )

500 400 0.00 -0.02 -0.04 -0.06 -0.08 -0.10 0 200 400 600 800 300 200 100

Period ( ps )

I M PC S

Heff, M are vector quantities comprehensive description of dynamics involves the modulus and orientation of M(t)

Static polar, longitudinal, transverse (p-pol):

z

M- M- M H

External static field

and time resolved: T/T = [T(t) T0]/T0 R/R = [R(t) R0]/R0 Pol/Pol = [Pol(t) Pol]/Pol Long/Long = [Long(t) Long]/Long Trans/Trans = [Trans(t) Trans]/Trans

M PC

Precession dynamics in 3D

Phys. Rev. Lett. 94, 237601 (2005)

Pol (10 )

-2

16 nm Co/Al203

Polar

0 -4 3 0 -3 2

0 -4

Long (10 )

3 0 -3 2 0

longitudinal

-2

Trans (10 )

transverse

-2

Delay (ps)

Delay (ns)

M PC

16 nm Co/Al203

I M PC S

Pol/Pol x 10-2

0 -5 -10 -15

0 200 400 600

Pol/Pol x 10-2

4 0 -4

100

200

300

Delay (ps)

Delay (ps)

M PC

* Electron/spin and lattice dynamics: two temperatures model

r dTe = G el (Tl (t) Te (t))+ P(t) e 2 Te (t, r) r dt r2 dT r C l l = G el (Te (t) Tl (t)) l Tl (t, r ) dt C e (Te )

Temperature

r r dM r r r dM = M H eff Te (t), Tl (t), M(t) dt dt relax

r r 2 M(Te (t)) = M s 1 - (Te /Tc ) for Te Tc and M = 0 for Te > Tc

10 l K a (Tl ) = K a (0) MS

M PC

In plane anisotropy

M PC

Co/MgO : excitation of 0 and 1st order standing spin waves

50 nm pol/Pol x 10-2

5 0 -5 -10 0.0 0.1 0.2

0 order SW

Delay (ns)

Fourier Transform (a.u.) 1

0 50 100

1st order SW

Frequency (GHz)

I M PC S

3.1 Ultrafast Magnetization Dynamics of thin ferromagnetic films

3.2 Ultrafast magnetization dynamics of nanostructures

M PC

MFM imaging of CoPt3 dots

(d=1 m) (d=250 nm)

I M PC S

amplified Ti:S

(800 nm)

(400 nm)

I M PC S

Magnet ( 0.4T)

H

PM F Analyzer F PM Scanning piezo

y x

/2

Pinhole (20 m)

.

R= 5x10- 4 R//

(400 nm) Polarization bridge

Polarizer

I M PC S

Gauss250nm Crenel500nm

Gauss300nm Gauss900nm

I M PC S

Differential Magnetization :

M (t ) M (t ) ( I + H ( t ) I H ( t )) = M stat stat ( I + H I H ) stat

0 M / M

e (spin)-l

6 4 2 2 4 6 8

-0.1 -0.2 -0.3 0 e-l = 2.27 ps P1aser= 3.8 mJcm-2 5 10 Delay (ps) 15 20

M PC

M PC

-20 10 0 20

50

M (u.a)

-50x10

-6

-10

15

M PC

10

15

10

Pump-probe delays

t = 300 fs t = 2 ps t = 10 fs

M PC

8 mJcm-2

MFM Images

M PC

0 P= 8 mJ cm-2 -0.5

damping = 946 ps

M/M

-0.5

10 Delay (ps)

20

M PC

E = KV sin H cos

2

(a)

0.5

E / KV

Anisotropy K

dipolar

E

(b)

0.5

0 01

12 1

E / KV

00

M PC S

KV (1 H / H K ) 2 k BT

HK =

2 KV

if d = 2 nm : = 0 ~ 10-10 s ; if d = 8 nm : ~ 1017 s !

I

D = 4 nm Co in Al2O3

0.0 0.0

t=0 t=1 ns

Pol/Pol (x10)

Long/Long

Pol/Pol

-0.5

-0.1

6 ps

-1.0

400 fs

Delay (ps)

1/p = 50 ps P = 90 ps

Long/Long (x10)

M PC S

dM dM V + h(t ) = 0M dt dt M

Gilbert damping Fluctuating field : Stationnary Gaussian Stochastic process

hi (t ) = 0 ;

hi t )h j (t + ) = ij (t )

The magnetic moment of one particle is distributed on a sphere with a density of probability W(,,t) which obeys a Fokker-Planck equation

avec : H c 2K 0 M S

2M S H c 2 (M S ) 2 + 0

0 VM SH c 2 k BT

incoherent term

coherent term

I M PC S

coherent term : 4.8 x 1010 s-1 with = 90ps incoherent term : 0.38

0 = 55 ps !

2.5 nm = 3

film = 0.02

10 nm = 0.43

4 nm = 0.46

Magnetization precession The Gilbert damping increases when the size decreases The characteristic times of the Nel-Brown model are close : 1/P = 50ps ; P = 90 ps ; 0 = 55ps

The process of magnetization reversal is probably not fully coherent

M PC S

Personal references on electrons and spins dynamics in metallic films and nanostructures A. Ultrafast dynamics of magnetic metals.

* A. Laraoui, M. Albrecht, J.-Y. Bigot Optics. Letters 32, 936-398 (2007). * L.H.F. Andrade, A. Laraoui, M. Vomir, D. Muller, J.-P. Stoquert, C. Estourns, E. Beaurepaire, and J.Y. Bigot Phys. Rev. Lett. 97, 127401 (2006). * M. Vomir, L. H.F. Andrade, L. Guidoni, E. Beaurepaire, J.-Y. Bigot Phys. Rev. Lett. 94, 237601 (2005) * J.-Y. Bigot, M. Vomir, L.H.F. Andrade, E. Beaurepaire Chem. Phys. 318, 137 (2005). * J.-Y. Bigot, L. Guidoni, E. Beaurepaire, P. N. Saeta Phys. Rev. Lett. 93, 077401 (2004). * L. Guidoni, E. Beaurepaire, J.-Y. Bigot Phys. Rev. Lett., 89, 17401-17404 (2002). * J.-Y. Bigot, C. R. Acad. Sci. Ser. IV (Paris) 2, 1483-1504 (2001). * J. S. Dodge, A. B. Schumacher, J.-Y. Bigot, D. S. Chemla, N. Ingle, M. R. Beasley Phys. Rev. Lett., 83, 4650-4653 (1999). * D. S. Chemla, J.-Y. Bigot Chem. Phys., 210, 135-154 (1996). * E. Beaurepaire, J.-C. Merle, A. Daunois, J.-Y. Bigot Phys. Rev. Lett., 76, 4250-4253 (1996). B. Ultrafast electron dynamics in metallic nanoparticles and nanostructured films. * I. Lisiecki, V. Halt, C. Petit, M.-P. Pileni and J.-Y. Bigot, Adv. Mat. 20,1-4, (2008) * V. Halt, A. Benabbas and J.-Y. Bigot Optics Express, 16, 11611 (2008). * V. Halt, A. Benabbas, J.-Y. Bigot Opt. Express 14, 2909-2920 (2006). * A. Benabbas, V. Halt, J.-Y. Bigot Opt. Express 13, 8730 (2005). * P.-A. Hervieux, J.-Y. Bigot Phys. Rev. Lett., 92, 177402-177406 (2004). * J.-Y. Bigot, V. Halt, J.-C. Merle, A. Daunois Chem. Phys., 251, 181-203 (2000). * T. V. Shahbazyan, I. E. Perakis, J.-Y. Bigot Phys. Rev. Lett., 81, 3120-3123 (1998). * J.-Y. Bigot, J.-C. Merle, O. Crgut, A. Daunois Phys. Rev. Lett., 75, 4702-4705 (1995).

I M PC S

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